无机-有机杂化光催化剂: 合成、机理及应用

doi:10.1016/S1872-2067(22)64096-8

催化学报 ›› 2022, Vol. 43 ›› Issue (8): 2111-2140.DOI: 10.1016/S1872-2067(22)64096-8

无机-有机杂化光催化剂: 合成、机理及应用

杨辉^a, 代凯^a^,^*(), 张金锋^a^,^#(), Graham Dawson^b

^a淮北师范大学绿色和精准合成化学及应用教育部重点实验室, 安徽淮北235000
^b西交利物浦大学化学系, 江苏苏州215123

收稿日期:2021-12-24 接受日期:2022-03-27 出版日期:2022-08-18 发布日期:2022-06-20
通讯作者: 代凯,张金锋
基金资助:
国家自然科学基金(51572103);国家自然科学基金(51973078);安徽省杰出青年基金(1808085J14);安徽省教育厅重大项目(KJ2020ZD005);安徽省教育厅重点项目(KJ2019A0595)

Inorganic-organic hybrid photocatalysts: Syntheses, mechanisms, and applications

Hui Yang^a, Kai Dai^a^,^*(), Jinfeng Zhang^a^,^#(), Graham Dawson^b

^aKey Laboratory of Green and Precise Synthetic Chemistry and Applications, Ministry of Education, Huaibei Normal University, Huaibei 235000, Anhui, China
^bDepartment of Chemistry, Xi’an Jiaotong Liverpool University, Suzhou 215123, Jiangsu, China

Received:2021-12-24 Accepted:2022-03-27 Online:2022-08-18 Published:2022-06-20
Contact: Kai Dai, Jinfeng Zhang
About author:Kai Dai (Huaibei Normal University) received his B.A. degree from Anhui University (China) in 2002, and Ph.D. degree from Shanghai University (China) in 2007. He worked in Suzhou Institute of Nano-Tech and Nano-Bionics, Chinese Academy of Sciences at 2007, and then in Huaibei Normal University at 2010. He is Distinguished Young Scholars Recipients of Natural Science Foundation of Anhui Province (2018) and head of Anhui Provincial Teaching Team (2019). His research interests mainly focus on semiconductor photocatalysis. He has published more than 120 peer-reviewed papers, including 6 hot paper of ESI and 19 highly cited papers of ESI.
Jinfeng Zhang (Huaibei Normal University) received his M.S. degree from Ningxia University (China) in 2007, and Ph.D. degree from Wuhan University of Technology (China) in 2016. He carried out postdoctoral research in Wuhan University of Technology from 2016 to 2018. Since the end of 2007, he has been working in Huaibei Normal University. His research interests mainly focus on semiconductor photocatalysis. As the first author or corresponding author, he has published more than 50 SCI papers in solar RRL, Appl. Catal. B: Environ., Chem. Eng. J and other international academic journals, including 3 hot paper of ESI and 12 highly cited papers of ESI. He has mainly undertaken more than 6 research projects, including the National Natural Science Foundation of China, China Postdoctoral Science Foundation and Anhui Provincial Department of education.
Supported by:
National Natural Science Foundation of China(51572103);National Natural Science Foundation of China(51973078);Distinguished Young Scholar of Anhui Province(1808085J14);Major projects of Education Department of Anhui Province(KJ2020ZD005);Key Foundation of Educational Commission of Anhui Province(KJ2019A0595)

摘要/Abstract

摘要：

由无机与有机组分组成的无机-有机杂化材料因其优异的性能及良好的物理化学性质在光催化领域得到了广泛的关注. 目前, 已经开发的单相光催化剂有很多种, 但其很难同时满足宽的光激发范围以及高的光吸收能力和强的氧化还原能力等需求, 因此, 科研人员开发了很多方法去解决上述问题,主要包括以下两大类. 第一类, 修饰光催化剂扩大光激发范围以及增强可见光吸收. 例如构建固溶体、引入表面缺陷、杂质掺杂、染料敏化和表面等离子体共振等策略. 第二类, 构建半导体异质结, 通过界面处的协同作用有效促进光生电子空穴对的转移与分离. 例如type II型、直接Z型以及S型异质结等.

有机成分与无机成分的杂化是有效解决上述问题的方法之一. 大部分有机材料具有成本低、吸光系数高以及比表面积大等优点; 但低的强度以及宽的带隙限制了有机材料在光催化上的应用. 而大部分无机材料具有高强度、窄带隙以及良好的光学性能. 但低韧性和较差的分散性限制了无机材料在光催化上的应用. 无机-有机杂化材料不仅保留了无机与有机组分的原有性质, 而且界面处组分之间的协同作用会产生新的性质, 如高的载流子传输能力和高的光吸收能力等. 无机-有机杂化材料是多相材料, 其中的一相是纳米材料, 从而保留了纳米材料的量子尺寸效应、小尺寸效应、表面效应和宏观量子隧道效应; 并且纳米结构的光催化剂相对于体相材料而言, 具有比表面积高、载流子输运距离短和电子结构可调等优势. 无机-有机杂化光催化材料既保留了高的光吸收能力, 又保留了高氧化性的空穴与高还原性的电子, 因而在光催化领域的应用越来越广泛.

