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Construction of Magnetic NiFe2O4-Based Composite Materials and Their Applications in Photocatalysis

Xiaowei Li , Lei Zhang , Qixin Xing , Jinyu Zan , Jin Zhou , Shuping Zhuo

Progress in Chemistry ›› 2022, Vol. 34 ›› Issue (4) : 950 -962.

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Progress in Chemistry ›› 2022, Vol. 34 ›› Issue (4) : 950-962 DOI: 10.7536/PC210442
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Construction of Magnetic NiFe2O4-Based Composite Materials and Their Applications in Photocatalysis
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Abstract

Environmental pollution and energy shortage caused by the rapid development of the economy have become two major problems in modern society. Accordingly, much research is currently focused on the exploitation of new alternative energy sources. Among various energy sources, solar energy is considered to be ideal and renewable energy. Under sunlight irradiation, photocatalysis, as a novel “green technology”, can directly convert organic pollutants into innoxious substances to solve both energy crisis and environmental pollution. However, the key to the success of this process is dependent on the rational design and fabrication of efficient photocatalysts. The NiFe2O4 possessing fast magnetism response and good photochemistry stability, is coupled with other semiconductor photocatalysts having a suited band gap in order to obtain greatly effective photocatalytic systems and achieve the magnetic separation, exhibiting wide application foreground. This paper mainly reviews the latest research progress on the synthesis and photocatalytic application of NiFe2O4-based composites, which may open a new avenue and idea for preparing highly active and magnetically separable composite photocatalysts. Finally, the future development of NiFe2O4-based photocatalytic materials is also prospected.

Contents

1 Introduction

2 NiFe2O4/carbon materials

2.1 NiFe2O4/graphene

2.2 NiFe2O4/g-C3N4

2.3 NiFe2O4/other carbon materials

3 NiFe2O4/Bismuth-based compounds

3.1 NiFe2O4/BiOX

3.2 NiFe2O4/Aurivillius Bismuth-based oxide

3.3 NiFe2O4/other Bismuth-based compounds

4 NiFe2O4/Silver-based compounds

4.1 NiFe2O4/Ag3PO4

4.2 NiFe2O4/AgX

5 NiFe2O4/TiO2

6 NiFe2O4/ZnO

7 Conclusion and outlook

Graphical abstract

Keywords

NiFe2O4 / magnetic / composites / photocatalysis

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Xiaowei Li, Lei Zhang, Qixin Xing, Jinyu Zan, Jin Zhou, Shuping Zhuo. Construction of Magnetic NiFe2O4-Based Composite Materials and Their Applications in Photocatalysis. Progress in Chemistry, 2022, 34(4): 950-962 DOI:10.7536/PC210442

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1 Introduction

In recent years, the rapid development of industry and economy has led to the increasingly serious problems of energy shortage and environmental pollution, so the development of new sustainable supply of clean energy is imminent. As a pollution-free and sustainable energy, solar energy radiates to the earth's surface every day 200 times the total energy consumed by all mankind in a year, and is recognized as one of the most potential clean energy sources. Semiconductor photocatalytic technology driven by solar energy can directly use solar energy to degrade pollutants in the environment into harmless substances, thus effectively solving the above two problems[1⇓⇓⇓⇓⇓⇓⇓⇓~10]. However, the core and key of photocatalytic technology lies in the design of photocatalyst. Since Fujishima and Honda reported the first report of hydrogen production from water photolysis of TiO2 single crystal in 1972, the development and study of new efficient and inexpensive semiconductor photocatalysts have attracted worldwide attention[11]. At present, researchers at home and abroad have done a lot of work in the exploration, synthesis and photocatalytic performance of photocatalytic materials, and have successfully developed a series of efficient and stable photocatalytic systems. Although these photocatalytic systems have achieved high activity, there are still many shortcomings, such as the difficulty of separation and recovery in the process of degrading organic pollutants, which leads to high economic costs and environmental pollution, thus seriously limiting their large-scale industrial application. Based on this, magnetic materials are used as carriers to compound with band-matched photocatalysts, which can not only realize the magnetic separation and recovery of photocatalysts, but also improve the utilization rate of photocatalysts in the recycling process, thus providing the possibility for the practical application of photocatalytic technology.
With the development of nanoscience and nanotechnology, a variety of new materials are coming out. Among them, nickel ferrite (NiFe2O4), as a spinel ferrite magnetic material, has attracted much attention because of its large specific surface area, unique magnetic separation characteristics and good photocatalytic activity[12⇓⇓⇓⇓⇓⇓⇓⇓⇓⇓~23]. When it is compounded with a semiconductor photocatalyst with a suitable band gap, it realizes the magnetic separation of the photocatalyst and shows excellent photocatalytic effect, so it shows potential application value and extremely broad market prospects in the field of photocatalysis. However, at present, there are many reports on NiFe2O4-based composite photocatalytic materials, but there are few reports on their design, synthesis and photocatalytic applications. So,In this paper, NiFe2O4 matrix composites (NiFe2O4/ carbon materials, NiFe2O4/Bi,Recent advances in the synthesis of NiFe2O4/Ag series, NiFe2O4/TiO2 and NiFe2O4/ZnO) and their photocatalytic applications,This will provide a good reference for the development and application of new efficient magnetic composite photocatalytic materials.

