缺陷态二维超薄材料用于光/电催化CO2还原的基础与展望

doi:10.3866/PKU.WHXB202308052

物理化学学报 >> 2025, Vol. 41 >> Issue (3): 100019.doi: 10.3866/PKU.WHXB202308052

所属专题：能源化学

缺陷态二维超薄材料用于光/电催化CO₂还原的基础与展望

陈润华¹^,†, 吴琼¹^,†, 罗婧宸¹, 祖小龙²^,*(), 朱姗³, 孙永福¹^,*()

¹ 中国科学技术大学合肥微尺度物质科学国家研究中心, 合肥 230026
² 福建省能源材料科学与技术创新实验室(IKKEM), 福建厦门 360015
³ 国网安徽省电力有限公司电力科学研究院, 合肥 230601

收稿日期:2023-08-31 修回日期:2023-10-04 录用日期:2023-10-17 发布日期:2023-12-20
通讯作者: Email: xiaolongzu@xmu.edu.cn (祖小龙)yfsun@ustc.edu.cn (孙永福)
作者简介:
^†These authors contributed equally to this work.
基金资助:
国家重点研发计划(2019YFA0210004); 国家重点研发计划(2022YFA1502904); 国家重点研发计划(2021YFA1501502); 国家自然科学基金(22125503); 国家自然科学基金(21975242); 国家自然科学基金(U2032212); 中国科学院青年创新促进会优秀会员(CX2340007003); 安徽省自然科学基金(2208085QB31)

Defective Ultrathin Two-Dimensional Materials for Photo-/Electrocatalytic CO₂ Reduction: Fundamentals and Perspectives

Runhua Chen¹, Qiong Wu¹, Jingchen Luo¹, Xiaolong Zu²^,*(), Shan Zhu³, Yongfu Sun¹^,*()

¹ Hefei National Research Center for Physical Sciences at Microscale, University of Science and Technology of China, Hefei 230026, China
² Innovation Laboratory for Sciences and Technologies of Energy Materials of Fujian Province (IKKEM), Xiamen 361005, Fujian Province, China
³ State Grid Anhui Electric Power Research Institute, Hefei 230601, China

Received:2023-08-31 Revised:2023-10-04 Accepted:2023-10-17 Published:2023-12-20
Contact: Email: xiaolongzu@xmu.edu.cn (Xiaolong Zu)yfsun@ustc.edu.cn (Yongfu Sun)
Supported by:
the National Key Research and Development Program of China(2019YFA0210004); the National Key Research and Development Program of China(2022YFA1502904); the National Key Research and Development Program of China(2021YFA1501502); the National Natural Science Foundation of China(22125503); the National Natural Science Foundation of China(21975242); the National Natural Science Foundation of China(U2032212); the Youth Innovation Promotion Association of CAS(CX2340007003); the Anhui Provincial Natural Science Foundation(2208085QB31)

摘要/Abstract

摘要：

太阳能、风能等可再生能源驱动的光/电催化还原二氧化碳(CO₂)制碳基燃料是一种非常吸引人的资源再生和能源存储策略，这对中国实现碳达峰和碳中和战略具有重要意义。然而，CO₂分子极高的热力学稳定性和极强的化学惰性导致CO₂还原反应的转化效率和选择性仍然不理想，这严重限制了CO₂转化技术的实际应用。得益于超薄的厚度、高比表面积和相对均一的暴露晶面等特性，二维超薄材料具有高活性、高密度以及高均一的催化位点，能够优化关键的热力学和动力学因素，进而有效改善CO₂光/电还原性能。需要指出的是，缺陷态二维超薄材料中的富电子催化位点能够更高效地吸附和活化CO₂分子，从而有效降低反应势垒，加速CO₂还原并提高产物选择性。此外，二维超薄材料的缺陷结构也有助于催化过程中的质子传递和电子转移等行为，从而进一步提高催化剂的反应活性。本文综述了缺陷态二维超薄材料在CO₂光/电催化还原方面的最新研究进展，详细介绍了几类常见的缺陷态二维超薄材料的可控制备方法和精细结构表征。结合典型实例，系统总结了表面缺陷结构对二维超薄材料的局域原子结构和电子结构的调制作用，以及对CO₂还原性能的影响。最后，展望了缺陷态二维超薄材料在CO₂还原领域所面临的挑战与机遇，为今后的研究提供了借鉴和启示。

关键词: 缺陷结构, 二维超薄材料, 二氧化碳还原, 光/电催化反应

Abstract:

Photo-/electrocatalytic reduction of carbon dioxide (CO₂) to carbon-based fuel molecules driven by renewable energy is an attractive strategy for resource regeneration and energy storage, especially for achieving carbon peak and carbon-neutral goals. However, the high thermodynamic stability and chemical inertness of CO₂ molecules make the conversion efficiency and selectivity of reduction products very low, which further hinders its application. In addition, different CO₂ reduction products have similar reduction potential and usually face severe hydrogen evolution competition under aqueous system conditions, which makes the selectivity of specific reduction products unable to be effectively controlled. To overcome these bottlenecks, researchers have been working for many years to develop efficient photo/electrocatalysts to enhance the activity and product selectivity of CO₂ reduction. Thanks to the ultrathin thickness and large specific surface area, ultrathin two-dimensional materials possess highly active sites with high density and high uniformity, which can effectively regulate the key thermodynamic and kinetic factors of CO₂ photo-/electroreduction reactions. As a typical two-dimensional material, the defective ultrathin two-dimensional materials can provide a large number of electron-rich catalytic sites to efficiently adsorb and highly activate CO₂ molecules, which can effectively reduce the reaction barrier, thus accelerating CO₂ reduction and enhancing product selectivity. Moreover, the local atomic and electronic structure of the defects can effectively stabilize the intermediate of CO₂ reduction reactions, thus further optimizing the kinetics of CO₂ reduction reactions. Furthermore, the surface defects are beneficial to the mass and electron transfer in the catalytic process, thus further improving the catalytic activity of the catalysts. In this review, we overview the latest research progress in CO₂ photo-/electrocatalytic reduction using defective ultrathin two-dimensional materials, including the controllable synthesis and fine structure characterization of defective ultrathin two-dimensional materials; the modulation effect of defect structure on the local atomic and electronic structure; the advantages of defective ultrathin two-dimensional materials for CO₂ reduction. We also discuss the challenges and opportunities of defective ultrathin two-dimensional materials for future development of CO₂ photo-/electrocatalytic reduction. It is expected that this review will provide a guide for designing highly efficient CO₂ reduction systems.

Key words: Defect, Ultrathin two-dimensional materials, CO₂ reduction, Photo-/Electrocatalysis

陈润华, 吴琼, 罗婧宸, 祖小龙, 朱姗, 孙永福. 缺陷态二维超薄材料用于光/电催化CO₂还原的基础与展望[J]. 物理化学学报, 2025, 41(3), 100019. doi: 10.3866/PKU.WHXB202308052

Runhua Chen, Qiong Wu, Jingchen Luo, Xiaolong Zu, Shan Zhu, Yongfu Sun. Defective Ultrathin Two-Dimensional Materials for Photo-/Electrocatalytic CO₂ Reduction: Fundamentals and Perspectives[J]. Acta Phys. -Chim. Sin. 2025, 41(3), 100019. doi: 10.3866/PKU.WHXB202308052

链接本文: https://www.whxb.pku.edu.cn/CN/10.3866/PKU.WHXB202308052

https://www.whxb.pku.edu.cn/CN/Y2025/V41/I3/100019

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2D materials	Vacancy types	syntdetic metdod	Characterization metdods	Product	Formation rate/ (μmol·g^-1·h^-1) or FEP%	Ref.
ZnIn₂S₄ atomic layers	Zn vacancies	hydrotdermal	HAADF-STEM, EPR, PAS	CO	33.2	26
BiOBr atomic layers	Oxygen vacancies	UV irradiation	XPS, EPR, XANES	CO	87.4	31
CuIn₂S₄ single-unit-cell layers	S vacancies	fast-calciination treatment	XPS, EPR	CH₄	8.7	36
BiVO₄ layers	V vacancies	hydrotdermal	PAS	CH₃OH	398.3	43
TiO₂ ultratdin layers	Oxygen vacancies	annealing treatment	XPS, PAS	CO	23.1	51
Bi₂O₂CO₃ nanosheets	Oxygen vacancies	UV irradiation	XPS, EPR	CO	275	55
ZnCo₂O₄ atomic layers	Ni-doping	adding reactants	XPS, ICP-AES	CO	31.4	56
WO₃ nanosheets	Ti-doping	adding reactants	XPS, XANES	CH₃OH	16.8	57
Co₃O₄ nanosheets	Oxygen vacancies	fast-calciination treatment	XPS, EPR, XANES	CH₃COOH	2.95	58
Zn₂GeO₄ nanobelts	Oxygen vacancies	vacuum aluminotdermic reduction	XPS, EPR	CH₃COOH	12.7	59
WO₃ layers	Oxygen vacancies	annealing treatment	XPS, EPR	CO	2.7	62
Bi₂WO₆ atomic layers	Oxygen vacancies	annealing treatment	HRTEM, XPS, Raman, EPR	CH₃OH	157	66
NiS₂ atomic layers	Co doping	adding reactants	XPS, ICP-AES	C₂H₄	2.5	68
Bi nanosheets	lattice-distorted	hydrotdermal	HAADF-STEM, Raman	HCOOH	100%	45
Co₃O₄ atomic layer	Oxygen vacancies	fast-calciination treatment	XAFS, XPS	HCOOH	85%	50
Cu_2-δSe nanosheets	Se vacancies	hydrotdermal	XPS, EPR, XANES	EtOH	68.1%	52
SnO₂ nanosheet	oxygen vacancies and N-doping	hydrotdermal	XPS, EPR	HCOOH	83%	71
Cu nanosheets	pits	electroreduction	HAADF-STEM	C₂H₄	83.2%	72

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缺陷态二维超薄材料用于光/电催化CO₂还原的基础与展望

Defective Ultrathin Two-Dimensional Materials for Photo-/Electrocatalytic CO₂ Reduction: Fundamentals and Perspectives

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