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| Complementary Operando Spectroscopy identification of in-situ generated metastable charge-asymmetry Cu2-CuN3 clusters for CO2 reduction to ethanol | |
| 2022-03-11 | |
| 发表期刊 | NATURE COMMUNICATIONS (IF:14.7[JCR-2023],16.1[5-Year]) |
| EISSN | 2041-1723 |
| 卷号 | 13期号:1 |
| 发表状态 | 已发表 |
| DOI | 10.1038/s41467-022-29035-8 |
| 摘要 | Copper-based materials can reliably convert carbon dioxide into multi-carbon products but they suffer from poor activity and product selectivity. The atomic structure-activity relationship of electrocatalysts for the selectivity is controversial due to the lacking of systemic multiple dimensions for operando condition study. Herein, we synthesized high-performance CORR catalyst comprising of CuO clusters supported on N-doped carbon nanosheets, which exhibited high C products Faradaic efficiency of 73% including decent ethanol selectivity of 51% with a partial current density of 14.4 mA/cm at −1.1 V vs. RHE. We evidenced catalyst restructuring and tracked the variation of the active states under reaction conditions, presenting the atomic structure-activity relationship of this catalyst. Operando XAS, XANES simulations and Quasi-in-situ XPS analyses identified a reversible potential-dependent transformation from dispersed CuO clusters to Cu-CuN clusters which are the optimal sites. This cluster can’t exist without the applied potential. The N-doping dispersed the reduced Cu clusters uniformly and maintained excellent stability and high activity with adjusting the charge distribution between the Cu atoms and N-doped carbon interface. By combining Operando FTIR and DFT calculations, it was recognized that the Cu-CuN clusters displayed charge-asymmetric sites which were intensified by CH adsorbing, beneficial to the formation of the high-efficiency asymmetric ethanol. |
| URL | 查看原文 |
| 收录类别 | SCIE |
| 语种 | 英语 |
| Scopus 记录号 | 2-s2.0-85126263261 |
| 来源库 | Scopus |
| 引用统计 | 正在获取...
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| 文献类型 | 期刊论文 |
| 条目标识符 | https://kms.shanghaitech.edu.cn/handle/2MSLDSTB/165036 |
| 专题 | 物质科学与技术学院_PI研究组_杨帆组 大科学中心_PI研究组_刘志组 物质科学与技术学院_硕士生 |
| 通讯作者 | Chen, Wenxing; Wang, Yu |
| 作者单位 | 1.Shanghai Synchrotron Radiation Facility,Zhangjiang Laboratory,Shanghai Advanced Research Institute,Chinese Academy of Sciences,Shanghai,201204,China 2.Beijing Key Laboratory of Construction Tailorable Advanced Functional Materials and Green Applications,School of Materials Science and Engineering,Beijing Institute of Technology,Beijing,100081,China 3.Department of Chemistry,Tsinghua University,Beijing,100084,China 4.Shanghai Institute of Applied Physics,Chinese Academy of Sciences,Shanghai,201800,China 5.National Synchrotron Radiation Laboratory,University of Science and Technology of China,Hefei,Anhui,230029,China 6.School of Physical Science and Technology,ShanghaiTech University,Shanghai,201210,China |
| 推荐引用方式 GB/T 7714 | Su, Xiaozhi,Jiang, Zhuoli,Zhou, Jing,et al. Complementary Operando Spectroscopy identification of in-situ generated metastable charge-asymmetry Cu2-CuN3 clusters for CO2 reduction to ethanol[J]. NATURE COMMUNICATIONS,2022,13(1). |
| APA | Su, Xiaozhi.,Jiang, Zhuoli.,Zhou, Jing.,Liu, Hengjie.,Zhou, Danni.,...&Wang, Yu.(2022).Complementary Operando Spectroscopy identification of in-situ generated metastable charge-asymmetry Cu2-CuN3 clusters for CO2 reduction to ethanol.NATURE COMMUNICATIONS,13(1). |
| MLA | Su, Xiaozhi,et al."Complementary Operando Spectroscopy identification of in-situ generated metastable charge-asymmetry Cu2-CuN3 clusters for CO2 reduction to ethanol".NATURE COMMUNICATIONS 13.1(2022). |
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