金属-有机框架衍生的多功能光催化剂

doi:10.1016/S1872-2067(21)63934-7

催化学报 ›› 2022, Vol. 43 ›› Issue (4): 971-1000.DOI: 10.1016/S1872-2067(21)63934-7

金属-有机框架衍生的多功能光催化剂

张亚萍^a^,^c, 徐继香^a^,^b^,^*(), 周洁^a^,^c, 王磊^a^,^c^,^#()

^a青岛科技大学生态化工国家重点实验室基地, 山东青岛266042
^b青岛科技大学化学与分子工程学院, 山东青岛266042
^c青岛科技大学环境与安全工程学院, 山东青岛266042

收稿日期:2021-06-03 接受日期:2021-06-03 出版日期:2022-03-05 发布日期:2022-03-01
通讯作者: 徐继香,王磊
基金资助:
国家自然科学基金(51772162);国家自然科学基金(52072197);山东省高校青年创新技术基金(2019KJC004);山东省杰出青年基金(ZR2019JQ14);泰山青年学者人才计划(tsqn201909114);重大科技创新项目(2019JZZY020405);山东省自然科学基金重大基础研究项目(ZR2020ZD09)

Metal-organic framework-derived multifunctional photocatalysts

Yaping Zhang^a^,^c, Jixiang Xu^a^,^b^,^*(), Jie Zhou^a^,^c, Lei Wang^a^,^c^,^#()

^aState Key Laboratory Base of Eco-chemical Engineering, Qingdao University of Science and Technology, Qingdao 266042, Shandong, China
^bCollege of Chemistry and Molecular Engineering, Qingdao University of Science & Technology, Qingdao 266042, Shandong, China
^cCollege of Environment and Safety Engineering, Qingdao University of Science and Technology, Qingdao 266042, Shandong, China

Received:2021-06-03 Accepted:2021-06-03 Online:2022-03-05 Published:2022-03-01
Contact: Jixiang Xu, Lei Wang
Supported by:
National Natural Science Foundation of China(51772162);National Natural Science Foundation of China(52072197);Youth Innovation and Technology Foundation of Shandong Higher Education Institutions, China(2019KJC004);Outstanding Youth Foundation of Shandong Province, China(ZR2019JQ14);Taishan Scholar Young Talent Program(tsqn201909114);Major Scientific and Technological Innovation Project(2019JZZY020405);Major Basic Research Program of Natural Science Foundation of Shandong Province(ZR2020ZD09)

摘要/Abstract

摘要：

在光催化过程中, 光催化剂被太阳能激发产生光生电子和空穴, 来实现环境净化或能量转换, 是应对全球变暖和能源短缺的有效途径之一. 然而, 光催化技术面临的主要瓶颈问题是光生载流子的低分离效率和高反应能垒. 而催化剂本身的特性对这一点起到了决定性的作用. 因此, 催化剂的合理设计和改性是提高光催化效率的关键. 金属有机框架(MOFs)是一类由金属节点和有机配体组成的新型结晶多孔材料. 基于结构多样性、超高比表面积、形状和尺寸可调的纳米孔或纳米通道等优异的特性, MOFs基材料在光催化领域引起了广泛关注. 然而, MOFs的主要问题之一是低导电性和稳定性, 这限制了其更广泛应用.
正是由于MOFs的不稳定性, 其可以作为牺牲模板制备纳米材料. 由MOFs衍生的纳米材料继承了MOFs的优异特性, 同时避免了MOFs较差的导电性和稳定性的问题. 并且可以通过选择特定的金属节点和有机配体对MOFs衍生的纳米材料进行调控, 从而实现光催化剂的多功能性. 因此, MOFs衍生物在光催化领域展现出更广阔的应用前景. 而且MOFs衍生物不仅可以作为半导体光催化剂, 还可以作为光催化析氢、CO₂还原、污染物降解等反应的助催化剂.
本文重点介绍MOFs衍生物在光催化领域的多功能应用. 从MOFs衍生物的制备、修饰和应用等方面对近年来的研究进行了分析和总结. 最后, 对MOFs衍生物应用于光催化领域的挑战进行了分析, 并对未来发展和机遇进行了展望, 以期为该领域的进一步研究提供更多参考, 并带来新的启示.

关键词: 金属有机框架衍生纳米材料, 半导体光催化剂, 助催化剂, 析氢反应, CO₂还原, 污染物降解

Abstract:

Metal-organic framework (MOF)-derived nanomaterials have attracted widespread attention, because the excellent features, such as high surface area, porosity and tunable properties are inherited from MOFs. Moreover, the derivatives avoid the poor conductivity and stability of MOFs. MOF-derived nanomaterials can easily be regulated by a specific selection of metal nodes and organic linkers, resulting in multifunctionality in photocatalysis. MOF derivatives can be used not only as semiconductor photocatalysts, but also as co-catalysts for photocatalytic hydrogen evolution, CO₂ reduction, pollutants degradation, etc. This review focuses on the multifunctional applications of MOF derivatives in the field of photocatalysis. The researches in recent years are analyzed and summarized from the aspects of preparation, modification and application of MOF derivatives. At the end of the review, the development and challenges of MOF derivatives applied in photocatalysis in the future are put forward, in order to provide more references for further research in this field and bring new inspiration.

Key words: MOF-derived nanomaterials, Semiconductor photocatalyst, Cocatalyst, H₂ evolution, CO₂ reduction, Pollution degradation

张亚萍, 徐继香, 周洁, 王磊. 金属-有机框架衍生的多功能光催化剂[J]. 催化学报, 2022, 43(4): 971-1000.

