光电催化与人工光合作用还原CO<sub>2</sub>研究进展

刘金瑞; 张妍; 孙诗书; 石建军; 孙天一; 史载锋

光电催化与人工光合作用还原CO₂研究进展

海南师范大学, 化学与化工学院, 海口市重点实验室, 海南省水污染治理与资源化重点实验室, 海南海口 570100

基金项目: 国家自然科学基金(22168017)；海南省自然科学基金(420QN259, 222CXTD513, 420QN251)

详细信息

通讯作者:
孙天一，博士，讲师，硕士生导师，研究方向：光催化，　E-mail：tianyi870328@163.com

史载锋，博士，教授，博士生导师，研究方向：材料化学。　E-mail：zaifengshi@163.com

中图分类号: TB333
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- HTML全文浏览量: 61
- 被引次数: 0
出版历程
- 收稿日期: 2023-11-13
- 修回日期: 2024-01-16
- 录用日期: 2024-01-20
- 网络出版日期: 2024-02-28

Advances in photoelectrocatalysis and artificial photosynthesis for the reduction of CO₂

Haikou Key Laboratory, Hainan Provincial Key Laboratory of Water Pollution Control and Resource Reuse, School of Chemistry and Chemical Engineering, Hainan Normal University, Haikou 570100, Hainan, China

Funds: National Natural Science Foundation of China (22168017); Hainan Provincial Natural Science Foundation of China (420QN259,222CXTD513, 420QN251)

摘要

摘要: 随着工业化的不断发展，化石燃料的过度使用产生的CO₂导致了温室效应等问题，已经引起国际社会的高度关注，并制定了一系列应对措施。因此，对大气中CO₂的还原回收技术研发具有迫切性和重要意义。光电催化是目前可用于还原CO₂的具有良好应用前景的技术之一，为了对该技术进行更深入的研究，推动其实际应用，本文首先阐述了光催化、电催化、光电催化还原CO₂的基本原理和优缺点，并举例介绍了各类催化剂还原CO₂的效率。因为光催化是光合作用中的重要步骤之一，接着重点分析了光合作用在还原CO₂研究现状和前景，提出人工光合作用还原CO₂可行性与潜力。本文旨在为人工光合作用还原CO₂提供新思路和参考，为减少大气中CO₂的积累和应对当前的环境挑战提供新的见解和视角。
- 太阳能 /
- 光合作用 /
- CO₂还原 /
- 催化剂 /
- 光催化 /
- 电催化 /
- 光电催化
Abstract: With the continuous development of industrialization, CO₂ produced by the excessive use of fossil fuels has led to problems such as the greenhouse effect, which has attracted great attention from the international community and a series of countermeasures have been formulated. Therefore, the research and development of technology for the reduction and recovery of CO₂ from the atmosphere is urgent and important. Photoelectrocatalysis is one of the technologies with good application prospects that can be used to reduce CO₂. In order to carry out a more in-depth research on this technology and promote its practical application, this paper firstly describes the basic principles and advantages and disadvantages of photocatalysis, electrocatalysis, and photoelectrocatalysis for CO₂ reduction, and gives examples of the efficiency of various types of catalysts for CO₂ reduction. Because photocatalysis is one of the important steps in photosynthesis, it then focuses on analyzing the current status and prospects of photosynthesis in reducing CO₂ research, and proposes the feasibility and potential of artificial photosynthesis for CO₂ reduction. The aim of this paper is to provide new ideas and references for the reduction of CO₂ by artificial photosynthesis, and to provide new insights and perspectives for reducing the accumulation of CO₂ in the atmosphere and addressing current environmental challenges.
- solar energy /
- photosynthesis /
- CO₂ reduction /
- catalyst /
- photocatalysis /
- electrocatalysis /
- photoelectrocatalysis

HTML全文

图 1 用于CO₂催化还原/转化为增值产品的常见光催化剂的分类^[10]

Figure 1. Classification of common photocatalysts for CO₂ catalytic reduction / conversion to value-added products^[10]

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图 2 用于二氧化碳催化还原/转化为增值产品的常见电催化剂的分类^[10]

Figure 2. Classification of common electrocatalysts for CO₂ catalytic reduction / conversion to value-added products^[10]

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图 3 叶绿素a与叶绿素b结构示意图

Figure 3. Structure diagram of chlorophyll a and chlorophyll b

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图 4 卟啉-石墨烯复合材料光生电子的转移过程^[143]

Figure 4. Photogenerated electron transfer process of porphyrin-graphene composites^[143]

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图 5 光合作用反应序列—明暗反应

Figure 5. Photosynthetic reaction sequence-light-dark reaction

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表 1 部分非金属或金属负载半导体光催化剂复合材料用于CO₂还原

Table 1. Several non-metallic or metalsupported semiconductor photocatalyst composites for CO₂ reduction

