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Electrochemical Advanced Oxidation and Adsorptive Enrichment of Emerging Contaminants： Mechanisms and Synergistic Potential

Xinyu Wang , Xu Liu , Xixue He , Qiao Li , Zhihua Qiao , Hao Xu

Progress in Chemistry ›› 2026, Vol. 38 ›› Issue (9) : 1664 -1680.

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Progress in Chemistry ›› 2026, Vol. 38 ›› Issue (9) : 1664-1680 DOI: 10.7536/PC20251217
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Electrochemical Advanced Oxidation and Adsorptive Enrichment of Emerging Contaminants： Mechanisms and Synergistic Potential
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Abstract

Emerging contaminants（ECs）have become a significant challenge in aquatic environments. Due to their common trace-level distribution， structural stability， and high mobility in aquatic systems， conventional water treatment processes exhibit notable deficiencies. Electrochemical advanced oxidation processes（EAOPs）are considered an effective approach for the efficient removal of ECs， owing to the in‑situ generation of highly reactive oxidative species and strong process controllability. However， in practical water treatment systems， EAOPs still face engineering bottlenecks including mass transfer limitations， reduced energy efficiency under low-conductivity conditions， incomplete degradation， and by‑product formation. Although adsorption technology is generally incapable of achieving complete mineralization， it holds unique advantages for the rapid enrichment of trace-level ECs. In recent years， coupling adsorption with EAOPs has been regarded as a crucial strategy to overcome the limitations of individual technologies and enhance both the removal efficiency and operational stability for ECs. This review summarizes the mechanisms， research progress， and key challenges of EAOPs and adsorption technology in ECs treatment. It focuses on delineating three typical modes of the adsorption-EAOPs coupled system： simultaneous adsorption‑EAOPs degradation， adsorption enrichment‑EAOPs degradation， and EAOPs degradation followed by post-treatment adsorption. The synergistic mechanisms of these coupled systems in enhancing mass transfer and mitigating secondary pollution are elucidated. Furthermore， the article analyzes the main obstacles currently facing the engineering application of adsorption-EAOPs coupled systems. Finally， considering the demands of real water treatment， it is proposed that future research should strengthen the systematic evaluation of the long-term continuous operational performance， material deactivation mechanisms， and environmental risks of the treated effluent， which is essential for facilitating the transition of adsorption‑EAOPs technology from laboratory research to practical engineering applications.

Contents

1 Introduction

2 Advances and challenges in EAOPs for the treatment of ECs

2.1 Classification and applicability of EAOPs

2.2 Research progress of EAOPs in ECs degradation

2.3 Characterization approaches and degradation mechanisms in EAOPs

2.4 Challenges and limitations of EAOPs

3 Advances and challenges in adsorption for the removal of ECs

3.1 Principles of adsorption and classification of adsorbents

3.2 Research progress on the removal of ECs by adsorption

3.3 Characterization of adsorption mechanisms and adsorption models

4 Adsorption-EAOPs coupling for the removal of ECs

4.1 Theoretical basis of adsorption‑EAOPs coupling

4.2 Coupling configurations and synergistic mechanisms

4.3 Key challenges for engineering applications

5 Conclusions and outlook

Graphical abstract

Keywords

emerging contaminants / electrochemical advanced oxidation processes / adsorption / coupled system / secondary pollution

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Xinyu Wang, Xu Liu, Xixue He, Qiao Li, Zhihua Qiao, Hao Xu. Electrochemical Advanced Oxidation and Adsorptive Enrichment of Emerging Contaminants： Mechanisms and Synergistic Potential. Progress in Chemistry, 2026, 38(9): 1664-1680 DOI:10.7536/PC20251217

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1 Introduction

Emerging contaminants (ECs) refer to chemical substances that have received widespread attention in recent years, pose potential hazards to ecosystems and human health, and currently lack a comprehensive regulatory framework[1-2]. ECs typically exhibit characteristics such as environmental persistence, bioaccumulation, and biological toxicity[3], and water bodies are an important environmental medium for them[4].
ECs mainly include categories such as Pharmaceuticals and Personal Care Products (PPCPs), Endocrine Disrupting Chemicals (EDCs), industrial organic pollutants (e.g., fluorinated organics, flame retardants, dyes, etc.), and emerging inorganic pollutants. Although they mostly exist at trace levels of ng/L to μg/L in the environment, they have been proven to exert significant impacts on ecosystems and human health. For instance, under antibiotic exposure at the ng/L level, microbial communities can still experience sustained selective pressure, leading to the enrichment of antibiotic resistance genes and resistant strains.[5]. Studies in multiple regions have also indicated[6]that even under exposure to endocrine hormones and their microbial metabolites (such as progesterone, androstenedione, 17α-hydroxyprogesterone) at ng/L or nmol/L levels, fish can exhibit typical endocrine disruption responses, including skewed sex ratios, impaired gonadal development, abnormally elevated Gonadosomatic Index (GSI), and induced liver detoxification enzyme activity. Some ECs possess high environmental mobility; for example, highly persistent pollutants like perfluoroalkyl and polyfluoroalkyl substances (PFAS, such as PFOA and PFOS) can be transported over long distances via the atmosphere and accumulate in precipitation, resulting in PFAS levels in precipitation across North America and Europe reaching 2–100 ng/L, with levels in some areas affected by point sources even exceeding current drinking water limits.[7]. In addition to organic ECs, certain inorganic pollutants also exhibit similar migration characteristics and environmental risks. In recent years, the behavior and potential risks of Rare Earth Elements (REEs) in environmental systems have gradually gained attention. Regarding environmental behavior, REEs share certain commonalities with some heavy metal ions; both can enhance their mobility in water bodies by complexing with organic matter, thereby demonstrating strong persistence in the environment.[8]. Toxicological studies further indicate[9]that REEs can induce oxidative stress, neurotoxicity, and tissue damage; some REEs may adversely affect neurocognitive development in children and are associated with potential reproductive toxicity risks.
Conventional water treatment processes generally have limited efficiency in removing ECs: physical methods (such as coagulation-flocculation) primarily remove suspended particles and are almost ineffective against dissolved ECs[10]; biological treatment relies on microbial metabolism[11], resulting in extremely low removal rates for antibiotics, flame retardants, and fluorinated organic compounds that have stable structures and are difficult to biodegrade; chemical disinfection (such as Cl2, O3) possesses certain oxidation capabilities but struggles to completely destroy the molecular skeleton of ECs, and tends to generate halogenated byproducts such as chlorates and bromates under halogen-containing conditions. Adsorption and membrane separation can effectively retain trace ECs, but essentially they remain "phase transfer" processes that not only fail to achieve true degradation and mineralization but also produce solid residues with high loads or concentrated liquids with high concentrations, becoming new potential pollution sources. This risk has been verified in actual operations[12]; for example, the content of quinolone antibiotics in sludge from multiple wastewater treatment plants in China can reach as high as 21.9 mg/kg; global surveys show[13]that PFAS levels in typical municipal sludge range from hundreds to thousands of μg/kg. When such sludge is applied to land, ECs enter the soil-water system directly; some highly persistent pollutants (especially PFAS) exhibit significant long-term accumulation and can migrate to deep soil and groundwater under leaching effects, forming an irreversible "secondary pollution" pathway. Therefore, there is an urgent need for water treatment technologies capable of directly destroying the molecular structure of ECs to compensate for the shortcomings of conventional processes.
In this context, advanced oxidation technologies capable of rapidly generating highly oxidizing species and thoroughly destroying the molecular structure of organic pollutants have received widespread attention. In recent years, electrochemical advanced oxidation processes (EAOPs), owing to their high controllability and ability to treat highly toxic and refractory pollutants, have been regarded as a potential core technical route for the efficient removal of ECs. However, the application of EAOPs in real water bodies still faces several key limitations. First, ECs are typically present at ultra-low concentrations of ng/L~μg/L[14-15], resulting in slow reaction kinetics; second, the conductivity of natural and municipal water bodies is generally low[16-17](approximately 0.1~2.0 mS/cm), and ohmic losses significantly constrain the actual energy efficiency of EAOPs. Furthermore, the oxidation process of EAOPs may not be complete[18], as some degradation intermediates (such as aromatic amines and quinone structures) possess potentially higher ecotoxicity. Meanwhile, in chloride-containing media, EAOPs also exhibit the behavior of oxidizing electrolytes to generate secondary pollutants such as chlorates and perchlorates, posing further challenges to their engineering applications.
EAOPs are easy to couple with other processes, providing new technical pathways to address the aforementioned bottlenecks. Although adsorption technology does not aim to destroy pollutant molecular structures, its selective enrichment capability enables rapid capture of trace ECs in water at the front end, elevating pollutant levels from environmental concentrations of ng/L~μg/L to local effective concentrations at the mg/L level at the adsorption interface. This enrichment-concentration effect not only significantly accelerates the reaction kinetics of electrochemical oxidation but also mitigates, to some extent, the increase in energy consumption caused by low conductivity, thereby laying a critical foundation for the efficient operation of EAOPs in real water bodies. Furthermore, adsorption enrichment and EAOPs can be carried out separately in space or stage, preventing the accumulation of certain potential oxidation by-products in the oxidation unit, thus further enhancing the stability and environmental safety of the treatment process.
This paper takes the pollution characteristics of ECs in real environments as a starting point to systematically review research progress, characterization methods, and action mechanisms regarding EC removal using EAOPs and adsorption technologies. Without altering the core research focus, this paper also appropriately introduces several cases of pollutants that share high similarities with ECs in terms of environmental behavior and treatment challenges, to support discussions on related technical mechanisms and applicability. Building on this, the synergistic mechanisms, engineering potential, and future development directions of these two types of technologies are further summarized, aiming to provide references for constructing efficient, widely applicable, and sustainable EC treatment strategies.

