Single-Atom Cu and Zn Vacancy Synergy in NiFe-LDH Boosts Metal–Support Interaction for High-Efficiency Nitrate-to-Ammonia Electroreduction

作者：Yifan Ren, Jiachen Wang, Lin Yang, Qiufeng Gao, Panpan Li, Yun Zhang, Yuecheng Xiong, Zhanxi Fan, Xie Quan, Yanbiao Liu · 发表于：Environmental Science & Technology · 年份：2025 · DOI：10.1021/acs.est.5c04310 · 被引用次数：40 · 研究领域：Ammonia Synthesis and Nitrogen Reduction、Advanced Photocatalysis Techniques、Nanomaterials for catalytic reactions

The electrochemical nitrate (NO 3 - )-to-ammonia conversion reaction (NO 3 RR) represents a transformative approach addressing dual challenges of environmental remediation and sustainable ammonia (NH 3 ) synthesis. Despite its promise, practical implementation remains constrained by parasitic hydrogen evolution and inherent kinetic limitations. We propose an innovative dual-site architecture through atomic-scale metal–support engineering, constructing single copper (Cu) atoms anchored on zinc-deficient NiFe-layered double hydroxide (CuSA/V-LDH). This strategic design achieves exceptional NO 3 RR performance, delivering 95.2% Faradaic efficiency and 2.08 mg h –1 cm –2 NH 3 yield at environmentally relevant NO 3 - levels (100 mg-N L –1 ), surpassing most reported catalysts in low-concentration scenarios. Operando spectroscopy and multiscale modeling uncover key synergistic effects that govern the system’s enhanced performance. Vacancy-mediated charge redistribution strengthens metal–support interactions and structural durability, while LDH-derived atomic hydrogen species exhibit prolonged lifetimes through CuSA coordination, which facilitates efficient hydrogenation of nitrogen intermediates. Additionally, the flow-through reactor configuration optimizes mass transport, further boosting the overall reaction kinetics. System-level validation and life cycle assessment highlight the reduced environmental footprint of the proposed technology. This work establishes a paradigm for va...