Yaping Zhang, Jixiang Xu, Jie Zhou, Lei Wang. Metal-organic framework-derived multifunctional photocatalysts[J]. Chinese Journal of Catalysis, 2022, 43(4): 971-1000.

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图/表 38

Fig. 1. Applications of MOF derivatives in photocatalysis.

Fig. 2. Schematic illustrating the process of the photocatalysis.

Fig. 3. The modification strategy of MOF derivatives.

Fig. 4. A summary illustration for the synthesis methods of MOF-derived semiconductors.

Fig. 6. (a) SEM image of ZIF-8; (b) TG curves of ZIF-8; (c) The synthesis process of ZnO; (d,e) SEM and TEM images of ZnO obtained by two-step calcination method. Reprinted with permission from Ref. [120]. Copyright 2016, Elsevier.

Fig. 7. (a) The products of MIL-88A(Fe) annealed in different atmosphere. Reprinted with permission from Ref. [122]. Copyright 2020, Elsevier. (b) The products of Zn-MOF annealed at different temperatures and atmospheres. Reprinted with permission from Ref. [123]. Copyright 2020, Elsevier.

Fig. 8. (a) Preparation of core-shell Fe3O4-CuO@carbon hollow sphere composite; (b) The illustration of freezing-replacement post-treatment on the structure of Fe3O4-CuO@carbon sphere; SEM images of original (c) and freezing-replacement treated (d) Fe3O4-CuO@carbon. Reprinted with permission from Ref. [126]. Copyright 2020, Elsevier.

Fig. 9. (a) Schematic illustration for preparing Co4S3. Reprinted with permission from Ref. [129]. Copyright 2018, Elsevier. (b) Schematic illustration for preparing Fe-Ni-P nanotubes using Fe-Ni-MOF as templates. Reprinted with permission from Ref. [131]. Copyright 2020, Elsevier.

Fig. 10. (a) Schematic preparation processes of Bismuth oxyhalides. Reprinted with permission from Ref. [102]. Copyright 2020, Elsevier. (b) Schematic diagram of two-step synthesis of Fe2N nanocubes. Reprinted with permission from Ref. [142]. Copyright 2020, The Royal Society of Chemistry.

Fig. 11. Schematic diagrams of different types of heterojunctions. (a) type-II heterojunction; (b) p-n heterojunction; (c) Z-scheme heterojunction.

Fig. 12. (a) Scheme illustration for the synthesis of ZIF-derived ZnS/ZnIn2S4 heterojunction; (b) The SEM image of the ZnS/ZnIn2S4 heterojunction; (c) Band structure and proposed charge transfer mechanism for ZnS/ZnIn2S4 heterojunction photocatalyst; (d) Photocatalytic hydrogen evolution by series photocatalysts. Reprinted with permission from Ref. [152]. Copyright 2020, The Royal Society of Chemistry.

Fig. 13. XRD patterns (a), H2 evolution rates (b) over MIL-125-NH2-derived TiO2 prepared at different temperatures; (c) The synthesis process of MIL-125-NH2-derived TiO2; (d) TEM images and selected-area electron diffraction pattern of MIL-125-NH2-derived TiO2 synthesized through calcination at 600 °C for 1 h. Reprinted with permission from Ref. [58]. Copyright 2018, American Chemical Society.

Fig. 14. (a) Self-recognition of mixed metal cations during the sulfuration of Co/Cd-MOF into Co9S8/CdS; (b) Scheme illustration for the transfer route of photogenerated carries in the Z-scheme Co9S8/CdS during H2 evolution and BA oxidation; (c) Photocatalytic H2 evolution with different catalysts; (d) Photocatalytic conversion rate of BA to BAD. Reprinted with permission from Ref. [164]. Copyright 2020, Elsevier.

Fig. 15. (a) Schematic preparation process of hollow Cu-TiO2/C; (b) SEM image of Cu-TiO2/C. Reprinted with permission from Ref. [172]. Copyright 2018, The Royal Society of Chemistry. (c) Schematic preparation process of hollow ZnFe2O4/AgCl/Ag/C nanotube; (d) SEM image of ZnFe2O4/AgCl/Ag/C; (e) The scattering path of incident light in the porous nanotube structure. Reprinted with permission from Ref. [173]. Copyright 2021, Elsevier.

Fig. 16. (a) Schematic illustration of the fabrication of ZnOZIF-8/rGO/carbon sponge; (b) Schematic diagram of the photogenerated carrier transfer process in ZnOZIF-8/rGO/carbon sponge. Reprinted with permission from Ref. [191]. Copyright 2018, American Chemical Society. (c) Schematic the synthesis process of CdS/ZCO nanocomposites; (d) Photocurrent response of CdS/ZCO; (e) Light irradiation route in CdS/ZCO. Reprinted with permission from Ref. [192]. Copyright 2018, The Royal Society of Chemistry.

Fig. 17. (a) Schematic preparation process of Co3O4/ZnO@ZnS photocatalysts; Calculated Fermi levels of ZnO (101) (b) and ZnS (111) (c) planes; (d) Possible mechanism for the photocatalytic over Co3O4/ZnO@ZnS; (e) H2 and O2 production rates of Co3O4/ZnO@ZnS without sacrificial agent. Reprinted with permission from Ref. [193]. Copyright 2020, Elsevier.

Table 1 A summary of MOF-derived photocatalysts for photocatalytic H2 evolution.