本文综述了无机-有机杂化材料的合成、机理以及在光催化领域的应用. 首先, 介绍了无机-有机光催化剂的作用、优缺点以及设计原则, 讨论了自上而下和自下而上制备无机-有机杂化材料的方法, 为设计杂化材料提供思路. 其次, 对有机组分与无机组分的相互作用力进行分类讨论. 再次, 阐述了无机-有机杂化材料的优势, 讨论了进一步改进无机-有机光催化剂的方法. 最后, 总结了无机-有机杂化材料在光催化领域面临的问题与挑战, 并对未来发展进行了展望.

关键词: 光催化剂, 无机-有机杂化, 合成, 机理, 应用

Abstract:

Inorganic-organic hybrid materials are promising for application in the field of photocatalysis because of their excellent properties. Therefore, their syntheses, mechanisms, and applications are reviewed in this paper. First, we introduce the role of inorganic-organic photocatalysts, their advantages and disadvantages, and their design principles. Second, we present the top-down and bottom-up synthesis methods of the hybrid materials. The interaction between inorganic and organic components in hybrid materials is discussed, followed by how to improve inorganic-organic photocatalysts. Third, the applications of hybrid materials in the field of photocatalysis, such as realizing hydrogen evolution, organic pollutant degradation, heavy metals and CO₂ reduction, sterilization, and nitrogen fixation, are examined. Finally, the application prospects and development directions of inorganic-organic hybrid materials are explored and the unsolved problems are described.

Key words: Photocatalyst, Inorganic-organic hybrid, Synthesis, Mechanism, Application

杨辉, 代凯, 张金锋, Graham Dawson. 无机-有机杂化光催化剂: 合成、机理及应用[J]. 催化学报, 2022, 43(8): 2111-2140.

Hui Yang, Kai Dai, Jinfeng Zhang, Graham Dawson. Inorganic-organic hybrid photocatalysts: Syntheses, mechanisms, and applications[J]. Chinese Journal of Catalysis, 2022, 43(8): 2111-2140.

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图/表 29

Fig. 1. Advantages of inorganic-organic hybrid materials.

Fig. 2. Statistics of publications and their citations with topics including “inorganic-organic hybrid materials” and “photocatalytic” based on a Web of Science search conducted on January 23, 2022.

Fig. 3. Photocatalytic reaction steps.

Fig. 4. Role of inorganic-organic hybrid materials.

Fig. 5. (a) Synthesis of Bi2WO6 with different morphologies using PVP as an inducer. (b) Different molar ratios of BDC and Cr(NO3)3·9H2O change the size of MIL-101(Cr)-Ag. (a) Reprinted with permission from Ref. [63]. Copyright 2016, Elsevier. (b) Reprinted with permission from Ref. [60]. Copyright 2019, American Chemical Society.

Fig. 6. (a) UV-vis DRS curves of the VO-BiOBr nanosheets and BiOBr nanoplates. The inset shows the color comparison of the VO-BiOBr nanosheets (left) and BiOBr nanoplates (right). (b) Corresponding Tauc ((Ahν)1/2 versus hν) plots, valence-band XPS spectra (c) and band alignments (d) of the VO-BiOBr nanosheets and BiOBr nanoplates. (e) Schematic of the photocatalytic ammonia synthesis process on the VO-BiOBr nanosheets and BiOBr nanoplates. Reprinted with permission from Ref. [71]. Copyright 2018, American Chemical Society.

Fig. 7. Schematic of CdS nanomaterials prepared using different inducers and CdS-PD-assisted photocatalytic reduction of CO2. Reprinted with permission from Ref. [75]. Copyright 2018, American Chemical Society.

Fig. 9. Design principles of inorganic-organic photocatalysts.

Fig. 10. Synthetic methods for preparing inorganic-organic hybrid materials.

Table 1 Overview of synthetic methods for preparing inorganic-organic photocatalysts.

