以石墨烯作用为导向的多功能石墨烯基复合光催化剂

doi:10.1016/S1872-2067(21)63871-8

催化学报 ›› 2022, Vol. 43 ›› Issue (3): 708-730.DOI: 10.1016/S1872-2067(21)63871-8

以石墨烯作用为导向的多功能石墨烯基复合光催化剂

李月华, 唐紫蓉^*(), 徐艺军^#()

福州大学化学学院, 能源与环境光催化国家重点实验室, 福建福州 350116

收稿日期:2021-05-07 修回日期:2021-05-07 出版日期:2022-03-18 发布日期:2022-02-18
通讯作者: 唐紫蓉,徐艺军
基金资助:
国家自然科学基金(22072023);国家自然科学基金(21872029);国家自然科学基金(U1463204);国家自然科学基金(21173045);国家万人计划科技创新领军人才(00387072);闽江学者特聘教授奖励计划;福建省首批青年拔尖创新人才和福建省自然科学基金(2017J07002);福建省首批青年拔尖创新人才和福建省自然科学基金(2019J0106)

Multifunctional graphene-based composite photocatalysts oriented by multifaced roles of graphene in photocatalysis

Yue-Hua Li, Zi-Rong Tang^*(), Yi-Jun Xu^#()

College of Chemistry, State Key Laboratory of Photocatalysis on Energy and Environment, Fuzhou University, Fuzhou 350116, Fujian, China

Received:2021-05-07 Revised:2021-05-07 Online:2022-03-18 Published:2022-02-18
Contact: Zi-Rong Tang, Yi-Jun Xu
Supported by:
National Natural Science Foundation of China(22072023);National Natural Science Foundation of China(21872029);National Natural Science Foundation of China(U1463204);National Natural Science Foundation of China(21173045);Program for National Science and Technology Innovation Leading Talents(00387072);Award Program for Minjiang Scholar Professorship, the 1st Program of Fujian Province for Top Creative Young Talents;Natural Science Foundation of Fujian Province(2017J07002);Natural Science Foundation of Fujian Province(2019J0106)

摘要/Abstract

摘要：

具有单层二维蜂窝状结构的石墨烯在材料科学和能源转化领域吸引了巨大的研究兴趣. 在光催化领域, 因其独特的二维平面结构、优异的电荷传输能力、超高的理论比表面积、良好的透光性和化学稳定性, 可作为高效的助催化剂, 以提高光催化体系的太阳能转换效率. 在一些特定的光催化体系中, 石墨烯还可以作为大分子光敏剂产生光生电子. 近年来, 石墨烯基复合光催化剂, 如石墨烯-半导体、石墨烯-金属和石墨烯-有机物复合材料, 已被广泛应用于光催化水分解制氢、环境净化、二氧化碳还原和选择性有机合成, 为缓解能源与环境问题提供了一种有效策略.
众所周知, 合成方法对石墨烯基复合光催化剂的形貌、尺寸、缺陷结构、表界面性质等影响很大, 这些性质与石墨烯基复合光催化剂的催化性能密切相关. 因此, 探索合适的合成方法制备具有目标功能结构的高效石墨烯基复合光催化剂, 具有重要的科学意义. 现有的合成方法主要包括: 水热/溶剂热法、煅烧法、低温油浴法、溶胶-凝胶法、超声辅助沉积法、微波辅助合成法、电化学沉积法、光化学还原法等. 根据概念进行归类, 可分为非原位合成法和原位合成法.
在非原位合成中, 预制的光活性材料的形貌和尺寸保持不变, 有利于实现对石墨烯基复合光催化剂微观结构的精确控制, 以及对空白光活性组分和复合光催化剂性能进行比较. 在原位合成中, 石墨烯或其前驱体不仅可以作为二维模板调控纳米晶的成核和生长, 合成具有可控形貌和良好界面接触的石墨烯基复合光催化剂, 还可以作为三维石墨烯凝胶的自组装模板. 此外, 氧化石墨烯作为常用的石墨烯前驱体, 可以同时作为模板和表面活性剂, 灵活调控一些特定复合材料的形貌、尺寸和缺陷结构等.
鉴于已有大量综述系统地总结了石墨烯基复合光催化剂的分类、合成方法、性质和应用等, 本文先介绍石墨烯基复合光催化剂的优化策略, 例如降低石墨烯的缺陷密度、化学掺杂、优化维数、沉积助催化剂、优化界面参数; 再以石墨烯在光催化中的基本作用为导向, 讨论石墨烯基复合光催化剂的合成. 最后, 对石墨烯基复合催化剂在光催化领域面临的挑战和优化策略进行了展望, 希望为多功能石墨烯基复合光催化剂的合理制备及高效利用提供参考.

关键词: 石墨烯, 复合光催化剂, 优化策略, 合成方法, 石墨烯的多重作用, 光催化应用

Abstract:

Graphene (GR), a single-layer carbon sheet with a hexagonal packed lattice structure, has displayed attractive potential and demonstrably become the research focus in artificial photocatalysis due to its enchanting properties in enhancing light absorption, electron transfer dynamics, and surface reactions. Currently, numerous efforts have shown that the properties of GR, which are closely correlated to the photocatalytic performance of GR-based composites are significantly affected by the synthesis methods. Herein, we first introduce the optimization strategies of GR-based hybrids and then elaborate the synthesis of GR-based composite photocatalysts oriented by manifold roles of GR in photoredox catalysis, containing photoelectron mediator and acceptor, improving adsorption capacity, regulating light absorption range and intensity, as well as macromolecular photosensitizer. Beyond that, a brief outlook on the challenges in this burgeoning research field and potential evolution strategies for enhancing the photoactivity of GR-based hybrids is presented and we anticipate that this review could provide some enlightenments for the rational construction and application of multifunctional GR-based composite photocatalysts.

