Citation: 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 Physico-Chimica Sinica, ;2025, 41(3): 230805. doi: 10.3866/PKU.WHXB202308052 shu

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

Runhua Chen ^{1, †} ,
Qiong Wu ^{1, †} ,
Jingchen Luo ¹ ,
Xiaolong Zu ^2,, ,
Shan Zhu ³ ,
Yongfu Sun ^1,,

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

Corresponding author: Xiaolong Zu, xiaolongzu@xmu.edu.cn Yongfu Sun, yfsun@ustc.edu.cn
Received Date: 31 August 2023
Revised Date: 4 October 2023
Accepted Date: 17 October 2023

Fund Project: the National Key Research and Development Program of China 2019YFA0210004the National Key Research and Development Program of China 2022YFA1502904the National Key Research and Development Program of China 2021YFA1501502the National Natural Science Foundation of China 22125503the National Natural Science Foundation of China 21975242the National Natural Science Foundation of China U2032212the Youth Innovation Promotion Association of CAS CX2340007003the Anhui Provincial Natural Science Foundation 2208085QB31

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.
- Defect,
- Ultrathin two-dimensional materials,
- CO₂ reduction,
- Photo-/Electrocatalysis
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通讯作者: 陈斌, bchen63@163.com

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沈阳化工大学材料科学与工程学院沈阳 110142

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

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通讯作者: 陈斌, bchen63@163.com

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