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Published on: December 6, 2021
Magnetic-Field-Induced Spin Transition in Single-Atom Catalysts for Nitrate Electrolysis to Ammonia
Xingchao You1,2, Zhongyuan Guo3,4, Qiuling Jiang3
1National Key Laboratory for Development and Utilization of Forest Food Resources, Zhejiang A&F University, Hangzhou 311300, China.
Abstract:
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 NH3 yield rate of ∼38 mg L-1 h-1 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 *NH2. Economic analysis hints at cost effectiveness and scalability. Overall, this study demonstrates that magnetic-field-induced spin modulation effectively optimizes NitRR electrocatalysts.
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