基于金属氧化物材料的二氧化碳电催化还原

doi:10.3866/PKU.WHXB202009033

物理化学学报 >> 2021, Vol. 37 >> Issue (7): 2009033.doi: 10.3866/PKU.WHXB202009033

所属专题：电催化

基于金属氧化物材料的二氧化碳电催化还原

郝磊端, 孙振宇()

有机-无机复合材料国家重点实验室，北京化工大学化学工程学院，北京 100029

收稿日期:2020-09-09 录用日期:2020-11-05 发布日期:2020-11-16
通讯作者: 孙振宇 E-mail:sunzy@mail.buct.edu.cn
作者简介:Zhenyu Sun was born in April 1977. He is currently a full professor in the College of Chemical Engineering at Beijing University of Chemical Technology (China). He completed his Ph.D. at Institute of Chemistry, Chinese Academy of Sciences in 2006. He did postdoctoral research in Trinity College Dublin (Ireland) from 2006 to 2008, at Ruhr University, Bochum (Germany) from 2011 to 2014, and University of Oxford from 2014 to 2015. He has obtained a Humboldt Research Fellowship for Experienced Researchers (Germany). His current research focuses on energy conversion reactions using two-dimensional materials
基金资助:
国家自然科学基金(21972010);北京市自然科学基金(2192039)

Metal Oxide-Based Materials for Electrochemical CO₂ Reduction

Leiduan Hao, Zhenyu Sun()

State Key Laboratory of Organic-Inorganic Composites, Beijing University of Chemical Technology, Beijing 100029, China

Received:2020-09-09 Accepted:2020-11-05 Published:2020-11-16
Contact: Zhenyu Sun E-mail:sunzy@mail.buct.edu.cn
About author:Zhenyu Sun, Email: sunzy@mail.buct.edu.cn. Tel.: +86-13301308339
Supported by:
National Natural Science Foundation of China(21972010);Beijing Natural Science Foundation, China(2192039)

摘要/Abstract

摘要：

电催化方法还原二氧化碳制备高附加值化学品，在降低二氧化碳浓度、平衡碳循环和储存可再生途径产生的电能等方面展现较大潜力。通过设计高效电催化剂来降低二氧化碳电催化还原过程所需的过电位并提高产物的选择性和电流密度，对电催化还原二氧化碳的发展和应用具有重要意义。本文总结了金属氧化物基材料作为电催化剂在二氧化碳电还原中的最新研究进展，深入探讨了金属氧化物在催化反应中的作用、稳定性及结构性能关系，并对金属氧化物基材料在二氧化碳电还原中未来的设计和研究方向做出思考。

关键词: 二氧化碳电化学还原, 金属氧化物, 电催化剂, 选择性, 稳定性

Abstract:

The CO₂ level in the atmosphere has been increasing since the industrial revolution owing to anthropogenic activities. The increased CO₂ level has led to global warming and also has detrimental effects on human beings. Reducing the CO₂ level in the atmosphere is urgent for balancing the carbon cycle. In this regard, reduction in CO₂ emission and CO₂ storage and usage are the main strategies. Among these, CO₂ usage has been extensively explored, because it can reduce the CO₂ level and simultaneously provide opportunities for the development in catalysts and industries to convert CO₂ as a carbon source for preparing valuable products. However, transformation of CO₂ to other chemicals is challenging owing to its thermodynamic and kinetic stabilities. Among the CO₂ utilization techniques, electrochemical CO₂ reduction (ECR) is a promising alternative because it is generally conducted under ambient conditions, and water is used as the economical hydrogen source. Moreover, ECR offers a potential route to store electrical energy from renewable sources in the form of chemical energy, through generation of CO₂ reduction products. To improve the energy efficiency and viability of ECR, it is important to decrease the operational overpotential and maintain large current densities and high product selectivities; the development of efficient electrocatalysts is a critical aspect in this regard. To date, many kinds of materials have been designed and studied for application in ECR. Among these materials, metal oxide-based materials exhibit excellent performance as electrocatalysts for ECR and are attracting increasing attention in recent years. Investigation of the mechanism of reactions that involve metallic electrocatalysts has revealed the function of trace amount of oxidized metal species—it has been suggested that the presence of metal oxides and metal-oxygen bonds facilitates the activation of CO₂ and the subsequent formation and stabilization of the reaction intermediates, thereby resulting in high efficiency and selectivity of the ECR. Although the stability of metal oxides is a concern as they are prone to reduction under a cathodic potential, the catalytic performance of metal oxide-based catalysts can be maintained through careful designing of the morphology and structure of the materials. In addition, introducing other metal species to metal oxides and fabricating composites of metal oxides and other materials are effective strategies to achieve enhanced performance in ECR. In this review, we summarize the recent progress in the use of metal oxide-based materials as electrocatalysts and their application in ECR. The critical role, stability, and structure-performance relationship of the metal oxide-based materials for ECR are highlighted in the discussion. In the final part, we propose the future prospects for the development of metal oxide-based electrocatalysts for ECR.