2 NiFe2O4/ carbon material

2.1 NiFe2O4/ graphene

Graphene and its composites are one of the most popular international frontiers. In 2010, two scientists, Geim and Novoselov, won the Nobel Prize in Physics for their outstanding contributions to graphene. At present, this research achievement has been widely used in the world. Graphene, as a new type of carbon material with two-dimensional planar structure, has the characteristics of large specific surface area, abundant surface functional groups, unique physical and chemical properties, good thermal stability and chemical stability, which is not only easy to be functionalized, but also can be used as a carrier to support or disperse a variety of photocatalytic materials. So far, many experts and scholars have conducted systematic and in-depth research on the preparation and application of graphene and its composite materials, but there are relatively few reports on the composite of NiFe2O4 and graphene for photocatalytic degradation, which are mainly concentrated in the work of the following groups.
In 2018, Liang et al. Successfully loaded NiFe2O4 nanoparticles with a particle size of about 11 nm on the surface of reduced graphene oxide (RGO) using a simple mechanical ball milling method to prepare composite NiFe2O4-RGO[24]. Further study found that when the content of graphene was 0.35, the activity of the composite was the best, and the simulated pollutant methylene blue (MB) could be degraded by 99.1% under visible light irradiation for 180 min. Such a high degradation efficiency was mainly due to the introduction of graphene, which accelerated the migration rate of photogenerated electrons and improved the separation efficiency of photogenerated carriers. The photocatalytic mechanism is shown in Figure 1. The cycle test showed that the NiFe2O4-RGO could be separated from the reaction system rapidly under the action of the external magnetic field after the reaction, and could be reused after pretreatment.The photocatalytic activity of the composite material did not decrease significantly after three times of use, which showed that the composite material had good stability. In addition, the synthesis method is simple and easy, and does not need to use organic solvents and toxic reducing agents. Therefore, this research work not only provides a new way to construct a new type of graphene-based composite photocatalyst with high efficiency and magnetic separation, but also provides an experimental basis for the application of ball milling method in industrial production.
In 2021, Bayantong et al. Used graphene oxide (GO) as substrate, nickel nitrate hexahydrate and ferric nitrate nonahydrate as nickel source and iron source, and successfully constructed a foam-type composite photocatalytic material NiFe2O4@GO under mild conditions by combustion method, which was used to degrade MB aqueous solution. The results showed that, compared with NiFe2O4 monomer,The composite has higher activity NiFe2O4@GO, and methylene blue can be almost completely decolorized under UV irradiation for 120 min when the dosage of the composite is 0. 5 G/L and the concentration of methylene blue solution is 0. 04 mmol/L, which is mainly due to the good conductivity of graphene oxide, which effectively improves the photocatalytic activity of the composite[25]. Otherwise, quenching experiments confirmed that photogenerated holes (h+) and hydroxyl radicals (· OH) were the main active species in the degradation process. The disadvantage of this study is that NiFe2O4@GO is a UV-driven photocatalyst, which can not make full use of visible light in the solar spectrum, which seriously restricts the promotion and application of NiFe2O4@GO.

