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Advances in Two-Dimensional Black Phosphorus-Based Nanostructures for Photocatalytic Applications

Xin Pang , Shixiang Xue , Tong Zhou , Hudie Yuan , Chong Liu , Wanying Lei

Progress in Chemistry ›› 2022, Vol. 34 ›› Issue (3) : 630 -642.

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Progress in Chemistry ›› 2022, Vol. 34 ›› Issue (3) : 630-642 DOI: 10.7536/PC210318
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Advances in Two-Dimensional Black Phosphorus-Based Nanostructures for Photocatalytic Applications
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Abstract

As a new two-dimensional (2D) monoelement material in post-graphene era, black phosphorus (BP) has gained broad prospects in photocatalysis due to its extraordinary physicochemical characteristics including unique anisotropic structures, high carrier mobility and thickness-controlled bandgap. Nevertheless, the extremely narrow bandgap of BP (≤ 1.5 eV) is detrimental for the efficient separation of photogenerated electron-hole pairs that limits the photoreactivity. And the isolated BP suffers from the severe degradation upon long-term exposure due to PxOy species formed by the reaction between the lone pair electrons onto the BP surfaces and oxygen in ambient environment, then BP will gradually corrode in water through the formation of phosphoric acid. Therefore, the lower photoreactivity and instability of BP material restrict its industrial implementation. To overcome these obstacles, various effective strategies like creating a wide range of plasmonic hybrid nanostructures and mixed-dimensional heterojunctions have been developed. Herein, the recent progress on BP-based nanostructures through hybridization with dissimilar components like metals, semiconductors, carbon materials, etc. has been summarized and its applications in photocatalytic reactions such as water splitting for hydrogen evolution, organic pollutant removal, CO2 photoreduction and N2 fixation have also been reviewed, together with the insights into the photocatalytic mechanism for the boosted photoreactivity and good recyclability. Lastly, the challenges and potential directions of BP-based nanostructures toward high-efficiency photocatalytic reactions are analyzed and provided.

Contents

1 Introduction

2 BP-based nanostructures for hydrogen evolution

2.1 Metal/BP hybrid

2.2 Semiconductor/BP hybrid

2.3 Carbon/BP hybrid

3 BP-based nanostructures for organic pollutant removal

3.1 Metal/BP hybrid

3.2 Semiconductor/BP hybrid

3.3 Carbon/BP hybrid

4 BP-based nanostructures for CO2photoreduction and N2fixation

5 Conclusions and perspectives

Graphical abstract

Keywords

black phosphorus-based nanostructures / photocatalysis / water splitting for hydrogen evolution / organic pollutants removal / CO2 photoreduction / N2 fixation

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Xin Pang, Shixiang Xue, Tong Zhou, Hudie Yuan, Chong Liu, Wanying Lei. Advances in Two-Dimensional Black Phosphorus-Based Nanostructures for Photocatalytic Applications. Progress in Chemistry, 2022, 34(3): 630-642 DOI:10.7536/PC210318

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1 Introduction

The rapid development of science and technology is accompanied by a huge consumption of energy, while bringing a series of environmental problems, such as water pollution, greenhouse effect and haze. At present, photocatalytic technology based on semiconductor materials can convert clean and renewable solar energy into chemical energy, which is considered as one of the ideal energy conversion technologies. Photocatalytic reactions include water splitting, degradation of organic pollutants, reduction of CO2 and nitrogen fixation[1⇓⇓~4]. In order to realize its industrial application, the construction of efficient and stable photocatalytic materials with broad-spectrum solar response is the key direction of development. Metal oxides (TiO2, CeO2, WO3, etc.), transition-metal chalcogenides (TMDs) and graphite-phase carbon nitride (g-C3N4) are currently the most studied semiconductor materials in the field of photocatalysis[5⇓⇓~8]. However, these materials have the following three problems: (1) The width of the band gap is large, and the utilization rate of sunlight is low. For example, the band gap of TiO2 is about 3.2 eV, which can only absorb 5% of the sunlight[9]. (2) Photogenerated carriers are easy to recombine, and the electrons and holes are quenched in the material before they migrate to the surface and undergo redox reaction, resulting in low photocatalytic performance; (3) The specific surface area of the bulk material (about hundreds of nanometers in size) is small, the concentration of exposed active sites is low, and the reactants are not easy to adsorb on the surface of the catalyst, which hinders the subsequent redox reaction[10]. Therefore, the narrow range of solar response and limited photocatalytic activity restrict the development and practical application of photocatalytic technology[11].
In order to solve the current limitations of photocatalytic technology, researchers are committed to finding a photocatalytic material with both broad spectral response and high carrier separation efficiency. Since 2014, black phosphorus (BP), as another single-element two-dimensional material in the post-graphene era, has attracted wide attention of researchers[12,13]. Because of its unique layered structure (Fig. 1A), in-plane anisotropy, ultra-high carrier mobility and controllable band gap, it has broad application prospects in the field of photocatalysis[14⇓~16]. The advantages of BP materials in the field of photocatalysis are mainly reflected in the following five aspects: (1) The band gap of BP decreases with the increase of layer thickness. As shown in Figure 1b, the band gap of bulk BP is 0.3 eV, and that of monolayer BP is 1.5 eV[17]. Therefore, the utilization rate of solar energy of the BP material is as high as 95%, and the BP material has the ability to absorb ultraviolet light, visible light and near-infrared light; (2) BP is a direct band gap semiconductor, which is beneficial to the strong interaction between light and matter and can increase the concentration of photogenerated carriers; (3) BP has ultrahigh carrier mobility (~1000 cm2·V-1·s-1), which is conducive to the rapid migration of carriers to the surface of the material; (4) As a two-dimensional material, the limited atomic thickness of BP can greatly reduce the migration distance of carriers, making it easier for them to migrate to the surface to participate in the subsequent redox reaction; (5) Due to the characteristics of the two-dimensional structure, BP has a large specific surface area and abundant active sites, which is more conducive to the surface adsorption of reactants and the occurrence of surface redox reactions. To sum up, the two-dimensional BP material is a new type of photocatalytic material with great potential.
However, the separation efficiency of photogenerated electron-hole pairs in a single BP material is still low, and the construction of heterojunction can further improve its catalytic activity and stability. The reasons for the improvement are mainly reflected in the following three points: (1) The formation of the heterojunction is helpful to synthesize the optical absorption properties of the material, broaden the optical absorption range, enhance the optical absorption, and increase the concentration of photogenerated carriers; (2) the heterojunction construction is beneficial to improving the separation rate of photogenerated carriers of the catalyst, accelerating the spatial separation of electron-hole pairs, and improving the stability of BP through the migration and reaction consumption of carriers; (3) The composite material can form a close interaction at the interface, which is beneficial to the effective separation of carriers at the interface on the one hand, and can improve the stability of BP on the other hand[18⇓⇓⇓~22]. In recent years, researchers have summarized and prospected the research status of BP materials in the field of photocatalysis. For example, Li et al systematically introduced the physical and chemical properties of BP materials, preparation methods and various modification methods to improve the performance of BP, and summarized the application of BP materials in the field of photocatalysis[23]. Sakthivel et al. reviewed the application progress of BP materials in environmental treatment, such as sewage treatment and air purification[24].
In this paper, the research progress of nanocomposites composed of 2D BP materials and metal, semiconductor and carbon materials in the fields of photocatalytic water splitting, degradation of organic pollutants, reduction of CO2 and nitrogen fixation is reviewed.Finally, the future research directions of 2D BP-based photocatalytic composites are analyzed and prospected.