Photocatalyst	Main products	Photocatalytic activity	Ref.
m-CeO₂/g-C₃N₄	CH₄ and CO	CH₄ 13.88 µmol·h⁻¹·g⁻¹; CO 11.8 µmol·h⁻¹·g⁻¹	[56]
SrCO₃/SrTiO₃	CO	CO 23.82 (100) μmol·h⁻¹·g⁻¹	[57]
Fe₂O₃/Cu₂O	CO	5.0 μmol·g·cat⁻¹	[58]
Cu₂ZnSnS₄-ZnO	CH₄	138.90 μmol·g⁻¹·L⁻¹	[59]
TiO₂-SiO₂	CH₄	2.42 μmol·g⁻¹	[60]
Cu/TiO₂	CH₃OH	1.8 μmol·cm⁻²·h^-1	[61]
Sulfur-doped g-C₃N₄	CH₃OH	1.12 μmol·g⁻¹	[62]
ZnPc/TiO₂	HCOOH	978.6 μmol·g·cat⁻¹	[63]
GO-TiO₂Composite	CH₃OH/C₂H₅OH	47.0 μmol·g⁻¹·h⁻¹/144.7 μmol·g⁻¹·h⁻¹	[64]
Bi₂S₃	HC(O)OCH₃	300.94 μmol·g⁻¹	[65]

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表 2 一些用于二氧化碳还原的选择性电催化剂

Table 2. Some selective electrocatalysts for CO₂ reduction

Electrocatalyst	Electrolyte	Main products	Corresponding overpotential	Ref.
Fe-N₄O	0.1 mol/L KHCO₃,6.8 pH	CO	470 mV	[91]
In(OH)₃-Cu₂O	0.7 mol/L KHCO₃	CO	290 mV	[92]
BiOI	0.5 mol/L NaHCO₃,6 pH	HCOOH	−0.40 V	[93]
Pyridoxine modification graphene oxide(GO-VB₆-Cu)	0.1 mol/L KHCO₃,6.8 pH	CH₃CH₂OH	0.14 V	[94]
Graphite/carbon NPs/Cu/ polytetrafluoroethylene(PTFE)	7 mol/L KOH,>14 pH	C₂H₄	−0.63 V	[95]
Cu₂O/ZnO/Graphene(GN)	0.5 mol/L NaHCO₃	C₃H₇OH	−0.90 V	[96]
Cu/TiO₂/Graphene(GN)	0.2 mol/L KI, 6.62 pH	C₂H₅OH	0.84 V	[97]
Bi nanosheet	0.1 mol/L KHCO₃, 6.8 pH	HCOOH	420 mV	[98]
nanoporous Au-Sn(NPAS)	0.5 mol/L KHCO₃, 7.2 pH	CO	0.45 V	[99]

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表 3 CO₂还原的主要产物及其对应电位(pH=7)

Table 3. Main products of CO₂ reduction and their corresponding potentials(pH=7)

Reaction	E^o(V vs. NHE)	Product
CO₂ + e⁻→CO₂	−1.90	·CO- 2 anion radical
2 CO₂ + 2 H⁺ + 2 e⁻ → H₂C₂O₄	−0.87	Oxalate
CO₂ + 2 H⁺ + 2 e⁻ → HCOOH	−0.61	Formic acid
CO₂ + 2 H⁺ + 2 e⁻ → CO + H₂O	−0.53	Carbon monoxide
CO₂ + 4 H⁺ + 4 e⁻ → HCHO + H₂O	−0.48	Formaldehyde
CO₂ + 6 H⁺ + 6 e⁻ → CH₃OH + H₂O	−0.38	Methanol
2 CO₂ + 12 H⁺ + 12 e⁻ → C₂H₅OH + 3 H₂O	−0.33	Ethanol
2 CO₂ + 14 H⁺ + 14 e⁻ → C₂H₆ + 4 H₂O	−0.27	Ethane
CO₂ + 8 H⁺ + 8 e⁻ → CH₄ + 2 H₂O	−0.24	Methane

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表 4 用于二氧化碳还原的几种光电催化界面

Table 4. Several photoelectrocatalytic interfaces for CO₂ reduction

catalyst	Number of electrons transferred	Main products	Yield [μmol/g-cat/h]	Ref.
Pt/TiO₂	8	CH₄	1361	[113]
Cu@TiO₂-Au	2	HCOOH	N.A.	[114]
Au-ZnTe/ZnO	2	CO	N.A.	[115]
Rh grain boundaries(GBs)/TiO₂	12	C₂H₅OH	12.1	[116]
NH₃/g-C₃N₄	8, 6	CH₄, CH₃OH	1.39, 1.87	[117]
NH₂-C/Cu₂O	2	HCOOH	138.65	[118]
Co-ZIF9/g-C₃N₄	2	CO	495	[119]
UiO-66/MoS₂	8	CH₃COOH	39	[120]
Ni(II) MOF/g-C₃N₄	2, 8	CO, CH₄	13.6	[121]

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光电催化与人工光合作用还原CO₂研究进展

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孙天一，博士，讲师，硕士生导师，研究方向：光催化，　E-mail：tianyi870328@163.com

史载锋，博士，教授，博士生导师，研究方向：材料化学。　E-mail：zaifengshi@163.com

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Advances in photoelectrocatalysis and artificial photosynthesis for the reduction of CO₂

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光电催化与人工光合作用还原CO2研究进展

通讯作者: 孙天一，博士，讲师，硕士生导师，研究方向：光催化， E-mail：tianyi870328@163.com 史载锋，博士，教授，博士生导师，研究方向：材料化学。 E-mail：zaifengshi@163.com

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Advances in photoelectrocatalysis and artificial photosynthesis for the reduction of CO2

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光电催化与人工光合作用还原CO₂研究进展

通讯作者:
孙天一，博士，讲师，硕士生导师，研究方向：光催化，　E-mail：tianyi870328@163.com

史载锋，博士，教授，博士生导师，研究方向：材料化学。　E-mail：zaifengshi@163.com

Advances in photoelectrocatalysis and artificial photosynthesis for the reduction of CO₂