2 Progress and Challenges in EAOPs for Treating ECs

2.1 Classification and Applicability of EAOPs

EAOPs refer to electrochemical methods that generate reactive species (such as ·OH, SO4·-, O2·-, etc.) in situ through electrode interface or bulk reactions under an applied electric field, thereby achieving deep oxidation of refractory organic pollutants. From an engineering operation perspective, EAOPs can be briefly classified into the following two categories based on whether external oxidants are introduced.
(1) Zero-dosing EAOPs: These technologies do not require the external addition of strong oxidants. They primarily rely on anodes with high catalytic oxidation activity (such as boron-doped diamond electrodes and lead oxide electrodes) to undergo anodic oxidation reactions under an applied electric field. Through direct electron transfer (DET) or in-situ generated adsorbed •OH (weakly adsorbed), they achieve non-selective oxidative degradation of refractory organic compounds such as ECs.
(2) Low-dosage EAOPs: These technologies require the participation of a small amount of exogenous reagents, such as Fe2+ in electro-Fenton/Fenton-like systems, or peroxymonosulfate/persulfate (PMS/PDS) in electro-activation systems, to achieve ·OH, SO4·- and other reactive species in large quantities.
The two types of EAOPs demonstrate differentiated advantages in practical water treatment scenarios. Zero-dosing EAOPs, requiring no external strong oxidants and offering high process controllability, are suitable for advanced treatment and effluent standard upgrading of refractory pollutants at low to medium concentrations. In contrast, low-dosing EAOPs (such as electro-Fenton and PMS/PDS electro-activation systems) can generate higher concentrations of ·OH or SO4·-, significantly enhancing oxidation intensity and making them more suitable for industrial wastewater with high concentration, high toxicity, and complex structures. Regarding continuous operational stability, zero-dosing systems are less affected by external reagents and typically exhibit better long-term performance; whereas low-dosing systems, while maintaining high reaction rates under a wide range of water quality conditions, may face engineering challenges such as electrode scaling and passivation, narrow pH applicability, and continuous reagent consumption. Concerning secondary pollution risks, byproduct risks in zero-dosing EAOPs are relatively concentrated, mainly stemming from the generation of halogen derivatives like chlorine oxides; in contrast, low-dosing EAOPs, due to the introduction of external activation components, require focused attention on the accumulation of iron-containing sludge, residual oxidants such as persulfates, and the ecological toxicity risks posed by potential release of dissolved metals. Therefore, specific process selection should be conducted based on a comprehensive trade-off of factors including pollutant types, target treatment levels, water conductivity, operating costs, and potential environmental risks.

2.2 Research progress on EAOPs in the degradation of ECs

Since ECs mostly exist at trace levels, mass transfer limitations have become the core bottleneck restricting their electrochemical degradation efficiency. To enhance the applicability and energy efficiency of EAOPs, recent research has shifted towards developing novel reactors based on flow-through and electrochemical membrane structures, as well as regulating interfacial reaction mechanisms. For example, Yang et al.[19] proposed Ti4O7 reactive electrochemical membranes (Ti4O7-REM), which achieve strong convective mass transfer via their porous structure (Figure 1a), can significantly compress the diffusion layer and intensify the DET process, removing 94%~97% of antibiotics within 30 s (Figure 1b); their apparent rate constant for norfloxacin is 4.3~34 times higher than that of traditional flow-through systems, while energy consumption is reduced by 80%~97%. This design for enhanced mass transfer was also successfully applied by Wang et al.[20] to the degradation of PFOS; they revealed the critical influence of REM anode composition and pore size on the electro-oxidation process. Ti3+ sites can enhance PFOS surface adsorption and lower the DET energy barrier (Figure 1c), making the PFOS degradation efficiency significantly superior to batch systems and achieving nearly complete defluorination. Overall, strategies that enhance interfacial electron transfer and mass transfer efficiency can be used for the efficient removal of ECs[21], but several challenges remain: the preparation of microporous electrode materials such as REMs is relatively difficult, clogging easily occurs during long-term operation, and oxidation pathways dominated by DET struggle to achieve complete mineralization; thus, combination with oxidation processes involving ·OH is still required to ensure effluent safety.
In recent years, some studies have begun to focus on enhancing the ·OH generation rate of anodes through material modification. For example, Xie et al.[22]introduced trace amounts of carbon materials into Ti4O7anodes and found that only 0.1% (by mass) of carbon could significantly reduce the charge transfer resistance (Rct), enhance interfacial electron absorption capacity, and suppress the oxygen evolution reaction, enabling the anode to achieve higher oxidation activity at lower potentials (Figure 1d). Furthermore, He et al.[24]constructed a Ti3C2 MXene-doped Ti4O7ceramic membrane, achieving dual enhancement of electronic structure optimization and exposure of reaction sites, which reduced the charge transfer impedance from 59.09 Ω to 4.21 Ω and increased the ·OH yield by 2.3–2.6 times, providing a technical foundation for the degradation of a wider range of ECs.
Secondary pollutant threats in EAOP processes cannot be ignored. The presence of halogens (including halogenated groups and free halide ions) is easily converted into highly toxic by-products such as chlorate/perchlorate under high potentials. Serna-Galvis et al.[25]detected toxic chlorinated by-products such as chloroform and dichloroacetic acid when treating ECs containing halogen substituents; other studies observed free Cl-further converting to ClO3-and ClO4-[23,26], where ClO4-belongs to typical persistent inorganic pollutants. Optimization and improvement of electrode materials help alleviate the above problems. For example, Wang et al.[23]compared the electro-oxidation behavior of PFOS on Ti4O7and boron-doped diamond (BDD) anodes, showing that the accumulation of ClO3-and ClO4-on Ti4O7anodes was significantly lower (Figure 1e, f); Li et al.[26]applied Ti4O7to drinking water electrochemical disinfection, where the generated ClO4-concentration could be controlled below the drinking water standard limits. Notably, the Ti[19]proposed by Yang et al.4O7-REM system, when operated under NaCl conditions, exhibited a ClO3-accumulation concentration of only about 43% of that in flow-through systems, with no detection of ClO4-formation, highlighting the advantage of the DET-dominated Ti4O7system in balancing EC removal (incomplete mineralization) efficiency with by-product risk control.
Overall, in recent years, research on the removal of ECs by EAOPs has gradually shifted from solely pursuing removal efficiency to emphasizing both "enhancing reaction kinetics through improved mass transfer" and "synergistic control of byproduct risks." Based on this, deeply revealing the dominant reactive species, degradation pathways, and key reaction behaviors such as dehalogenation under different electrode/reactor systems has become a prerequisite for further optimization and engineering scale-up of EAOPs.