Preparation method	Photocatalyst	Ref.
Epitaxial growth	Fe₃O₄@UiO-66-NH₂	[119]
	HZSM-5@UIO-66-NH₂/Pd	[120]
	CdS-TiO₂@g-C₃N₄	[98]
	Au@Pd@MOF-74	[121]
	MAF-7	[93]
Mechanical grinding	MoNi@MoO₂-8%/g-C₃N₄	[122]
	Perylenetetracarboxylic acid diimide polymer@TiO₂	[123]
	Co₂ZrO₅/g-C₃N₄	[124]
	WO_x/Ni-g-C₃N₄	[125]
Pyrolysis	Co nanoparticles decorated with nitrogen-doped carbon nanotubes	[126]
	Cellulose-derived carbon nanofibers/BiOBr	[127]
	N-C-TiO₂/C	[128]
	Fe(OH)₃@nickel PDI	[129]
	WC_1‒_x/g-C₃N₄	[130]
Chemical intercalation	Ethylenediamine-intercalated quasimonolayer BP	[131]
	Bi₂O₃-bentonite	[132]
	Co₃O₄/C₃N₄	[107]
Electrospray	Zn/PbO/PC-Zn/MAPbBr₃	[97]
Hydrothermal/solvothermal	CdS/polybenzothiadiazole (B-BT-1,4-E, noted as BE)	[133]
	CdS/DETA	[134]
	Carbonized polymer dots/Bi₄O₅Br₂	[86]
	WO₃/CdS-DETA	[135]
	Zn₃In₂S₆/fluorinated polymeric carbon nitride	[88]
	Pt/CdS-DETA	[136]
	CdS-NiPc	[137]
	ZnS(propylamine)	[138]
	Cu₂S/CdS-DETA	[139]
	Ag/AgCl/NH₂-UiO-66	[140]
	Au@Void@g‑C₃N₄/SnS	[141]
	BiOI/g‐C₃N₄	[142]
	g-C₃N₄/N-doped carbon dots/MoS₂	[143]
	NH₂-MIL-125 (Ti)@Bi₂MoO₆	[144]
	Bi₂WO₆/g-C₃N₄	[145]
	ZnIn₂S₄@PCN-224 (a MOF composed of porphyrin linkers and Zr clusters)	[146]
	g-C₃N₄/CdS	[147]
	g-C₃N₄/ZnIn₂S₄	[148]
	MASnI₃/TiO₂ (MA represents CH₃NH₃⁺)	[149]
Evaporation-solvent assembly	TiO₂/g-C₃N₄	[150]
	MIL-125	[151]
	WO₃/g-C₃N₄	[152]
	Nd₂O₃/g-C₃N₄	[153]
	SnO₂/Polyaniline	[154]
Sol-gel	Aluminum-doped zinc oxide-polyaniline	[155]
	g-C₃N₄/N-doped-LaTiO₃	[156]
	calixarene dye (HO-TPA)/TiO₂	[157]
Template	MIL-125(Ti)	[158]
	TB-TiO₂@MFA	[159]
	SiO₂/g-C₃N₄	[160]
	pg-C₃N₄/Co₃O₄/CoS	[161]
	AgCl/g-C₃N₅	[162]
	Bi₅O₇I/g-C₃N₄	[163]
	ZnO@zeolitic imidazolate frameworks-8	[164]
	MOF-derived bimetallic Fe-Ni-P nanotubes	[165]
	MIL-125/TiO₂@SiO₂	[166]
LBL self-assembly	Ag-AgCl/WO₃/g-C₃N₄ nanoparticles on a polydopamine (PDA)-modified melamine sponge	[167]
	MoS₂/ZIF-8	[168]
	Polypyrrole/CdS	[169]
	Poly(styrene sulfonate) sodium salt/TiO₂	[170]
	BiOCl/g-C₃N₄/kaolinite	[171]
	TiO₂/poly(sodium styrenesulfonate)	[172]

Table 1 Overview of synthetic methods for preparing inorganic-organic photocatalysts.

