Cage-Confined Cu Clusters Boost Carbon Dioxide Electroreduction into Methane
The microgeometric structures of Cu play important roles in regulating the catalytic selectivity of CO<sub>2</sub> electroreduction. Herein, we fabricated sub-nanometer Cu clusters confined in a metal organic framework (UIO-66-NDC) with certain tetrahedral/octahedral cages for efficient methane (CH<sub>4</sub>) synthesis. During CO<sub>2</sub> electroreduction, Cu clusters confined in UIO-66-NDC exhibited a faradaic efficiency for CH<sub>4</sub> as high as 72.0% and a partial current density of -361.0 mA cm<sup>-2</sup>. Based on <i>in situ</i> characterizations, we revealed that Cu clusters with a coordination number of around 7 were <i>in situ</i> generated in the octahedral cages of UIO-66-NDC during electrolysis. <i>In situ</i> spectroscopy measurements unraveled that *CO with bridge adsorption (*CO<sub>bridge</sub>) was favorable to be adsorbed on the surface of Cu clusters. Theoretical calculations suggested that *CO<sub>bridge</sub> was more inclined to be protonated into *CHO and then into *CH<sub>2</sub>O rather than going through the C-C coupling path on Cu clusters, thus boosting CH<sub>4</sub> selectivity.
Authors
- Zifan Xu
- Zhigang Geng (ORCID: https://orcid.org/0000-0003-3183-5900)
- Zheng Han (ORCID: https://orcid.org/0000-0002-9424-5759)
- Xiangdong Kong
- Minghui Fan (ORCID: https://orcid.org/0009-0005-7481-3164)
- Zhengwu Yang
- Zhi Zhao
- Jiangchen Zhu
Institutions
- University of Science and Technology of China (CN)
- Hefei National Center for Physical Sciences at Nanoscale (CN)
- Microscale (United States) (US)
Publication Details
- Journal
- Nano Letters
- Published
- 2025-11-07
- DOI
- https://doi.org/10.1021/acs.nanolett.5c04563
- Citations
- 2
- Primary Topic
- CO2 Reduction Techniques and Catalysts
- Type
- article
- Field-Weighted Citation Impact
- 0.73