MOF precursors	Photocatalyst	Synthesis strategy	Light	Sacrificial agent	Activity (μmol h^-1g^-1)	Ref.
In-MOF	In₂O₃/g-C₃N₄	calcined annealing (In-MOF precursor + melamine)	visible light	TEOA	1374	[168]
NH₂-MIL-125(Ti/Cu)	TiO₂/Cu_xO/C	one-step direct carbonization	UV-visible light	CH₃OH	3298	[186]
ZIF-67	TiO₂-Ti₃C₂-CoS_x	solvothermal method	UV-visible light	CH₃OH	950	[187]
Cd-MOF	CdS/MoS₂	sulfurization	UV-visible light	Na₂S + Na₂SO₃	5587	[189]
HKUST-1	Cu-TiO₂/C nanospheres	calcination and etching	simulated sunlight	CH₃OH	14049	[172]
Ni-MOF	CdS-NiO-P	annealing and ultrasonication	UV-visible light	DMPO	14250	[179]
NH₂-MIL-125(Ti)	MoS₂@TiO₂	thermally treated (thiourea and sodium molybdate dihydrate)	visible light	TEOA	10046	[169]
MIL-68(In)	In₂O₃@g-C₃N₄	annealing	visible light	0.5 mol/L Na₂SO₃ + Na₂S	258.8	[182]
MOF-74-Zn/Fe	ZnFe₂O₄/AgCl/Ag/C	thermal treatment	visible light	0.1 mol/L Na₂SO₃ + 0.1 mol/L Na₂S	7524	[173]
MIL-125	g-C₃N₄/TiO₂	facile pyrolysis	UV-visible light	TEOA	606	[183]
ZIF-8	ZnO_ZIF-8/rGO/carbon sponge	dipping-pyrolysis	simulated solar light	CH₃OH	14.6	[191]
Cd-Zn-Fe PBA	Cd_0.5Zn_0.5S	solvothermal	visible light	Na₂S (0.35 mol/L) + Na₂SO₃ (0.25 mol/L)	4341.6	[105]
Cd-Fe-PBA	CdS	microwave-assisted hydrothermal process	visible light	Na₂S + Na₂SO₃	3051.4	[174]
NH₂-MIL-125	NiS/CdS/TiO₂	hydrolysis combining sulfidation process	visible light	Na₂SO₃ (0.25 mol/L) + Na₂S (0.35 mol/L)	2149.15	[170]
Ce-ZIF-8	CeO₂/ZnS-CuS	calcining and vulcanizing and in-situ cation exchange method	visible light	CH₃OH	13470	[180]
Fe-MOF	g-Fe₂O₃/rGO-w	thermolysis and wet chemical technique	visible light	TEA	318	[185]
Al-MOF	CdX-g-C₃N₄-NPC	annealing	simulated solar light	lactic acid	116.5	[188]
NH₂-MIL-125	H-TiO₂/CdS	post solvothermal method	visible light	Na₂S (0.2 mol/L) + Na₂SO₃ (0.3 mol/L)	2997.482	[171]
MOF-199	Cu-Cu₂O/TiO₂	calcining	UV-visible light	glycerol	15130	[190]
Co-MOF	Co₄S₃/CdS	hydrothermal reaction	visible light	lactic acid	5892.6	[181]
ZnCo-MOFs	Co₃O₄/ZnO@ZnS	calcining and solvothermal method	780 nm > λ > 320 nm	CH₃OH	3853	[193]
ZIF-67	Co₉S₈@ZnAgInS	sulfidation reaction and thermal treatment	simulated solar light	TEOA	9395.3	[146]
ZnCo-ZIF	CdS/ZnXCo_3‒_xO₄	aminated in an oil bath and hydrothermal method	UV-visible light	lactic acid	3978.6	[192]
ZIF-8	Co/NGC@ZnIn₂S₄	situ solution growth method and high-temperature pyrolysis and acid leaching	visible light	TEOA	11270	[194]
ZnCo-ZIF	Pt-ZnO-Co₃O₄ Pt-ZnS-CoS Pt-Zn₃P₂-CoP	oxidation sulfurization phosphidation	UV-vis light	methanol	7800 8210 9150	[130]
Prussian blue	Fe₂N	annealing + ammoniated	visible light	TEOA	14500	[142]
Fe-Ni-MIL-88	Fe-Ni-P nanotubes	phosphating method	visible light	TEOA	5420	[131]
Co-MOF	Co₄S₃/CdS	annealing + sulfurization	simulated solar light	lactic acid	12360	[129]
CAU-17	Bi_0.5Y_0.5VO₄	annealing	UV-vis light	—	124.2	[30]
ZIF-8	ZnS/ZnIn₂S₄	sulfurization	simulated solar light	TEOA	453.4	[152]
MIL-125@ZIF-67 HMOF	TiO₂/Co₃O₄/Ni	annealing	UV-visible light	free	122.67	[153]
MIL-125-NH₂	TiO₂	annealing	UV-visible light	methanol	1394	[58]
Co/Cd-MOF	Co₉S₈/CdS	sulfurization	visible light	free	61924	[164]
NH₂-MIL-125(Ti)	N-C-TiO₂/C	one-step pyrolysis	UV-visible light	methanol	426	[162]

Table 1 A summary of MOF-derived photocatalysts for photocatalytic H2 evolution.

