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

doi:10.13801/j.cnki.fhclxb.20240204.003

光电催化与人工光合作用还原CO₂研究进展

doi: 10.13801/j.cnki.fhclxb.20240204.003

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，研究方向为光催化　E-mail: tianyi870328@163.com

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

中图分类号: TB333
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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: 2024-02-06
- 刊出日期: 2024-10-15

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, 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。由于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^[8]

Figure 1. Classification of common photocatalysts for CO₂ catalytic reduction/conversion to value-added products^[8]

ZIF—Zeolitic imidazolate framework; PMOF—Polymeric metal-organic frameworks; MIL—Materials of institut lavoisier; MOF—Metal-organic frameworks

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图 2 用于CO₂催化还原/转化为增值产品的常见电催化剂的分类^[8]

Figure 2. Classification of common electrocatalysts for CO₂ catalytic reduction/conversion to value-added products^[8]

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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^[136]

Figure 4. Photogenerated electron transfer process of porphyrin-graphene composites^[136]

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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

NADP—Nicotinamide adenine dinucleotide phosphate; ADP—Adenosine diphosphate; NADPH—Nicotinamide adenine dinucleotide phosphate; ATP—Adenosine triphosphate

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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 metal supported semiconductor photocatalyst composites for CO₂ reduction

Photocatalyst	Main product	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	[54]
SrCO₃/SrTiO₃	CO	CO: 23.82 (100) μmol·h⁻¹·g⁻¹	[55]
Fe₂O₃/Cu₂O	CO	5.0 μmol·g⁻¹ catalyst	[56]
Cu₂ZnSnS₄-ZnO	CH₄	138.90 μmol·g⁻¹·L⁻¹	[57]
TiO₂-SiO₂	CH₄	2.42 μmol·g⁻¹	[58]
Cu/TiO₂	CH₃OH	1.8 μmol·cm⁻²·h⁻¹	[59]
Sulfur-doped g-C₃N₄	CH₃OH	1.12 μmol·g⁻¹	[60]
ZnPc/TiO₂	HCOOH	978.6 μmol·g⁻¹ catalyst	[61]
GO-TiO₂	CH₃OH/C₂H₅OH	47.0 μmol·g⁻¹·h⁻¹/144.7 μmol·g⁻¹·h⁻¹	[62]
Bi₂S₃	HC(O)OCH₃	300.94 μmol·g⁻¹	[63]
Notes: m-CeO₂—Mesoporous-CeO₂; GO—Graphene oxide; ZnPc—Zinc-phthalocyanine.

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表 2 一些用于CO₂还原的选择性电催化剂

Table 2. Some selective electrocatalysts for CO₂ reduction

Electrocatalyst	Electrolyte	Main product	Corresponding overpotential	Ref.
Fe-N₄O	0.1 mol/L KHCO₃, pH=6.8	CO	470 mV	[88]
In(OH)₃-Cu₂O	0.7 mol/L KHCO₃	CO	290 mV	[89]
BiOI	0.5 mol/L NaHCO₃, pH=6	HCOOH	−0.40 V	[90]
Pyridoxine modification graphene oxide (GO-VB₆-Cu)	0.1 mol/L KHCO₃, pH=6.8	CH₃CH₂OH	0.14 V	[84]
Graphite/carbon nanoparticle (NPs)/ Cu/polytetrafluoroethylene (PTFE)	7 mol/L KOH, pH>14	C₂H₄	−0.63 V	[91]
Cu₂O/ZnO/Graphene (GN)	0.5 mol/L NaHCO₃	C₃H₇OH	−0.90 V	[92]
Cu/TiO₂/GN	0.2 mol/L KI, pH=6.62	C₂H₅OH	0.84 V	[93]
Bi nanosheet	0.1 mol/L KHCO₃, pH=6.8	HCOOH	420 mV	[94]
Nanoporous Au-Sn (NPAS)	0.5 mol/L KHCO₃, pH=7.2	CO	0.45 V	[95]

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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(vs NHE)/V	Product
CO₂ + e⁻→•$\text{CO}_{2}^{-} $	−1.90	•$\text{CO}_{2}^{-} $ anion radical
2CO₂ + 2H⁺ + 2e⁻ → H₂C₂O₄	−0.87	Oxalate
CO₂ + 2H⁺ + 2e⁻ → HCOOH	−0.61	Formic acid
CO₂ + 2H⁺ + 2e⁻ → CO + H₂O	−0.53	Carbon monoxide
CO₂ + 4H⁺ + 4e⁻ → HCHO + H₂O	−0.48	Formaldehyde
CO₂ + 6H⁺ + 6e⁻ → CH₃OH + H₂O	−0.38	Methanol
2CO₂ + 12H⁺ + 12e⁻ → C₂H₅OH + 3H₂O	−0.33	Ethanol
2CO₂ + 14H⁺ + 14e⁻ → C₂H₆ + 4H₂O	−0.27	Ethane
CO₂ + 8H⁺ + 8e⁻ → CH₄ + 2H₂O	−0.24	Methane
Notes: E^o—Standard electrode potential; NHE—Normal hydrogen electrode.

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表 4 用于CO₂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 product	Yield/(μmol·g_cat⁻¹·h⁻¹)	Ref.
Pt/TiO₂	8	CH₄	1361	[108]
Cu@TiO₂-Au	2	HCOOH	N.A.	[100]
Au-ZnTe/ZnO	2	CO	N.A.	[109]
Rh grain boundaries (GBs)/TiO₂	12	C₂H₅OH	12.1	[110]
NH₃/g-C₃N₄	8, 6	CH₄, CH₃OH	1.39, 1.87	[111]
NH₂-C/Cu₂O	2	HCOOH	138.65	[112]
Co-ZIF9/g-C₃N₄	2	CO	495	[113]
UiO-66/MoS₂	8	CH₃COOH	39	[114]
Ni(II) MOF/g-C₃N₄	2, 8	CO, CH₄	13.6	[115]
Note: N.A.—Not available.

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光电催化与人工光合作用还原CO₂研究进展

doi: 10.13801/j.cnki.fhclxb.20240204.003

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

史载锋，博士，教授，博士生导师，研究方向为材料化学　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

doi: 10.13801/j.cnki.fhclxb.20240204.003

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

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Advances in photoelectrocatalysis and artificial photosynthesis for the reduction of CO2

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目录

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，研究方向为光催化　E-mail: tianyi870328@163.com

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

Advances in photoelectrocatalysis and artificial photosynthesis for the reduction of CO₂