Preparation method	Photocatalyst	Ref.
Epitaxial growth	Fe₃O₄@UiO-66-NH₂	[119]
	HZSM-5@UIO-66-NH₂/Pd	[120]
	CdS-TiO₂@g-C₃N₄	[98]
	Au@Pd@MOF-74	[121]
	MAF-7	[93]
Mechanical grinding	MoNi@MoO₂-8%/g-C₃N₄	[122]
	Perylenetetracarboxylic acid diimide polymer@TiO₂	[123]
	Co₂ZrO₅/g-C₃N₄	[124]
	WO_x/Ni-g-C₃N₄	[125]
Pyrolysis	Co nanoparticles decorated with nitrogen-doped carbon nanotubes	[126]
	Cellulose-derived carbon nanofibers/BiOBr	[127]
	N-C-TiO₂/C	[128]
	Fe(OH)₃@nickel PDI	[129]
	WC_1‒_x/g-C₃N₄	[130]
Chemical intercalation	Ethylenediamine-intercalated quasimonolayer BP	[131]
	Bi₂O₃-bentonite	[132]
	Co₃O₄/C₃N₄	[107]
Electrospray	Zn/PbO/PC-Zn/MAPbBr₃	[97]
Hydrothermal/solvothermal	CdS/polybenzothiadiazole (B-BT-1,4-E, noted as BE)	[133]
	CdS/DETA	[134]
	Carbonized polymer dots/Bi₄O₅Br₂	[86]
	WO₃/CdS-DETA	[135]
	Zn₃In₂S₆/fluorinated polymeric carbon nitride	[88]
	Pt/CdS-DETA	[136]
	CdS-NiPc	[137]
	ZnS(propylamine)	[138]
	Cu₂S/CdS-DETA	[139]
	Ag/AgCl/NH₂-UiO-66	[140]
	Au@Void@g‑C₃N₄/SnS	[141]
	BiOI/g‐C₃N₄	[142]
	g-C₃N₄/N-doped carbon dots/MoS₂	[143]
	NH₂-MIL-125 (Ti)@Bi₂MoO₆	[144]
	Bi₂WO₆/g-C₃N₄	[145]
	ZnIn₂S₄@PCN-224 (a MOF composed of porphyrin linkers and Zr clusters)	[146]
	g-C₃N₄/CdS	[147]
	g-C₃N₄/ZnIn₂S₄	[148]
	MASnI₃/TiO₂ (MA represents CH₃NH₃⁺)	[149]
Evaporation-solvent assembly	TiO₂/g-C₃N₄	[150]
	MIL-125	[151]
	WO₃/g-C₃N₄	[152]
	Nd₂O₃/g-C₃N₄	[153]
	SnO₂/Polyaniline	[154]
Sol-gel	Aluminum-doped zinc oxide-polyaniline	[155]
	g-C₃N₄/N-doped-LaTiO₃	[156]
	calixarene dye (HO-TPA)/TiO₂	[157]
Template	MIL-125(Ti)	[158]
	TB-TiO₂@MFA	[159]
	SiO₂/g-C₃N₄	[160]
	pg-C₃N₄/Co₃O₄/CoS	[161]
	AgCl/g-C₃N₅	[162]
	Bi₅O₇I/g-C₃N₄	[163]
	ZnO@zeolitic imidazolate frameworks-8	[164]
	MOF-derived bimetallic Fe-Ni-P nanotubes	[165]
	MIL-125/TiO₂@SiO₂	[166]
LBL self-assembly	Ag-AgCl/WO₃/g-C₃N₄ nanoparticles on a polydopamine (PDA)-modified melamine sponge	[167]
	MoS₂/ZIF-8	[168]
	Polypyrrole/CdS	[169]
	Poly(styrene sulfonate) sodium salt/TiO₂	[170]
	BiOCl/g-C₃N₄/kaolinite	[171]
	TiO₂/poly(sodium styrenesulfonate)	[172]

Fig. 11. (a) MOF structure of the hydrophilic and hydrophobic layers of Zn grown on the PES membrane. (b) Schematic of the synthetic pathway of Ni-CPNS/CdS heterostructure. (c) Schematic of the synthesis path of PVAD-g-TiO2 prepared via pyrolysis. (d) Schematic of inorganic-organic (top arrow) and columnar inorganic (bottom arrow) materials prepared through the intercalation of IPC-1P precursor. (e) Synthesis and structure principle of Zn/PbO/PC-Zn/MAPbBr3 heterojunction materials using the electrospray method. (a) Reprinted with permission from Ref. [93]. Copyright 2021, Elsevier. (b) Reprinted with permission from Ref. [94]. Copyright 2019, The Royal Society of Chemistry. (c) Reprinted with permission from Ref. [95]. Copyright 2014, American Chemical Society. (d) Reprinted with permission from Ref. [96]. Copyright 2014, American Chemical Society. (e) Reprinted with permission from Ref. [97]. Copyright 2021, John Wiley and Sons.

Fig. 12. (a) Schematic of the synthesis path of ZnxCd1-xSe-DETA and NiS/Zn0.5Cd0.5Se-DETA using the solvothermal method. (b) Multications: α,α'-bis(4-cyano-l-pyridino)-o-xylene dibromide [O-CN·Br2], α,α'-bis(4-cyano-l-pyridino)-m-xylene dibromide [M-CN·Br2], α,α'-bis(4-cyano-l-pyridino)-p-xylene dibromide [P-CNP·Br2], and 1,2,4,5-four[(4-cyanopyridyl)-N-methylene] benzene) [Multi-CN·Br4]. (c) Structure and the optimized structure of cone-calixarene-based dye Calix-3. (d) Illustration of the formation process of hierarchically porous titanium phosphonates using dual templates. (e) LBL self-assembly construction process of coating. (a) Reprinted with permission from Ref. [108]. Copyright 2020, Elsevier. (b) Reprinted with permission from Ref. [109]. Copyright 2020, Elsevier. (c) Reprinted with permission from Ref. [110]. Copyright 2019, The Royal Society of Chemistry. (d) Reprinted with permission from Ref. [111]. Copyright 2018, John Wiley and Sons. (e) Reprinted with permission from Ref. [112]. Copyright 2019, American Chemical Society.