2 Application of Black Phosphorus-based Nanomaterials in Cracking Aquatic Hydrogen

Hydrogen is a kind of important renewable and clean energy.Since Fujishima and Honda first discovered that hydrogen could be produced by splitting water with TiO2 electrode in 1972, solar-driven hydrogen production has been regarded as a green hydrogen production technology, which can effectively alleviate the existing energy problems[25⇓⇓⇓⇓⇓~31]. The reaction equation for hydrogen production from water cracking is as follows:
H 2 O = 1 / 2 O 2 + H 2 　 △ G = + 237 k J / m o l
Photocatalytic water splitting is an endothermic reaction.In order to drive the reaction, the band gap of the semiconductor material should be greater than 1. 23 eV, and the lowest position of the conduction band should be more negative than the hydrogen reduction potential (H+/H2:0.0 eV vs.NHE,pH=0).Under this condition, electrons have strong reduction ability and can reduce H+ to H 2 [32][33-34]. Zhu et al. reported that 2D BP nanosheets have certain hydrogen production performance under alkaline conditions, but the hydrogen production performance is low and the stability is poor[35]. The in-situ modification of BP surface, such as partial oxidation, functional group modification and in-situ growth of metal phosphide, can improve the stability of the material to a certain extent, but its hydrogen production performance is still low[36⇓⇓~39]. Therefore, the introduction of metals, semiconductors or carbon materials to form heterojunctions with BP can greatly improve the effective separation of photogenerated electron-hole pairs and further enhance the photocatalytic hydrogen production performance, on the other hand, it can broaden the utilization range of sunlight and improve the stability of BP materials.