2.2 NiFe2O4/g-C3N4

Graphite-like carbon nitride (g-C3N4) is the most stable allotrope of carbon nitride, with a graphite-like layered structure. As an inorganic non-metallic semiconductor material, the band gap of g-C3N4 is about 2.7 eV.Because of its simple preparation method, chemical stability, unique electronic structure and response to visible light, it has become a hot research topic in the field of photocatalysis and has shown great potential in photocatalytic applications[26⇓⇓⇓⇓⇓~32]. However, g-C3N4still have some limitations in photocatalytic reaction, such as high recombination rate of photogenerated electron-hole pairs, low quantum yield and difficulty in recycling, which lead to unsatisfactory photocatalytic activity and low recycling rate of photocatalyst. Therefore, scientists have done a lot of research on the modification of g-C3N4. In 2018, based on the principle of band matching, Zheng et al. Coupled two semiconductors, NiFe2O4 and g-C3N4, to prepare a heterostructured composite photocatalytic system NiFe2O4/g-C3N4[33]. Compared with the single-component NiFe2O4 and g-C3N4, the photocatalytic performance of the obtained composite NiFe2O4/g-C3N4 is greatly improved, which is attributed to the energy level difference between them, which enhances the absorption of the composite to visible light and promotes the separation of photogenerated charges. As can be seen from the above, the coupling of heterogeneous semiconductor materials is an effective way to break through the properties of a single material. Generally speaking, three factors should be considered to construct an ideal heterointerface: (1) band matching; (2) intimate interfacial contact; (3) The effective interface is large.
Mani et al. Deposited NiFe2O4 nanoparticles on the surface of g-C3N4 by sol-gel method and high temperature calcination method to prepare nanocomposite NiFe2O4-g-C3N4, which was successfully used for the degradation of rhodamine B (RhB) and MB.The results show that the compact heterointerface structure formed between the NiFe2O4 and the g-C3N4 effectively promotes the charge transfer, inhibits the recombination of photogenerated electrons and holes, and improves the photocatalytic activity of the composite material[34]. The material showed high activity for RhB and MB under both visible and solar light. Interestingly, compared with visible light, the composite has superior activity under direct sunlight irradiation, which can degrade 99% of RhB and MB in 225 min. For RhB, the degradation rate of composite is 13 times of monomer NiFe2O4 and 1.6 times of C3N4, while for MB, the degradation rate is 33 times of monomer NiFe2O4 and 12 times of C3N4. The possible reason for this phenomenon is that under sunlight, the reaction temperature (30 ~ 35 ℃) is conducive to the decomposition of hydrogen peroxide to produce more decisive active species hydroxyl radical · OH, which reacts with dye molecules to degrade them into pollution-free small molecules such as carbon dioxide and water.
Gebreslassie et al. Prepared the composite photocatalyst g-C3N4/NiFe2O4 by a one-pot hydrothermal method and proposed the degradation mechanism of methyl orange (MO) (Fig. 2)[35]. According to the experimental results, they attributed the enhancement of photocatalytic activity to the formation of a Z-shaped mechanism between the two, in which NiFe2O4 and g-C3N4 are simultaneously excited to produce electrons and holes under visible light irradiation.Under the action of an internal electric field, electrons in the conduction band of the NiFe2O4 are transferred and combined with holes in the valence band of the g-C3N4, so that the electrons and the holes are respectively gathered in the conduction band and the valence band of the g-C3N4,At this time, the accumulated electrons react with the adsorbed O2 on the surface of the catalyst to produce superoxide radicals (·O2-), while the holes can directly participate in the oxidation reaction or oxidize H2O to · OH for the oxidative decomposition of MO. In addition, the research group also studied the recycling performance of g-C3N4/NiFe2O4, and found that the degradation efficiency decreased by 3.6% after three times of recycling.
Chen et al. Also prepared g-C3N4/NiFe2O4 by compounding NiFe2O4 and g-C3N4, and inhibited the recombination of photogenerated electron-hole pairs by using the different valence band positions of the two, which significantly improved the degradation efficiency of MB[36]. When the content of NiFe2O4 was 12%, the activity was the best, and the degradation rate of methylene blue could reach 100% under visible light irradiation for 75 min, which was 7 times higher than that of monomer g-C3N4. The difference between this study and other reports is that there is no need to add hydrogen peroxide in the photocatalytic reaction.
Element doping is an important means to change the energy band structure of semiconductors.Doping a small amount of metal or non-metal elements into g-C3N4 can effectively change the energy band structure of g-C3N4, and improve its absorption of visible light and photocatalytic performance. For example, Kamal et al. First prepared B-doped g-C3N4(BCN) by thermal polycondensation using dicyandiamide and boric acid as precursors, and then compounded with NiFe2O4 to obtain composite BCN/NiFe2O4, which achieved efficient degradation of MB under visible light[37]. The cycle test showed that the degradation rate of BCN/NiFe2O4 decreased from 97. 68% to 95. 99% after three times of use, which showed the good stability of photocatalyst. Parida's group also carried out similar research work, and P-doped g-C3N4(P-CN) was prepared by calcining melamine and ammonium dihydrogen phosphate at 520 ℃ for 2 H, and then coupled with NiFe2O4 to construct Z-type NiFe2O4@P-CN photocatalyst. When the loading of NiFe2O4 was 20%, it showed high activity in the photocatalytic oxidation of phenol and visible light photocatalytic hydrogen production, and the hydrogen production rate was as high as 904μmol·h-1[38].
Graphene has also been used to modify g-C3N4 due to its good conductivity and excellent electron transfer ability. At present, there are many studies on the preparation of composite photocatalytic materials by using graphene to modify g-C3N4, but there are few reports on the construction of photocatalysts by using graphene and magnetic NiFe2O4. In 2019, the Gebreslassie team developed a new and efficient all-solid-state Z-type ternary composite photocatalytic system g-C3N4/graphene/NiFe2O4, whose photocatalytic mechanism is shown in Figure 3, in which graphene, as an electron mediator, inhibits the recombination of electrons and holes on the one hand, and on the other hand, retains the strong reducibility of conduction band electrons of g-C3N4 and valence band holes of NiFe2O4.Electrons in the conduction band of g-C3N4 reduce O2 to ·O2-,NiFe2O4 holes in the valence band oxidize water to ·OH,·O2- and · OH as active species to participate in MO degradation, and the composite system with the optimal ratio can completely degrade MO in 120 min under visible light irradiation, thus showing a strong application prospect in the field of photocatalysis[39].

2.3 NiFe2O4/ other types of carbon materials

It can be seen from the above introduction that the photocatalyst prepared by using graphene and graphite-like carbon nitride as substrates and NiFe2O4 can effectively degrade various dyes. At present, except for graphene and graphite-like carbon nitride, there are only a few reports on the photocatalytic degradation of other types of carbon materials composite NiFe2O4. For example, Chen's research group first synthesized ammonium polyacrylate nanospheres containing Fe2+ and Ni2+ by using polyacrylic acid nanospheres as a hard template, and then obtained the NiFe2O4/C composite material as shown in Fig. 4 after removing the template by hydrolysis and calcination. It can be seen from the figure that the NiFe2O4/C is a spherical structure with uniform size (diameter 200 – 400 nm), and the sphere has both an inner core and an outer shell[40]. The photocatalytic degradation of tetracycline hydrochloride (TC) by NiFe2O4/C under visible light irradiation showed that the photocatalytic performance of NiFe2O4/C was significantly better than that of monomer.Surprisingly, the photocatalytic performance of NiFe2O4/C was significantly improved by introducing a small amount of hydrogen peroxide into the reaction system, and the degradation rate was 97. 25% after 60 min of irradiation, and the degradation rate could still reach more than 90% after 5 times of reuse. The reason is that the core-shell structure of NiFe2O4/C has stronger visible light absorption ability, larger specific surface area (72.23 m2/g) and more exposed active sites relative to NiFe2O4, which is beneficial to mass transfer and nucleus transfer. It can be seen that the synergistic effect of the above factors plays a vital role in the improvement of photocatalytic activity.
In 2020, Nawaz et al. Introduced multi-walled carbon nanotubes (MWCNT) into NiFe2O4 through a simple hydrothermal reaction to obtain 10% -50% NiFe2O4-MWCNT composites with different mass ratios[41]. It was found that the composite containing 25% (mass fraction) MWCNT exhibited 38% higher photocatalytic degradation of sulfamethoxazole than that of NiFe2O4 under optimized conditions, which was mainly due to the fact that the interaction between NiFe2O4 and MWCNT accelerated the transfer of photogenerated electrons and inhibited the recombination of electron-hole pairs, resulting in a significant increase in photodegradation efficiency. Unfortunately, the stability of the NiFe2O4-MWCNT was poor, and the degradation rate decreased by 20% after 5 cycles, which may be due to the loss of metallic iron during the degradation process.
From the above introduction, it can be seen that although the photocatalytic materials prepared by NiFe2O4 and carbon materials can effectively degrade various organic dyes and pollutants (Table 1), with the development of social economy and the deepening of research, people have higher and higher requirements for photocatalytic materials.Therefore, it is still a challenging task to select cheap raw materials to synthesize NiFe2O4-based composite photocatalytic materials with novel structure, excellent photocatalytic activity and recycling performance, and researchers still need to continue their efforts.