Fig. 13. Bonding types of inorganic-organic hybrid materials.

Table 2 Overview of the bonding types of inorganic-organic photocatalysts.

Bond	Photocatalyst	Ref.
Electrostatic interactions	CdS/mercaptopropionic acid (MPA)	[181]
	MOF (Ni₃HITP₂)/rGO	[182]
	ZnIn₂S₄/g-C₃N₄	[183]
	g-C₃N₄/Au/BiVO₄	[184]
	g-C₃N₄/ZnO	[185]
	BaSnO₃/poly(dimethyl- Diallylammonium chloride)/Ti₃C₂T_x	[186]
	Triptycene covalent polymer@CdS	[187]
	Ru@Cu-HHTP	[188]
Van der Waals force	Geopolymer spheres/CdS	[189]
	Co-rGO/C₃N₄	[190]
	PDINH/Bi₂WO₆	[191]
	FLI₂/CNNS	[174]
Hydrogen bond	In₂S₃@MIL-125(Ti)	[192]
	Regenerated cellulose/TiO₂	[179]
	polyaniline-titanium dioxide (PANI)/TiO₂	[193]
	PDINH/TiO₂	[175]
Ionic bond	CNFs/ZnIn₂S₄	[176]
	Mn-adsorbed g-C₃N₄	[194]
	Barium-embedded g-C₃N₄	[195]
Covalent bond	ZnIn₂S₄/g-C₃N₄	[180]
	COF-318-TiO₂	[177]
	C₃N₄/CoP_x	[196]
	MIL-53(Fe)/PDI	[197]
	Co-phosphide/p-C₃N₄	[198]
	O-g-C₃N₄/TiO₂	[199]

Fig. 14. (a) Schematic of the synthesis path of EDTA-mediated Cd0.5Zn0.5S@halloysite nanotubes. (b) Schematic of the processes of preparing the FLI2/CNNs-X composite. (c) Schematic of the photocatalytic reaction mechanism of PDINH/TiO2 under simulated sunlight. (d) Diagram of the synthesis path of CNFs/ZnIn2S4. (e) Schematic of the preparation of COF-318-SCs via the condensation of COF-318 and semiconductor materials. (a) Reprinted with permission from Ref. [173]. Copyright 2019, John Wiley and Sons. (b) Reprinted with permission from Ref. [174]. Copyright 2022, Elsevier. (c) Reprinted with permission from Ref. [175]. Copyright 2021, Elsevier. (d) Reprinted with permission from Ref. [176]. Copyright 2019, Elsevier. (e) Reprinted with permission from Ref. [177]. Copyright 2020, John Wiley and Sons.

Fig. 15. Method for enhancing light excitation and absorption.

Fig. 16. Photocatalytic application of inorganic-organic hybrid materials.

Table 3 Overview of the catalytic efficiency of inorganic-organic photocatalysts.