2.1 Metal/BP

Noble metal materials, such as Pt, Ag and Au, have excellent conductivity, which is beneficial to the rapid transfer of photogenerated carriers in semiconductor materials, thus improving the separation efficiency of electron-hole pairs[20][40][41]. After introducing 20 wt% Pt as a co-catalyst, the hydrogen production performance of the composite increased by about 30 times (447μmol·h-1·g-1) under visible light irradiation when the BP nanosheets were synthesized by a simple solvothermal method at 60 – 140 ° C by Tian et al[42]. In order to make the cocatalyst Pt stably supported on the surface of the support, Xue et al. Grown Pt nanoparticles on the surface of BP nanosheets in situ, which could enhance the interaction between Pt and BP interface[20]. Impedance spectroscopy (EIS) shows that the formation of Pt/BP heterojunction is beneficial to improve the charge transfer rate. Under illumination, due to the low overpotential of Pt, the photogenerated charges on the conduction band of BP will quickly migrate to the surface of Pt and react with the adsorbed H+ to generate H2, while the holes remain on the valence band of BP and react with the OH- in water to generate oxidative free radicals, which are captured by TEOA, and the electron-hole pairs are effectively separated, greatly improving the hydrogen production activity of the material.
In order to further improve the photocatalytic activity of the material and enhance the absorption of sunlight, Zhu et al. constructed a ternary BP/Pt/RGO composite photocatalytic material with reduced graphene oxide (RGO) as the charge transfer channel, Pt as the cocatalyst, and BP nanosheets as the catalyst. The hydrogen production rates under visible light (λ > 420 nm) and near-infrared light (λ > 780 nm) were 840μmol·h-1·g-1 and 590μmol·h-1·g-1, respectively, in the presence of sacrificial agent EDTA[32]. Both the enhanced photocurrent density and the smaller resistance indicate that the introduction of RGO accelerates the rate of interfacial charge transfer and suppresses the recombination quenching of photogenerated carriers, thereby enhancing the rate of hydrogen production. Under illumination, BP is excited and the electrons in the valence band jump to the conduction band. Because of the ultrafast carrier mobility of RGO, the electrons on BP can be quickly transferred to Pt through RGO, and then reduced with H+ to generate H2. In addition, tungsten nitride (WN) with metal-like properties is also used to improve the hydrogen production performance of BP[43].
Noble metal nanoparticles, such as Au and Ag, have a significant localized surface plasmon resonance (LSPR) effect. When the frequency of incident light is the same as the oscillation frequency of free electrons on the surface of noble metal particles, the electrons on the surface of noble metal particles will oscillate violently and absorb solar energy[44]. Based on this characteristic, the introduction of noble metal nanoparticles on the surface of BP nanosheets is one of the development ideas to improve its solar energy utilization and enhance its hydrogen production performance. Zhu et al. used Au nanoparticles as a "binder" to form a ternary BP/Au/La2Ti2O7 composite. Due to the LSPR effect of Au nanoparticles and the interfacial interaction between BP and Au/La2Ti2O7, the ternary composite had a good hydrogen production performance in the near-infrared region of λ > 780 nm, and the hydrogen production rate could reach 300μmol·h-1·g-1. The hydrogen production mechanism under visible and near-infrared light conditions is shown in Figure 2[41]. Under visible light, the electrons on the surface of Au are excited due to the LSPR effect, and these electrons can overcome the Schottky barrier at the interface between Au and La2Ti2O7 and transfer to the conduction band of La2Ti2O7, reducing H+ to H2. At this time, the Au is converted into an electron-deficient state, and the electrons generated on the BP are rapidly transferred to the Au particles, while the holes on the BP are captured by the sacrificial agent methanol, and the electron-hole pairs are effectively separated in space. When the BP/Au/La2Ti2O7 is excited by near-infrared light, electron-hole pairs will be generated in the electronic States of BP and the interface between BP and Au/La2Ti2O7. Because the electronic state of the interface between BP and Au/La2Ti2O7 is higher than the work function of Au and the valence band position of BP, the photogenerated electrons on BP will migrate to the electronic state of the interface between BPand Au/La2Ti2O7, and then flow into the conduction band of La2Ti2O7 for reduction. To sum up, the loading of noble metals has a good effect on the hydrogen production performance of BP materials.