MOF precursors	Photocatalyst	Synthesis strategy	Light	Sacrificial agent	Activity (μmol h^-1g^-1)	Ref.
In-MOF	In₂O₃/g-C₃N₄	calcined annealing (In-MOF precursor + melamine)	visible light	TEOA	1374	[168]
NH₂-MIL-125(Ti/Cu)	TiO₂/Cu_xO/C	one-step direct carbonization	UV-visible light	CH₃OH	3298	[186]
ZIF-67	TiO₂-Ti₃C₂-CoS_x	solvothermal method	UV-visible light	CH₃OH	950	[187]
Cd-MOF	CdS/MoS₂	sulfurization	UV-visible light	Na₂S + Na₂SO₃	5587	[189]
HKUST-1	Cu-TiO₂/C nanospheres	calcination and etching	simulated sunlight	CH₃OH	14049	[172]
Ni-MOF	CdS-NiO-P	annealing and ultrasonication	UV-visible light	DMPO	14250	[179]
NH₂-MIL-125(Ti)	MoS₂@TiO₂	thermally treated (thiourea and sodium molybdate dihydrate)	visible light	TEOA	10046	[169]
MIL-68(In)	In₂O₃@g-C₃N₄	annealing	visible light	0.5 mol/L Na₂SO₃ + Na₂S	258.8	[182]
MOF-74-Zn/Fe	ZnFe₂O₄/AgCl/Ag/C	thermal treatment	visible light	0.1 mol/L Na₂SO₃ + 0.1 mol/L Na₂S	7524	[173]
MIL-125	g-C₃N₄/TiO₂	facile pyrolysis	UV-visible light	TEOA	606	[183]
ZIF-8	ZnO_ZIF-8/rGO/carbon sponge	dipping-pyrolysis	simulated solar light	CH₃OH	14.6	[191]
Cd-Zn-Fe PBA	Cd_0.5Zn_0.5S	solvothermal	visible light	Na₂S (0.35 mol/L) + Na₂SO₃ (0.25 mol/L)	4341.6	[105]
Cd-Fe-PBA	CdS	microwave-assisted hydrothermal process	visible light	Na₂S + Na₂SO₃	3051.4	[174]
NH₂-MIL-125	NiS/CdS/TiO₂	hydrolysis combining sulfidation process	visible light	Na₂SO₃ (0.25 mol/L) + Na₂S (0.35 mol/L)	2149.15	[170]
Ce-ZIF-8	CeO₂/ZnS-CuS	calcining and vulcanizing and in-situ cation exchange method	visible light	CH₃OH	13470	[180]
Fe-MOF	g-Fe₂O₃/rGO-w	thermolysis and wet chemical technique	visible light	TEA	318	[185]
Al-MOF	CdX-g-C₃N₄-NPC	annealing	simulated solar light	lactic acid	116.5	[188]
NH₂-MIL-125	H-TiO₂/CdS	post solvothermal method	visible light	Na₂S (0.2 mol/L) + Na₂SO₃ (0.3 mol/L)	2997.482	[171]
MOF-199	Cu-Cu₂O/TiO₂	calcining	UV-visible light	glycerol	15130	[190]
Co-MOF	Co₄S₃/CdS	hydrothermal reaction	visible light	lactic acid	5892.6	[181]
ZnCo-MOFs	Co₃O₄/ZnO@ZnS	calcining and solvothermal method	780 nm > λ > 320 nm	CH₃OH	3853	[193]
ZIF-67	Co₉S₈@ZnAgInS	sulfidation reaction and thermal treatment	simulated solar light	TEOA	9395.3	[146]
ZnCo-ZIF	CdS/ZnXCo_3‒_xO₄	aminated in an oil bath and hydrothermal method	UV-visible light	lactic acid	3978.6	[192]
ZIF-8	Co/NGC@ZnIn₂S₄	situ solution growth method and high-temperature pyrolysis and acid leaching	visible light	TEOA	11270	[194]
ZnCo-ZIF	Pt-ZnO-Co₃O₄ Pt-ZnS-CoS Pt-Zn₃P₂-CoP	oxidation sulfurization phosphidation	UV-vis light	methanol	7800 8210 9150	[130]
Prussian blue	Fe₂N	annealing + ammoniated	visible light	TEOA	14500	[142]
Fe-Ni-MIL-88	Fe-Ni-P nanotubes	phosphating method	visible light	TEOA	5420	[131]
Co-MOF	Co₄S₃/CdS	annealing + sulfurization	simulated solar light	lactic acid	12360	[129]
CAU-17	Bi_0.5Y_0.5VO₄	annealing	UV-vis light	—	124.2	[30]
ZIF-8	ZnS/ZnIn₂S₄	sulfurization	simulated solar light	TEOA	453.4	[152]
MIL-125@ZIF-67 HMOF	TiO₂/Co₃O₄/Ni	annealing	UV-visible light	free	122.67	[153]
MIL-125-NH₂	TiO₂	annealing	UV-visible light	methanol	1394	[58]
Co/Cd-MOF	Co₉S₈/CdS	sulfurization	visible light	free	61924	[164]
NH₂-MIL-125(Ti)	N-C-TiO₂/C	one-step pyrolysis	UV-visible light	methanol	426	[162]

Table 2 The different products of CO2 reduction and the corresponding reduction potentials (pH = 7).

Equation	Reaction	E⁰vs. NHE
1	CO₂ + 2H⁺+ 2e^-→ HCOOH	-0.61 V
2	CO₂ + 2H⁺+ 2e^-→ CO + H₂O	-0.53 V
3	CO₂ + 4H⁺+ 4e^-→ HCHO + H₂O	-0.48 V
4	CO₂ + 6H⁺+ 6e^-→ CH₃OH + H₂O	-0.38 V
5	CO₂ + 8H⁺+ 8e^-→ CH₄ + 2H₂O	-0.24 V
6	2H⁺+ 2e^-→ H₂	-0.41 V

Fig. 18. Scheme illustration for the preparation and SEM images of In2S3-CdIn2S4 (a) and ZnIn2S4-In2O3 (b). Reprinted with permission from Ref. [210]. Copyright 2017, American Chemical Society. Reprinted with permission from Ref. [211]. Copyright 2018, American Chemical Society. (c) SEM image of holey Co3O4 nanosheets; (d) The theoretical calculation models of CO2 molecule adsorbed on the surface of Co3O4 bulk (left) and Co3O4 monolayer (right) based on DFT calculations; (e) Evolution of CO and H2 under various reaction conditions. Reprinted with permission from Ref. [212]. Copyright 2019, Elsevier.