2.3 Characterization methods and degradation mechanisms of EAOPs

With the increasing demand for precise identification of dominant active species, interfacial reaction behaviors, and degradation pathways, the synergistic application of cutting-edge technologies such as electrochemistry, spectroscopy, mass spectrometry, and theoretical simulations is becoming a key means to understand the essence of EAOPs reactions. These technologies mainly focus on three aspects: the identification of active species, the analysis of intermediates and degradation pathways, and the characterization of electrode interface structures and electronic behaviors, collectively forming a systematic mechanistic cognition framework for EAOPs.
The core of EAOPs lies in the generation and transformation of reactive species (·OH, SO4·-,1O2, O2·-, etc.). Wang et al.[27]combined electron paramagnetic resonance (EPR), Raman spectroscopy, and Fourier transform infrared spectroscopy (FTIR) to systematically analyze the degradation behavior on the BDD electrode interface, confirming a non-selective oxidation pathway dominated by ·OH. In contrast, the reaction mechanism of electro-Fenton/Fenton-like systems is more complex. Yang et al.[28]after constructing the PA-OCNTs@CoFe2-LDH electro-Fenton membrane, achieved individual identification of ·OH, O2·-and1O2using EPR and various spin traps (DMPO, TEMP). Among these, the typical 1:2:2:1 quartet peak of DMPO-OH confirmed the generation of ·OH, while the triplet signal of TEMP-1O2and its significant enhancement in D2O confirmed the contribution of1O2in the system. Furthermore, the appearance of the DMPO-O2·-quartet peak in the methanol system indicated that superoxide radicals also participated in the reaction. This "EPR + multiple quenchers + isotope effect" strategy has become an important method for elucidating synergistic mechanisms of multiple reactive species. Related approaches are equally applicable in other systems; for example, Yu et al.[29]distinguished the contributions of photogenerated holes (h+) and ·OH in a photocatalytic system using KI and IPA, and combined with DMPO-EPR to clarify the key role of ·OH.
After identifying the dominant active species, precisely recognizing the intermediates generated during ECs degradation is a key step to further understanding EAOPs reaction pathways. Ji et al.[30]utilized LC-MS to systematically analyze fragments obtained from doxycycline degradation in an electro-Fenton system, categorizing their transformation into three parallel pathways: a side-chain cleavage pathway driven by demethylation/deamidation; a deep ring-opening pathway induced by dehydroxylation plus demethylation; and a nitrogen-containing side-chain cleavage pathway dominated by demethylation/demethylamination/deamination. These three pathways are interwoven, with multi-level fragments undergoing further oxidation and ultimately trending toward mineralization. Notably, unlike antibiotics which are pollutants with relatively small molecular weights, ECs such as PFAS possess high chemical stability; their degradation intermediates have short lifespans, and the defluorination/bond-breaking processes highly depend on electron transfer kinetics, making it difficult for traditional LC-MS to fully capture their transformation processes. To address this, Li et al.[31]employed Density Functional Theory (DFT) simulations to reveal the electron gain/loss behavior of perfluoroalkyl acids (PFAAs), the adsorption activation pathways of PMS, and the energy barriers for radical generation. Their research indicates that the HOMO/LUMO energy gap of PFAAs shows a good linear correlation with their degradation rates (R2 ≈ 0.98), suggesting that stronger electron transfer capability facilitates bond-breaking/defluorination processes. By further integrating radical contribution distributions, reaction energy diagrams, and Fukui indices of key reaction sites, the study constructed a mechanistic framework of "electron transfer → radical attack → functional group cleavage → defluorination/mineralization," providing important theoretical and methodological references for elucidating EAOPs reaction pathways for such ECs.
Analyzing the electrode interface structure, pore accessibility, and electron transfer behavior is key to understanding the differences in EAOPs reaction kinetics. Xie et al.[22]Through structural analysis of Ti4O7and Ti9O17anodes, it was pointed out that different phase contents and carbon doping significantly affect interfacial charge transfer behavior; electrochemical impedance spectroscopy (EIS) results show that the charge transfer resistance of Ti4O7can systematically decrease with phase purity, pore structure, and doping status, indicating that its interfacial electron behavior can be significantly improved through material regulation. Further combined with pore structure characterization, it is known that micrometer-scale pores facilitate convective mass transfer, while nanopores are more likely to lead to restricted ion migration; these microstructural differences jointly determine the anode's conductivity and charge transfer capability. Zhuo et al.[32]further systematically revealed the profound impact of surface chemical regulation on interfacial electron behavior by constructing a high oxygen vacancy ratio Ti4O7-E/F anode. Linear sweep voltammetry (LSV) tests indicated that the oxygen evolution potential of this anode (2.164 V vs Ag/AgCl) is higher than that of the original Ti4O7, making it more conducive to maintaining electron utilization efficiency for organic oxidation while suppressing the oxygen evolution reaction; CV curves showed that etching and fluorination significantly expanded the electroactive region, reflecting a higher electrochemically accessible area. EIS analysis further provided quantitative evidence: etched Ti4O7-E reduced the Rct from 44.31 to 4.18 Ω·cm2, while fluorinated Ti4O7-E/F, although causing an increase in Rct to 20.66 Ω·cm2 due to F occupancy and increased hydrophobicity, remained far lower than that of BDD electrodes. The synergistic effect of oxygen vacancies and F substitution not only enhanced interfacial electron transport capability but also increased the generation rate of surface ·OH (1.38~3.2 times that of the original Ti4O7), thereby significantly improving the area-normalized kinetic constant. These results indicate that electrochemical characterizations such as linear sweep voltammetry (LSV), cyclic voltammetry (CV), and EIS play a key role in revealing the interfacial electron behavior of anodes, establishing a clear link between the enhancement of macroscopic electrocatalytic performance and the regulation of microscopic electronic structures. They hold important reference value for the design of EAOPs anode materials.
In summary, the analysis of active species, tracking of degradation intermediates, and characterization of electron behavior at the electrode interface together constitute the three pillars of EAOPs mechanism research. The synergistic advancement of these three approaches has clarified the overall mechanistic model of EAOPs and provided a systematic theoretical foundation for the design of efficient and stable anode materials.

2.4 Challenges and Limitations of EAOPs

Although regulating interfacial electron transfer, optimizing the exposure of electrode active sites, and enhancing the generation flux of ·OH and SO4</sup>and other reactive species can significantly strengthen the degradation performance of EAOPs on ECs, their application in real water bodies still faces multiple engineering bottlenecks:
1) ECsoften exist only at trace levels[14-15], severely limiting their diffusion to the electrode surface and significantly constraining the degradation kinetics of traditional two-dimensional reactors. Although three-dimensional electrodes and REMs[19,33]and other intensified structures can compress the diffusion layer and partially alleviate mass transfer bottlenecks, three-dimensional granular electrodes suffer from difficulties in recovery, easy loss, and insufficient long-term operational stability; meanwhile, the microporous structure of REMs is prone to clogging and irreversible fouling, limiting their promotion in practical industrial scenarios.
2) ECsContaminated water bodies generally exhibit low conductivity[16-17], under these conditions, energy loss caused by ohmic drop increases significantly, leading to a notable decline in the overall energy efficiency of EAOPs. Unlike the aforementioned mass transfer limitations, the low conductivity environment further constrains reaction efficiency from the perspective of the system's electrical properties. Although advanced oxidation technologies such as photocatalytic oxidation or photoelectrocatalysis, which do not rely on added electrolytes, can operate in low-conductivity water environments[29], they remain limited by issues such as high catalyst preparation costs and the susceptibility of active sites to contamination by natural organic matter (NOM), posing challenges for engineering applications. Furthermore, NOM and various inorganic ions commonly present in actual water bodies (such as Ca2+/Mg2+, HCO3-/CO32-, etc.) synergistically affect system performance through multiple mechanisms. First, background organic matter such as humic substances can preferentially consume reactive oxygen species, reducing the degradation efficiency of target pollutants[34]. Second, small-molecule organic compounds and carbonate systems can act as radical scavengers[19], reacting with highly active species such as ·OH to convert them into less reactive species (e.g., carbonate radicals), thereby weakening the contribution of non-selective oxidation processes. Meanwhile, Ca2+ and Mg2+ are prone to forming deposits under locally high pH conditions at the cathode (such as CaCO3, Mg(OH)2)[35], leading to electrode surface scaling, increased interfacial resistance, and hindered mass transfer, which further deteriorates system performance. Therefore, in actual water bodies, EAOPs are affected by interfacial competition, quenching of active species, and electrode deactivation; these factors may further alter reaction pathways and influence subsequent degradation behavior.
3) EAOPsThe issue of incomplete degradation and the generation of secondary pollutants cannot be ignored either[18]. Under actual conditions, due to limited reaction kinetics, partial oxidation products of ECs are often difficult to fully mineralize and remain in the water body, and the accumulation of these products may be further exacerbated under low-concentration conditions[36-37]. Existing studies have shown that incomplete degradation products of ECs may still retain certain biological activity, genotoxicity, or endocrine-disrupting effects[21,38]. In the treatment of ECs containing halogenated structures, some incompletely dehalogenated aromatic amine and quinone intermediates even exhibit higher ecological risks than the parent pollutants. Meanwhile, Cl-is widely present in natural water bodies and municipal wastewater[39], which is easily further oxidized on high-potential anodes to form ClO3-, ClO4-and other highly persistent inorganic by-products[40]. The aforementioned risks indicate that EAOPs in real-world scenarios need to focus heavily on the accumulation of incomplete degradation products and the generation and release of by-products, thereby imposing higher requirements for ensuring effluent safety.