2.2 Semiconductor/BP

Combining other semiconductor materials with 2D BP nanosheets to form heterojunctions can effectively solve the problem of easy recombination of carriers and enhance the cycle stability of BP[45]. The heterojunctions formed by the semiconductor/BP composite materials include I-type heterojunction, II-type heterojunction, Z-type heterojunction, S-type heterojunction and multi-component heterojunction photocatalysts, wherein the multi-component heterostructure means that two or more heterostructures are contained in the reaction system[46⇓⇓~49].
TiO2 is the most widely studied semiconductor photocatalyst, which has good chemical stability and cost advantages. However, the utilization rate of sunlight is low, and the photocatalytic performance is not good. In order to solve the above problems, it can be combined with the semiconductor with broad spectral response to form a heterojunction, which can broaden the optical absorption range and accelerate the spatial separation of carriers[50]. Elbanna et al. prepared BP/TMC composites by compounding TiO2 mesogens (TMC) with BP. By virtue of the broad-spectrum solar response of BP nanosheets, the composites have good hydrogen production rates under visible light (λ > 420 nm) and near-infrared light (λ > 780 nm), which can reach 950μmol·h-1·g-1 and 205μmol·h-1·g-1, respectively[51]. According to the valence band spectrum and Mott-Schottky spectrum, the conduction band energy levels of BP and TMC are located at 1.06 eV and 0.45 eV, respectively, and the valence band energy levels are located at -0.23 eV and -2.75 eV, respectively. The energy band structure after recombination conforms to the type II heterojunction, as shown in Figure 3A. Under illumination, the electrons on the BP conduction band are transferred to the adjacent TMC conduction band, the holes are captured by the sacrificial agent methanol, and the composite material realizes the effective separation of photogenerated carriers.
Sulfides have attracted much attention in the field of visible-light photocatalytic hydrogen production due to their suitable band gap. However, the rapid recombination of photogenerated carriers and the problem of photocorrosion restrict their development. Qiao et al. compounded two-dimensional BP nanosheets with different sulfides (CdS, ZnS) to form composite photocatalysts, and explored the improvement of the photocatalytic performance of sulfides by BP with different thicknesses[52]. This study pointed out that the few-layer BP nanosheets (thickness of about 4 ~ 5 nm, 5 ~ 6 layers) had a great effect on the hydrogen production rate of sulfides, and when 1 wt% of the few-layer BP nanosheets were loaded on the surface of CdS, the visible light hydrogen production performance was the best, and the hydrogen production rate could reach 11 192μmol·h-1·g-1 with a quantum yield of about 37%. At the same time, the introduction of BP can also improve the stability of sulfide. On this basis, Qiao et al. prepared 0D/2D composite photocatalyst by loading 0D ZnxCd1-xS nanoparticles on BP. The results of X-ray near-edge absorption spectroscopy (XANES) and ultraviolet photoelectron spectroscopy (UPS) showed that the interface of BP/Znx Cd 1 - x S composite had strong interaction, and the photogenerated electron-hole pairs were effectively separated at the interface, thus improving the hydrogen production rate of the material under visible light[53]. Other sulfides such as ZnIn2S4 have also been used to improve the catalytic performance of BP materials[54].
TMDs also have excellent visible light response ability, among which MoS2 is considered to be an ideal semiconductor photocatalyst by virtue of its excellent hydrogen production performance. It has a layered structure similar to BP material, and can form 2D/2D contact with BP to shorten the charge transfer distance and improve the hydrogen production activity. Yuan et al. constructed a 2D/2D heterojunction composite BP/MoS2, and the hydrogen generation rate under visible light can reach 1286μmol·h-1·g-1, which is much higher than Pt/BP(432μmol·h-1·g-1)[55]. In addition, the photocatalytic performance of the 2D/2D composite decreased by only 8% after three cycles, showing good cycle stability. There are two reasons for the improvement of hydrogen production performance: (1) After the combination of BP and MoS2, the photogenerated electrons on BP migrate to the surface of MoS2 under illumination, and react with the adsorbed H+ to form H2; At the same time, the holes in the valence band of BP are captured and consumed by the sacrificial agent, and the photogenerated carriers are effectively separated. (2) Compared with the point-point contact formed between Pt/BP, the tight surface-surface contact formed between BP and MoS2 can greatly shorten the charge transport distance, which is conducive to the rapid separation of photogenerated carriers. In order to further broaden the spectral response range, Reddy et al. compounded BP/MoS2 with 1D CdS nanorods by hydrothermal method. With the excellent light absorption ability and abundant active sites of CdS nanorods, the hydrogen production rate of the ternary composite BP/MoS2/CdS under visible light can reach 183.24 mmol h-1·g-1[18]. In addition, the WS2 has a low work function (5. 57 eV), which is beneficial to the photogenerated charge transfer and hydrogen evolution reaction of BP conduction band. When WS2 was introduced, the hydrogen production rate of the composite BP/WS2 in the near-infrared region was increased by 21 times compared with that of the single BP[56].
In addition to the above common semiconductor materials, bismuth-based materials also have a certain application prospect in the field of photocatalytic hydrogen production due to their good visible light response ability[57⇓~59]. Hu et al. modified Bi2WO6 on the surface of BP nanosheets by hydrothermal method and self-assembly technology to form BP/Bi2WO6 composite materials stacked layer by layer[60]. Due to the excellent light absorption properties of BP materials, the absorption peak intensity of the composites at 400 ~ 800 nm increases with the increase of BP content. When the loading amount of BP reaches 12 wt%, the composite exhibits the best visible light hydrogen evolution performance of about 4208.4μmol·h-1·g-1. The carrier migration path under illumination is shown in Figure 3B. Because Fermi energy level of that BP and the Bi2WO6 are different, a built-in electric field is for on an interface after the BP and the Bi2WO6 are in close contact, the direction of the electric field point from the BP to the Bi2WO6, and under the illumination condition, photo-generated electrons formed by the Bi2WO6 are transfer to the BP under the action of the built-in electric field,And is compounded with holes on a BP valence band, so that electrons with stronger reducibility on a BP conduction band and holes with stronger oxidizability on a Bi2WO6 valence band are reserved, and the hydrogen production driving force of the material is improved while the space separation of photo-generated carriers is realized. On this basis, Zhu et al. Prepared BP/BiVO4 composite materials and realized the photocatalytic-driven water splitting reaction[61]. The hydrogen/oxygen production capacity of the composite under visible light can reach 160/102μmol·h-1·g-1, respectively. The mechanism of hydrogen production is similar to that of BP/Bi2WO6, and the reasonable construction of Z-type heterojunction can improve the carrier recombination problem of photocatalytic materials and enhance their redox ability. In addition, because the BP material itself is a direct band gap semiconductor whose band gap varies with the thickness of the layer, Zhu et al. Composite the bulk BP with BP nanosheets to construct a single-element, noble-metal-free type I semiconductor heterojunction BP/BM (ball-milled BP)[35]. Under visible light irradiation, the hydrogen production rate of the composite BP/BM was about 18 times higher than that of the pure bulk BP, reaching 512μmol·h-1·g-1. Similarly, Liu et al. Synthesized Z-type heterojunction semiconductor BP/RP by one-step wet chemical method using red phosphorus (RP) as raw material. Compared with single BP, the hydrogen production performance and stability of the composite material were improved[62]. To sum up, the construction of semiconductor heterojunction can significantly improve the photocatalytic hydrogen production performance and cycle stability of the material.