Key words: Graphene, Composite photocatalyst, Optimization strategies, Synthesis method, Multifarious roles of graphene, Photocatalytic applications

李月华, 唐紫蓉, 徐艺军. 以石墨烯作用为导向的多功能石墨烯基复合光催化剂[J]. 催化学报, 2022, 43(3): 708-730.

Yue-Hua Li, Zi-Rong Tang, Yi-Jun Xu. Multifunctional graphene-based composite photocatalysts oriented by multifaced roles of graphene in photocatalysis[J]. Chinese Journal of Catalysis, 2022, 43(3): 708-730.

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Entry	Composite photocatalyst	Light source	Reaction type	Reaction conditions	Ref. Year
1	TNTAs@rGO/MoS₂^a	300 W Xe lamp, 320-780 nm	H₂ evolution	vacuum, methanol (10 vol%) or lactic acid (10 vol%)	[58] 2018
2	Ni₂P-FGR ^b	300 W Xe lamp, ≥ 420 nm	H₂ evolution	vacuum, TEOA^c (10 vol%), Eosin Y	[59] 2018
3	CdS-EGR^dCdS-rGO	300 W Xe lamp, ≥ 420 nm	H₂ evolution	vacuum, lactic acid (10 vol%)	[60] 2018
4	CH₃NH₃PbI₃/rGO	300 W Xe lamp, ≥ 420 nm	H₂ evolution	HI solution	[61] 2018
5	Fe₂O₃/rGO/PCN^e	300 W Xe lamp, ≥ 420 nm	overall water splitting	H₂O, H₂PtCl₆	[62] 2019
6	graphene/carbon nitride	¹300 W Xe lamp, ≥ 420 nm ²LED solar simulator	¹H₂ evolution ²photooxidation of 1,4-DHP^f	¹N₂, TEOA (10 vol%), H₂PtCl₆ ²10^‒4 mol/L 1,4-DHP	[63] 2020
7	rGO-CoO_x/BiVO₄- Pt-metal sulfides^g	300 W Xe lamp, ≥ 420 nm	overall water splitting CO₂ reduction to CO	Ar gas flow, H₂O CO₂ gas flow, H₂O	[64] 2016
8	CsPbBr₃ QD/GO^h	100 W Xe lamp, AM 1.5 G	CO₂ reduction to CO	CO₂, ethyl acetate	[65] 2017
9	nanographene-rhenium complex	100 W tungsten lamp, ≥ 490 nm	CO₂ reduction to CO	CO₂, tetrahydrofuran, TEOA	[66] 2017
10	NH₂-rGO/Al-PMOFⁱ	125 W medium-pressure mercury lamp	CO₂ reduction to formate	CO₂, TEOA/acetonitrile (v:v = 1:5)	[9] 2018
11	hypercrosslinked polymer-TiO₂-GR	300 W Xe lamp, ≥ 420 nm	CO₂ reduction to CH₄ and CO	CO₂, H₂O	[30] 2019
12	N-doped GR/CdS	350 W Xe lamp, ≥ 420 nm	CO₂ reduction to CO and CH₄	CO₂, H₂O	[28] 2019
13	α-Fe₂O₃/amine-rGO/ CsPbBr₃	150 W Xe lamp, ≥ 420 nm or AM 1.5 G	CO₂ reduction to CH₄ and CO	CO₂, H₂O	[67] 2020
14	CsPbBr₃/USGO/α-Fe₂O₃^j	300 W Xe lamp, ≥ 400 nm	CO₂ reduction to CO	CO₂, acetonitrile/H₂O (v:v = 200:1)	[68] 2020
15	Cs₄PbBr₆/rGO	300 W Xe lamp, ≥ 400 nm	CO₂ reduction to CO	CO₂, ethyl acetate/H₂O (v:v = 1000:1)	[69] 2020
16	ZnPc/GR/BiVO₄^k	300 W Xe lamp, ≥ 420 nm	CO₂ reduction to CH₄ and CO	CO₂, H₂O
17	TaON@GR	300 W Xe lamp, ≥ 420 nm	CO₂ reduction to CH₄	CO₂, H₂O	[27] 2020
18	transition metal hydroxide-GR^l	300 W Xe lamp, ≥ 420 nm	CO₂ reduction to CO	CO₂, TEOA, acetonitrile/H₂O (v:v = 3:2), [Ru(bpy)₃]Cl₂·6H₂O	[48] 2020
19	Co-metal-organic layers@GR	Blue LED, λ = 450 nm	CO₂ reduction to CO	CO₂, TEOA, acetonitrile/H₂O (v:v = 4:1), [Ru(phen)₃] (PF₆)₂	[70] 2021
20	single Co atoms/GR	300 W Xe lamp, ≥ 420 nm	CO₂ reduction to CO	CO₂, acetonitrile/TEOA/H₂O (v:v:v = 3:1:1), [Ru(bpy)₃]Cl₂·6H₂O	[71] 2018