3 Progress and Challenges in the Removal of ECs by Adsorption

3.1 Adsorption Principles and Classification of Adsorption Materials

The adsorption process is generally classified into physical adsorption and chemical adsorption; their adsorption types, dominant forces, and characteristics are summarized inTable 1.
From the perspective of material composition, common adsorbents can be classified into carbon-based materials, mineral materials, metals and their oxides, polymer materials, and metal-organic frameworks (MOFs). Different material systems exhibit distinct adsorption behaviors due to variations in their surface structures, pore characteristics, and chemical functional groups. Yu et al.[41]used oxidized multi-walled carbon nanotubes (MWCNTs) to remove quinolone antibiotics from water. The results indicated that their adsorption process is primarily dominated by physical adsorption mechanisms such as π-π interactions and hydrophobic effects. Due to the low bonding energy and high reversibility of these forces, the adsorption-desorption process is easily achievable, providing favorable conditions for material regeneration and reuse. Carbon materials have an extremely wide range of sources[42], for example, carbon materials prepared from various raw materials such as activated carbon, fruit shells, bamboo charcoal, bone charcoal, and coffee grounds have all been confirmed to exhibit excellent performance in the adsorption of various types of pharmaceuticals.
Unlike carbon-based materials, which primarily rely on non-specific interfacial interactions such as hydrophobic effects and π-π interactions, clay minerals exhibit distinctly different and more selective dominant mechanisms during adsorption and enrichment processes, owing to their layered structure, high surface charge density, and abundant exchangeable cation sites. For ECs, including rare earth ligand-based contrast agents and heavy metal-organic complexes, further removal is required through methods such as adsorption, ion exchange, or sedimentation filtration. Bishop et al.[43]systematically evaluated the adsorption and migration behavior of rare earth elements on clay minerals through batch adsorption experiments and EXAFS. The results showed that under neutral to slightly alkaline conditions (pH ≈ 7.5), adsorption efficiency exceeded 95% regardless of clay type or ionic strength variations, highlighting the critical role of clay minerals in metal enrichment and environmental migration control. Beyond the diversity of natural clays (such as bentonite, montmorillonite, and kaolinite), composite adsorbents formed by combining clay minerals with other functional materials demonstrate superior overall performance compared to single clays. Relevant studies indicate that clay-carbon composites can increase adsorption capacity for removing organic pollutants by 50% to 250%.[44], with this enhancement effect mainly stemming from the stable heterogeneous interfaces formed during the compounding process and richer surface functional groups, rather than a mere increase in specific surface area (SSA).
Metal-based materials, due to their active metal surfaces capable of participating in electron rearrangement and interfacial reactions, often exhibit a distinctly different adsorption pattern. Fang et al.[45]pointed out that nano-zero-valent iron (nZVI), relying on its high SSA and abundant active sites, can rapidly adsorb PFOA and PFOS through electrostatic interactions and an electron participation mechanism at the iron interface, with electron transfer behavior playing a crucial role in this process.
Polymer materials and MOF-based adsorbents have gradually become an important direction in adsorption material research in recent years due to their highly designable pore structures, rich and tunable ligand chemistry, and the ability to achieve specific recognition sites. Chitosan itself is rich in amino, amide, and hydroxyl groups, making it one of the most promising natural polymer materials; however, its original form suffers from limitations such as strong swelling, easy dissolution under acidic conditions, and slow adsorption kinetics. Elanchezhiyan et al.[46]constructed magnetic reduced graphene oxide-zinc ferrite composite microspheres (rGO-ZF@CB) using chitosan as a matrix, significantly improving these issues. In this system, rGO-ZF@CB not only possesses excellent magnetic separation properties but also achieves significant adsorption enhancement for typical long-chain PFAS (such as PFOA and PFOS), with maximum adsorption capacities reaching 16.07 and 21.64 mg/g, respectively, which are markedly superior to single chitosan materials. Mechanism analysis indicates that electrostatic attraction and hydrophobic interactions jointly drive PFAS adsorption, while the introduction of rGO and ferrite further enhances interfacial activity and functional group density, thereby endowing the composite material with higher adsorption efficiency.
On the other hand, due to the wide variety of ECs, their generally low environmental concentrations, and their extensive pollution range, relying solely on materials with high costs or complex preparation processes still presents limitations in practical applications. To meet the demands for large-scale treatment and sustainable development, green adsorbents prepared from agricultural waste or biomass have gradually gained attention in recent years. These materials offer advantages such as widespread raw material availability, low cost, and simple preparation processes, and they demonstrate good performance in removing various types of organic pollutants. For example, Nguyen et al.[51]utilized H3PO4-activated sunflower seed shell biochar to achieve efficient adsorption of various antibiotics, demonstrating the potential application value of biomass adsorbents in practical water treatment.
Overall, adsorption materials from different sources and structures exhibit unique mechanisms and application advantages in the removal of ECs. However, the performance of adsorbents in actual water bodies is still influenced by multiple factors such as pH, background ions, coexisting pollutants, and kinetics. Therefore, it is necessary to further combine the structural characteristics and environmental behaviors of ECs to systematically evaluate the treatment performance and application potential of different materials in real-world scenarios.

