粉体光催化全水分解技术研究进展

doi:10.16085/j.issn.1000-6613.2023-0603

摘要/Abstract

摘要：

光催化全水分解制氢可以直接将太阳能转变为绿色氢能，该技术具有过程简单、成本低等优势，受到广泛关注的同时展现出了良好的应用前景。半导体光催化剂的性能是光催化全水分解技术发展的核心因素，目前该领域主要围绕光催化反应的三个基本步骤对其性能进行提升：光吸收、载流子分离与迁移以及表面反应。本文从光催化基本原理出发，围绕以上三方面概述了应对相应挑战的有效策略与近年来的研究进展，在此基础上总结了设计、制备高效光催化全水分解材料的重要方法，分析了当前影响该水分解制氢技术工业化应用的难点，指出该领域的核心问题是开发高效的窄带隙光催化材料，同时未来需着重解决逆反应严重、催化剂稳定性不足以及大规模实施过程中的氢氧混合气体分离等技术问题。

关键词: 太阳能, 光催化, 全水分解, 制氢, 催化剂, 可再生能源

Abstract:

Photocatalytic overall water splitting (POWS) is a simple and cost-effective approach to directly transforming solar energy into green hydrogen, which attracts great attention and demonstrates a bright prospect. The performance of photocatalyst is recognized as the key factor in the development of POWS. The strategies for improving the performance mainly focus on the three fundamental steps of photocatalysis, i.e., light absorption, carrier separation and migration and surface reaction. This paper reviews the recent achievements from the perspectives of valid strategies in coping with the challenges in these steps. Based on this, we summarize the important strategies of designing and preparing efficient photocatalysts for POWS and analyze the remaining obstacles to the industrial application of POWS. It is pointed out that the main challenge at present is to develop efficient narrow-gap photocatalysts. Meanwhile, the problems of serious backward reaction, the instability of the materials, and the technological problems like the separation of H₂-O₂ mixture during large-scale operations should also be addressed in the future.

Key words: solar energy, photocatalysis, overall water splitting, hydrogen production, catalyst, renewable energy

中图分类号:

TQ116.2

吴晨赫, 刘彧旻, 杨昕旻, 崔记伟, 姜韶堃, 叶金花, 刘乐全. 粉体光催化全水分解技术研究进展[J]. 化工进展, 2024, 43(4): 1810-1822.

WU Chenhe, LIU Yumin, YANG Xinmin, CUI Jiwei, JIANG Shaokun, YE Jinhua, LIU Lequan. Particulate photocatalysts for light-driven overall water splitting[J]. Chemical Industry and Engineering Progress, 2024, 43(4): 1810-1822.

图/表 5

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催化剂	吸光范围/nm	反应溶液	效率	参考文献
NiO-NaTaO₃∶La	<300	纯水	AQY：56%@270nm	[36]
Rh_0.5Cr_1.5O₃-Ga₂O₃∶Zn	<280	纯水	AQY：71%@254nm	[37]
Rh_0.5Cr_1.5O₃-AgTaO₃	<364	纯水	AQY：40%@340nm	[38]
Pt@C/CoOOH-SrTiO₃	<385	纯水	AQY：44%@360nm	[39]
Rh/Cr₂O₃/CoOOH-SrTiO₃∶Al	<385	纯水	AQY：95.9%@360nm，STH：0.65%	[5]
PtO _x /CoO _x -(g-C₃N₄)	<440	纯水	AQY：0.3%@405nm	[28]
Pt/Co(OH)₂-(Cl-g-C₃N₄)	<440	纯水	AQY：6.9%@420nm	[40]
RhCrO₃-(Ga_1-_x Zn _x )(N_1-_x O _x )	<470	硫酸溶液（pH=4.5）	AQY：5.9%@420~440nm	[14]
IrO₂-SrTiO₃∶Rh，Sb	<500	硫酸溶液（pH=3）	AQY：0.1%@420nm	[10]
NiO _x -InTaO₄∶Ni	<540	纯水	AQY：0.66%@402nm	[11]
RhCrO _x -LaMg_1/3Ta_2/3O₂N	<590	纯水	AQY：0.03%@（440±30）nm	[16]
Rh/Cr₂O₃-Ta₃N₅/KTaO₃	<600	纯水	AQY：0.22%@（420±25）nm，STH：0.014%	[21]
Ru/Cr₂O₃/IrO₂-TaON∶Zr	<600	NaOH溶液（pH=8）	AQY：0.66%@420nm，STH：0.009%	[22]
Ru/CrO _x /IrO₂-SrTaO₂N	<600	NaOH溶液（pH=8）	AQY：0.34%@（429±30）nm，STH：0.0063%	[23]
Rh/Cr₂O₃/Co₃O₄-InGaN/GaN	<630	纯水	STH：9.2%（343K），0.5%（303K）	[35]
RhCrO₃/Ir, FeCoO _x - (ZrO₂/TaON)/BiVO₄	ZrO₂/TaON<530 BiVO₄<530	Na₃PO₄溶液（pH=6.8）离子对[Fe(CN)₆]^3-/4-	AQY：12.3%@（420±10）nm， STH：0.6%	[41]
Ru/Cr₂O₃-SrTiO₃∶La, Rh/Au/BiVO₄∶Mo	SrTiO₃∶La,Rh<520 BiVO₄∶Mo<520	纯水	AQY：30%@419nm，STH：1.1%	[42]
Ru/RuO _x -SrTiO₃∶La, Rh/C/BiVO₄∶Mo	SrTiO₃∶La,Rh<520 BiVO₄∶Mo<520	纯水	STH：1.2%（331K，10kPa）， 1%（331K，91kPa）	[43]
Pt/Co(OH)₂-BDCNN₃₅₀/ BDCNN₄₂₅	BDCNN₃₅₀<470 BDCNN₄₂₅<580	纯水	AQY：23.52%@420nm， STH：1.16%	[31]

