Magnetic-Field-Induced Spin Transition in Single-Atom Catalysts for Nitrate Electrolysis to Ammonia
Xingchao You, Zhongyuan Guo, Qiuling Jiang, Junkai Xia, Suwen Wang, Xiaohui Yang, Zechao Zhuang, Yongfu Li, Hai Xiang, Hao Li, Bing Yu
Abstract
High Resolution Image Download MS PowerPoint Slide 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 3 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 *NH 2 . Economic analysis hints at cost effectiveness and scalability. Overall, this study demonstrates that magnetic-field-induced spin modulation effectively optimizes NitRR electrocatalysts.