3.2 Research progress on adsorption in the removal of ECs

Traditional adsorbent material design strategies mainly revolve around three levels: 1) increasing SSA to enhance the density of potential adsorption sites; 2) introducing specific surface functional groups to strengthen the recognition and binding capacity for pollutants; 3) regulating the microstructure of materials to improve mass transfer efficiency.
However, relying solely on the aforementioned traditional strategies still presents significant limitations. First, macroscopic improvements in SSA are difficult to adapt to the molecular structure, size, and electronic characteristics of pollutants, resulting in a lack of quantitative design basis for material-molecule matching. Second, adsorption interfaces often involve the coupling of multiple mechanisms, making it difficult to accurately distinguish their contribution ratios and dominant pathways through conventional characterization techniques. Finally, the regulation of pore structures and functional groups remains at an experience-dominated level, lacking refined design based on molecular recognition, which makes it difficult to achieve high selectivity and specific recognition for specific categories of ECs.
Recent research has gradually shifted from experience-driven to mechanism-driven approaches, with relevant frontier technologies advancing the field of adsorption along two complementary pathways: on one hand, computational methods such as Density Functional Theory (DFT), Molecular Dynamics (MD) simulations, and Monte Carlo (MC) simulations can reveal the mechanisms of interaction at adsorption interfaces at the atomic and electronic scales, elucidating bonding modes, coordination structures, and dynamic interfacial evolution; on the other hand, data-driven methods like machine learning further transform these microscopic insights into actionable design criteria for guiding the construction of specific sites, pore regulation, and surface chemical modulation, thereby achieving rational design and performance optimization of adsorption materials.
DFT can directly obtain electronic structure information of adsorption systems and is considered one of the most explanatory theoretical tools for revealing adsorption mechanisms[52]. Liu et al.[53]used AHP to treat sesame straw biochar and applied it to the adsorption of Cd2+. Through joint analysis of DFT calculations and experimental data (Figure 2a~d), the synergistic contributions of multiple mechanisms during Cd2+ adsorption, including ion exchange, surface coordination, co-precipitation, and Cd2+-π interactions, were clarified. The coordination characteristics where oxygen-containing functional groups provide lone pair electrons and aromatic structures provide π electrons were elucidated at the electronic level. The maximum adsorption capacity of the finally prepared adsorbent for Cd2+was significantly improved (approximately 87.13 mg/g), revealing the critical role of DFT in quantitatively analyzing the electronic structure and reaction pathways at the adsorption interface. Unlike DFT, which emphasizes electronic structure and energy minimization pathways, MD focuses on the dynamic evolution of the adsorption process, capturing details of changes in the interfacial microenvironment over time. Based on this advantage, MD has been widely used to analyze the adsorption behavior of non-steroidal anti-inflammatory drugs (NSAIDs) in MOFs[54]. Taking UiO-66-(COOH)2as an example, Younes et al.[55]first used MC to determine the lowest energy configuration of diclofenac (DCF) on the material surface, finding that incompletely coordinated Zr6clusters containing Zr4+can act as Lewis acid sites, undergoing strong coordination and π-π interactions with carboxyl groups or aromatic rings in drug molecules. MD simulations further demonstrated the stable conformation and local environmental regulation after the drug entered the adsorbent pores (Figure 2e~g), providing dynamic evidence to elucidate the adsorption mechanism of NSAIDs in Zr-MOFs. Similarly, the high-capacity adsorption of DCF by the MOF-type adsorbent MIL-100(Fe) was also confirmed through multi-scale simulations[56]: MC simulations showed that DCF molecules are preferentially located in the characteristic pentagonal pore regions of MIL-100, while MD simulations revealed their spontaneous diffusion within the pores and the final stable adsorption configuration, explaining from a structural perspective why this material achieves a monolayer adsorption capacity as high as 773 mg/g. In summary, DFT, MC, and MD can provide complementary information from different levels, enabling a complete analysis of the adsorption process.
With deepening understanding at the mechanism level, research is gradually shifting towards how to map microscale information into material design rules, thereby achieving predictable and controllable regulation of adsorbent structure and function. Yazid et al.[58]systematically analyzed key molecular parameters such as charge distribution and HOMO-LUMO energy levels of target herbicide molecules in neutral and charged states through DFT calculations. Based on this, they identified preferred binding sites during interaction with adsorbents, providing a quantitative design basis for regulating surface functional groups of adsorption materials. Leveraging these microscopic electronic structure insights, researchers further prepared modified activated carbon material AC-Ws using walnut shells as precursors. This material demonstrated significantly enhanced adsorption performance in removing the target herbicide 2,4-D, with a maximum adsorption capacity reaching 290.2 mg/g, notably higher than most conventional activated carbon materials reported in literature (typically around 80~240 mg/g), validating the effectiveness of DFT-driven rational material design in optimizing adsorbent performance. Building on mechanism-driven research, data-driven material design methods are becoming another important direction in adsorbent development. Li et al.[57]constructed a machine learning (ML)-based biochar design framework, achieving full-process prediction and optimization from material preparation conditions to adsorption performance. Researchers established two XGBoost models (Fig. 2h~j): one to predict the effects of different raw material ash content and pyrolysis temperature on SSA and pore structure; the other to predict the adsorption capacity Qeof biochar for organic pollutants, where the adsorption model exhibited high prediction accuracy (R2 ≈ 0.97). On this basis, the two models were further coupled via particle swarm optimization, enabling reverse design of "preparation parameters → material structure → adsorption performance." This hybrid ML framework can automatically screen optimal raw materials and pyrolysis parameters for preparing customized biochar targeting specific antibiotics. Optimization results showed that using pine wood as a precursor and pyrolyzing within the 500~700 ℃ range yields biochar with higher SSA, exhibiting excellent adsorption capacity for various antibiotics including sulfamethoxazole, ciprofloxacin, and tetracycline. Additionally, the model captured a negative correlation trend between antibiotic molecular weight and the required optimal SSA, indicating that larger pollutant molecule sizes exhibit weaker dependence on high SSA. This study achieved quantitative coupling of "preparation parameters–material properties–adsorption performance," providing an intelligent route for precise design of adsorption materials. Such data-driven design strategies possess good universality and have been applied in multiple systems such as heavy metal capture and gas adsorption[59-60], demonstrating the cross-system and transferable advantages of machine learning in developing novel adsorbents. Furthermore, high-throughput screening (HTS) is an accelerated screening technology capable of rapidly evaluating performance across vast material libraries. Compared to methods like DFT and MD that focus on mechanistic analysis, the advantage of HTS lies in its ability to traverse candidate structures orders of magnitude larger within short timeframes, providing a highly parallel and systematic search pathway for material discovery. Currently, this strategy is mainly applied to structural optimization and multi-component gas adsorption performance prediction of crystalline porous materials such as MOFs[61-62], and has already formed a relatively mature simulation screening system. However, in the field of aqueous organic pollutant adsorption, the application of HTS remains relatively limited. With the gradual accumulation of adsorption databases and the precise development of interfacial force fields and solvation models, HTS is expected to deeply integrate with DFT, MD, and ML models to construct a high-throughput screening framework oriented toward aqueous adsorption systems, enabling rapid identification of preferred adsorbents with specific pore structures, surface functional groups, or interfacial affinities from large-scale candidate material libraries.

3.3 Characterization of Adsorption Mechanisms and Adsorption Models

In practical research, elucidating the interaction mechanism between pollutants and adsorbents is crucial. To this end, researchers usually combine multiple characterization techniques[63-64], such as FTIR, X-ray photoelectron spectroscopy (XPS), Raman spectroscopy, and scanning electron microscopy (SEM), to support an in-depth analysis of the adsorption process.
FTIR is one of the commonly used characterization methods. Wang et al.[65]utilized FTIR to analyze the adsorption behavior and mechanisms of four typical microplastics towards three antibiotics (amoxicillin AMX, ciprofloxacin CIP, and tetracycline TC). The FTIR results showed that no new functional group peaks appeared on the material surface before and after AMX adsorption, indicating that its removal is mainly achieved through physical actions such as surface adsorption and pore filling; whereas the adsorption of CIP and TC was accompanied by the enhancement of characteristic peaks (e.g., 1600~1631, 1364~1378 cm-1) and the appearance of new peaks (e.g., 2711~2718 cm-1, 690~775 cm-1), reflecting hydrogen bonding interactions and changes in C―H and O―H vibrations respectively, suggesting a tendency towards a multi-site chemical adsorption mechanism. To further obtain a more comprehensive mechanistic analysis, Cho et al.[66]integrated techniques such as Small-Angle X-ray Scattering (SAXS), Attenuated Total Reflectance Fourier Transform Infrared Spectroscopy (ATR-FTIR), and XPS to conduct a higher-dimensional structural-chemical joint analysis of the mechanism of triclosan adsorption by kenaf biochar. SAXS showed that the surface fractal dimension of the material decreased from 3 to 2.8 after adsorption, indicating that triclosan entering the pores made the material surface smoother; in FTIR, the benzene ring C―C skeleton vibration (1435 cm-1) and C―Cl absorption peak (876 cm-1) were enhanced, indicating the participation of aromatic ring structures and halogen groups in adsorption; XPS further confirmed the disappearance of inorganic chlorine signals and the enhancement of organic chlorine after adsorption, while the ―OH component in O 1s was enhanced, and changes in C 1s indicated the existence of π-π interactions. Comprehensive analysis reveals the synergistic contributions of specific surface area, aromatic structure, π-π interactions, hydrogen bonding, and surface functional groups to triclosan adsorption. Overall, the joint analysis of multiple characterization techniques provides multi-dimensional experimental evidence for elucidating the participation of functional groups, the evolution of surface chemical environments, and changes in microstructure during the adsorption process. However, such characterization results still struggle to directly quantify transient interfacial processes, competition for adsorption sites, and the relative dominance of different forces under actual operating conditions. Therefore, characterizing adsorption mechanisms usually requires combination with kinetic models, isothermal adsorption models, and theoretical calculations to construct a more systematic mechanistic understanding framework.
In adsorption studies, kinetic models and isotherm adsorption models are empirical auxiliary tools for analyzing adsorption behavior. Researchers widely utilize pseudo-first-order (PFO) and pseudo-second-order (PSO) kinetic models to fit experimental data[51], to characterize the rate features of the adsorption process[49-50]; or introduce Langmuir and Freundlich isotherm models to compare the apparent adsorption capacity and affinity of different adsorbents. The fitting results of these models are often used to assist in judging the rate characteristics and possible mechanisms of the adsorption process, and to reveal the energy heterogeneity of the adsorbent surface and the coverage characteristics of the adsorbate (monolayer or multilayer adsorption).