Fig. 19. (a) Illustration of the synthetic process of hierarchical FeCoS2-CoS2 double-shelled nanotubes. Reprinted with permission from Ref. [216]. Copyright 2020, Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim. (b) The synthetic procedure of Co3O4 hierarchical nanosheets; (c) CO2 photoreduction activity and selectivity of different samples. Reprinted with permission from Ref. [217]. Copyright 2019, The Royal Society of Chemistry.

Fig. 20. (a) A schematic synthesis process for the Co1.11Te2@C material. Theoretical calculation results of (b) valence band XPS of Co1.11Te2, (c) DOS/PDOS diagrams, (d) band structure of Co1.11Te2. (e) Photocatalytic CO2 reduction activities of Co1.11Te2@C. Reprinted with permission from Ref. [221]. Copyright 2019, The Royal Society of Chemistry.

Fig. 21. (a) The effect of different samples on the product; (b) The mechanism diagram for photocatalytic CO2 reduction over the composited photocatalyst. Reprinted with permission from Ref. [222]. Copyright 2019, American Chemical Society.

Table 3 A summary of MOF-derived photocatalysts for photocatalytic CO2 reduction.

MOF precursor	Photocatalyst	Synthesis strategy	Light	Product	Activity (μmol h^-1g^-1)	Ref.
In-MIL-68	In₂S₃-CdIn₂S₄	liquid phase sulfidation process + cation exchange reaction	visible light	CO	825	[210]
In-MIL-68	ZnIn₂S₄-In₂O₃	thermal annealing + hydrothermal Reaction	visible light	CO	3075	[211]
ZIF-67	Co₃O₄	ion-assistant solvothermal + annealing	visible light	CO	9040	[212]
In-MIL-68	MnS/In₂S₃	one-step sulfurizing method	300 W Xe lamp, 100 mW cm^-2	CO	58	[219]
ZnCo-ZIFs	ZnO/Co₃O₄	annealing	300 W Xe lamp	CO	537.5	[220]
MIL-88A	FeCoS₂-CoS₂	ion-exchange + sulfidation reaction + thermal annealing	visible light	CO	56200	[216]
Co-MOF	Co₃O₄	annealing	visible light	CO	1985	[217]
ZnMn₂-ptcda MOF	ZnMn₂O₄	annealing	500 W Xenon arc lamp	CO CH₄	0.024 —	[104]
Zn-Ni MOF	ZnO/NiO	annealing	300 W full-spectrum Xe lamp	CH₃OH	1.57	[215]
Cu/Zn MOF	Cu/Zn bimetallic oxide	annealing	300 W Xe lamp with full spectrum	CH₃OH	3710	[214]
ZIF-67	Co₃O₄	annealing	AM 1.5, 100 W/cm²	CO	46.3	[218]
ZIF-67	Co_1.11Te₂	annealing + Te powder	200 W white LEDs lamp	CO	11400	[221]
MIL-101(Fe)	Fe@C	two-step calcination	300 W Xe lamp	CO	18301	[90]
MIL-125(Ti)	Co-Cu/TiO₂	annealing	300 W Xe lamp	CO CH₄ C₂H₆ C₃H₈	501.9 565.97 892 33.57	[222]
NH₂-MIL-125	Au/TiO₂	solvothermal synthesis	200 W Hg/Xe (200-750 nm) lamp	CH₄	—	[224]
ZIF-8	CuO_X@p-ZnO	aerobic pyrolysis	300 W Xe lamp	CO CH₄ C₂H₄	3.3 2.2 2.7	[223]

Fig. 22. (a) The synthetic process of core-shell ZnO@C-N-Co; (b,c) TEM images of ZnO@C-N-Co; (d) Photodegradation mechanism of organic pollutants over the prepared core-shell ZnO@C-N-Co photocatalyst; (e) Recyclability of the ZnO@C-N-Co nanocomposites in the MO degradation. Reprinted with permission from Ref. [235]. Copyright 2017, The Royal Society of Chemistry.

Fig. 23. (a) Schematic synthesis process of AgCl/Ag/In2O3; (b) The photocatalytic mechanism of Z-scheme AgCl/Ag/In2O3 system; The work function of In2O3 (c), AgCl (d) and Ag (e); (f) Photocatalytic degradation of tetracycline by the various photocatalysts; (g) Photocatalytic Cr (VI) reduction of the various photocatalysts. Reprinted with permission from Ref. [249]. Copyright 2021, Elsevier.

Table 4 A summary of MOF-derived photocatalysts for photocatalytic degradation of pollutants.