2.3 Carbon material/BP

In order to promote the practical application of photocatalytic materials and reduce the use of noble metal materials with low storage and high cost, the research of non-noble metal photocatalytic materials has attracted wide attention. Among them, carbon materials are cheap and abundant, which can greatly promote the industrial application of photocatalytic technology. For example, g-C3N4 is a potential semiconductor photocatalyst due to its ability to respond to visible light, large specific surface area and abundant active sites. Zhu et al. Synthesized 2D/2D BP/g-C3N4 heterojunction materials and applied them to photocatalytic water splitting for hydrogen production, which showed good hydrogen production activity under visible and near-infrared light[63]. The study indicates that the I-type heterojunction formed by the recombination of BP/g-C3N4, the intimate contact of 2D/2D structure and the formation of P — N covalent bond at the interface are beneficial to the capture and separation of photogenerated charges, thus improving the hydrogen production rate and material stability. The hydrogen production mechanism is shown in fig. 4A. In addition, Ran et al. also constructed a 2D/2D BP/g-C3N4 heterojunction, and the XANES characterization and DFT theoretical calculation results showed that the two were recombined through the van der Waals force (Fig. 4B). The formation of the van der Waals force heterojunction is also conducive to the effective migration of photogenerated charges between the g-C3N4 and the BP interface[64]. The mechanism of hydrogen production is shown in Figure 4C. In this two-dimensional composite system, the addition of BP can promote the photogenerated electrons and holes on the g-C3N4 to migrate to the surface of BP, and then reduce and oxidize with H+ and sacrificial agents, respectively. In addition, Zhang et al. skillfully utilized the intercalation effect of volume expansion after liquid freezing, and combined with ultrasonic method to obtain few-layer BP nanosheets under low power[65]. The obtained BP nanosheets could be uniformly dispersed in isopropanol (IPA) solution without aggregation and precipitation.After adding g-C3N4, a large number of precipitates were formed at the bottom of the solution, and the supernatant was gradually clarified, indicating that the BP/g-C3N4 composite was formed. The electrostatic interaction force between BP and g-C3N4 in the BP-IPA-g-C3N4 mixed solution was fully utilized in this composite manner (BP was positively charged and g-C3N4 was negatively charged) to achieve rapid and efficient 2D/2D self-assembly, and the resulting BP/g-C3N4 photocatalyst had a high hydrogen production rate and excellent recyclability.
In order to further improve the photocatalytic performance of the composite, Boppella et al. introduced Ni2P as a co-catalyst to prepare a ternary composite Ni2P@BP/g-C3N4[66]. The unique Ni2P@BP coating structure provides a large contact area, excellent electron transport rate and abundant active sites for the photocatalytic hydrogen production reaction, and can also improve the stability of the composite material. The larger surface area of the two-dimensional Ni2P increases the intimate contact with the BP surface and shortens the charge transport distance, so that the charges can be effectively separated at the interface, thereby improving the hydrogen production activity of the catalyst. Zhu et al. Also constructed a MoS2-BP/GO of ternary composite photocatalytic system, whose light response range covers the visible to near-infrared region, and the hydrogen production rate reaches 8675μmol·h-1·g-1 in this range[67]. In addition, porous g-C3N4 with large surface area and pore structure are also used to prepare BP-g-C3N4 composite materials, which can significantly improve the hydrogen production rate of the catalyst[68]. The application of carbon materials in the field of photocatalytic hydrogen production can significantly reduce the cost of hydrogen production and promote the industrialization of hydrogen production technology.

3 Application of Black Phosphorus-based Nanomaterials in Degradation of Organic Pollutants

A large amount of polluted wastewater is discharged in the process of industrial production, which has a great impact on the water environment. At present, the common treatment methods of water pollution include physical adsorption, electrochemical degradation, biological degradation and so on, but these methods have some problems, such as difficult recovery of adsorbent, easy to cause secondary pollution, high treatment cost, large area and incomplete treatment. Photocatalytic technology can degrade organic pollutants efficiently, simply and at low cost. Under the condition of light, photocatalyst can produce strong oxidative hydroxyl radical (— OH) and singlet oxygen (1O2) and other active substances, which have the ability to degrade organic pollutants in water[69]. In the degradation of organic pollutants, the generation of effective and strong oxidizing active free radicals is the most critical step. However, there are two problems in the application of single BP material in the photocatalytic degradation of organic pollutants: on the one hand, the carriers are easy to recombine and annihilate, resulting in the decrease of the concentration of photogenerated electron-hole pairs in the valence band and conduction band of semiconductors; On the other hand, the position of the energy band does not meet the conditions for the generation of active radicals and cannot drive the subsequent redox reaction. These two reasons inhibit the photocatalytic activity of BP materials. The construction of the heterojunction is beneficial to the effective transmission of carriers, and the electron-hole pair is in a favorable energy band position, so that the photodegradation efficiency is effectively improved. This section summarizes the research progress in the field of degradation of organic pollutants by the photocatalytic system constructed by BP and metal, semiconductor and carbon materials.

