低浓度二氧化碳还原光催化剂结构设计的研究进展

doi:10.16085/j.issn.1000-6613.2024-0584

摘要/Abstract

摘要：

光催化二氧化碳（CO₂）转化为增值化学品和燃料是缓解全球变暖、实现“碳中和”目标的有前途的策略之一。为了推进该领域的发展，高效光催化剂的设计合成至关重要。相比于前期研究，近五年研究学者集中在低浓度CO₂光还原的研究上。基于此，本文综述了低浓度二氧化碳还原光催化剂结构设计的研究进展。首先介绍了光催化CO₂还原的机理、路径及其影响因素；其次总结了基于金属有机骨架材料、共价有机框架材料、金属氧化物、单原子这四类光催化剂的结构特征和调控策略；深入探讨了催化剂的CO₂吸附和富集能力、电子-空穴分离迁移能力及表面位点活性等重要因素对低浓度CO₂光催化还原效率和选择性的影响；最后，针对低浓度CO₂还原光催化剂在产物选择性、转化效率、高值C₂产品合成方面存在的挑战，本文从催化剂结构设计方向提供了相关的解决思路和策略。

关键词: 二氧化碳捕集, 光化学, 催化剂, 碳氢化合物

Abstract:

Photocatalytic conversion of carbon dioxide (CO₂) into value-added chemicals and fuels is one of the promising strategies for mitigating global warming and achieving the goal of carbon neutrality. In order to promote the development of this field, the design and synthesis of efficient photocatalysts is critical. Compared with previous studies, low-concentration CO₂ photoreduction received intensive research in the past five years. Hence, this review explores the latest advancements in structure design of photocatalyst for diluted CO₂ reduction. Firstly, the mechanism and pathways of CO₂ photoreduction as well as their influencing factors are briefly introduced. Secondly, the structural characteristics and regulation strategies are reviewed in term of four types of photocatalyst, including metal-organic framework, covalent organic framework, metal oxides, and single atom photocatalysts. The effects of CO₂ adsorption and enrichment, electron-hole separation and migration and surface site activity on the efficiency and selectivity were deeply investigated. Finally, in response to the opportunities and challenges of photocatalyst for efficient diluted CO₂ reduction, including product selectivity, conversion efficiency and the synthesis of high-value C₂ products, we proposed relevant solutions and strategies regarding catalyst structure design.

Key words: carbon dioxide capture, photochemistry, catalyst, hydrocarbons

中图分类号:

O644

于梦洁, 吴语童, 罗发祥, 豆义波. 低浓度二氧化碳还原光催化剂结构设计的研究进展[J]. 化工进展, 2024, 43(S1): 335-350.

YU Mengjie, WU Yutong, LUO Faxiang, DOU Yibo. Research progress on structural design of photocatalysts for diluted carbon dioxide reduction[J]. Chemical Industry and Engineering Progress, 2024, 43(S1): 335-350.

图/表 13

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还原半反应	E₀/V
CO₂+e^-CO₂^-	-1.85
CO₂+2H⁺+2e^-CO+H₂O	-0.53
CO₂+2H⁺+2e^-HCOOH	-0.61
CO₂+4H⁺+4e^-HCHO+H₂O	-0.48
CO₂+6H⁺+6e^-CH₃OH+H₂O	-0.38
CO₂+8H⁺+8e^-CH₄+2H₂O	-0.24
2CO₂+12H⁺+12e^-C₂H₄+4H₂O 2CO₂+14H⁺+14e^-C₂H₆+4H₂O	-0.35 -0.27

还原半反应	E₀/V
CO₂+e^-CO₂^-	-1.85
CO₂+2H⁺+2e^-CO+H₂O	-0.53
CO₂+2H⁺+2e^-HCOOH	-0.61
CO₂+4H⁺+4e^-HCHO+H₂O	-0.48
CO₂+6H⁺+6e^-CH₃OH+H₂O	-0.38
CO₂+8H⁺+8e^-CH₄+2H₂O	-0.24
2CO₂+12H⁺+12e^-C₂H₄+4H₂O 2CO₂+14H⁺+14e^-C₂H₆+4H₂O	-0.35 -0.27