4 Adsorption-EAOPs coupling for ECs removal

4.1 Theoretical Foundation of Coupling

Both EAOPs and adsorption technologies have inherent limitations in addressing EC pollution: although EAOPs can achieve efficient oxidative removal, they are often constrained by insufficient interfacial mass transfer, declining energy efficiency, and the potential accumulation of intermediates; adsorption typically fails to effectively degrade ECs and may lead to pollutant re-release due to adsorbent saturation or fluctuations in environmental conditions. In this context, constructing a coupled adsorption-EAOP system holds clear significance, primarily reflected in the following three aspects.
(1) Complementary effects of mass transfer and interfacial reactions: Since the reactive species (such as ·OH) that play a dominant role in EAOPs have extremely short lifetimes (nanosecond to microsecond scale)[67-68], their effective action radius is often confined to an extremely thin reaction layer on the electrode surface. This forces pollutant molecules to cross a relatively thick liquid-phase diffusion layer (typically reaching about 10~100 μm) to enter the reaction zone, resulting in mass transfer limitations and insufficient local concentration at the interface. Consequently, a large number of free radicals undergo ineffective quenching before they can timely contact the target pollutants. The adsorption process can in situ enrich pollutants at the electrode-electrolyte interface, significantly increasing the effective concentration of target molecules within the reactive layer, thereby enhancing interfacial reaction kinetics, alleviating the mass transfer bottleneck of EAOPs, and substantially improving the utilization efficiency of reactive species such as free radicals.
(2) Energy efficiency optimization and byproduct control: The electrolyte concentration in actual water bodies is far lower than that in laboratory systems (e.g., the commonly used 0.05~0.10 mol/L sodium sulfate)[16-17], which leads to a significant increase in ohmic drop, thereby reducing the energy efficiency of EAOPs. The adsorption process is hardly affected by water conductivity; its coupling with EAOPs allows enrichment and deep degradation to be implemented in stages under different operating conditions, thus reducing energy loss, improving overall removal efficiency, and inhibiting the accumulation of byproducts and intermediates.
(3) Pollutant degradation and secondary pollution control: Adsorbents are prone to re-release of target pollutants when saturated or when encountering fluctuations in conditions such as temperature, pH, electrolyte type/concentration[69-70], posing potential risks of secondary pollution. The oxidation of adsorbed pollutants by EAOPs facilitates the in-situ regeneration of adsorbents, thereby extending their service life.
In summary, the adsorption-EAOPs coupled system is expected to overcome the bottlenecks of single technologies in terms of interfacial mass transfer, energy efficiency loss under complex water matrix conditions, and the risk of adsorbent re-release, providing an effective strategy for the efficient and safe removal of ECs.