3.1 Metal/BP

Similar to the role of metal nanoparticles in the process of hydrogen production, the enhanced light absorption and fast charge transfer make the BP-base composite photocatalyst modified by metal nanoparticles have excellent degradation activity in the field of organic degradation. Lei et al. Used chemical reduction method to grow Ag nanoparticles on the surface of BP to construct Ag/BP plasma composite[40]. Which exhibits enhanced photocatalytic RhB degradation performance under visible light excitation. The photocatalytic enhancement mechanism of the composite mainly includes the following three aspects: firstly, the LSPR effect of noble metal Ag can increase the light absorption intensity of the composite in the visible light region; Secondly, under the irradiation of visible light, the local electric field enhancement phenomenon will occur at the boundary of Ag metal particles (Figure 5A), which promotes the rapid transfer of photogenerated charges generated near the surface of BP to Ag nanoparticles, and reacts with O2 adsorbed on the surface to generate · O 2 -, which degrades organic molecules adsorbed on the surface. Finally, the photogenerated hole is retained on the valence band of BP and also has the ability to degrade RhB.
In addition, the degradation rate of methylene blue in the BP/Ag/TiO2 ternary nanocomposites constructed by Wang et al. Was almost 100% after 80 min of visible light irradiation[70]. UV-Vis absorption spectra showed that the light absorption of the material was enhanced in the range of 500 ~ 600 nm due to the introduction of noble metal Ag nanoparticles.Compared with GO-Ag/TiO2, the solar light absorption range of BP-Ag/TiO2 material almost covered the visible and near-infrared regions. After 85 min of visible light (λ > 420 nm) irradiation, the methylene blue solution with a concentration of 1×10-4mol/L was completely degraded by the BP/Ag/TiO2 material; The degradation rate of methylene blue can also reach 25% under the irradiation of near-infrared light with λ > 780 nm. In addition, Wang et al. Also deposited Ag nanoparticles on the surface of BP by in-situ reduction, and then compounded with GO to form ternary nanocomposites Ag/BP/GO[71]. Under the irradiation of visible light, the Ag nanoparticles quickly capture photogenerated electrons to realize the effective separation of photogenerated carriers; At the same time, the electrons and the O2 adsorbed on the surface of the material are reduced to form a O 2 - with strong oxidizability, which can effectively degrade methylene blue. In this ternary material, the introduction of GO as the substrate material not only makes the distribution of Ag/BP uniform, but also improves the stability of the composite. Therefore, the LSPR effect and high conductivity of noble metals can significantly improve the visible light degradation ability of BP materials for organic pollutants.

3.2 Semiconductor/BP

The construction of semiconductor heterojunction can control the energy band structure of the composite material, so that the photogenerated electrons and holes can be quickly separated, thereby achieving efficient degradation of pollutants. Shen et al. Used the in-situ growth method to grow BP nanoparticles on the surface of red phosphorus (RP) to obtain the RP/BP single-element composite, which has an enhanced absorption peak in the visible light region of 600-800 nm[72]. After visible light (λ > 420 nm) irradiation for 30 min, the degradation rate of RhB can reach 89%, which is twice as high as that of pure BP material, and the degradation mechanism is shown in Fig. 5B. Because the conduction band position of RP is higher than that of BP, and BP has excellent carrier mobility, the photogenerated charge on the conduction band of RP flows into the conduction band of BP under illumination. At the same time, the holes on the valence band of RP react with the adsorbed water molecules to produce strong oxidizing · OH, thus realizing the effective degradation of RhB. The composite material also has a great cost advantage, which provides a guiding direction for the development of non-metallic semiconductor composite materials. However, the single BP material will be oxidized in the air and water environment, resulting in poor stability in the degradation of pollutants and affecting the cycle life of the material. Liu et al. Supported TiO2 with good stability on the surface of BP and obtained a composite photocatalyst with excellent cycle performance[73]. Due to the formation of 2D/2D structure between TiO2 nanosheets and BP (Figure 5C), the degradation rate of RhB reached 98% after 120 min of reaction with RhB under UV-visible light, and the degradation rate could still be maintained at 92.5% after three cycle experiments.
In order to achieve efficient degradation of organic pollutants in the visible light region, Shao et al. Further introduced MXene materials to synthesize ternary BP/TiO2/MXene composites[74]. Due to the lower Fermi level, good conductivity and excellent visible light absorption ability of MXene materials, the photogenerated electrons on BP first transfer to the surface of TiO2 under visible light, and then migrate to MXene. Finally, the photogenerated electrons react with the O2 adsorbed on the surface of MXene to form · O 2 -, which degrades the pollutants into CO2, H2O and other small molecules. The reaction mechanism is shown in Figure 5d. In addition, BiOBr is a layered material with a low valence band position (2. 53 eV), which can efficiently degrade organic pollutants in water. Li et al. Synthesized BiOBr/BP composites by self-assembly, which had excellent tetracycline removal ability[76].
Materials with porous structure are also used to composite with BP, and their excellent pore structure can be used to improve the adsorption performance of reactants, thereby improving the degradation efficiency. ZIF-8 is a kind of metal organic framework (MOF) material with high density of pore structure, adjustable pore size and large specific surface area, which has strong organic adsorption ability. Wang et al. Prepared ZIF/BP nanocomposites by in-situ growth of ZIF-8 on the surface of BP (Fig. 5e)[75]. The degradation rate of RhB can reach 90% after 60 min of UV irradiation, and the degradation rate constant is 4.49×10-2min-1. Compared with BP, the degradation performance of organic pollutants was significantly improved. The theoretical calculation results show that the highest occupied molecular orbital (HOMO) and lowest unoccupied molecular orbital (LUMO) of ZIF-8 are 1. 9 eV and -3. 6 eV, respectively. Under illumination, the electrons at the LUMO position of ZIF-8 will be rapidly transferred to the conduction band of BP, and the holes on the HOMO will be effectively retained and transferred to the surface to degrade the adsorbed pollutants. This study provides a new research idea for improving the performance of photocatalytic materials and broadens the selection range of composite materials.