3 NiFe2O4/Bi compound

3.1 NiFe2O4/BiOX

Bismuth-based compounds are a hot topic in the field of photocatalysis because of their unique structure and excellent light absorption ability[42⇓⇓⇓~46]. Bismuth oxyhalide (BiOX, X = Cl, Br, I), as a narrow band gap semiconductor, has become an ideal photocatalyst because of its special electronic structure, good optical properties and catalytic properties[47⇓⇓~50]. However, BiOX has some problems, such as low quantum yield, band gap mismatch with solar spectrum, easy recombination of photogenerated carriers and difficult separation of catalysts. Therefore, researchers have modified or modified BiOX by various means, such as morphology control, element doping, dye sensitization and semiconductor recombination, to obtain high-performance photocatalysts with visible light response. Among them, the composite of NiFe2O4 and BiOX can not only improve the photocatalytic activity of BiOX, but also realize the magnetic separation of photocatalyst, which provides a good theoretical support for the degradation of pollutants and the treatment of sewage. In 2016, Lv et al. Prepared the heterojunction photocatalyst NiFe2O4/BiOBr by calcination method, and the degradation ability of RhB after compounding was increased by two times compared with pure BiOBr[51]. This is due to the formation of heterojunction between NiFe2O4 and BiOBr, which on the one hand enhances the absorption of NiFe2O4/BiOBr in the visible region and on the other hand suppresses the recombination of photogenerated carriers. The cycle test showed that the NiFe2O4/BiOBr had good stability, and the activity did not decrease significantly after 6 cycles. In the same year, the hybrid material formed by the combination of NiFe2O4 and BiOBr by chemical adsorption method in Xu's group also showed good catalytic activity in the experiment of RhB degradation under visible light[52].
Our research group has also carried out related work on the construction and photocatalytic application of NiFe2O4/BiOBr composites, such as the preparation of NiFe2O4/BiOBr composites by simple hydrothermal reaction, and the TEM photos are shown in Figure 5[53]. It can be seen from the figure that the NiFe2O4 nanorods with a length of about 300 nm are uniformly dispersed on the surface of the BiOBr nanosheets, and a "face-rod" contact mode is formed between them. The photodegradation of MB showed that the activity of the composite increased first and then decreased with the increase of NiFe2O4, and the optimal activity was obtained when the doping amount was 20%.The degradation rate of MB was 90% under visible light irradiation for 60 min, which was 22. 4 times and 3. 2 times higher than that of single phase NiFe2O4 and BiOBr, respectively. On this basis, we also prepared NiFe2O4 nanoparticles with a particle size of 20 – 40 nm by changing the raw materials and experimental conditions, and coupled them with BiOBr nanosheets to obtain NiFe2O4/BiOBr composite materials with different morphologies, and the TEM images are shown in Fig. 6[54]. When the proportion of NiFe2O4 is 10%, the degradation ability is the strongest, and the removal rate of RhB is 95% under visible light irradiation for 15 min. The reason for the improved photodegradability of the two different morphologies of NiFe2O4/BiOBr may be that :(1)NiFe2O4 and BiOBr have matching valence and conduction bands; (2) The flat exposed surface of BiOBr nanosheets forms strong "face-rod" and "face-point" interface contact with NiFe2O4 nanorods or nanoparticles; (3) The formation of heterojunction between them is beneficial to the transfer and separation of photogenerated charges.
In addition to BiOBr, the composite NiFe2O4/Bi24O31Br10 formed by coupling the photocatalyst Bi24O31Br10 composed of Bi, O, and Br with NiFe2O4 has also been reported. In this report, Xia et al. Analyzed the morphology and structure of NiFe2O4/Bi24O31Br10 and the reasons for the improvement of photocatalytic performance by means of XRD, SEM, XPS, UV-vis DRS, and photoluminescence spectroscopy (PL)[55]. The results showed that the NiFe2O4 nanoparticles were deposited on the Bi24O31Br10, and the degradation of crystal violet (CV) by the composite was better than that by the pure phase material.The degradation effect was the best when the content of NiFe2O4 in the composite was 20%, and the activity decreased when the content of NiFe2O4 continued to increase, because the NiFe2O4 with low activity occupied part of the active sites. NiFe2O4/Bi24O31Br10 also has strong photostability and reusability, and its activity remains basically unchanged after five times of reuse. In addition, they also proposed the reaction mechanism of CV degradation of the composite under visible light. According to the experimental results, the improvement of photocatalytic activity was attributed to the effective transfer and separation of photogenerated electron-hole pairs, which was also confirmed by PL spectra.
The research group also developed a novel flower-like NiFe2O4/BiOI composite material with ferric chloride, nickel chloride, bismuth nitrate and potassium iodide as precursors under solvothermal conditions, and investigated the degradation effect of NiFe2O4/BiOI on RhB, MB and CV dyes with xenon lamp as light source.It was found that when the doping amount of NiFe2O4 was 15%, the dosage of the complex was 100 mg, and the concentration of the dye aqueous solution was 20 mg/L, the NiFe2O4/BiOI showed excellent decomposition effect on the three dyes, and the energy band structure and possible charge transfer path were shown in Figure 7[56]. Jiang et al. Also developed a photocatalyst NiFe2O4/BiOI with similar structure and high efficiency for MO degradation under hydrothermal conditions, and revealed that photogenerated holes were the main active species in the degradation process[57].