Entry	Composite photocatalyst	Light source	Reaction type	Reaction conditions	Ref. Year
21	MIL-53(Fe)-GR	500 W Xe lamp, ≥ 400 nm	photooxidation of benzyl alcohols	CCl₄, benzyl alcohols	[72] 2016
22	Eu-based MOF/GO	5 W LED	photooxidation of benzyl alcohol	N₂, benzyl alcohol, acetonitrile/H₂O (v:v = 2:1)	[12] 2017
23	Cu₂O-MoS₂/GR	24 W compact fluorescent bulb	oxidative C-C bond formation	N-aryl-tetrahydroisoquinoline and nitromethane	[73] 2017
24	GR/Ag/α-Al₂O₃	0.5 W laser, 514.5 nm	photo-epoxidation of ethylene	C₂H₄ and air	[74] 2018
25	Ni₂P-graphene-TiO₂	300 W Xe lamp, ≥ 420 nm	photooxidation of benzyl alcohol coupled with H₂ evolution	N₂, benzyl alcohol solution	[75] 2019
26	Cu₂S:NiS₂@C/rGO	300 W Xe lamp, 400-800 nm	¹chan-Lam coupling reaction ²cyclization reaction³oxidative homocoupling reaction	¹phenylboronic acid and imidazole, methanol/H₂O (v:v = 3:1) ²1,2-phenylenediamine, aromatic aldehyde, ethanol ³benzylamine, acetonitrile	[76] 2021
27	CdS/GR	500 W tungsten-halogen lamp	photodegradation of Rhodamine B	rhodamine B solution	[77] 2017
28	BiOI/GO	5 W LED, ≥ 400 nm	photodegradation of phenol	phenol solution	[78] 2020
29	GR/ZnO	125 W, λ = 365 nm	photodegradation of Rhodamine B, methyl orange, and Methylene blue	rhodamine B solution, methyl orange solution, and Methylene blue solution	[79] 2021
30	Fe₃O₄/polypyrrole/rGO	250 W tungsten-halogen lamp (two)	degradation of acetaminophen	acetaminophen solution, pH = 6.7 ± 0.2	[80] 2021
31	TiO₂/g-C₃N₄/GR	300 W Xe lamp	reduction of nitrobenzene	N₂, nitrobenzene, methanol solution	[81] 2017
32	g-C₃N₄/aromatic diimide/GR	2 kW Xe lamp, ≥ 420 nm	H₂O₂ production	O₂, H₂O	[82] 2016
33	Bismuth-graphene	direct sunshine (0.039-0.048 W cm^‒2)	¹degradation of Methyl orange ²reduction of Cr (VI)	methyl orange solution (pH = 2)	[83] 2017
34	3DG-organic hybrid^m	300 W Xe lamp, ≥ 420 nm	reduction of 4-nitroaniline reduction of Cr (VI)	N₂, 4-nitroaniline solution, TEOA N₂, Cr (VI) solution, TEOA	[19] 2018
35	Ti₃C₂T_x/GO-Eosin Y	300 W Xe lamp, ≥ 420 nm	reduction of Cr (VI)	N₂, Cr (VI) solution (pH = 7), TEOA	[84] 2019
36	Carbon QDs/GR aerogelⁿ	300 W Xe lamp, 200-780 nm	reduction of Cr (VI)	N₂, Cr (VI) solution, TEOA	[20] 2019
37	NCQDs/GA^o	300 W Xe lamp, ≥ 420 nm	reduction of Cr (VI)	N₂, Cr (VI) solution, TEOA	[18] 2019
38	CdSe QDs/graphene/TiO₂	350 W Xe lamp, ≥ 420 nm	E. coli disinfection	e. coli, 0.9% NaCl solution, 37 °C	[85] 2018
39	GR/AgBr/Ag aerogel	300 W Xe lamp, ≥ 400 nm	E. coli disinfection	e. coli, phosphate-buffered saline buffer (pH = 7.4), 25 °C	[52] 2019
40	GO@polyoxometalate	300 W Xe lamp	N₂ fixation	N₂, H₂O, Nessler’s reagent	[86] 2019
41	rGO/red phosphorus	300 W Xe lamp, ≥ 400 nm	N₂ fixation	N₂, H₂O, Nessler’s reagent	[87] 2021

