Ferromagnetic single-atom spin catalyst for boosting water splitting

doi:10.1038/s41565-023-01407-1

淡江大學機構典藏 > 理學院 > 物理學系暨研究所 > 期刊論文 > Item 987654321/125605

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题名:	Ferromagnetic single-atom spin catalyst for boosting water splitting
作者:	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
日期:	2023-05-25
上传时间:	2024-07-30 12:06:54 (UTC+8)
出版者:	Springer Nature
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.
關聯:	Nature Nanotechnology 18, p.763-771
DOI:	10.1038/s41565-023-01407-1
显示于类别:	[物理學系暨研究所] 期刊論文

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