催化剂	吸光范围/nm	反应溶液	效率	参考文献
NiO-NaTaO₃∶La	<300	纯水	AQY：56%@270nm	[36]
Rh_0.5Cr_1.5O₃-Ga₂O₃∶Zn	<280	纯水	AQY：71%@254nm	[37]
Rh_0.5Cr_1.5O₃-AgTaO₃	<364	纯水	AQY：40%@340nm	[38]
Pt@C/CoOOH-SrTiO₃	<385	纯水	AQY：44%@360nm	[39]
Rh/Cr₂O₃/CoOOH-SrTiO₃∶Al	<385	纯水	AQY：95.9%@360nm，STH：0.65%	[5]
PtO _x /CoO _x -(g-C₃N₄)	<440	纯水	AQY：0.3%@405nm	[28]
Pt/Co(OH)₂-(Cl-g-C₃N₄)	<440	纯水	AQY：6.9%@420nm	[40]
RhCrO₃-(Ga_1-_x Zn _x )(N_1-_x O _x )	<470	硫酸溶液（pH=4.5）	AQY：5.9%@420~440nm	[14]
IrO₂-SrTiO₃∶Rh，Sb	<500	硫酸溶液（pH=3）	AQY：0.1%@420nm	[10]
NiO _x -InTaO₄∶Ni	<540	纯水	AQY：0.66%@402nm	[11]
RhCrO _x -LaMg_1/3Ta_2/3O₂N	<590	纯水	AQY：0.03%@（440±30）nm	[16]
Rh/Cr₂O₃-Ta₃N₅/KTaO₃	<600	纯水	AQY：0.22%@（420±25）nm，STH：0.014%	[21]
Ru/Cr₂O₃/IrO₂-TaON∶Zr	<600	NaOH溶液（pH=8）	AQY：0.66%@420nm，STH：0.009%	[22]
Ru/CrO _x /IrO₂-SrTaO₂N	<600	NaOH溶液（pH=8）	AQY：0.34%@（429±30）nm，STH：0.0063%	[23]
Rh/Cr₂O₃/Co₃O₄-InGaN/GaN	<630	纯水	STH：9.2%（343K），0.5%（303K）	[35]
RhCrO₃/Ir, FeCoO _x - (ZrO₂/TaON)/BiVO₄	ZrO₂/TaON<530 BiVO₄<530	Na₃PO₄溶液（pH=6.8）离子对[Fe(CN)₆]^3-/4-	AQY：12.3%@（420±10）nm， STH：0.6%	[41]
Ru/Cr₂O₃-SrTiO₃∶La, Rh/Au/BiVO₄∶Mo	SrTiO₃∶La,Rh<520 BiVO₄∶Mo<520	纯水	AQY：30%@419nm，STH：1.1%	[42]
Ru/RuO _x -SrTiO₃∶La, Rh/C/BiVO₄∶Mo	SrTiO₃∶La,Rh<520 BiVO₄∶Mo<520	纯水	STH：1.2%（331K，10kPa）， 1%（331K，91kPa）	[43]
Pt/Co(OH)₂-BDCNN₃₅₀/ BDCNN₄₂₅	BDCNN₃₅₀<470 BDCNN₄₂₅<580	纯水	AQY：23.52%@420nm， STH：1.16%	[31]

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