3.3 Carbon/BP composites

It is of great significance to find the earth's abundant and low-cost photocatalysts for environmental governance, and the research of non-metallic photocatalytic composites has gradually become a new trend. Therefore, high-conductivity and low-cost carbon materials such as g-C3N4, RGO and C60 exhibit great application advantages and prospects. In view of this, Wen et al. Prepared metal-free composite BP/g-C3N4, which exhibited excellent RhB degradation ability[77]. Under illumination, the electrons on the conduction band of BP react with the O2 adsorbed on the surface of the material to form a O 2 -, which can quickly oxidize RhB molecules in the solution and completely degrade them after 25 min of illumination. Ge et al. coated RGO on the surface of BP by combining freeze-drying and ultrasonic self-assembly methods to form an RGO/BP/RGO coated structure (Figure 6a)[78]. Relying on the good stability of RGO, the composite has good cycle stability (Fig. 6 B, C). At the same time, due to the high conductivity of RGO, the photogenerated electrons on BP can be quickly transferred to the surface of RGO, which promotes the effective separation of photogenerated electron-hole pairs on BP and greatly improves the photodegradation rate.
However, it is still challenging to adjust the structure of BP at the atomic scale and improve its degradation activity. The C60 is a very stable molecular material of the "carbon family". Zhu et al. selectively anchored the C60 at the edge of the BP nanosheet (Fig. 6d). This structure can play a very good role in protecting the BP nanosheet, so that the BP has a very good stability in the photocatalytic process[79]. Moreover, the anchoring of C60 also makes the conduction band position of BP/C60 more negative, which is easier for the generation of · O 2 - radicals. Meanwhile, C60 has the similar effect with GO, which is beneficial to the separation of photogenerated carriers on the composite, and the degradation mechanism is shown in Fig. 6e. The photocurrent density test confirmed that after the modification of C60, the photocurrent density of the material was about ten times higher than that of BP nanosheets, and the degradation rate constant reached 6.70 h-1 under visible light irradiation. In addition to the above carbon materials, other non-metallic materials, such as covalent triazine skeleton polymers, also have good visible light degradation ability of RhB after being compounded with BP[80]. Compared with metal materials, carbon materials and non-metallic materials have rich structures, which can obtain BP-base composite materials with multi-dimensional structure, improve the adsorption capacity of organic pollutants, and thus obtain composite photocatalysts with low cost and high degradation performance.

4 Application of black phosphorus-based nanomaterials in CO2 reduction and nitrogen fixation

BP-based photocatalytic materials also have a certain application prospect in CO2 reduction and nitrogen fixation. Through photocatalytic technology, BP-based composites can convert CO2 and N2 into high value-added chemicals. Zhu et al. Obtained a stable monolayer BP (M-BP-OH) with hydroxyl group modification in situ by liquid nitrogen-assisted stripping method[81]. Upon visible light irradiation, this monolayer BP nanosheet (with a thickness of about 0.62 nm) exhibits a CO generation rate of up to 112.6μmol·h-1·g-1. VB and Tauc patterns show that the band gap of M-BP-OH is 2. 2 eV, and the top of valence band (VBM) and the bottom of conduction band (CBM) are located at -2. 85 eV and -5. 05 eV, respectively, which meets the requirement of CO2/CO reduction potential. The surface photovoltage (SPV) and photoluminescence (PL) results showed that M-BP-OH had a strong absorption peak at 300 ~ 500 nm due to interband transition, and the PL intensity was weaker than that of bulk BP, indicating that M-BP-OH had a more efficient photogenerated charge separation. The CO2 reduction process comprises the following three steps: (1) photogenerated electrons react with CO2 molecules adsorbed on the surface of a material to generate CO 2 -;(2) CO 2 - interacts with protons to generate an intermediate product COOH*;(3) the intermediate product COOH* is reduced to CO. At this time, the combination of — OH and the lone pair electrons on the surface of BP can prevent the oxidation reaction of monolayer BP with oxygen and improve the chemical stability of the material. g-C3N4 also has excellent CO2 adsorption and reduction ability because of its unique two-dimensional structure[82]. Zhang et al. studied the CO2 reduction process of BP/g-C3N4 by theoretical calculations, and DFT calculations showed that the complex was a S-type heterojunction[83]. However, due to the different Fermi levels of the two materials, band bending occurs at the interface and a built-in electric field is formed. Under this action, the photogenerated electrons on BP flow into the g-C3N4 from the conduction band of BP and recombine with the holes on the valence band of BP, so that the holes on the valence band of BP and the electrons on the conduction band of g-C3N4 are retained. Because that conduction band position of the g-C3N4 satisfy the reduction condition of the CO2, the final CO2 can be reduced to the CH3OH:CO2→COOH*→HCOOH→HCO*→H2CO→CH2OH*→CH3OH through the follow steps. The reaction mechanism is shown in Figure 7A.
Perovskite materials have many advantages, such as stable crystal structure, adjustable photoresponse ability, high photoluminescence rate and high carrier mobility, which make it a very potential new photocatalytic material. Wang et al. Dispersed perovskite nanocrystalline CsPbBr3 on the surface of two-dimensional BP nanosheets by self-assembly[84]. Compared with the original CsPbBr3, the introduction of BP provides more active sites, which can promote the activation of CO2 and increase the production rate of CO2. Under photoexcitation, the electrons of the CsPbBr3 can be rapidly transferred to BP through the Pb-P bond at the interface, which suppresses the recombination quenching of electron-hole pairs. At the same time, the formation of Pb-P bond is also helpful to improve the stability of the material. To sum up, photocatalytic technology has great application advantages in the reduction of CO2, which can not only alleviate global warming to a certain extent, but also generate a series of carbonaceous fuels to cope with the worsening energy crisis through clean and pollution-free light-chemical energy conversion process.
Ammonia is a very important chemical substance for agricultural production. The Haber ammonia process used in industrial production has harsh reaction conditions and huge energy consumption, so it is very important to find a green and energy-saving ammonia synthesis method. Photocatalytic nitrogen fixation technology has attracted wide attention in the field of ammonia synthesis because of its advantages of low cost and no pollution[85]. The theoretical calculation shows that the edge position of BP nanosheets can become the adsorption center of N2. Based on this, Bian et al. prepared BP nanosheets (eBP) with "polycrystal-like structure" with rich edges, as shown in Fig. 7B[86][87]. This "polycrystal-like structure" exposes more unsaturated sites, which is beneficial to the adsorption of N2 molecules and the occurrence of nitrogen fixation. According to XPS analysis, the valence band and conduction band of eBP are located at 0. 5 eV and -1. 0 eV, respectively, and the nitrogen fixation reaction can occur (the reduction potential of N2 is -0. 092 eV). Under the excitation of visible light, electron-hole pairs were generated on eBP, and the photogenerated electrons were captured by the N2 adsorbed on the surface for nitrogen fixation, while the holes were consumed by the SO 3 2 - /S2- in the solution (as shown in Figure 7c), and the material showed efficient nitrogen fixation performance.
In addition, the two-dimensional BP/g-C3N4 composite synthesized by Qiu et al. Has excellent nitrogen fixation performance without adding a sacrificial agent, and the nitrogen fixation rate can reach 337.2μmol·h-1·g-1 under visible light conditions. The enhanced nitrogen fixation ability of the composite is mainly due to the following three reasons: (1) the C — P covalent bond formed between BP and g-C3N4 can accelerate electron transfer and improve the separation efficiency of carriers[88]; (2) The formation of C — P bond leads to the rearrangement of electrons on the neighboring P and C atoms in BP and g-C3N4, so that the multi-electron P atom acts as an electron donor in the photocatalyst; (3) The existence of C-P bond changes the stable π-conjugated system in the g-C3N4, which is more conducive to the excitation of electrons in the photocatalyst. After Shen et al compounded BP with CdS, the nitrogen fixation rate was increased by about 3.69 times compared with that of CdS alone, and the stability of the material was also improved[89]. The reaction mechanism is shown in Figure 7d. Under visible light, the photogenerated electrons on CdS are transferred to the conduction band of BP, and NH3 can be generated on BP because the position of the conduction band of BP is lower than the reduction potential of the N2/NH3. At the same time, the holes in the valence band of CdS react with methanol to form HCHO.
In addition to the above photocatalytic reactions, the two-dimensional BP-nanocomposites also have certain application value in antibacterial, antibiotic treatment and seawater treatment[90][91][92].