Entry	Composite photocatalyst	Light source	Reaction type	Reaction conditions	Ref. Year
1	TNTAs@rGO/MoS₂^a	300 W Xe lamp, 320-780 nm	H₂ evolution	vacuum, methanol (10 vol%) or lactic acid (10 vol%)	[58] 2018
2	Ni₂P-FGR ^b	300 W Xe lamp, ≥ 420 nm	H₂ evolution	vacuum, TEOA^c (10 vol%), Eosin Y	[59] 2018
3	CdS-EGR^dCdS-rGO	300 W Xe lamp, ≥ 420 nm	H₂ evolution	vacuum, lactic acid (10 vol%)	[60] 2018
4	CH₃NH₃PbI₃/rGO	300 W Xe lamp, ≥ 420 nm	H₂ evolution	HI solution	[61] 2018
5	Fe₂O₃/rGO/PCN^e	300 W Xe lamp, ≥ 420 nm	overall water splitting	H₂O, H₂PtCl₆	[62] 2019
6	graphene/carbon nitride	¹300 W Xe lamp, ≥ 420 nm ²LED solar simulator	¹H₂ evolution ²photooxidation of 1,4-DHP^f	¹N₂, TEOA (10 vol%), H₂PtCl₆ ²10^‒4 mol/L 1,4-DHP	[63] 2020
7	rGO-CoO_x/BiVO₄- Pt-metal sulfides^g	300 W Xe lamp, ≥ 420 nm	overall water splitting CO₂ reduction to CO	Ar gas flow, H₂O CO₂ gas flow, H₂O	[64] 2016
8	CsPbBr₃ QD/GO^h	100 W Xe lamp, AM 1.5 G	CO₂ reduction to CO	CO₂, ethyl acetate	[65] 2017
9	nanographene-rhenium complex	100 W tungsten lamp, ≥ 490 nm	CO₂ reduction to CO	CO₂, tetrahydrofuran, TEOA	[66] 2017
10	NH₂-rGO/Al-PMOFⁱ	125 W medium-pressure mercury lamp	CO₂ reduction to formate	CO₂, TEOA/acetonitrile (v:v = 1:5)	[9] 2018
11	hypercrosslinked polymer-TiO₂-GR	300 W Xe lamp, ≥ 420 nm	CO₂ reduction to CH₄ and CO	CO₂, H₂O	[30] 2019
12	N-doped GR/CdS	350 W Xe lamp, ≥ 420 nm	CO₂ reduction to CO and CH₄	CO₂, H₂O	[28] 2019
13	α-Fe₂O₃/amine-rGO/ CsPbBr₃	150 W Xe lamp, ≥ 420 nm or AM 1.5 G	CO₂ reduction to CH₄ and CO	CO₂, H₂O	[67] 2020
14	CsPbBr₃/USGO/α-Fe₂O₃^j	300 W Xe lamp, ≥ 400 nm	CO₂ reduction to CO	CO₂, acetonitrile/H₂O (v:v = 200:1)	[68] 2020
15	Cs₄PbBr₆/rGO	300 W Xe lamp, ≥ 400 nm	CO₂ reduction to CO	CO₂, ethyl acetate/H₂O (v:v = 1000:1)	[69] 2020
16	ZnPc/GR/BiVO₄^k	300 W Xe lamp, ≥ 420 nm	CO₂ reduction to CH₄ and CO	CO₂, H₂O
17	TaON@GR	300 W Xe lamp, ≥ 420 nm	CO₂ reduction to CH₄	CO₂, H₂O	[27] 2020
18	transition metal hydroxide-GR^l	300 W Xe lamp, ≥ 420 nm	CO₂ reduction to CO	CO₂, TEOA, acetonitrile/H₂O (v:v = 3:2), [Ru(bpy)₃]Cl₂·6H₂O	[48] 2020
19	Co-metal-organic layers@GR	Blue LED, λ = 450 nm	CO₂ reduction to CO	CO₂, TEOA, acetonitrile/H₂O (v:v = 4:1), [Ru(phen)₃] (PF₆)₂	[70] 2021
20	single Co atoms/GR	300 W Xe lamp, ≥ 420 nm	CO₂ reduction to CO	CO₂, acetonitrile/TEOA/H₂O (v:v:v = 3:1:1), [Ru(bpy)₃]Cl₂·6H₂O	[71] 2018
Entry	Composite photocatalyst	Light source	Reaction type	Reaction conditions	Ref. Year
21	MIL-53(Fe)-GR	500 W Xe lamp, ≥ 400 nm	photooxidation of benzyl alcohols	CCl₄, benzyl alcohols	[72] 2016
22	Eu-based MOF/GO	5 W LED	photooxidation of benzyl alcohol	N₂, benzyl alcohol, acetonitrile/H₂O (v:v = 2:1)	[12] 2017
23	Cu₂O-MoS₂/GR	24 W compact fluorescent bulb	oxidative C-C bond formation	N-aryl-tetrahydroisoquinoline and nitromethane	[73] 2017
24	GR/Ag/α-Al₂O₃	0.5 W laser, 514.5 nm	photo-epoxidation of ethylene	C₂H₄ and air	[74] 2018
25	Ni₂P-graphene-TiO₂	300 W Xe lamp, ≥ 420 nm	photooxidation of benzyl alcohol coupled with H₂ evolution	N₂, benzyl alcohol solution	[75] 2019
26	Cu₂S:NiS₂@C/rGO	300 W Xe lamp, 400-800 nm	¹chan-Lam coupling reaction ²cyclization reaction³oxidative homocoupling reaction	¹phenylboronic acid and imidazole, methanol/H₂O (v:v = 3:1) ²1,2-phenylenediamine, aromatic aldehyde, ethanol ³benzylamine, acetonitrile	[76] 2021
27	CdS/GR	500 W tungsten-halogen lamp	photodegradation of Rhodamine B	rhodamine B solution	[77] 2017
28	BiOI/GO	5 W LED, ≥ 400 nm	photodegradation of phenol	phenol solution	[78] 2020
29	GR/ZnO	125 W, λ = 365 nm	photodegradation of Rhodamine B, methyl orange, and Methylene blue	rhodamine B solution, methyl orange solution, and Methylene blue solution	[79] 2021
30	Fe₃O₄/polypyrrole/rGO	250 W tungsten-halogen lamp (two)	degradation of acetaminophen	acetaminophen solution, pH = 6.7 ± 0.2	[80] 2021
31	TiO₂/g-C₃N₄/GR	300 W Xe lamp	reduction of nitrobenzene	N₂, nitrobenzene, methanol solution	[81] 2017
32	g-C₃N₄/aromatic diimide/GR	2 kW Xe lamp, ≥ 420 nm	H₂O₂ production	O₂, H₂O	[82] 2016
33	Bismuth-graphene	direct sunshine (0.039-0.048 W cm^‒2)	¹degradation of Methyl orange ²reduction of Cr (VI)	methyl orange solution (pH = 2)	[83] 2017
34	3DG-organic hybrid^m	300 W Xe lamp, ≥ 420 nm	reduction of 4-nitroaniline reduction of Cr (VI)	N₂, 4-nitroaniline solution, TEOA N₂, Cr (VI) solution, TEOA	[19] 2018
35	Ti₃C₂T_x/GO-Eosin Y	300 W Xe lamp, ≥ 420 nm	reduction of Cr (VI)	N₂, Cr (VI) solution (pH = 7), TEOA	[84] 2019
36	Carbon QDs/GR aerogelⁿ	300 W Xe lamp, 200-780 nm	reduction of Cr (VI)	N₂, Cr (VI) solution, TEOA	[20] 2019
37	NCQDs/GA^o	300 W Xe lamp, ≥ 420 nm	reduction of Cr (VI)	N₂, Cr (VI) solution, TEOA	[18] 2019
38	CdSe QDs/graphene/TiO₂	350 W Xe lamp, ≥ 420 nm	E. coli disinfection	e. coli, 0.9% NaCl solution, 37 °C	[85] 2018
39	GR/AgBr/Ag aerogel	300 W Xe lamp, ≥ 400 nm	E. coli disinfection	e. coli, phosphate-buffered saline buffer (pH = 7.4), 25 °C	[52] 2019
40	GO@polyoxometalate	300 W Xe lamp	N₂ fixation	N₂, H₂O, Nessler’s reagent	[86] 2019
41	rGO/red phosphorus	300 W Xe lamp, ≥ 400 nm	N₂ fixation	N₂, H₂O, Nessler’s reagent	[87] 2021

