Ferromagnetic single-atom spin catalyst for boosting water splitting

Ferromagnetic single-atom spin catalyst for boosting water splitting

Nature Nanotechnology

10.1038/s41565-023-01407-1

https://doi.org/10.1038/s41565-023-01407-1

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

25 May 2023

Sun, T., Tang, Z., Zang, W., Li, Z., Li, J., Li, Z., Cao, L., Dominic Rodriguez, J. S., Mariano, C. O. M., Xu, H., Lyu, P., Hai, X., Lin, H., Sheng, X., Shi, J., Zheng, Y., Lu, Y.-R., He, Q., Chen, J., … Lu, J. (2023). Ferromagnetic single-atom spin catalyst for boosting water splitting. Nature Nanotechnology, 18(7), 763–771. https://doi.org/10.1038/s41565-023-01407-1

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.

Publisher Copyright

This research / project is supported by the Agency for Science, Technology and Research (A*STAR) - Low Carbon Energy Research Finding Initiative (LCERFI01-0033 | U2102d2006)
Grant Reference no. : U2102d2006

This research / project is supported by the Ministry of Education - Academic Research Fund Tier 2
Grant Reference no. : MOE2019-T2-2-044 and MOE-T2EP50121-0008

This research / project is supported by the Ministry of Education - Research Centre of Excellence programme
Grant Reference no. : EDUN C-33-18-279-V12

This research / project is supported by the National Research Foundation - National Research Foundation Fellowship
Grant Reference no. : NRF-NRFF11-2019-0002

This is a post-peer-review, pre-copyedit version of an article published in Nature Nanotechnology. The final authenticated version is available online at: http://dx.doi.org/10.1038/s41565-023-01407-1

https://oar.a-star.edu.sg/communities-collections/articles/22691

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Institute of Sustainability for Chemicals, Energy and Environment