Ferromagnetic single-atom spin catalyst for boosting water splitting
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
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機構典藏連結 ( http://tkuir.lib.tku.edu.tw:8080/dspace/handle/987654321/125605 )