Application Type	Photocatalyst	Photocatalytic target	Efficiency	Ref.
Photocatalytic degradation of organic pollutants	5% Citric acid/CeO₂	25 mg L^-1 glyphosate	100% in 30 min	[245]
	30% Perylene imide/Bi₂WO₆	50 mL of 10 ppm bisphenol A	100% in 180 min	[246]
	[BHMTA] [Cu₂I₃]_n	20 mg L^-1 tetracycline	96.2% in 180 min	[294]
	Ag₃PO₄/PDI organic supermolecules	20 mg L^-1 tetracycline hydrochloride	82.8% in 8 min	[248]
	H₁₂SubPcB-OPhCOPh/TiO₂	20 mg L^-1 tetracycline	100% in 180 min	[295]
	30% WO₃@Cu@PDI	10 mg L^-1 tetracycline hydrochloride	75% in 15 min	[296]
	Tetra (4-carboxyphenyl) porphyrin/Bi₂MoO₆	20 mg L^-1 tetracycline hydrochloride	85.7% in 15 min	[297]
	PW₁₂/CN@Bi₂WO₆	30 mg L^-1 tetracycline hydrochloride	97.5% in 100 min	[298]
	ZnSe/polyaniline	10 mg L^-1 methylene blue (MB)	90%-100% in 180 min	[299]
Photocatalytic reduction of heavy metals	PANI@SnS₂@carbon	80 mg Cr(VI)	100% in 20 min	[300]
	MIL-53(Fe)	1.0 g L^-1 Cu-EDTA	91% in 60 min	[250]
	TiO₂-WO₃-PANI	10 mg L^-1 Cr(VI)	67.62% in 60 min	[301]
	PVP/Bi₂S₃	Cr(VI)	95.2% in 5 min	[251]
	Polyaniline/Zn₃In₂S₆	50 mg L^-1 Cr(VI)	100% in 20 min	[24]
	PDPB-ZnO	50 mg L^-1 Cr(VI)	99.8% in 90 min	[302]
	PW₁₂/CN@Bi₂WO₆	20 mg L^-1 Cr(VI)	98.7% in 90 min	[298]
Photocatalytic hydrogen production	ZnIn₂S₄/TCP	H₂O	1432.8 μmol h^-1 g^-1 H₂	[262]
	Titanium-phosphonate MOF	H₂O	1260 μmol h^-1 g^-1 H₂	[263]
	Pyrene-benzene polymer/MoS₂	H₂O	27 μmol h^-1 H₂	[303]
	CdS@TCP	H₂O	104.51 μmol h^-1 g^-1 H₂	[49]
	Polytriptycene@CdS	H₂O	9480 μmol h^-1 g^-1 H₂	[187]
	Polyaniline/ZnO	H₂O	9.4 mmol h^-1 g^-1 H₂	[304]
Photocatalytic carbon dioxide reduction	Graphdiyne/Bi₂WO₆	CO₂ and H₂O	2.13 mmol h^-1 g^-1 CH₃OH 0.23 mmol h^-1 g^-1 CH₄	[305]
	L-cysteine/In₄SnS₈	CO₂ and H₂O	10.70 μL h^-1 CH₄ 9.39 μL h^-1 CO	[306]
	Cu-HHTP	CO₂	130 mmol h^-1 g^-1 CO	[188]
	Zr(IV)-MOF BUT-110-65%-Co	CO₂ and H₂O	70.8 μmol h^-1 g^-1 CH₄ 9.0 μmol h^-1 g^-1 CO	[307]
	InVO₄/g-C₃N₄	CO₂ and H₂O	69.8 μmol h^-1 g^-1 CO	[281]
	UiO-66-NH₂-LV	CO₂	35 μmol h^-1 g^-1 CO	[308]
	Imidazolium-modified ZnSe	CO₂	2.4 mmol h^-1 g^-1 CO	[280]
	Pd-hypercrosslinked polymers-TiO₂	CO₂ and H₂O	237.4 μmol h^-1 g^-1 CH₄	[309]
	SnNb₂O₆/CdSe-DETA	CO₂ and H₂O	36.16 μmol h^-1 g^-1 CO	[279]
Photocatalytic sterilization	TiO₂/chlorophyll	Escherichia coli	sterilization (2.94 × 10⁷ cfu cm^-2 180 min)	[310]
	CeO₂/polymeric carbon nitride	staphylococcus aureus (S. aureus)	88.1% sterilization	[89]
	P-doped MoS₂/g-C₃N₄	escherichia coli (E. coli)	99.99% sterilization	[79]
	α-Fe₂O₃/g-C₃N₄	Escherichia coli	sterilization (7 log₁₀ cfu mL^-1 in 120 min)	[282]
	Sn₃O₄/perylene-3,4,9,10-tetracarboxylic diimide	staphylococcus aureus and escherichia coli	94% and 92% sterilization efficiencies for S. aureus and E. coli, respectively	[284]
Photocatalytic nitrogen fixation	Al-PMOF (porphyrin-based metal-organic framework)	N₂	127 μg h^-1 g^-1 NH₃	[293]
	NH₂-MIL-125(Ti)	N₂	12.3 μmol h^-1 g^-1 NH₃	[292]
	Polyacrylonitrile/BiOBr-Cl	N₂	234.4 μmol h^-1 g^-1 NH₃	[311]
	MIL-101(Fe)	N₂	50.355 μmol h^-1 g^-1 NH₃	[312]
	Zn/PbO/PC-Zn/MAPbBr₃	N₂	46.87 μmol h^-1 g^-1 NH₃	[97]

Table 3 Overview of the catalytic efficiency of inorganic-organic photocatalysts.

