Magnetic-Field-Induced Spin Transition in Single-Atom Catalysts for Nitrate Electrolysis to Ammonia
Electrochemical nitrate reduction (NitRR) using single-atom catalysts (SACs) offers a promising pathway for sustainable ammonia production. Herein, we explore the use of external magnetic fields to regulate the spin state of Ru SACs supported on nitrogen-doped carbon (Ru-N-C), aiming to optimize their catalytic performance toward NitRR. Under magnetic field conditions, Ru-N-C exhibits a remarkable NH<sub>3</sub> yield rate of ∼38 mg L<sup>-1</sup> h<sup>-1</sup> and a Faradaic efficiency of ∼95% over 200 h. Our spectroscopic and magnetic characterization demonstrates that the external magnetic field induces a spin transition to a high-spin state in Ru SACs/N-C. Theoretical analysis further suggests that the increased spin state of Ru shifts the density of states away from the Fermi level, weakening the adsorption affinity for *NH<sub>2</sub>. Economic analysis hints at cost effectiveness and scalability. Overall, this study demonstrates that magnetic-field-induced spin modulation effectively optimizes NitRR electrocatalysts.
Authors
- Zechao Zhuang (ORCID: https://orcid.org/0000-0003-4788-1119)
- Suwen Wang (ORCID: https://orcid.org/0009-0000-1385-8426)
- Xiaohui Yang (ORCID: https://orcid.org/0000-0002-4647-6253)
- Zhongyuan Guo (ORCID: https://orcid.org/0000-0002-5445-1400)
- Bing Yu
- Qiuling Jiang
- Hao Li (ORCID: https://orcid.org/0000-0002-7577-1366)
- Yongfu Li (ORCID: https://orcid.org/0000-0002-8324-5606)
- Hai Xiang (ORCID: https://orcid.org/0000-0002-5170-3000)
- Xingchao You
- Junkai Xia
Institutions
- Zhejiang A & F University (CN)
- Tohoku University (JP)
- Institute for Materials Research, Tohoku University
- Zhejiang University (CN)
- Tsinghua University (CN)
Publication Details
- Journal
- Nano Letters
- Published
- 2025-05-14
- DOI
- https://doi.org/10.1021/acs.nanolett.5c01516
- Citations
- 15
- Primary Topic
- Ammonia Synthesis and Nitrogen Reduction
- Type
- article
- Field-Weighted Citation Impact
- 5.83
Funders
- National Natural Science Foundation of China
- China Postdoctoral Science Foundation
- Japan Society for the Promotion of Science
- National Key Research and Development Program of China
- Scientific Research Foundation of Zhejiang A and F University
- Science and Technology Department of Zhejiang Province