Mechanistic Studies of Stimulus–Response Integrated Catalysis of Single-Atom Alloys under Electric Fields for Electrochemical Nitrogen Reduction

作者：Shan Li, Chang-Wei Wang, Xiang Zhao, Jingshuang Dang, Jun Li · 发表于：The Journal of Physical Chemistry Letters · 年份：2024 · DOI：10.1021/acs.jpclett.4c00711 · 被引用次数：9 · 研究领域：Ammonia Synthesis and Nitrogen Reduction、Nanomaterials for catalytic reactions、Electrocatalysts for Energy Conversion

The present work introduces a novel catalytic strategy to promote the nitrogen reduction reaction (NRR) by employing a cooperative Cu-based single-atom alloy (SAA) and oriented external electric fields (OEEFs) as catalysts. The field strength ( F )-dependent reaction pathways are investigated by means of first-principles calculations. Different dipole-induced responses of intermediates to electric fields break the original scaling relationships and effectively tune not only the activity but also the product selectivity of the NRR. When the most active Os 1 Cu SAA is taken as an example, in the absence of an OEEF, the overpotential (η) of the NRR is 0.62 V, which is even larger than that of the competitive hydrogen evolution reaction (HER). A negative field not only reduces η but switches the preference to the NRR over the HER. In particular, η at F = −1.14 V/Å reaches the bottom of 0.18 V, which is 70% lower than that in the field-free state.