4.2 Coupling Mode Classification and Synergistic Mechanisms

The adsorption-EAOPs coupled system can be primarily categorized into the following three typical modes, each providing differentiated solution pathways tailored to the environmental behavior characteristics of specific ECs and water treatment objectives:
(1) Synchronous adsorption-EAOPs degradation mode: applicable to scenarios where trace-level ECs suffer from diffusion limitations leading to excessively low interfacial reaction efficiency[19], this mode leverages the selective adsorption of pollutants by materials to significantly increase the local enrichment of pollutants at the electrode interface, enhance the utilization efficiency of reactive species, and thereby alleviate the mass transfer bottleneck of EAOPs.
(2) Adsorption enrichment-EAOPs degradation mode: Suitable for scenarios with complex water matrices where EAOPs cannot operate stably directly[19,32], such as water bodies with high salinity, low conductivity, high natural organic matter load, or containing large amounts of radical scavengers (Cl-, HCO3-, PO43-, etc.). This mode typically requires ECs to have a strong adsorption tendency, enabling pollutants to be transferred to an independent EAOPs reaction system for subsequent degradation.
(3) EAOPs Degradation-Terminal Adsorption Mode: Suitable for scenarios where EAOPs can rapidly achieve preliminary degradation or transformation, but the generated harmful intermediates and by-products are difficult to further mineralize. This mode is applicable for deep treatment requirements, such as removing incompletely degraded products, adsorbing metal ions released during the EAOPs process (e.g., REEs or heavy metal complexes), improving effluent stability, or meeting stricter discharge standards.
In summary, the three coupling modes demonstrate the functional complementarity between adsorption and electrochemical processes in the enrichment, transformation, and removal of pollutants.
The synchronous adsorption-EAOPs degradation mode has developed rapidly in recent years. Its core lies in the synergistic design of interface structure and reaction space to reconstruct the coupling relationship among pollutant enrichment, reactive species generation, and electrochemical reaction processes at the nanoscale. Wang et al.[71]based on a cellulose-chitosan skeleton, combined with in-situ nitrogen doping and molecular imprinting technology, constructed a single-cathode carbon electrode (CSF-MIP-800) with nano-confined reaction spaces, achieving synchronous adsorption-electrocatalytic degradation of PFOA in an electro-Fenton system (Figure 3a). The imprinted cavities match PFOA molecules highly in terms of spatial scale and functional groups, enabling preferential adsorption and enrichment on the cathode surface and within the pores; DFT calculations further indicate that pyridinic N sites in the confined space have the highest adsorption energy for PFOA, serving as "synergistic sites" to simultaneously anchor PFOA and catalyze O2 to generate H2O2 via the 2-electron pathway of the oxygen reduction reaction (ORR). Compared to non-imprinted electrodes, CSF-MIP-800 significantly enhanced ORR activity and the generation capacity of reactive species: oxygen conversion efficiency increased from 17.9% to 61.2%, and the effective concentrations of ·OH and O2·- increased by approximately 2–3 times. Under conditions of pH ≈ 3 and an electrocatalyst dosage of 1.8 g/L, this single-cathode EF system achieved 96.7% PFOA removal within 120 min, corresponding to a total organic carbon (TOC) removal rate of about 83% and a defluorination rate of about 60.3%. In this system, the confined space constructed by molecular imprinting possesses the dual functions of selective adsorption of target molecules and in-situ generation of reactive oxygen species (such as ·OH and O2·-), greatly shortening the mass transfer distance between reactive species and pollutants and significantly improving interfacial reaction efficiency. The synchronous adsorption-EAOPs degradation mode can also be extended to the anode side. Zhang et al.[72]utilized bifunctional metal-organic frameworks (Fe-MOFs) to prepare electrodes possessing both excellent adsorption performance and strong anodic oxidation capability: the MIL-101(Fe) skeleton provided abundant adsorption sites for sulfosalicylic acid and acetaminophen, while α-FeOOH generated in-situ during anodic oxidation became the active center, accelerating charge transfer and driving the generation and utilization of reactive oxygen species (1O2, O2·-, ·OH, etc.) (Figure 3b). This synergistic effect of adsorption and anodic oxidation continues at the porous interface, not only maintaining a high local pollutant concentration on the electrode surface but also achieving in-situ regeneration of active sites. Thanks to this, the system achieved approximately 94% removal of PPCPs in actual pharmaceutical wastewater, with energy consumption as low as 31.2 kWh kgCOD-1, verifying the significant advantages of this coupled mode in enhancing interfacial reaction efficiency and energy efficiency. At the kinetic level, this system no longer fully follows the pseudo-first-order reaction behavior common in EAOPs but rather conforms more closely to the Langmuir-Hinshelwood surface reaction model, where the reaction rate is controlled simultaneously by surface coverage of pollutants and the electrochemical reaction rate. For molecules with strong adsorption tendencies (such as sulfosalicylic acid), the reaction process exhibits obvious characteristics of adsorption-reaction coupling, indicating that such coupled modes alter the reaction control steps and kinetic structure. However, in actual water bodies, the interfacial advantages of the synchronous adsorption-EAOPs degradation mode may also be interfered with by natural organic matter. NOM represented by humic acid has a complex molecular structure and exhibits significant competitive adsorption behavior at the electrode interface, which can preferentially occupy active sites and reduce the interfacial enrichment efficiency of target pollutants. Meanwhile, the amphiphilic characteristics of humic acid make it prone to forming an adsorption layer on the electrode surface, affecting the generation and transport of reactive species[34], thereby triggering interfacial fouling and electrode passivation. To alleviate these problems, pretreatment methods (such as activated carbon adsorption, ultrafiltration, etc.)[73]can be used to remove or transform NOM before EAOPs, reducing the risk of interfacial fouling from the source. During the reaction process, introducing intensification technologies such as ultrasound[74]can strip deposited layers from the electrode surface and enhance interfacial mass transfer through cavitation effects, thereby slowing down the passivation process. In addition, pulsed current or periodic reverse polarity operations[75-76], as well as chemical cleaning methods (such as acid washing or alkali washing), can be employed to maintain the activity and stability of the electrode surface. Therefore, the operational performance of this mode in actual water bodies highly depends on the synergistic regulation of interfacial fouling and water matrix.
Correspondingly, the core of the adsorption enrichment-EAOPs degradation mode is to first enrich and separate pollutants from complex water bodies, and then achieve adsorbent regeneration under a controllable electrochemical environment. Ersan et al.[77]proposed a proof-of-concept system for the in-situ electro-regeneration of adsorption-saturated activated carbon (F400), achieving electro-driven desorption and capacity recovery of PFAS-enriched adsorbents. This system first utilizes the high specific surface area and hydrophobicity of activated carbon to efficiently enrich long-chain PFOA; during the regeneration phase, saturated F400 serves as the cathode, where OH-generated by water reduction causes a significant local pH increase on the carbon surface, thereby electro-driving the desorption of negatively charged PFOA molecules. These PFOA molecules desorbed into the solution are expected to undergo subsequent ex-situ degradation treatment via EAOPs. Multiple adsorption-regeneration cycles indicate that this method can recover approximately 60% of the initial adsorption capacity and maintain high regeneration stability over 4 consecutive cycles; energy consumption is only about 0.70 kWh kg-1, offering distinct advantages over traditional regeneration technologies such as incineration. This demonstrates that electrochemical processes can serve as an effective means for adsorbent regeneration and create conditions for subsequent deep oxidation treatment of concentrated PFAS solutions. Another category of strategies involves constructing interface sites with enrichment functions, allowing pollutants to be pre-enriched on the electrode surface and subsequently degraded through EAOPs. Roth et al.[78]constructed a microtubular gas diffusion electrode (CNT-GDE) composed of multi-walled carbon nanotubes (MWCNTs) and adopted an operational strategy of adsorption enrichment followed by electro-Fenton degradation, circumventing the reliance of traditional electro-Fenton processes on acidic conditions and iron sludge separation. In this system, the CNT-GDE functions as both a porous adsorbent and a cathode, first enriching Acid Red 14 from raw water without an applied electric field; subsequently, the electrode is transferred to an independent acidic electrolyte (0.05 M Na2SO4, pH ≈ 3), where in-situ pollutant degradation and electrode regeneration are achieved via the electro-Fenton reaction: at a current density of approximately 4.1 mA/cm2and with 0.7 mmol/L Fe2+, the adsorption capacity of the CNT-GDE can be restored to 97%~100%, while achieving a COD removal rate of approximately 70%. This coupled mode separates low-concentration pollutants from wastewater with complex matrices and introduces a controllable electrochemical reaction environment, enabling the synergistic occurrence of adsorbed pollutants, H2O2generation and ·OH-mediated oxidation reactions within the same microscopic space. This effectively weakens the non-selective quenching effect of the water matrix on ·OH generation and utilization, significantly improving interfacial reaction efficiency and the stability of the water treatment process.
In contrast, the EAOPs degradation-terminal adsorption mode is logically closer to the combination of traditional EAOPs and post-treatment water units in terms of process logic. Its adsorption process does not primarily aim to directly enhance the interfacial reactions or reaction rates of EAOPs, but rather serves as a supplementary means to further remove residual degradation intermediates or by-products after EAOPs treatment, thereby improving the overall stability and safety of the effluent quality. For example, methylene blue often generates aromatic or conjugated structure intermediates with significant biological toxicity during the EAOPs process. Wang et al.[79]achieved effective removal of these highly toxic intermediates by introducing fly ash (4 g/L) as a terminal adsorption unit, reducing the light inhibition rate of the anodically oxidized solution on luminescent bacteriaVibrio fischerifrom >80% significantly to about 7%. This result indicates that the EAOPs degradation-terminal adsorption mode can effectively compensate for the shortcomings of EAOPs in deep mineralization and demonstrates unique advantages in improving effluent safety. During the EAOPs process, the formation of disinfection by-products (DBPs) such as chlorinated oxides is usually unavoidable[23,26], and it is difficult to remove them through further EAOPs or natural attenuation. The terminal control strategy centered on adsorption has been proven to be a path with clear engineering feasibility, and the key to this strategy lies in constructing a functionalized adsorption interface with anion affinity and exchange capabilities. A typical approach is to use adsorbent materials that have undergone cationic modification; for example, Sanchez-Cano et al.[80]significantly enhanced the capture capacity for ClO2-and ClO3-by introducing quaternary ammonium salt structures on the surface of granular activated carbon (GAC), forming stable positive potential sites. Under static conditions, the modified GAC achieved approximately 100% removal of ClO2-within 2 hours, while simultaneously achieving a removal rate of about 80% for ClO3-; under continuous flow fixed-bed conditions, the material maintained high-efficiency retention of ClO3-during multi-cycle operations and demonstrated good stability and regeneration potential. It is worth noting that for free metal ions released during the EAOPs process, researchers often prefer to achieve removal through sedimentation filtration, electrochemical reduction, or electric-driven enrichment, rather than relying primarily on adsorption processes: Mao et al.[81]proposed a dual-cathode electro-Fenton system without added reagents, achieving efficient removal of Cu-EDTA. During the EAOPs process, Cu(I) undergoes a Fenton-like reaction with H2O2to produce ·OH, while part of Cu(II) is further oxidized to Cu(III) and acts as a selective oxidant to revert to Cu(II). Under optimized conditions, the Cu-EDTA decomplexation and Cu recovery rates of this dual-cathode system reached 94.8% and 93.4%, respectively, with corresponding apparent rate constants of 0.017 min-1, both significantly superior to the single-cathode system; its energy consumption was only 0.011 kWh/g (decomplexation) and 0.057 kWh/g (Cu recovery). Similar coupling strategies are also common in the treatment of metal complexes such as copper, nickel, and zinc[82-83]. This can be attributed to the fact that metal ions typically possess distinct valence transformation characteristics and electrochemical activity, making them easier to achieve targeted separation and resource recovery compared to diverse organic intermediates or by-products.
In summary, the three coupling modes exhibit essential differences in operating strategies, coupling sequences, and functional priorities, reflecting the division of labor and synergistic complementarity between EAOPs and adsorption processes in key stages such as pollutant enrichment, speciation transformation, and degradation/mineralization, thereby providing feasible process pathways for enhancing treatment performance and ensuring effluent safety.

