High-throughput Design of Single-atom Catalysts with Nonplanar and Triple Pyrrole-N Coordination for Highly Efficient H2O2 Electrosynthesis
文献类型：期刊论文
| 作者 | Jia, Jingjing1; Li, Zhenxin1; Sang, Zhiyuan1,2; Liu, Xiaoqing1; Peng, Wei1; Chen, Rui1; Jiang, Qiao1; Li, Xia1; Ren, Zhizhen3,4; Hao, Weichang3,4 |
| 刊名 | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
 |
| 出版日期 | 2025-01-12 |
| 页码 | 12 |
| ISSN号 | 1433-7851 |
| DOI | 10.1002/anie.202421864 |
| 通讯作者 | Sang, Zhiyuan(sangzhiyuan@tju.edu.cn) ; Hao, Weichang(whao@buaa.edu.cn) ; Yin, Lichang(lcyin@imr.ac.cn) ; Liang, Ji(liangji@tju.edu.cn) |
| 英文摘要 | Single-atom catalysts (SACs) with nonplanar configurations possess unique capabilities for tailoring the oxygen reduction reaction (ORR) catalytic performance compared with the ones with planar configurations, owing to the additional orbital rearrangement arising from the asymmetric coordination atoms. However, the systematic investigation of these nonplanar SACs has long been hindered by the difficulty in screening feasible nonplanar configurations and precisely controlling the coordination structures. Herein, we demonstrate a combined high-throughput screening and experimental verification of nonplanar SACs (ppy-MN3) with metal atoms triple-coordinated by pyrrole-N, for highly active and selective 2e- ORR electrocatalysis. With the additional p-orbital rearrangement of N-ligands for ppy-MN3 during catalysis, a new descriptor on the energy difference between d-band center of metal sites and p-band centers of N-ligands (Delta & varepsilon;d-p) is proposed to accurately identify the relationship between their catalytic activities and electronic structures, on top of the conventional d-band center theory. Consequently, ppy-ZnN3 is identified with excellent 2e- ORR activity (eta=0.08 eV) and selectivity, as well as a low 2e- ORR kinetic barrier under alkaline condition owing to a strong hydrogen bonding between OOH* intermediate and interfacial water, which is then experimentally verified by its high electrocatalytic H2O2 yield (43 mol g-1 h-1) and selectivity (92 %) under alkaline condition. This study thus presents a proof-of-concept demonstration of the performance-oriented and precise coordination design of nonplanar SACs for efficient H2O2 electrosynthesis, and, more importantly, provides an essential complement to the d-band theory for more accurately predicting the catalytic activities of catalysts with nonplanar configurations for series potential electrochemical processes. |
| 资助项目 | the National Natural Science Foundation of China[22379111] ; the National Natural Science Foundation of China[22179093] ; National Natural Science Foundation of China ; Tianjin Graduate Research Innovation Project |
| WOS研究方向 | Chemistry |
| 语种 | 英语 |
| WOS记录号 | WOS:001396316300001 |
| 出版者 | WILEY-V C H VERLAG GMBH |
| 资助机构 | the National Natural Science Foundation of China ; National Natural Science Foundation of China ; Tianjin Graduate Research Innovation Project |
| 源URL |  |
| 专题 | 金属研究所_中国科学院金属研究所 |
| 通讯作者 | Sang, Zhiyuan; Hao, Weichang; Yin, Lichang; Liang, Ji |
| 作者单位 | 1.Tianjin Univ, Sch Mat Sci & Engn, Key Lab Adv Ceram & Machining Technol, Minist Educ, Tianjin 300072, Peoples R China 2.Peking Univ, Sch Mat Sci & Engn, Beijing 100871, Peoples R China 3.Beihang Univ, Sch Phys, Beijing 100191, Peoples R China 4.Beihang Univ, Anal & Testing Ctr, Beijing 100191, Peoples R China 5.Chinese Acad Sci, Inst Met Res, Shenyang Natl Lab Mat Sci, Shenyang 110016, Peoples R China |
| 推荐引用方式 GB/T 7714 | Jia, Jingjing,Li, Zhenxin,Sang, Zhiyuan,et al. High-throughput Design of Single-atom Catalysts with Nonplanar and Triple Pyrrole-N Coordination for Highly Efficient H2O2 Electrosynthesis[J]. ANGEWANDTE CHEMIE-INTERNATIONAL EDITION,2025:12. |
| APA | Jia, Jingjing.,Li, Zhenxin.,Sang, Zhiyuan.,Liu, Xiaoqing.,Peng, Wei.,...&Liang, Ji.(2025).High-throughput Design of Single-atom Catalysts with Nonplanar and Triple Pyrrole-N Coordination for Highly Efficient H2O2 Electrosynthesis.ANGEWANDTE CHEMIE-INTERNATIONAL EDITION,12. |
| MLA | Jia, Jingjing,et al."High-throughput Design of Single-atom Catalysts with Nonplanar and Triple Pyrrole-N Coordination for Highly Efficient H2O2 Electrosynthesis".ANGEWANDTE CHEMIE-INTERNATIONAL EDITION (2025):12. |
入库方式： OAI收割
来源：金属研究所
浏览0
下载0
收藏0
其他版本
除非特别说明，本系统中所有内容都受版权保护，并保留所有权利。