3.2 NiFe2O4/Aurivillius type Bi-based oxides

Bismuth tungstate (Bi2WO6) is one of the simplest members of the Aurivillius family, and its special layered structure and visible light response endow Bi2WO6 with good photocatalytic properties. However, like most single photocatalysts, the photogenerated electron-hole recombination of Bi2WO6 leads to the decrease of photocatalytic activity, which seriously restricts the promotion and application of Bi2WO6. Based on this, scientists used Bi2WO6 and other photocatalysts to prepare composite photocatalytic systems with different morphologies as an effective strategy. Zhang et al. Showed that the Bi2WO6/NiFe2O4 formed by building NiFe2O4 and Bi2WO6 together could inhibit the recombination of photogenerated charges by means of the synergistic effect between them, thus degrading RhB efficiently under visible light[58⇓⇓⇓⇓~63][64].
Bismuth oxycarbonate (Bi2O2CO3) is also a member of the Aurivillius family, and Farhadi's research team prepared a composite material Bi2O2CO3/NiFe2O4 of flower-like Bi2O2CO3 loaded with NiFe2O4 nanoparticles.It was used to catalyze the reduction of nitroaromatics, and the highest performance was obtained when the content of NiFe2O4 was 15%, the conversion of 4-nitrophenol could reach 100% at room temperature for 26 min, and the rate constant was also as high as 0.14 min-1[65]. At the same time, the composite material has strong stability Bi2O2CO3/NiFe2O4 and still maintains high activity after being used for four times. This study not only broadens the application of NiFe2O4/Bi composite materials in the field of catalysis, but also opens up a new path for the removal of nitroaromatics in sewage.

3.3 NiFe2O4/ of other Bi-based compound

In addition to bismuth oxyhalides and Aurivillius-type Bi-based oxides, other Bi-based photocatalysts such as bismuth vanadate (BiVO4) and bismuth ferrite (Bi2Fe4O9) complexed with NiFe2O4 have been reported in a few literatures[66⇓~68]. For example, Wang et al. Successfully prepared NiFe2O4 modified BiVO4 composite NiFe2O4/BiVO4 for photocatalytic hydrogen production by electrophoretic deposition in 2017. They attributed the improvement of hydrogen production performance to the formation of n-n type heterojunction, the broadening of visible light absorption range and the effective separation of photogenerated electrons and holes[69]. Recently, Sakhare et al. Prepared a composite photocatalyst NiFe2O4/BiVO4 by combining hydrothermal and co-precipitation methods, and evaluated the photocatalytic activity of the material by degradation of MB under sunlight[70]. Happily, the obtained material showed a very good degradation performance for MB under solar irradiation, the degradation rate was 98%.NiFe2O4/BiVO4 in 30 min, and the degradation rate was still high (95%) after 4 times of continuous use. The XRD characterization showed that the crystal phase of NiFe2O4/BiVO4 did not change after continuous use, which fully proved that the composite had high photochemical stability.
Ji et al. Compounded NiFe2O4 and Bi2Fe4O9 to form a p-n heterojunction photocatalyst Bi2Fe4O9/NiFe2O4. The formation of the heterojunction inhibited the recombination of electrons and holes and improved the ability of Bi2Fe4O9 to degrade MB under UV light. In addition, · OH and h+ acted as active species to degrade MB by redox reaction[71].
In summary, the composite photocatalytic materials based on NiFe2O4 and Bi-based compounds have been successfully used to degrade various organic dyes, and show good photocatalytic activity and recycling performance.How to better modify, regulate and optimize the composite to further reduce the dosage of photocatalyst and improve the catalytic activity and stability will be a challenging task in the future.

4 NiFe2O4/Ag compound

Silver semiconductor materials have become a hot topic in the field of photocatalysis because of their special electronic structure, excellent visible light absorption ability and efficient photocatalytic activity. Silver semiconductor materials are mainly compounds containing elemental silver, and for elemental silver, there are only a few reports on the construction of photocatalysts with NiFe2O4[72,73].