Key words: Electrochemical CO₂ reduction, Metal oxides, Electrocatalysts, Selectivity, Stability

MSC2000:

O642

郝磊端, 孙振宇. 基于金属氧化物材料的二氧化碳电催化还原[J]. 物理化学学报, 2021, 37(7): 2009033.

Leiduan Hao, Zhenyu Sun. Metal Oxide-Based Materials for Electrochemical CO₂ Reduction[J]. Acta Phys. -Chim. Sin., 2021, 37(7): 2009033.

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Table 1

Summary of representative metal oxide-based materials for ECR."

Electrocatalyst	Electrolyte	Major product and maximum FE	Current density ^b	Stability	Ref.
O₂ plasma treated Cu	0.1 mol∙L⁻¹ KHCO₃	C₂H₄, 60.0% at −0.9 V versus RHE	N.A.	1 h	22
Cyclic voltammetry (CV)-treated Cu	0.1 mol∙L⁻¹ KHCO₃	C₂H₄, 40.0% at −1.0 V versus RHE	N.A.	N.A.	45
Multihollow Cu₂O	2 mol∙L⁻¹ KOH	C₂₊ (C₂H₄, ethanol, propanol, acetic acid), 75.2% at −0.61 V versus RHE	C₂₊: 267 mA·cm⁻² at −0.61 V versus RHE	> 3 h	47
Cu-Cu₂O/Cu	0.1 mol∙L⁻¹ KCl	C₂ (ethanol, acetic acid), 80.7% at −0.4 V versus RHE	C₂: 11.5 mA·cm⁻² at −0.4 V versus RHE	24 h	48
Cu₂O@CuMOF	0.1 mol∙L⁻¹ KHCO₃	CH₄, 63.2% at −1.71 V versus RHE	CH₄: 8.4 mA·cm⁻² at −1.71 V versus RHE	1 h	50
Cu₂O-MWCNTs	0.5 mol∙L⁻¹ NaHCO₃	CH₃OH, 38.0% at −0.8 V versus Ag/AgCl	7.5 mA·cm⁻² at −0.8 V versus Ag/AgCl	> 20 min	51
Cu₃NiOC	0.5 mol∙L⁻¹ KHCO₃	HCOO⁻, 95.9% at −0.57 V versus RHE	HCOO⁻: 10.9 mA·cm⁻² at −0.57 V versus RHE	25 h	64
Cu/La₂CuO₄	1 mol∙L⁻¹ KOH	CH₄, 56.3% at −1.4 V versus RHE	CH₄: 117 mA·cm⁻² at −1.4 V versus RHE	> 20 min	67
SnO_x	0.1 mol∙L⁻¹ KHCO₃	HCOO⁻, 64.0% at −1.2 V versus Ag/AgCl	3 mA·cm⁻² at −1.2 V versus Ag/AgCl	2 h	74
SnO_x/Sn	0.1 mol∙L⁻¹ KHCO₃	HCOO⁻, 89.0% at −1.7 V versus Ag/AgCl	6 mA·cm⁻² at −1.7 V versus Ag/AgCl	10 times of reuse	75
Cu/SnO₂	0.5 mol∙L⁻¹ KHCO₃	CO, 93.0% at −0.7 V versus RHE	4.6 mA·cm⁻² at −0.7 V versus RHE	N.A.	83
Cu/SnO_x	0.1 mol∙L⁻¹ KHCO₃	CO, 89.0% at −0.99 V versus RHE	CO: 11.3 mA·cm⁻² at −0.99 V versus RHE	N.A.	84