MOF precursor	Photocatalysts	Synthesis strategy	Pollutant	Reactive species	Ref.
MIL-88B	AgPt@γ-Fe₂O₃/CuO	annealing	4-nitrophenol	^•OH/^•O₂^-	[245]
MOF-NiZn	ZnO/Ni_0.9Zn_0.1O	annealing	MB	^•OH	[230]
MIL-125(Ti)	CeO_x@C-TiO₂	annealing	tetracycline	^•OH/^•O₂^-	[243]
Co/Fe-MOF	CoP/Fe₂P@mC	annealing (NaH₂PO₂)	RhB	h⁺/^•OH/^•O₂^-	[242]
ZIF-8@MIL-68(In)	ZnO@In₂O₃	one-step calcination	tetracycline	^•OH/^•O₂^-	[236]
Cu-BTC	Cu-doped TiO₂	ultrasonic-assisted precipitation technique	ofloxacin	^•OH/^•O₂^-	[232]
In-MIL-68	In₂O₃@SnIn₄S₈	oil-bath method	Cr (VI)	e^-	[248]
Zn/Co-ZIF	ZnO@C-N-Co	directly pyrolyzing	MO	^•OH/^•O₂^-	[235]
Zn_1‒_xCo_x-ZIF	Zn_1‒_xCo_x-ZIF@Zn_1‒_xCo_xO	in situ transformation	RhB	^•OH/^•O₂^-	[229]
MIL-68 (In)	AgCl/Ag/In₂O₃	annealing	tetracycline/Cr (VI)	^•O₂^-/e^-/ h⁺	[249]
Ti-Fe-MOF	TiO₂/Au/Fe₂O₃	hydrothermal + annealing	2,4 dichlorophenol and 4-bromophenol	^•OH/^•O₂^-	[246]
MOF-5	C-doped ZnO	annealing	RhB	^•O₂^-/h⁺	[233]
MIL-53-NH₂	g-C₃N₄@CoFe₂O₄/Fe₂O₃	annealing	tetracycline	^•OH	[255]
MIL-125/Co	C-TiO₂/CoTiO₃	annealing	ciprofloxacin	^•OH	[247]
MIL-100(Fe)	CdS QDs/Fe₂O₃	two-step calcination	bisphenol A	^•OH/h⁺	[244]
MIL-125	g-C₃N₄/TiO₂	annealing	RhB	^•O₂^-/h⁺	[241]
Cu-Zn-BTC	Ag₂O/ZnO/CuO	annealing	acid blue 92	^•OH	[240]
MIL-68(In)	MoS₂/In₂S₃	two-step hydrothermal	MO	^•OH/^•O₂^-	[239]
MIL-101(Fe)	Fe₂O₃/TiO₂	microwave-assisted sol-gel	NSAIDs	h⁺	[238]
NH2-MIL-125(Ti)	N-doped TiO₂	annealing	MB	e^-	[231]
CAU-17	Bi₂O₂CO₃/g-C₃N₄	wet chemistry and calcination	tetracycline	^•O₂^-	[250]
UiO-66	TiO₂/ZrO₂	annealing	RhB	^•OH/^•O₂^-	[237]
In-BDC	In₂O₃	annealing	perfluorooctanoic acid	^•OH	[234]
MIL-68(In)	MWCNT@In₂S₃	thiourea sulfuration	tetracycline	^•O₂^-/h⁺	[253]
Fe-MIL-88B	α-Fe₂O₃/C	annealing	MB	^•OH/^•O₂^-	[251]
Cd-MOF	CdS/NC-T	annealing	tetracycline	^•OH/^•O₂^-/h⁺	[254]
HKUST-1	GCNO_X/Cu₂O@C	annealing	RhB ciprofloxacin	^•OH	[252]
MIL-88A	ZnIn₂S₄@Fe₃O₄ ZnIn₂S₄@α-Fe₂O₃	annealing + in-situ self-assembly strategy	RhB, MO, MB and BPA	^•O₂^-/h⁺ ^•OH/^•O₂^-	[122]
CuBTC/SA	Fe₃O₄-CuO@carbon	ferrocene CVD and pyrolysis	MB, acid red 73, X-3B, BPA	^•OH/e^-/h⁺	[126]
Ag/Bi-MOF	Ag/AgCl/BiOCl	halogenation treatment	tetracycline	^•O₂^-/h⁺	[132]
Bi-BTC	BiOBr/Bi₂₄O₃₁Br₁₀	Bromination-annealing route	RhB	h⁺/^•O₂^-/¹O₂	[133]
Bi-BTC	BiOX, X= Cl, Br, I	solvothermal method in sealed autoclaves	RhB	^•O₂^-/h⁺	[102]
Prussian blue	CuFe₂O₄	annealing	RhB	^•OH	[115]
MOF-5	C-doped ZnO	annealing	RhB	^•O₂^-/h⁺	[121]
Zn-MOF	ZnO/C	annealing	MB	—	[123]
MOF-5	ZnO/C	one-step carbonization	MB	^•OH/^•O₂^-	[125]
ZIF-8	C-doped ZnO	two-step calcination	RhB	—	[120]
MIL-68-In	In₂S₃	sulfidation	MO and tetracycline	^•O₂^-/h⁺	[128]
[NH₃CH₃][Cu(HCOO)₃]	Cu₂O	direct one-step pyrolysis	MO	^•O₂^-/h⁺	[118]
Co/In-MOFs	In₂O₃/Co₃O₄-palygorskite	one-pot solvothermal method	MB and TC	^•O₂^-/h⁺/^•OH	[117]

Table 4 A summary of MOF-derived photocatalysts for photocatalytic degradation of pollutants.

