期刊論文
| 學年 | 111 |
|---|---|
| 學期 | 2 |
| 出版（發表）日期 | 2023-05-25 |
| 作品名稱 | Ferromagnetic single-atom spin catalyst for boosting water splitting |
| 作品名稱（其他語言） | |
| 著者 | Tao Sun, Zhiyuan Tang, Wenjie Zang, Zejun Li, Jing Li , Zhihao Li, Liang Cao, Jan Sebastian Dominic Rodriguez, Carl Osby M. Mariano, Haomin Xu, Pin Lyu, Xiao Hai, Huihui Lin, Xiaoyu Sheng, Jiwei Shi, Yi Zheng, Ying-Rui Lu, Qian He, Jingsheng Chen, Kostya S. Novoselov, Cheng-Hao Chuang, Shibo Xi, Xin Luo, Jiong Lu |
| 單位 | |
| 出版者 | |
| 著錄名稱、卷期、頁數 | Nature Nanotechnology 18, p.763-771 |
| 摘要 | Heterogeneous single-atom spin catalysts combined with magnetic fields provide a powerful means for accelerating chemical reactions with enhanced metal utilization and reaction efficiency. However, designing these catalysts remains challenging due to the need for a high density of atomically dispersed active sites with a short-range quantum spin exchange interaction and long-range ferromagnetic ordering. Here, we devised a scalable hydrothermal approach involving an operando acidic environment for synthesizing various single-atom spin catalysts with widely tunable substitutional magnetic atoms (M1) in a MoS2 host. Among all the M1/MoS2 species, Ni1/MoS2 adopts a distorted tetragonal structure that prompts both ferromagnetic coupling to nearby S atoms as well as adjacent Ni1 sites, resulting in global room-temperature ferromagnetism. Such coupling benefits spin-selective charge transfer in oxygen evolution reactions to produce triplet O2. Furthermore, a mild magnetic field of ~0.5 T enhances the oxygen evolution reaction magnetocurrent by ~2,880% over Ni1/MoS2, leading to excellent activity and stability in both seawater and pure water splitting cells. As supported by operando characterizations and theoretical calculations, a great magnetic-field-enhanced oxygen evolution reaction performance over Ni1/MoS2 is attributed to a field-induced spin alignment and spin density optimization over S active sites arising from field-regulated S(p)–Ni(d) hybridization, which in turn optimizes the adsorption energies for radical intermediates to reduce overall reaction barriers. |
| 關鍵字 | |
| 語言 | en |
| ISSN | 1748-3387; 1748-3395 |
| 期刊性質 | 國外 |
| 收錄於 | SCI |
| 產學合作 | |
| 通訊作者 | |
| 審稿制度 | 否 |
| 國別 | DEU |
| 公開徵稿 | |
| 出版型式 | ,電子版 |
| 相關連結 |
機構典藏連結 ( http://tkuir.lib.tku.edu.tw:8080/dspace/handle/987654321/125605 ) |