PbSnO₃/C	0.1 mol∙L⁻¹ nBu₄NPF₆ in PC ^a	C₂O₄²⁻, 85.1% at −1.9 V versus Ag/Ag⁺	C₂O₄²⁻: 2.0 mA·cm⁻² at −1.9 V versus Ag/Ag⁺	N.A.	85
Zn₂SnO₄/SnO₂	0.1 mol∙L⁻¹ KHCO₃	HCOO⁻, 77.0% at −1.08 V versus RHE	HCOO⁻: 5.77 mA·cm⁻² at −1.18 V versus RHE	24 h	86
1D wire in tube SnO₂	0.1 mol∙L⁻¹ KHCO₃	HCOO⁻, 63.0% at −0.99 V versus RHE	N.A.	14 h	87
SnO₂ quantum wires	0.1 mol∙L⁻¹ KHCO₃	HCOO⁻, 87.3% at −1.156 V versus RHE	HCOO⁻: 13.7 mA·cm⁻² at −1.156 V versus RHE	7	88
3D SnO₂ nanosheets on carbon cloth	0.5 mol∙L⁻¹ NaHCO₃	HCOO⁻, 87.0% at −1.6 V versus Ag/AgCl	50 mA·cm⁻² at −1.6 V versus Ag/AgCl	24 h	89
Co₃O₄ layer of 1.72 nm thickness	0.1 mol∙L⁻¹ KHCO₃	HCOO⁻, 64.3% at −0.88 V versus SCE	0.68 mA·cm⁻² at −0.88 V versus SCE	20 h	95
Bi₂O₃	0.5 mol∙L⁻¹ KHCO₃	HCOO⁻, 91.0% at −0.9 V versus RHE	HCOO⁻: 8 mA·cm⁻² at −0.9 V versus RHE	24 h	102
Bi₂O₃@C	0.5 mol∙L⁻¹ KHCO₃	HCOO⁻, 92.0% at −0.9 V versus RHE	HCOO⁻: 7.5 mA·cm⁻² at −0.9 V versus RHE	10 h	103
In₂O₃@C	0.5 mol∙L⁻¹ KHCO₃	HCOO⁻, 87.6% at −0.9 V versus RHE	14.8 mA·cm⁻² at −0.9 V versus RHE	12 h	111
ZnO nanosheets	0.1 mol∙L⁻¹ KHCO₃	CO, 83.0% at −1.1 V versus RHE	CO: 16.1 mA·cm⁻² at −1.1 V versus RHE	8 h	117
ZrO₂/N-doped carbon	0.5 mol∙L⁻¹ KHCO₃	CO, 64.0% at −0.4 V versus RHE	2.6 mA·cm⁻² at −0.4 V versus RHE	5 h	119
Ga₂O₃	3.0 mol∙L⁻¹ KCl	HCOOH, 80.0% at −2 V versus Ag/AgCl	0.3 mA·cm⁻² at −2 V versus Ag/AgCl	50 cycles	120
RuO₂-coated diamond	pH = 3.9 aqueous solution	HCOOH, 40.0% at −0.6 V versus SCE	N.A.	N.A.	123

Table 1

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基于金属氧化物材料的二氧化碳电催化还原

Metal Oxide-Based Materials for Electrochemical CO₂ Reduction

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基于金属氧化物材料的二氧化碳电催化还原

Metal Oxide-Based Materials for Electrochemical CO2 Reduction

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Metal Oxide-Based Materials for Electrochemical CO₂ Reduction