Application Type	Photocatalyst	Photocatalytic target	Efficiency	Ref.
Photocatalytic degradation of organic pollutants	5% Citric acid/CeO₂	25 mg L^-1 glyphosate	100% in 30 min	[245]
	30% Perylene imide/Bi₂WO₆	50 mL of 10 ppm bisphenol A	100% in 180 min	[246]
	[BHMTA] [Cu₂I₃]_n	20 mg L^-1 tetracycline	96.2% in 180 min	[294]
	Ag₃PO₄/PDI organic supermolecules	20 mg L^-1 tetracycline hydrochloride	82.8% in 8 min	[248]
	H₁₂SubPcB-OPhCOPh/TiO₂	20 mg L^-1 tetracycline	100% in 180 min	[295]
	30% WO₃@Cu@PDI	10 mg L^-1 tetracycline hydrochloride	75% in 15 min	[296]
	Tetra (4-carboxyphenyl) porphyrin/Bi₂MoO₆	20 mg L^-1 tetracycline hydrochloride	85.7% in 15 min	[297]
	PW₁₂/CN@Bi₂WO₆	30 mg L^-1 tetracycline hydrochloride	97.5% in 100 min	[298]
	ZnSe/polyaniline	10 mg L^-1 methylene blue (MB)	90%-100% in 180 min	[299]
Photocatalytic reduction of heavy metals	PANI@SnS₂@carbon	80 mg Cr(VI)	100% in 20 min	[300]
	MIL-53(Fe)	1.0 g L^-1 Cu-EDTA	91% in 60 min	[250]
	TiO₂-WO₃-PANI	10 mg L^-1 Cr(VI)	67.62% in 60 min	[301]
	PVP/Bi₂S₃	Cr(VI)	95.2% in 5 min	[251]
	Polyaniline/Zn₃In₂S₆	50 mg L^-1 Cr(VI)	100% in 20 min	[24]
	PDPB-ZnO	50 mg L^-1 Cr(VI)	99.8% in 90 min	[302]
	PW₁₂/CN@Bi₂WO₆	20 mg L^-1 Cr(VI)	98.7% in 90 min	[298]
Photocatalytic hydrogen production	ZnIn₂S₄/TCP	H₂O	1432.8 μmol h^-1 g^-1 H₂	[262]
	Titanium-phosphonate MOF	H₂O	1260 μmol h^-1 g^-1 H₂	[263]
	Pyrene-benzene polymer/MoS₂	H₂O	27 μmol h^-1 H₂	[303]
	CdS@TCP	H₂O	104.51 μmol h^-1 g^-1 H₂	[49]
	Polytriptycene@CdS	H₂O	9480 μmol h^-1 g^-1 H₂	[187]
	Polyaniline/ZnO	H₂O	9.4 mmol h^-1 g^-1 H₂	[304]
Photocatalytic carbon dioxide reduction	Graphdiyne/Bi₂WO₆	CO₂ and H₂O	2.13 mmol h^-1 g^-1 CH₃OH 0.23 mmol h^-1 g^-1 CH₄	[305]
	L-cysteine/In₄SnS₈	CO₂ and H₂O	10.70 μL h^-1 CH₄ 9.39 μL h^-1 CO	[306]
	Cu-HHTP	CO₂	130 mmol h^-1 g^-1 CO	[188]
	Zr(IV)-MOF BUT-110-65%-Co	CO₂ and H₂O	70.8 μmol h^-1 g^-1 CH₄ 9.0 μmol h^-1 g^-1 CO	[307]
	InVO₄/g-C₃N₄	CO₂ and H₂O	69.8 μmol h^-1 g^-1 CO	[281]
	UiO-66-NH₂-LV	CO₂	35 μmol h^-1 g^-1 CO	[308]
	Imidazolium-modified ZnSe	CO₂	2.4 mmol h^-1 g^-1 CO	[280]
	Pd-hypercrosslinked polymers-TiO₂	CO₂ and H₂O	237.4 μmol h^-1 g^-1 CH₄	[309]
	SnNb₂O₆/CdSe-DETA	CO₂ and H₂O	36.16 μmol h^-1 g^-1 CO	[279]
Photocatalytic sterilization	TiO₂/chlorophyll	Escherichia coli	sterilization (2.94 × 10⁷ cfu cm^-2 180 min)	[310]
	CeO₂/polymeric carbon nitride	staphylococcus aureus (S. aureus)	88.1% sterilization	[89]
	P-doped MoS₂/g-C₃N₄	escherichia coli (E. coli)	99.99% sterilization	[79]
	α-Fe₂O₃/g-C₃N₄	Escherichia coli	sterilization (7 log₁₀ cfu mL^-1 in 120 min)	[282]
	Sn₃O₄/perylene-3,4,9,10-tetracarboxylic diimide	staphylococcus aureus and escherichia coli	94% and 92% sterilization efficiencies for S. aureus and E. coli, respectively	[284]
Photocatalytic nitrogen fixation	Al-PMOF (porphyrin-based metal-organic framework)	N₂	127 μg h^-1 g^-1 NH₃	[293]
	NH₂-MIL-125(Ti)	N₂	12.3 μmol h^-1 g^-1 NH₃	[292]
	Polyacrylonitrile/BiOBr-Cl	N₂	234.4 μmol h^-1 g^-1 NH₃	[311]
	MIL-101(Fe)	N₂	50.355 μmol h^-1 g^-1 NH₃	[312]
	Zn/PbO/PC-Zn/MAPbBr₃	N₂	46.87 μmol h^-1 g^-1 NH₃	[97]