4.1 NiFe2O4/Ag3PO4

Silver phosphate is a common silver salt, which has great potential in the field of photocatalysis[74⇓~76]. In 2010, Ye's research group first reported the research work on the degradation of organic pollutants and water photolysis to hydrogen by Ag3PO4 under visible light, and the results showed that Ag3PO4 had excellent visible light catalytic activity[77]. Since then, the research of Ag3PO4 in the field of photocatalysis has begun. However, the chemical properties of Ag3PO4 are unstable and vulnerable to photocorrosion, which makes it difficult to maintain the photocatalytic activity and limits the practical application. Therefore, the improvement and enhancement of its stability, photocatalytic activity and recycling performance have become the focus of attention of researchers all over the world. In 2015, Patil et al. Prepared a visible light-driven and magnetically separated n-n heterojunction composite photocatalyst Ag3PO4/NiFe2O4 by precipitation method. The formation of heterojunction broadens the response of photocatalyst to visible light, enhances the absorption of visible light, and inhibits the recombination of photogenerated carriers, thus increasing the degradation rate by 1.8 times compared with monomer Ag3PO4[78]. In addition, the recombination of NiFe2O4 makes the electrons on the surface of Ag3PO4 react with O2 to generate ·O2-, which avoids the reduction of Ag+ by photogenerated electrons and reduces the occurrence of photocorrosion. They also further analyzed the active substances and reaction mechanism in the degradation reaction. In 2016, Zhao's research team also prepared the heterojunction composite NiFe2O4/Ag3PO4 by ion exchange deposition method. The Ag3PO4 modified by NiFe2O4 not only extended the absorption range of visible light, but also increased the specific surface area from 0.51 m2·g-1 to 5% of the loading of 2.95 m2·g-1(NiFe2O4), so that the adsorption capacity and removal efficiency of the composite for MB were significantly improved. The adsorption-desorption equilibrium could be achieved in 10 min, and the removal rate was 92.63% in 30 min of visible light[79]. Similar studies include the Ag3PO4@NiFe2O4 of the complex reported by Huang et al. Photocurrent measurements, electrochemical impedance spectroscopy and photoluminescence spectra show that the combination of the two greatly promotes the migration and separation of photogenerated charges, and improves the activity and stability of Ag3PO4[80].
In 2018, Dong et al. Developed a Z-type ternary composite photocatalyst Ag3PO4/Ag/NiFe2O4 by using in-situ deposition combined with photoreduction method. The Ag3PO4/Ag/NiFe2O4 with the best ratio can completely degrade 20 mg/L MB in water under visible light irradiation for 25 min, and its activity is much higher than that of monobasic Ag3PO4 and binary Ag3PO4/Ag. However, the disadvantage is that the activity of the Ag3PO4/Ag/NiFe2O4 decreases to a certain extent during repeated use, so its stability needs to be improved[81]. The photocatalytic mechanism is shown in Fig. 8. Under the excitation of visible light, both Ag3PO4 and NiFe2O4 generate electron-hole pairs. The holes in the valence band of NiFe2O4 combine with the electrons in the conduction band of Ag3PO4 through the electron mediator Ag, while the holes in the valence band of Ag3PO4 can directly oxidize and degrade MB on the one hand, and on the other hand, they can react with water to generate hydroxyl radicals, both of which act as active species to degrade MB. In the same year, Zhang's group also constructed a visible-light-driven Z-type ternary composite photocatalyst Ag3PO4/GO/NiFe2O4 for RhB degradation by ion-exchange precipitation method[82]. From the SEM image (Fig. 9), it can be seen that the morphological structure of the composite has a slight photocorrosion compared with that before the reaction, which indicates that the introduction of GO and NiFe2O4 plays a certain role in protecting the photocorrosion of Ag3PO4. Total organic carbon (TOC) test showed that the mineralization rate of rhodamine B was 43% after 30 min of illumination. In order to clarify the photocatalytic mechanism of Ag3PO4/GO/NiFe2O4 (Fig. 10), the researchers of this group also carried out the capture experiment of active species by using disodium ethylenediaminetetraacetate, isopropanol and ascorbic acid, revealing that superoxide radicals and photogenerated holes play a major role in the degradation process.
In addition to graphene, the introduction of PANI and metal-organic framework (MOF) is also beneficial to inhibit the photocorrosion of Ag3PO4. For example, in 2019, Chen et al. Wrapped PANI on the surface of Ag3PO4 and immobilized NiFe2O4 nanoparticles on the surface of PANI/Ag3PO4 to obtain a Z-shaped ternary composite photocatalyst PANI/Ag3PO4/NiFe2O4. The close combination of the three improved the separation efficiency of photogenerated carriers, thus showing excellent performance. The degradation efficiency of RhB and MO was 100% and 94.97% under visible light irradiation for 40 and 25 min, respectively, and the degradation rate was 12.1 times and 15.4 times that of Ag3PO4[83]. For MB and other colorless pollutants such as tetracycline hydrochloride, nitrobenzene and bisphenol A, the PANI/Ag3PO4/NiFe2O4 also showed good degradation effect under the optimized conditions. Compared with the Ag3PO4, the PANI/Ag3PO4/NiFe2O4 showed higher stability in the cycle experiment, and the degradation rate of RhB could still reach 91. 7% after three cycles. This may be due to two factors. First, a small amount of Ag+ is reduced to Ag during the synthesis of PANI/Ag3PO4/NiFe2O4, and Ag acts as a transfer medium to accelerate the transfer of electrons and prevent the photocorrosion of Ag3PO4. Secondly, the unique magnetic response of NiFe2O4 enables PANI/Ag3PO4/NiFe2O4 to be rapidly separated and recovered from the reaction system under the action of an external magnetic field, which reduces the loss of photocatalyst. Zhang's group first prepared NiFe2O4 and MOF, and prepared ternary Z-shaped photocatalyst Ag3PO4/MOF/NiFe2O4(AFO/MOF/NFO) with different proportions by adjusting the amount of MOF. The removal rate of RhB by the composite containing 20% MOF reached 93% under visible light irradiation for 30 min, which realized the rapid degradation of RhB[84]. Fluorescence spectroscopy, photocurrent testing, AC impedance, and radical trapping further explain that the separation and transfer of charge during photodegradation is consistent with a Z-type photocatalytic mechanism (Fig. 11). The Z-type composite photocatalyst can not only ensure the enhancement of activity, but also broaden the application of MOF in the field of photocatalysis, thus showing a stronger application prospect.