Entry	Composite photocatalyst	Precursor of GR	Precursor of other component	Preparation method	Ref. Year
1	GR@TiO₂	GO prepared by modified Hummers’ method	tetrabutyl orthotitanate	GR@TiO₂ prepared by sol-gel process (in the mixture of ethanol, benzyl alcohol and H₂O), calcination (N₂, 450 °C, 2 h)	[117] 2014
2	TiO₂/GR	GO prepared by modified Hummers’ method	commercial TiO₂	TiO₂/GR prepared by mechanical mixing of GO and TiO₂ in 1-butyl alcohol (ultrasonication 0.5 h), catalysts dried at 100 °C	[139] 2017
3	TiO₂/GR	GO prepared by conventional Hummers’ method	P25	GO and P25 mixed in NH₃ solution (60 °C, 2 h), GO reduced by N₂H₄, catalysts dried at 200 °C	[140] 2017
4	TiO₂@rGO	GO prepared by modified Hummers’ method	P25	GO and P25 mixed in ethanol, GO reduced under ultraviolet light (N₂)	[141] 2017
5	TNTAs@rGO/ MoS₂	GO prepared by modified Hummers’ method	Ti foil	TNTAs prepared by anodic oxidization of Ti foil, rGO electrodeposited on TNTAs, MoS₂ photodeposited on TNTAs@rGO	[58] 2018
6	TiO₂/graphene	graphite powder	titanium tetra-n-butoxide	graphene obtained by chemical exfoliation of graphite in titanium tetra-n-butoxide (60 °C, 4 h, N₂), TiO₂ prepared by sol-gel method	[142] 2018
7	hypercross-linked polymer-TiO₂-GR	GO prepared by modified Hummers’ method	lamellar protonated titanate	solvothermal method (lamellar protonated titanate, GO, isopropyl alcohol, fluoric acid, glucose, 180 °C, 12 h)	[30] 2020
8	ZnO/rGO	GO prepared by modified Hummers’ method	Zn(CH₃COO)₂·2H₂O	ZnO/rGO prepared by solvothermal method (ethanol, NaOH, 160 °C, 24 h)	[143] 2016
9	ZnO nanoring/rGO	GO prepared by modified Hummers’ method	Zn(CH₃COO)₂·2H₂O	ZnO nanoring/rGO prepared by hydrolysis and chemical etching approach (cetyltrimethylammonium bromide, dimethyl sulfoxide, heat in an oven, 70 °C, 1.5 h)	[144] 2017
10	ZnO/Thermally reduced graphene	GO prepared by modified Hummers’ method	Zn(CO₃)₂(OH)₆	ZnO/thermally reduced graphene synthesized by ball milling of GO and Zn(CO₃)₂(OH)₆, calcination (inert gas, 400 °C, 2 h)	[145] 2019
11	GR/ZnO	GO prepared by modified Hummers’ method	Zn(CH₃COO)₂·2H₂O	GR/ZnO prepared by dissolving Zn(CH₃COO)₂·2H₂O in GO suspension and stirring for 3 h, GO reduced by adding N₂H₄ and stirring for 3 h	[146] 2020
12	ZnO-GO	GO prepared by modified Hummers’ method	Zn(CH₃COO)₂·2H₂O	ZnO-GO prepared by ultrasonic mixing and freeze-drying	[147] 2020
13	WO₃/rGO	GO prepared by modified Hummers’ method	Na₂WO₄·2H₂O, NaCl	WO₃/rGO prepared by hydrothermal method (180 °C, 15 h)	[148] 2018
14	SnO₂ microspheres-GOs	GO prepared by modified Hummers’ method	Na₂SnO₃·4H₂O	SnO₂ microspheres-GOs prepared by hydrothermal method (180 °C, 15 h)	[149] 2016
15	SnO₂-rGO	GO prepared by modified Hummers’ method	SnSO₄	SnSO₄ first dissolved in H₂SO₄ and GO solution, then reduced by ultraviolet light	[150] 2017
16	Cu₂O-dG^a	Alginic acid sodium salt	Cu(NO₃)₂·H₂O	dG prepared by alginate pyrolysis (inert gas, 200 °C, 2 h; 900 °C, 2 h), Cu₂O-dG prepared by heating the mixture of Cu(NO₃)₂·H₂O, dG and ethylene glycol at 900 °C for 2 h	[151] 2018
17	GO/TiO₂/ Bi₂WO₆	GO manufactured by the XFNANO of China	Bi(NO₃)₃·5H₂O, Na₂WO₆·2H₂O	GO/TiO₂/Bi₂WO₆ prepared by hydrothermal process (160 °C, 15 h)	[89] 2019
18	rGO/BiOBr	GO prepared by modified Hummers’ method	Bi(NO₃)₃·5H₂O, KBr	GO reduced to rGO by l-ascorbic acid, rGO/BiOBr obtained by hydrothermal process (160 °C, 12 h)	[152] 2019
19	ZnPc/GR/BiVO₄	Polyacrylic weak-acid cation-exchanged resin	BiCl₃, NaVO₃	GR prepared by in situ self-generating template route, BiVO₄ prepared by hydrothermal process (120 °C, 12 h), GR/BiVO₄ obtained by hydroxyl-induced assembly method (150 °C, 4 h), ZnPc/GR/BiVO₄ obtained by assembly process in absolute ethyl alcohol	[153] 2020
Entry	Composite photocatalyst	Precursor of GR	Precursor of other component	Preparation method	Ref. Year
20	GNs-CdS QDs^b	GO prepared by modified Hummers’ method	Na₂S, CdCl₂	CdS QDs prepared by heat injection method, GNs-CdS QDs prepared by layer-by-layer self-assembly method	[154] 2014