MOF precursor	Photocatalysts	Synthesis strategy	Pollutant	Reactive species	Ref.
MIL-88B	AgPt@γ-Fe₂O₃/CuO	annealing	4-nitrophenol	^•OH/^•O₂^-	[245]
MOF-NiZn	ZnO/Ni_0.9Zn_0.1O	annealing	MB	^•OH	[230]
MIL-125(Ti)	CeO_x@C-TiO₂	annealing	tetracycline	^•OH/^•O₂^-	[243]
Co/Fe-MOF	CoP/Fe₂P@mC	annealing (NaH₂PO₂)	RhB	h⁺/^•OH/^•O₂^-	[242]
ZIF-8@MIL-68(In)	ZnO@In₂O₃	one-step calcination	tetracycline	^•OH/^•O₂^-	[236]
Cu-BTC	Cu-doped TiO₂	ultrasonic-assisted precipitation technique	ofloxacin	^•OH/^•O₂^-	[232]
In-MIL-68	In₂O₃@SnIn₄S₈	oil-bath method	Cr (VI)	e^-	[248]
Zn/Co-ZIF	ZnO@C-N-Co	directly pyrolyzing	MO	^•OH/^•O₂^-	[235]
Zn_1‒_xCo_x-ZIF	Zn_1‒_xCo_x-ZIF@Zn_1‒_xCo_xO	in situ transformation	RhB	^•OH/^•O₂^-	[229]
MIL-68 (In)	AgCl/Ag/In₂O₃	annealing	tetracycline/Cr (VI)	^•O₂^-/e^-/ h⁺	[249]
Ti-Fe-MOF	TiO₂/Au/Fe₂O₃	hydrothermal + annealing	2,4 dichlorophenol and 4-bromophenol	^•OH/^•O₂^-	[246]
MOF-5	C-doped ZnO	annealing	RhB	^•O₂^-/h⁺	[233]
MIL-53-NH₂	g-C₃N₄@CoFe₂O₄/Fe₂O₃	annealing	tetracycline	^•OH	[255]
MIL-125/Co	C-TiO₂/CoTiO₃	annealing	ciprofloxacin	^•OH	[247]
MIL-100(Fe)	CdS QDs/Fe₂O₃	two-step calcination	bisphenol A	^•OH/h⁺	[244]
MIL-125	g-C₃N₄/TiO₂	annealing	RhB	^•O₂^-/h⁺	[241]
Cu-Zn-BTC	Ag₂O/ZnO/CuO	annealing	acid blue 92	^•OH	[240]
MIL-68(In)	MoS₂/In₂S₃	two-step hydrothermal	MO	^•OH/^•O₂^-	[239]
MIL-101(Fe)	Fe₂O₃/TiO₂	microwave-assisted sol-gel	NSAIDs	h⁺	[238]
NH2-MIL-125(Ti)	N-doped TiO₂	annealing	MB	e^-	[231]
CAU-17	Bi₂O₂CO₃/g-C₃N₄	wet chemistry and calcination	tetracycline	^•O₂^-	[250]
UiO-66	TiO₂/ZrO₂	annealing	RhB	^•OH/^•O₂^-	[237]
In-BDC	In₂O₃	annealing	perfluorooctanoic acid	^•OH	[234]
MIL-68(In)	MWCNT@In₂S₃	thiourea sulfuration	tetracycline	^•O₂^-/h⁺	[253]
Fe-MIL-88B	α-Fe₂O₃/C	annealing	MB	^•OH/^•O₂^-	[251]
Cd-MOF	CdS/NC-T	annealing	tetracycline	^•OH/^•O₂^-/h⁺	[254]
HKUST-1	GCNO_X/Cu₂O@C	annealing	RhB ciprofloxacin	^•OH	[252]
MIL-88A	ZnIn₂S₄@Fe₃O₄ ZnIn₂S₄@α-Fe₂O₃	annealing + in-situ self-assembly strategy	RhB, MO, MB and BPA	^•O₂^-/h⁺ ^•OH/^•O₂^-	[122]
CuBTC/SA	Fe₃O₄-CuO@carbon	ferrocene CVD and pyrolysis	MB, acid red 73, X-3B, BPA	^•OH/e^-/h⁺	[126]
Ag/Bi-MOF	Ag/AgCl/BiOCl	halogenation treatment	tetracycline	^•O₂^-/h⁺	[132]
Bi-BTC	BiOBr/Bi₂₄O₃₁Br₁₀	Bromination-annealing route	RhB	h⁺/^•O₂^-/¹O₂	[133]
Bi-BTC	BiOX, X= Cl, Br, I	solvothermal method in sealed autoclaves	RhB	^•O₂^-/h⁺	[102]
Prussian blue	CuFe₂O₄	annealing	RhB	^•OH	[115]
MOF-5	C-doped ZnO	annealing	RhB	^•O₂^-/h⁺	[121]
Zn-MOF	ZnO/C	annealing	MB	—	[123]
MOF-5	ZnO/C	one-step carbonization	MB	^•OH/^•O₂^-	[125]
ZIF-8	C-doped ZnO	two-step calcination	RhB	—	[120]
MIL-68-In	In₂S₃	sulfidation	MO and tetracycline	^•O₂^-/h⁺	[128]
[NH₃CH₃][Cu(HCOO)₃]	Cu₂O	direct one-step pyrolysis	MO	^•O₂^-/h⁺	[118]
Co/In-MOFs	In₂O₃/Co₃O₄-palygorskite	one-pot solvothermal method	MB and TC	^•O₂^-/h⁺/^•OH	[117]

Fig. 24. (a) The fabrication process of the hollow porous carbon (HPC)-immobilized ultrahigh content of single Zn atoms. Reprinted with permission from Ref. [266]. Copyright 2019, Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim. (b) Schematic preparation process of the Fe-N/GNs. Reprinted with permission from Ref. [267]. Copyright 2020, Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

Fig. 25. (a) Schematic preparation process of Co-NxPS/C/CdS photocatalyst; (b) Aberration-corrected STEM images of Co-NxPS/C cocatalyst; (c) H2 amounts of series photocatalysts; (d) Photocatalytic mechanism for H2 evolution. Reprinted with permission from Ref. [280]. Copyright 2021, Elsevier.