4.2 NiFe2O4/AgX

Silver halide AgX (X = Cl, Br, I) is a kind of semiconductor material which is easy to prepare and has photosensitivity. Because of its photosensitivity, its stability is poor. Therefore, AgX is rarely used as a photocatalytic material alone. In order to improve the practical application value of AgX, researchers often compound AgX with other semiconductor materials to improve the photocatalytic activity and stability while reducing the cost. Ge group reported a magnetic composite photocatalyst AgBr/NiFe2O4 by combining hydrothermal method and ultrasound-assisted precipitation method. The morphology, structure, photocatalytic activity and active species of the magnetic composite photocatalyst were systematically studied, and the photocatalytic mechanism was proposed[85]. On the basis of the above work, the research group prepared ternary composite heterojunction photocatalyst Ag/AgBr/NiFe2O4 by immobilizing Ag on the surface of AgBr in 2017. The results showed that the incorporation of Ag significantly enhanced the photocatalytic activity of Ag/AgBr/NiFe2O4 and improved the degradation efficiency of RhB, which was mainly due to the formation of heterostructure and the surface plasmon resonance effect of Ag[86].
It can be seen from the above research that the composite of NiFe2O4 and Ag-based compounds has obvious advantages as a photocatalyst, and is more and more widely used in the field of photocatalysis.However, some of their own drawbacks have hindered the practical application of these materials in industrial production to a large extent, such as the synthesis process of some materials is more cumbersome, the stability of materials is poor, and these problems need to be further studied and explored by researchers.

5 NiFe2O4/TiO2

Titanium dioxide (TiO2), as a green semiconductor material, has become an important and potential photocatalyst for wastewater treatment because of its low cost, easy availability, non-toxicity and chemical stability. However, the single phase of TiO2 has a wide band gap (about 3.2 eV) and can only absorb ultraviolet light in the solar spectrum (about 4% of sunlight). In addition, the high recombination rate of photogenerated carriers, the difficulty in controlling the catalytic activity and the difficulty in recycling have limited the application and development of TiO2. In order to overcome these shortcomings and broaden the response range of TiO2 to visible light, the development of efficient magnetic TiO2 composite photocatalysts has become an important development direction in this field. In 2016, Gao et al. Successfully impregnated and deposited NiFe2O4 nanoparticles on one-dimensional ordered nanorod TiO2 film to obtain composite photocatalyst NiFe2O4/TiO2[87]. The photocurrent test showed that the photocurrent intensity of the NiFe2O4/TiO2 modified by NiFe2O4 was 8 times higher than that of the pure TiO2, which meant that the NiFe2O4/TiO2 had better photodegradation ability, and the degradation rate of UDMH was increased from 7. 86% to 22. 06% after 180 min of illumination, although the degradation rate was improved, there was still a big gap from the practical application, so further research and discussion were needed.
Liu et al. Used the sol-gel method to obtain the core-shell structure of TiO2@NiFe2O4, which was used to catalyze the amination of 4-phenyl-n-butyric acid and aniline[88]. Similar studies include the core-shell nanocomposite NiFe2O4@TiO2 reported by Baig et al., which showed some activity in the degradation of MO[89]. Ma's research group placed the photocatalyst NiFe2O4@TiO2 in a mixed atmosphere of H2/N2, and investigated the effects of the existing form, element valence and crystal phase change of the products obtained by calcination at different temperatures on the photocatalytic activity[90]. Šutka et al. Prepared a binary composite TiO2/NiFe2O4 and a silver-sensitized ternary composite TiO2/Ag/NiFe2O4, and investigated and compared their photocatalytic properties with MO as a model pollutant[91].
Chen et al. Prepared composite photocatalyst N-TiO2/NiFe2O4/ diatomite by using diatomite as the loading material of TiO2 and NiFe2O4.Under the joint action of the superior adsorbability of diatomite, the degradation capability of TiO2 and the synergistic effect of “TiO2 and NiFe2O4, the removal efficiency of RhB is greatly improved[92]. It should be pointed out that the activity of the composite decreased significantly after five cycles, and the removal rate decreased from 93% to 89.9%, so they speculated that the reason might be the loss of the catalyst in the separation and washing process.
In 2018, Wang et al. Used TiO2 to coat magnetic NiFe2O4 nanoparticles and anchored them on the surface of reduced graphene oxide to prepare core-shell ternary heterojunction composite NiFe2O4@TiO2/RGO, which was found by UV-Vis absorption spectroscopy to degrade RhB under the condition of mercury lamp as light source.This is attributed to two factors: (1) the electrons in the outermost carbon atom of RGO are easy to form a π-conjugated structure, which facilitates the rapid transfer of electrons from the conduction band of TiO2 to RGO, thereby reducing the recombination rate of electron-hole pairs[93]; The electrons on the surface of (2)TiO2 react with water to produce · OH for the oxidative degradation of RhB. However, the defects of the complex are as follows: (1) the reusability is not ideal, and the activity is greatly reduced after being used for 6 times; (2) The composite is a UV-driven photocatalyst, which cannot fully utilize sunlight. In 2019, Saravani et al. Mixed tetraisopropyl titanate, NiFe2O4 and graphene, and obtained graphene-supported ternary composite TiO2/NiFe2O4/RGO after hydrolysis[94]. Different from the above studies, the TiO2/NiFe2O4/RGO in this study can respond to both visible light and ultraviolet light, and under the same conditions (pH 11, 0. 02 G photocatalyst, methylene blue solution with 0.01 mL H2O2,200 mL concentration of 10 mg/L), the degradation rates of MB were 71% and 87% after 90 min of visible light and ultraviolet light, respectively. Unfortunately, the activity of the complex gradually decreased during recycling, and the degradation rate decreased from 71% to 59% after the fourth use.
To sum up, the composite of NiFe2O4 and TiO2 can not only extend the spectral response wavelength of TiO2 to the visible region, but also endow the composite with unique magnetic separation characteristics, thus simplifying the operation process of material reuse in photocatalytic degradation. However, from the current point of view, most of the NiFe2O4/TiO2 composites have the problems of less reuse times and serious material deactivation, so more efforts should be made to improve the visible light catalytic activity and reuse performance of the composites.