21	CdS-rGO	GO prepared by modified Hummers’ method	Cd(CH₃CO₂)₂·2H₂O, thiourea	CdS-rGO prepared by hydrothermal method (180 °C, 12 h)	[155] 2017
22	CdS/ m-TiO₂/G^c	GO prepared by modified Hummers’ method	Cd(CH₃COO)₂·2H₂O, dimethyl sulfoxide	m-TiO₂ prepared by sol-gel and hydrothermal process, CdS/m-TiO₂/G prepared by solvothermal method (180 °C, 12 h)	[156] 2018
23	Ni-NG/CdS^d	GO prepared by modified Hummers’ method	commercial CdS	Ni-NG prepared by impregnation and calcination process (NH₃, 750 °C, 1 h), Ni-NG/CdS prepared by self-assembly route	[157] 2018
24	N-doped GR/CdS	GO prepared by modified Hummers’ method	CdCl₂, sodium citrate, ammonia, thiourea	CdS/SiO₂ prepared by using SiO₂ as sacrificial template, N-doped GR deposited on CdS/SiO₂ by a chemical vapor deposition at 700 °C	[28] 2019
25	NiS_x/Cd_0.8Zn_0.2S/rGO	GO prepared by modified Hummers’ method	Zn(NO₃)₂·6H₂O, CdCl₂·2.5H₂O, Ni(NO₃)₂·6H₂O, glucose, L-cysteine	NiS_x/Cd_0.8Zn_0.2S/rGO prepared by hydrothermal method (160 °C, 2 h)	[158] 2018
26	ZnIn₂S₄-GR	GO prepared by modified Hummers’ method	ZnCl₂, InCl₃·4H₂O, thioacetamide	ZnIn₂S₄-GR prepared by refluxing wet chemistry method (95 °C, 5 h)	[116] 2014
27	CdS/ZnIn₂S₄/ rGO	GO prepared by modified Hummers’ method	Cd(NO₃)₂, sulfur powder, ethanediamine, thioacetamide, In (NO₃)₃, Zn(CH₃COO)₂	CdS/ZnIn₂S₄ prepared by solvothermal method, GO reduced by N₂H₄ and NH₃ solution (95 °C, 1 h), CdS/ZnIn₂S₄/rGO prepared by electrostatic self-assembly process	[159] 2017
28	rGO/ZnIn₂S₄	GO prepared by modified Hummers’ method	ZnSO₄·7H₂O, In(NO₃)₃·4H₂O, thioacetamide	rGO/ZnIn₂S₄ prepared by alcohothermal method (ethanol, glycerol, 180 °C, 12 h)	[160] 2019
29	Ag:ZnIn₂S₄/ rGO	GO prepared by modified Hummers’ method	In(OOCCH₃)₃, Zn(CH₃COO)₂·2H₂O	Ag:ZnIn₂S₄/rGO prepared by hydrothermal method (180 °C, 12 h)	[161] 2020
30	CsPbBr₃QDs/GO	GO prepared by modified Hummers’ method	Cs-oleate, PbBr₂	CsPbBr₃QDs and CsPbBr₃QDs/GO prepared by antisolvent precipitation method	[65] 2017
31	LaCoO₃/ attapulgite/ rGO	GO prepared by modified Hummers’ method	La(NO₃)₃·6H₂O Co(NO₃)₂·6H₂O	LaCoO₃/attapulgite prepared by sol-gel method and calcination (600 °C, 2 h), LaCoO₃/attapulgite/rGO prepared by self-assembly process	[162] 2018
32	CsPbBr₃/USGO/ α-Fe₂O₃	GO prepared by modified Hummers’ method	Cs₂CO₃, PbBr₂	CsPbBr₃prepared by heat injection method, USGO/α-Fe₂O₃ prepared by hydrothermal process (180 °C, 12 h), CsPbBr₃/USGO/α-Fe₂O₃ prepared by electrostatic self-assembly process	[68] 2020
33	α-Fe₂O₃/Amine-rGO/ CsPbBr₃	GO prepared by modified Hummers’ method	Cs-oleate, PbBr₂	α-Fe₂O₃ nanorod array film prepared by hydrothermal process, α-Fe₂O₃/Amine-rGO prepared by electrostatic self-assembly process, α-Fe₂O₃/Amine-rGO/CsPbBr₃ prepared by solvent evaporation deposition approach	[67] 2020
34	Cs₂AgBiBr₆/ rGO	GO prepared by modified Hummers’ method	BiBr₃, AgBr, HBr acid, CsBr	Cs₂AgBiBr₆ prepared by oil bath method, Cs₂AgBiBr₆/rGO prepared by photoreduction process	[163] 2020
35	MIL-LIC-1(Eu) @GO	GO prepared by modified Hummers’ method	EuCl₃·6H₂O, 2-aminotere-phthalic acid	MIL-LIC-1(Eu) prepared by solvothermal method (N,N′-dimethylformamide, 120 °C, 20 h), MIL-LIC-1(Eu)@GO prepared by heating the mixture of GO/H₂O and MIL-LIC-1(Eu)/H₂O at 120 °C for 12 h	[12] 2017
36	NH₂-rGO/ Al-PMOF	Graphenea	AlCl₃, 4-carboxyphenyl porphyrin	NH₂-rGO obtained by solvothermal method (ammonia water, 180 °C, 10 h), NH₂-rGO/Al-PMOF obtained by hydrothermal method (180 °C, 24 h),	[9] 2018
37	Co-MOL@GO^e	GO prepared by modified Hummers’ method	CoCl₂·6H₂O, 5-(1H-1,2,4-triazol-1-yl) isophthalic acid	Co@GO obtained by oil bath (80 °C, 24 h), Co-MOL@GO obtained by solvothermal method (N,N′-dimethylformamide, H₂O, acetic acid, 130 °C, 4 h)	[70] 2021
38	rGO- TpPa-1-COF^f	GO prepared by modified Hummers’ method	1,3,5-Triformylphloroglucinol, p-Phenylenediamine	rGO-TpPa-1-COF obtained by heating the mixture of precursors, N,N′-dimethylformamide and acetic acid at 120 °C for 72 h	[164] 2020