Fig. 26. (a) Schematic fabrication process of CoSx/g-C3N4 photocatalysts; Schematic illustration of the morphology of ZIF-67 (b) and hollow CoSx polyhedron (c); FESEM images of ZIF-67 (d), hollow CoSx polyhedron (e) and CoSx/g-C3N4 composites (f). Reprinted with permission from Ref. [286]. Copyright 2018, American Chemical Society.

Fig. 27. (a) The synthesis processes of CoP/g-C3N4. Reprinted with permission from Ref. [287]. Copyright 2018, The Royal Society of Chemistry. (b) Synthesis of Ni2P/CdS composite. Reprinted with permission from Ref. [288]. Copyright 2016, American Chemical Society.

Fig. 28. (a) The illustration for the synthesis procedure of the Ni/SiO2 catalysts. Reprinted with permission from Ref. [285]. Copyright 2015, Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim. (b) Schematic process for the preparation of Ni/g-C3N4. Reprinted with permission from Ref. [289]. Copyright 2019, The Royal Society of Chemistry.

Fig. 29. (a) PL spectra of pure g-C3N4 and CoSx/g-C3N4; (b) Linear sweep voltammograms of g-C3N4/FTO, CoSx/FTO, and CoSx/g-C3N4/FTO electrodes; (c) Photocatalytic H2 evolution rate of g-C3N4 and CoSx/g-C3N4 photocatalysts with different CoSx contents; (d) Schematic mechanism for photocatalytic H2 evolution over CoSx/g-C3N4 photocatalyst. Reprinted with permission from Ref. [286]. Copyright 2018, American Chemical Society.

Fig. 30. (a) EIS of CdS and Ni2P/CdS; (b) Photocatalytic H2 generation rate of different photocatalysts. (a,b) Reprinted with permission from Ref. [288]. Copyright 2016, American Chemical Society. (c) Steady-state PL spectra of g-C3N4 and Ni/g-C3N4 with different Ni loadings; (d) Photocatalytic activity of H2 evolution over Ni/CN with different Ni loadings. (c,d) Reprinted with permission from Ref. [289]. Copyright 2019, The Royal Society of Chemistry. (e) The HER polarization curves of various catalysts; (f) PL spectra for g-C3N4, Pt/g-C3N4, and 1 wt% C-ZIF/g-C3N4 composite under 375 nm excitation. (e,f) Reprinted with permission from Ref. [301]. Copyright 2019, The Royal Society of Chemistry.

Fig. 31. (a) TRPL spectra of EY sensitized g-C3N4, CN/FeP/g-C3N4 and CN/FeNi7.47P/g-C3N4 composites; (b) Possible mechanism of photocatalytic H2 evolution over the EY-sensitized CN/FeNiP/g-C3N4 composite. (a,b) Reprinted with permission from Ref. [303]. Copyright 2019, Elsevier. (c) EIS for g-C3N4, g-C3N4/C@Ni2P, and g-C3N4/C@Ni3S4/Ni2P with different phosphating times; (d) Schematic preparation process of the g-C3N4/C@Ni3S4/Ni2P composite; (e) The proposed mechanism of photocatalytic H2 evolution over EY-sensitized g-C3N4/C@Ni3S4/Ni2P composite. (c?e) Reprinted with permission from Ref. [304]. Copyright 2019, Elsevier. (f) Photocurrent responses of g-C3N4, MoO2-8%/g-C3N4 and MoNi@MoO2-8%/g-C3N4; (g) Schematic process of charge transfer and H2 production over MoNi@MoO2/g-C3N4 composite. (f,g) Reprinted with permission from Ref. [305]. Copyright 2020, Elsevier.

Fig. 32. (a) Schematic synthesis process of the NixCo1?xO@C/CdS nanocomposites; (b) Schematic process of photogenerated carries separation and transfer in the NixCo1?xO@C/CdS system; (c) Photocatalytic activity of H2 evolution over CdS, Pt/CdS and NixCo1?xO@C/CdS. (a?c) Reprinted with permission from Ref. [307]. Copyright 2020, Elsevier. (d) Schematic preparation process of CoP/Co@NPC/g-C3N4 photocatalysts; (e) Schematic process of charge transfer and H2 production; (f) H2 generation over Co@NC/g-C3N4 and CoP/Co@NPC/g-C3N4 with different phosphidation time [308]. (d?f) Reprinted with permission from Ref. [308]. Copyright 2020, American Chemical Society.

Fig. 33. Schematic preparation process of ZIF-8-derived ZnO and ZIF-8@ZIF-67-derived ZnO@Co3O4 polyhedron. Reprinted with permission from Ref. [310]. Copyright 2016, The Royal Society of Chemistry.

Fig. 34. TEM images of ZnO photocatalyst derived from ZIF-8 before (a) and after (b) photocatalytic CO2 reduction; TEM images of ZnO@Co3O4 photocatalyst derived from ZIF-8@ZIF-67 before (c) and after (d) photocatalytic CO2 reduction; (e) Schematic diagram of ZnO and ZnO@Co3O4 participating in photocatalytic CO2 reduction; (f) CO and (g) CH4 evolution by various photocatalysts. Reprinted with permission from Ref. [310]. Copyright 2016, The Royal Society of Chemistry.

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金属-有机框架衍生的多功能光催化剂

Metal-organic framework-derived multifunctional photocatalysts

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