6 NiFe2O4/ZnO

As a widely studied photocatalytic material, ZnO has attracted much attention because of its low cost, non-toxicity, and high efficiency. However, due to the large band gap of ZnO, it can only absorb ultraviolet light, and the utilization rate of sunlight is low. In addition, ZnO has poor photostability and is prone to photocorrosion, which seriously limits its practical application. Therefore, many scholars have been exploring various methods to modify or modify ZnO in order to improve the quantum yield, photocatalytic activity and stability. Among them, the composite of ZnO and other semiconductors is one of the most commonly used and effective methods. In 2016, Jiang's team used hydrothermal method to compound NiFe2O4 and ZnO to obtain NiFe2O4/ZnO, which not only effectively regulated the energy band of ZnO, but also accelerated the transfer of electrons between interfaces.The recombination of photogenerated electron-hole pairs was inhibited, and the activity and stability of the photocatalyst were enhanced.The decolorization rate of Congo red was 98. 43% after 80 min of simulated sunlight irradiation, and the decolorization rate of Congo red was still as high as 97. 23% after 5 times of reuse[22]. Compared with ZnO, the stability is greatly improved. In the same year, Rahmayeni's research group also constructed a series of composite ZnO-NiFe2O4 with wide spectral response by using ethanol as solvent through solvothermal reaction. Photocatalytic experiments showed that the introduction of NiFe2O4 broadened the absorption of ZnO in the visible region. When the molar ratio of ZnO to NiFe2O4 was 1: 0.01, the ZnO-NiFe2O4 had the best photocatalytic effect under sunlight irradiation, and 99% of RhB could be degraded in 3 H, which was much better than that of single ZnO and NiFe2O4[95].
In 2018, Theivasanthi's team used solid-state synthesis to mix NiFe2O4, ZnO and thiourea at a ratio of 1:20:10 and then calcined them at 800 ℃ to obtain the composite ZnO/NiFe2O4, which showed significantly improved activity in the reaction of photodegradation of MB[96]. Torres-Mart Martínez et al. Studied the activity of NiFe2O4-ZnO heterojunction composite for hydrogen production by water photolysis, and the study showed that under UV irradiation, the composite doped with 3% ZnO had the best activity, and the hydrogen production rate was 3.65 times that of monomer ZnO[97]. NiFe2O4@ZnO synthesized by Ramazani et al. Showed high degradation ability for direct blue 129 and reactive blue 21[98]. Similarly, Yousefi et al. Also studied and compared the degradation behavior of Coomassie blue G-250 catalyzed by NiFe2O4/ZnO composite under UV light (30 min, degradation rate of 96.90%) and visible light (30 min, degradation rate of 68.55%), and found that the catalytic activity was more excellent under UV light[99].
As mentioned above, the introduction of NiFe2O4 into ZnO can not only control the band gap of ZnO, but also improve and enhance the photocatalytic activity and stability, but from the perspective of practical application, the response range of photocatalyst to visible light needs to be further extended. Therefore, the development of photocatalysts with high visible light utilization, high quantum yield and high stability is still the frontier and hot spot in the field of photocatalysis.

7 Conclusion and prospect

NiFe2O4-based composite photocatalytic materials have been successfully used in water photolysis for hydrogen production and degradation of various organic dyes due to their excellent catalytic activity, stability and easy separation and reuse.This provides an effective way for the development of new energy and the treatment of sewage, and also lays a solid foundation for the large-scale application of NiFe2O4-based composite photocatalytic materials in industrial production. This paper mainly summarizes the preparation and application of NiFe2O4/ carbon materials, NiFe2O4/Bi system, NiFe2O4/Ag system, NiFe2O4/TiO2 and NiFe2O4/ZnO composite photocatalytic system. Through the above introduction, we found that although some achievements have been made in the synthesis and application of NiFe2O4-based composite photocatalytic system, these achievements only evaluate the electron transfer and photocatalytic activity of the composite system in the photodegradation process by simulating the removal of simple dyes or common organic pollutants in the laboratory.There is little research on the microscopic mechanism of photocatalytic reaction and the removal of pollutants in complex water, so strictly speaking, it is still in an exploratory stage.If we want to put these composite photocatalytic materials into practical application, there are still many scientific problems to be solved, and the follow-up needs continuous exploration and systematic and in-depth research by researchers. It is believed that through continuous research and efforts, this kind of material will play its role in solving the energy crisis and controlling environmental pollution in the near future, and its development is worth looking forward to.

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Funding

National Natural Science Foundation of China(51502162)

National Natural Science Foundation of China(21975001)

Key Project of Natural Science Research for Colleges and Universities of Anhui Province of China(KJ2019A0115)

Young Teacher Supporting Fund of Shandong University of Technology

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