Fig. 18. Density functional theory simulation. (a) Band structure of Ag3PO4. Position of the Fermi level is set as 0 eV. (b) PDOS and TDOS of Ag3PO4. (c) Band structure of the Ag3PO4/PDI composite. (d) Simulated electron density difference of the Ag3PO4/PDI composite. (e) Schematic of the formation of an internal electric field. (f) Schematic of carrier migration on Ag3PO4/PDI under the influence of an internal electric field. Reprinted with permission from Ref. [248]. Copyright 2020, Elsevier.

Fig. 19. (a) Photocatalytic activity for Cu-EDTA degradation. (b) XRD patterns of MIL-53(Fe)-13. (c) Schematic of possible degradation mechanisms of Cu-EDTA via MIL-53(Fe) photocatalysis. Reprinted with permission from Ref. [250]. Copyright 2021, Elsevier.

Fig. 20. (a) SEM images of TCP. (b) HRTEM image of ZnIn2S4/TCP. (c) Photocatalytic H2 production of TCP, ZnIn2S4, and ZnIn2S4/TCP composites. (d) Stability tests for photocatalytic H2 evolution over the optimized ZnIn2S4/TCP. (e) Charge transfer over a ZnIn2S4/TCP composite under visible-light irradiation. Reprinted with permission from Ref. [262]. Copyright 2021, American Chemical Society.

Fig. 21. UV-vis DRS (a) and VB-XPS (b) spectra of anatase TiO2 and TiPNW. The inset of (a) shows the corresponding Tauc plots for the bandgap determination. 3D charge density differences for TiPNW (c) and TiPNW-Br (d) with an isovalue of 3 × 10-4 e Å-3, and the corresponding 2D charge density difference mapping inserted with planar-averaged charge density difference and electrostatic potential at the interfaces of TiPNW and TiPNW-Br. Red ball: O, cyan ball: Ti, gray ball: C, violet ball: P, white ball: H, and brown ball: Br. Apparently, the strong electron-donating feature of -OH induces a more pronounced electron transfer from the organophosphonic ligand to the modeled Ti-oxo cluster. Reprinted with permission from Ref. [263]. Copyright 2020, John Wiley and Sons.

Fig. 22. (a) Schematic of self-polymerization processes of dopamine and the structural diagrams of TiO2@PDA composites. (b) Photocatalytic yields of CH4 and CH3OH for pure TiO2 and TiO2@PDA composites (TP1, TP2, TP3, and TP4). (c) Recycling activity of TP3 for photocatalytic CO2 reduction; Schematic illustration of the relative band energy positions of TiO2 and PDA before contact (d), after contact (e) and under irradiation (f) and the S-scheme charge transfer mechanism between TiO2 and PDA under irradiation. Reprinted with permission from Ref. [278]. Copyright 2021, Elsevier.

Fig. 24. (a) Statistical counts of colonies under illumination and without illumination, respectively. (b) Bacteria removal efficiency over the prepared samples under visible-light illumination (λ ≥ 420 nm). The calculated work function and the corresponding structural model of the (111) plane of CeO2 (c) and the calculated work function and the corresponding structural model of the (001) plane of polymeric C3N4 (d). (e) The planar-averaged electron density difference ∆ρ and side view of the charge density difference over the CeO2/polymeric C3N4 heterojunction. The orange and purple areas represent the depletion and accumulation of electrons, respectively. Reprinted with permission from Ref. [89]. Copyright 2020, John Wiley and Sons.

Fig. 25. (a) UV-vis spectra of MIL-12 (Ti), NH2-MIL-125 (Ti), OH-MIL-125 (Ti), and CH3-MIL-125 (Ti). (b) Schematic images of NH2-MIL-125 (Ti) reveal defect sites in the cluster. (c) Production yield rates of ammonia over photocatalysts for 15 h. (d) Proposed mechanism for photocatalytic N2 fixation over NH2-MIL-125 (Ti). Reprinted with permission from Ref. [292]. Copyright 2020, Elsevier.

Fig. 26. (a) View of the charge difference map (yellow, positive density difference; cyan, negative density difference) for Al-PMOF(Fe)-adsorbing N2: C, gray; N, blue; H, white; O, red; Al, pink; Fe, purple. Free energy diagram of the associative alternating (b) and distal (c) pathways in Al-PMOF(Fe). Reprinted with permission from Ref. [293]. Copyright 2021, American Chemical Society.

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无机-有机杂化光催化剂: 合成、机理及应用

Inorganic-organic hybrid photocatalysts: Syntheses, mechanisms, and applications

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