4.3 Key challenges facing engineering applications

Although the adsorption-EAOPs coupled system has demonstrated significant advantages at the laboratory scale, its transition to engineering applications still faces key challenges. Existing research mostly focuses on short-term removal efficiency or performance enhancement under single operating conditions, while systematic evaluations of material manufacturability, reactor scale effects, and long-term operational stability remain insufficient.
At the material level, preparation cost and performance stability are factors that must be considered in engineering applications. Biochar, due to its wide availability, low cost, and abundant surface functional groups, is widely regarded as an adsorption carrier with application potential. However, Fan et al.[84]revealed that biochars derived from different raw materials exhibit significant differences in their adsorption performance for sulfonamide antibiotics. These differences are reflected not only in adsorption kinetics and maximum adsorption capacity but also further affect the overall removal performance of the system. Related studies indicate that this phenomenon is usually attributed to significant differences in carbon skeleton maturity and oxygen-containing functional group abundance among biochars from different raw materials. The inherent variations in raw materials can lead to large dispersion in adsorption performance, bringing engineering-level uncertainties to process standardization and the long-term stable operation of water treatment effects. In contrast, highly designable functional materials represented by MOFs demonstrate clearer structural advantages. MOFs possess regular and tunable pore structures, high specific surface areas, and precisely introducible metal nodes and functional groups[72], making them more capable of achieving efficient, stable, and selective enrichment of pollutants such as ECs in coupled adsorption-EAOPs systems. However, most MOFs rely on sophisticated chemical synthesis routes[85-86], where their raw material costs, solvent consumption, and synthesis cycles are significantly higher than those of traditional carbon-based materials. More critically, the long-term durability of MOFs in electrochemical environments still faces intrinsic challenges. During actual operation, multiple degradation pathways often occur simultaneously. Under acidic or alkaline conditions, OH-can engage in coordination competition with metal centers and induce ligand exchange, while H+weakens metal-ligand bonds through protonation of the ligands, thereby reducing framework structural stability. At higher anodic potentials, organic ligands may also undergo direct electrochemical oxidation, leading to bond cleavage and local structural disintegration. Furthermore, the electric double layer formed at the electrode interface causes local ion enrichment and pH shifts, thereby exacerbating coordination environment disturbances and promoting structural evolution processes[87]. The above processes are typically accompanied by metal ion leaching and defect structure generation, further reducing the overall stability of the material. Under continuous electrochemical polarization conditions, these processes usually do not occur in isolation but gradually accumulate and couple over operating time, causing the MOF to evolve from interfacial structural disturbances toward overall framework structural development, ultimately potentially leading to structural reconstruction or a significant decline in stability. Similar concerns also exist in spatially confined materials and molecularly imprinted polymer systems constructed based on polymers or biological substrates[71]. Considering that existing research lacks systematic characterization of the evolution behavior and deactivation mechanisms of the material framework itself under strong oxidative environments, the lifespan and reliability of such materials in actual long-cycle, high-intensity electrochemical water treatment processes remain subject to considerable uncertainty.
At the reactor scale, non-uniform current distribution in electrochemical reactors is one of the major limiting factors for the engineering application of EAOPs. Compared to the ideal uniform electric field distribution in laboratory-scale setups, significant ohmic losses and polarization effects in engineering-scale reactors lead to a redistribution of current density on the electrode surface (Figure 4). This non-uniform distribution typically manifests as significant edge effects, which not only cause elevated local overpotentials, triggering severe side reactions such as oxygen/hydrogen evolution, but also result in an imbalance in the spatial generation rates of reactive species, thereby reducing their overall utilization efficiency. Furthermore, prolonged local high current loads accelerate electrode passivation or coating detachment, severely constraining the stable operation of EAOPs systems at the engineering scale.
Furthermore, it should be noted that different adsorption-EAOPs coupling modes exhibit significant differences in their functional positioning for engineering applications, which is particularly critical in energy consumption evaluation and process optimization (Table 2). Systems represented by the adsorption enrichment-EAOPs mode primarily alleviate mass transfer limitations by increasing the local concentration of pollutants at the interface, thereby improving current efficiency to a certain extent and reducing energy consumption per unit of pollutant removal; meanwhile, synchronous adsorption-EAOPs systems enhance energy efficiency by intensifying interfacial reaction processes. However, for coupling modes such as EAOPs degradation followed by terminal adsorption, the primary purpose of introducing the adsorption unit is typically not to directly reduce energy consumption, but rather to serve as a post-treatment step for removing residual organic matter, intermediates, or potentially toxic by-products (e.g., dissolved organic matter or free metal ions) generated during electrochemical degradation. The former two types focus more on reaction efficiency and energy optimization, whereas the latter emphasizes effluent water quality safety and environmental risk control.
Overall, during the transition of adsorption-EAOPs coupled systems toward engineering applications, the core bottlenecks are concentrated in insufficient stability and controllability under long-term continuous operating conditions. Existing research is mostly limited to ideal water matrices and model pollutants, often evaluating removal efficiency and energy consumption within short operational cycles. However, in real water environments, complex ionic backgrounds[88], the coexistence of natural organic matter[89], as well as common electrode fouling[90], corrosion, and side reaction processes[91], often generate cumulative effects during long-term operation, gradually exacerbating issues such as material deactivation, deterioration of current distribution, and attenuation of interfacial reaction kinetics. For the adsorption unit within the coupled system, during long-term use, it not only faces challenges in controlling regeneration frequency after adsorption saturation[92], but is also constrained by problems such as irreversible decay of adsorption capacity, competitive blockage of pores by non-target macromolecular organic compounds, and a significant reduction in regeneration efficiency after multiple regeneration cycles. Therefore, future research urgently needs to shift from short-term feasibility verification to long-term operational stability assessment, conducting multi-cycle, long-duration continuous operation experiments under real water conditions; and combining methods such as in-situ electrochemical characterization, tracking of material structural evolution, and monitoring of effluent biological toxicity to systematically reveal the main failure modes of adsorption-EAOPs coupled systems in engineering applications, thereby providing a more reliable theoretical basis for their practical promotion.

5 Conclusion and Outlook

The adsorption-EAOPs coupled system provides a technically promising pathway for the efficient and safe removal of ECs. This paper systematically reviews the environmental behavior characteristics of ECs and research progress on their removal via EAOPs, focusing on key bottlenecks faced by EAOPs in real water bodies, such as mass transfer limitations, reduced energy efficiency, incomplete degradation, and byproduct formation. From a mechanistic perspective, it elucidates the supplementary role of the adsorption process in pollutant enrichment, reaction interface reconstruction, and effluent safety control. Based on differences in process organization and functional focus, this paper categorizes adsorption-EAOPs coupled systems into three typical coupling modes. These modes expand the performance scope of single EAOPs or adsorption technologies to some extent by increasing interfacial pollutant concentrations, optimizing the utilization efficiency of active species, and inhibiting the accumulation of toxic intermediates and byproducts. They demonstrate significant advantages, particularly in the removal of trace ECs, adaptability to complex water matrices, and control of effluent toxicity. Meanwhile, this paper also points out that the engineering application of adsorption-EAOPs coupled systems still faces multiple challenges, including limitations in cost, structural stability, and scalable preparation of adsorption and electrocatalytic materials; issues of uneven current distribution and energy efficiency attenuation caused by reactor scale-up; and the lack of systematic evaluation regarding material deactivation and system reliability under long-term continuous operation conditions. These issues remain insufficiently studied and constitute one of the major factors restricting the transition of such technologies from the laboratory to practical applications. Future research should synergistically advance the development of adsorption-EAOPs coupled systems across three levels: materials, reactors, and process control. This involves reducing material complexity and operational risks through functional decoupling and modular design; mitigating scale effects through refined electrochemical and fluid process regulation; and conducting long-term operation and environmental risk assessments under real water body conditions. Furthermore, addressing potential structural deterioration and performance attenuation of functional materials within coupled systems under actual operating conditions, future research urgently needs to establish standardized accelerated aging and deactivation evaluation systems. At the macro level, accelerated testing should be conducted by constructing multi-ion coexistence systems consistent with actual application scenarios (rather than traditional single electrolyte solutions), combined with fluctuations in electrochemical operating conditions and key performance indicators (such as removal efficiency, current efficiency, mineralization degree, and structural stability) to establish quantitative evaluation methods for rapid assessment of material lifespan and deactivation behavior. At the micro level, it is also necessary to further clarify the dominant mechanisms of material deactivation (such as structural reconstruction, loss of active sites, or surface passivation) to guide material optimization and improvements in reactor operation strategies, thereby enhancing the long-term stability and reliability of adsorption-EAOPs coupled systems in engineering applications. Through these efforts, adsorption-EAOPs coupled systems are expected to gradually evolve from the concept validation stage to engineering feasibility, providing more reliable technical support for the sustainable governance of ECs in complex water bodies.

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Funding

National Natural Science Foundation of China(52270078)

Xi’an Jiaotong University Fundamental Research Program(xzy022025024)

Shanxi Provincial Science Fund for Distinguished Young Scholars(2025JC-JCQN-027)

Shandong Provincial Key Research and Development Program(2025TSGCCZZB0684)

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