光催化剂	光源	反应条件	反应气组成	主要产物	生成速率 /μmol∙g^-1∙h^-1	选择性 /%	量子效率 /%	参考文献
TiO₂/UiO-66	300W 氙灯（λ>300nm）	H₂O	10%CO₂+90%Ar	CH₄	17.9	90.4	—	[56]
Pt/Co@NC	500W氙灯（λ>200nm）	H₂O	400μg/g CO₂	CH₄	14.4	100	—	[71]
CoAl-LDH	500W氙灯（λ>200nm）	H₂O	400μg/g CO₂	CH₄	4.3	92	—	[74]
TpBb-COF	300W氙灯（λ>420nm）	H₂O	30%CO₂+70%N₂	CO	89.9	100	—	[61]
TpPa/ZIF-8	40W LED 灯	H₂O	10%CO₂+90%Ar	CO	84.9	100	—	[62]
BA-PDI-Ni	300W氙灯（λ>200nm）	[Ru(bpy)₃]Cl₂,CH₃CN,三乙醇胺，H₂O	10%CO₂+90%Ar	CO	2262	100	0.2	[73]
MAF-34-CoRu	300W氙灯（λ>420nm）	CH3CN/H2O	15%CO₂+85%N2	CO	4.26	—	—	[55]
Ni-Co₃O₄	300W氙灯（λ≥420nm）	[Ru(bpy)₃]Cl₂,CH₃CN,三乙醇胺，H₂O	10%CO₂+90%Ar	合成气	CO：89100 H₂：80100	—	3.7	[67]
Zn-S-COF	300W氙灯（λ≥420nm）	H₂O	15%CO₂+85%Ar	合成气	CO:105.8 H₂: 3.4	—	—	[65]
Ni-TP-CON	300W氙灯 λ>300nm	[Ru(bpy)₃]Cl₂,CH₃CN,三乙醇胺，H₂O	15%CO₂+85%Ar	合成气	CO: 3200 H₂：200	—	1.2	[63]
VoHCo₃O₄/ OMNC	300W氙灯（λ>420nm）	H₂O	10%CO₂+90%Ar	合成气	CO: 337.8 H₂：95.2	—	4.2	[69]

光催化剂	光源	反应条件	反应气组成	主要产物	生成速率 /μmol∙g^-1∙h^-1	选择性 /%	量子效率 /%	参考文献
TiO₂/UiO-66	300W 氙灯（λ>300nm）	H₂O	10%CO₂+90%Ar	CH₄	17.9	90.4	—	[56]
Pt/Co@NC	500W氙灯（λ>200nm）	H₂O	400μg/g CO₂	CH₄	14.4	100	—	[71]
CoAl-LDH	500W氙灯（λ>200nm）	H₂O	400μg/g CO₂	CH₄	4.3	92	—	[74]
TpBb-COF	300W氙灯（λ>420nm）	H₂O	30%CO₂+70%N₂	CO	89.9	100	—	[61]
TpPa/ZIF-8	40W LED 灯	H₂O	10%CO₂+90%Ar	CO	84.9	100	—	[62]
BA-PDI-Ni	300W氙灯（λ>200nm）	[Ru(bpy)₃]Cl₂,CH₃CN,三乙醇胺，H₂O	10%CO₂+90%Ar	CO	2262	100	0.2	[73]
MAF-34-CoRu	300W氙灯（λ>420nm）	CH3CN/H2O	15%CO₂+85%N2	CO	4.26	—	—	[55]
Ni-Co₃O₄	300W氙灯（λ≥420nm）	[Ru(bpy)₃]Cl₂,CH₃CN,三乙醇胺，H₂O	10%CO₂+90%Ar	合成气	CO：89100 H₂：80100	—	3.7	[67]
Zn-S-COF	300W氙灯（λ≥420nm）	H₂O	15%CO₂+85%Ar	合成气	CO:105.8 H₂: 3.4	—	—	[65]
Ni-TP-CON	300W氙灯 λ>300nm	[Ru(bpy)₃]Cl₂,CH₃CN,三乙醇胺，H₂O	15%CO₂+85%Ar	合成气	CO: 3200 H₂：200	—	1.2	[63]
VoHCo₃O₄/ OMNC	300W氙灯（λ>420nm）	H₂O	10%CO₂+90%Ar	合成气	CO: 337.8 H₂：95.2	—	4.2	[69]

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