Entry	Composite photocatalyst	Precursor of GR	Precursor of other component	Preparation method	Ref. Year
1	GR@TiO₂	GO prepared by modified Hummers’ method	tetrabutyl orthotitanate	GR@TiO₂ prepared by sol-gel process (in the mixture of ethanol, benzyl alcohol and H₂O), calcination (N₂, 450 °C, 2 h)	[117] 2014
2	TiO₂/GR	GO prepared by modified Hummers’ method	commercial TiO₂	TiO₂/GR prepared by mechanical mixing of GO and TiO₂ in 1-butyl alcohol (ultrasonication 0.5 h), catalysts dried at 100 °C	[139] 2017
3	TiO₂/GR	GO prepared by conventional Hummers’ method	P25	GO and P25 mixed in NH₃ solution (60 °C, 2 h), GO reduced by N₂H₄, catalysts dried at 200 °C	[140] 2017
4	TiO₂@rGO	GO prepared by modified Hummers’ method	P25	GO and P25 mixed in ethanol, GO reduced under ultraviolet light (N₂)	[141] 2017
5	TNTAs@rGO/ MoS₂	GO prepared by modified Hummers’ method	Ti foil	TNTAs prepared by anodic oxidization of Ti foil, rGO electrodeposited on TNTAs, MoS₂ photodeposited on TNTAs@rGO	[58] 2018
6	TiO₂/graphene	graphite powder	titanium tetra-n-butoxide	graphene obtained by chemical exfoliation of graphite in titanium tetra-n-butoxide (60 °C, 4 h, N₂), TiO₂ prepared by sol-gel method	[142] 2018
7	hypercross-linked polymer-TiO₂-GR	GO prepared by modified Hummers’ method	lamellar protonated titanate	solvothermal method (lamellar protonated titanate, GO, isopropyl alcohol, fluoric acid, glucose, 180 °C, 12 h)	[30] 2020
8	ZnO/rGO	GO prepared by modified Hummers’ method	Zn(CH₃COO)₂·2H₂O	ZnO/rGO prepared by solvothermal method (ethanol, NaOH, 160 °C, 24 h)	[143] 2016
9	ZnO nanoring/rGO	GO prepared by modified Hummers’ method	Zn(CH₃COO)₂·2H₂O	ZnO nanoring/rGO prepared by hydrolysis and chemical etching approach (cetyltrimethylammonium bromide, dimethyl sulfoxide, heat in an oven, 70 °C, 1.5 h)	[144] 2017
10	ZnO/Thermally reduced graphene	GO prepared by modified Hummers’ method	Zn(CO₃)₂(OH)₆	ZnO/thermally reduced graphene synthesized by ball milling of GO and Zn(CO₃)₂(OH)₆, calcination (inert gas, 400 °C, 2 h)	[145] 2019
11	GR/ZnO	GO prepared by modified Hummers’ method	Zn(CH₃COO)₂·2H₂O	GR/ZnO prepared by dissolving Zn(CH₃COO)₂·2H₂O in GO suspension and stirring for 3 h, GO reduced by adding N₂H₄ and stirring for 3 h	[146] 2020
12	ZnO-GO	GO prepared by modified Hummers’ method	Zn(CH₃COO)₂·2H₂O	ZnO-GO prepared by ultrasonic mixing and freeze-drying	[147] 2020
13	WO₃/rGO	GO prepared by modified Hummers’ method	Na₂WO₄·2H₂O, NaCl	WO₃/rGO prepared by hydrothermal method (180 °C, 15 h)	[148] 2018
14	SnO₂ microspheres-GOs	GO prepared by modified Hummers’ method	Na₂SnO₃·4H₂O	SnO₂ microspheres-GOs prepared by hydrothermal method (180 °C, 15 h)	[149] 2016
15	SnO₂-rGO	GO prepared by modified Hummers’ method	SnSO₄	SnSO₄ first dissolved in H₂SO₄ and GO solution, then reduced by ultraviolet light	[150] 2017
16	Cu₂O-dG^a	Alginic acid sodium salt	Cu(NO₃)₂·H₂O	dG prepared by alginate pyrolysis (inert gas, 200 °C, 2 h; 900 °C, 2 h), Cu₂O-dG prepared by heating the mixture of Cu(NO₃)₂·H₂O, dG and ethylene glycol at 900 °C for 2 h	[151] 2018
17	GO/TiO₂/ Bi₂WO₆	GO manufactured by the XFNANO of China	Bi(NO₃)₃·5H₂O, Na₂WO₆·2H₂O	GO/TiO₂/Bi₂WO₆ prepared by hydrothermal process (160 °C, 15 h)	[89] 2019
18	rGO/BiOBr	GO prepared by modified Hummers’ method	Bi(NO₃)₃·5H₂O, KBr	GO reduced to rGO by l-ascorbic acid, rGO/BiOBr obtained by hydrothermal process (160 °C, 12 h)	[152] 2019
19	ZnPc/GR/BiVO₄	Polyacrylic weak-acid cation-exchanged resin	BiCl₃, NaVO₃	GR prepared by in situ self-generating template route, BiVO₄ prepared by hydrothermal process (120 °C, 12 h), GR/BiVO₄ obtained by hydroxyl-induced assembly method (150 °C, 4 h), ZnPc/GR/BiVO₄ obtained by assembly process in absolute ethyl alcohol	[153] 2020
Entry	Composite photocatalyst	Precursor of GR	Precursor of other component	Preparation method	Ref. Year
20	GNs-CdS QDs^b	GO prepared by modified Hummers’ method	Na₂S, CdCl₂	CdS QDs prepared by heat injection method, GNs-CdS QDs prepared by layer-by-layer self-assembly method	[154] 2014
21	CdS-rGO	GO prepared by modified Hummers’ method	Cd(CH₃CO₂)₂·2H₂O, thiourea	CdS-rGO prepared by hydrothermal method (180 °C, 12 h)	[155] 2017