5 Conclusion and prospect

Due to its special layered structure, excellent photoresponse ability, tunable energy band structure and ultrahigh carrier mobility, two-dimensional BP nanomaterials have been widely used in photocatalytic water splitting, degradation of organic pollutants, reduction of CO2, nitrogen fixation and other fields. By means of compounding the two-dimensional BP material with metal, semiconductor and carbon materials, on the one hand, the separation efficiency of photogenerated electron-hole pairs can be effectively improved; On the other hand, it can also enhance the light absorption performance of the material and improve the stability of the photocatalyst. Noble metal nanoparticles, due to their low overpotential, are easy to accept electrons generated by semiconductors and accelerate the reduction of H+, which can greatly improve the hydrogen production performance of BP materials. Carbon materials are one of the ideal cocatalysts because of their ultra-high electrical conductivity, special crystal structure and abundant reserves in the earth. In addition, there are many kinds of semiconductor materials, which can provide more choices for BP-based composites. By constructing different kinds of semiconductor heterojunctions (type Ⅰ, type Ⅱ, type Z, and type S), the band structure of the composite can be adjusted and the redox driving force can be improved. At present, the two-dimensional BP composite material has a certain theoretical basis in the field of photocatalysis, but it still faces great challenges.
First of all, the preparation methods of 2D BP nanosheets are divided into top-down and bottom-up methods. From top to bottom, it mainly includes mechanical stripping, liquid phase stripping and electrochemical stripping. Bottom-up include chemical vapor deposition (CVD) or wet chemical methods, etc. The peeling method has the advantages of simple operation, low manufacturing cost and large yield. However, the size and thickness of the obtained nanosheets are uncontrollable, and BP is prone to oxidation during the exfoliation process. In contrast, the CVD method can precisely control the thickness of BP nanosheets, but the yield is lower and the cost is higher. By combining various preparation methods, it is expected to realize the large-scale preparation of 2D BP nanosheets with uniform thickness and size.
Secondly, combined with advanced preparation methods (such as atomic layer deposition) and characterization methods (such as spherical aberration correction scanning transmission electron microscopy and synchrotron radiation), the structure optimization, defect structure, atom doping and heterojunction construction of BP materials can be realized on the atomic and molecular scale, and the efficient photocatalyst with good stability can be obtained accurately.
Finally, by means of in-situ testing and theoretical simulation, it is helpful to explore the structural change of photocatalytic materials and the micro-kinetic process in the catalytic reaction, and the in-depth study of photocatalytic mechanism provides a way to design a reasonable catalyst structure.
In this review, the recent progress in the application of different materials in the field of photocatalysis was summarized, and some composite methods and modification mechanisms were briefly introduced, hoping to provide some new inspiration for researchers to develop low-cost, efficient and stable photocatalysts as soon as possible.

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Funding

National Natural Science Foundation of China(51902243)

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