Coupling ZnN 4 Atomic Sites with Graphitic Nitrogen for Enhanced Ammonium Production via Electrocatalytic Nitrate Reduction

作者：Qing Li, Yixuan Ma, Qingling Zeng, Wenjun Liu, Chunfeng Wang, Shun Han, Peijiang Cao, Deliang Zhu, Ming Fang · 发表于：Small · 年份：2024 · DOI：10.1002/smll.202409925 · 被引用次数：5 · 研究领域：Ammonia Synthesis and Nitrogen Reduction、Advanced Photocatalysis Techniques、Nanomaterials for catalytic reactions

Abstract The electrocatalytic nitrate reduction reaction (NO 3 RR) presents a promising alternative to the traditional Haber‐Bosch process for synthesizing ammonium (NH 3 ) under mild conditions. Supported single atoms have emerged as active catalysts for this conversion; however, the efficiency of NH 3 production are limited by the modest activity and selectivity of these catalysts. In this study, it is demonstrated that zinc single atoms supported on nitrogen‐doped carbon (ZnNCs), derived from zeolitic imidazolate framework‐8 (ZIF‐8), possess remarkable catalytic performance for this conversion, achieving an unprecedented selectivity (exceeding 90%) for NH 3 formation across a broad potential range (−0.4–−0.8 V vs. RHE). Comprehensive analyses reveal that the incorporation of a graphitic nitrogen atom adjacent to the Zn‐N 4 site precisely modulates the reaction pathway, enabling a unique dual‐site adsorption and cascading reaction route for NH 3 formation. These findings not only uncover a novel reaction mechanism for the NO 3 RR but also have the potential to inspire the development of more efficient NO 3 RR catalysts.