22	CdS/ m-TiO₂/G^c	GO prepared by modified Hummers’ method	Cd(CH₃COO)₂·2H₂O, dimethyl sulfoxide	m-TiO₂ prepared by sol-gel and hydrothermal process, CdS/m-TiO₂/G prepared by solvothermal method (180 °C, 12 h)	[156] 2018
23	Ni-NG/CdS^d	GO prepared by modified Hummers’ method	commercial CdS	Ni-NG prepared by impregnation and calcination process (NH₃, 750 °C, 1 h), Ni-NG/CdS prepared by self-assembly route	[157] 2018
24	N-doped GR/CdS	GO prepared by modified Hummers’ method	CdCl₂, sodium citrate, ammonia, thiourea	CdS/SiO₂ prepared by using SiO₂ as sacrificial template, N-doped GR deposited on CdS/SiO₂ by a chemical vapor deposition at 700 °C	[28] 2019
25	NiS_x/Cd_0.8Zn_0.2S/rGO	GO prepared by modified Hummers’ method	Zn(NO₃)₂·6H₂O, CdCl₂·2.5H₂O, Ni(NO₃)₂·6H₂O, glucose, L-cysteine	NiS_x/Cd_0.8Zn_0.2S/rGO prepared by hydrothermal method (160 °C, 2 h)	[158] 2018
26	ZnIn₂S₄-GR	GO prepared by modified Hummers’ method	ZnCl₂, InCl₃·4H₂O, thioacetamide	ZnIn₂S₄-GR prepared by refluxing wet chemistry method (95 °C, 5 h)	[116] 2014
27	CdS/ZnIn₂S₄/ rGO	GO prepared by modified Hummers’ method	Cd(NO₃)₂, sulfur powder, ethanediamine, thioacetamide, In (NO₃)₃, Zn(CH₃COO)₂	CdS/ZnIn₂S₄ prepared by solvothermal method, GO reduced by N₂H₄ and NH₃ solution (95 °C, 1 h), CdS/ZnIn₂S₄/rGO prepared by electrostatic self-assembly process	[159] 2017
28	rGO/ZnIn₂S₄	GO prepared by modified Hummers’ method	ZnSO₄·7H₂O, In(NO₃)₃·4H₂O, thioacetamide	rGO/ZnIn₂S₄ prepared by alcohothermal method (ethanol, glycerol, 180 °C, 12 h)	[160] 2019
29	Ag:ZnIn₂S₄/ rGO	GO prepared by modified Hummers’ method	In(OOCCH₃)₃, Zn(CH₃COO)₂·2H₂O	Ag:ZnIn₂S₄/rGO prepared by hydrothermal method (180 °C, 12 h)	[161] 2020
30	CsPbBr₃QDs/GO	GO prepared by modified Hummers’ method	Cs-oleate, PbBr₂	CsPbBr₃QDs and CsPbBr₃QDs/GO prepared by antisolvent precipitation method	[65] 2017
31	LaCoO₃/ attapulgite/ rGO	GO prepared by modified Hummers’ method	La(NO₃)₃·6H₂O Co(NO₃)₂·6H₂O	LaCoO₃/attapulgite prepared by sol-gel method and calcination (600 °C, 2 h), LaCoO₃/attapulgite/rGO prepared by self-assembly process	[162] 2018
32	CsPbBr₃/USGO/ α-Fe₂O₃	GO prepared by modified Hummers’ method	Cs₂CO₃, PbBr₂	CsPbBr₃prepared by heat injection method, USGO/α-Fe₂O₃ prepared by hydrothermal process (180 °C, 12 h), CsPbBr₃/USGO/α-Fe₂O₃ prepared by electrostatic self-assembly process	[68] 2020
33	α-Fe₂O₃/Amine-rGO/ CsPbBr₃	GO prepared by modified Hummers’ method	Cs-oleate, PbBr₂	α-Fe₂O₃ nanorod array film prepared by hydrothermal process, α-Fe₂O₃/Amine-rGO prepared by electrostatic self-assembly process, α-Fe₂O₃/Amine-rGO/CsPbBr₃ prepared by solvent evaporation deposition approach	[67] 2020
34	Cs₂AgBiBr₆/ rGO	GO prepared by modified Hummers’ method	BiBr₃, AgBr, HBr acid, CsBr	Cs₂AgBiBr₆ prepared by oil bath method, Cs₂AgBiBr₆/rGO prepared by photoreduction process	[163] 2020
35	MIL-LIC-1(Eu) @GO	GO prepared by modified Hummers’ method	EuCl₃·6H₂O, 2-aminotere-phthalic acid	MIL-LIC-1(Eu) prepared by solvothermal method (N,N′-dimethylformamide, 120 °C, 20 h), MIL-LIC-1(Eu)@GO prepared by heating the mixture of GO/H₂O and MIL-LIC-1(Eu)/H₂O at 120 °C for 12 h	[12] 2017
36	NH₂-rGO/ Al-PMOF	Graphenea	AlCl₃, 4-carboxyphenyl porphyrin	NH₂-rGO obtained by solvothermal method (ammonia water, 180 °C, 10 h), NH₂-rGO/Al-PMOF obtained by hydrothermal method (180 °C, 24 h),	[9] 2018
37	Co-MOL@GO^e	GO prepared by modified Hummers’ method	CoCl₂·6H₂O, 5-(1H-1,2,4-triazol-1-yl) isophthalic acid	Co@GO obtained by oil bath (80 °C, 24 h), Co-MOL@GO obtained by solvothermal method (N,N′-dimethylformamide, H₂O, acetic acid, 130 °C, 4 h)	[70] 2021
38	rGO- TpPa-1-COF^f	GO prepared by modified Hummers’ method	1,3,5-Triformylphloroglucinol, p-Phenylenediamine	rGO-TpPa-1-COF obtained by heating the mixture of precursors, N,N′-dimethylformamide and acetic acid at 120 °C for 72 h	[164] 2020

以石墨烯作用为导向的多功能石墨烯基复合光催化剂

Multifunctional graphene-based composite photocatalysts oriented by multifaced roles of graphene in photocatalysis

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