Boosting Electrocatalytic Nitrate Reduction to Ammonia on a Hierarchical Nanoporous Ag,Ni-Codoped Cu Catalyst via Trimetallic Synergistic and Nanopore Enrichment Effects

作者：Yuhuan Cui, Changning Sun, Yuexuan He, Zixuan Feng, Guopeng Ding, Qingqing Dai, Tonghui Wang, Zhili Wang, Qing Jiang · 发表于：Nano Letters · 年份：2025 · DOI：10.1021/acs.nanolett.4c05376 · 被引用次数：29 · 研究领域：Ammonia Synthesis and Nitrogen Reduction、Caching and Content Delivery、Nanomaterials for catalytic reactions

The electrochemical nitrate (NO 3 – ) reduction reaction (NO 3 – RR) offers a promising route for NO 3 – wastewater treatment and sustainable ammonia (NH 3 ) synthesis. However, the reaction still faces the challenges of unsatisfactory productivity and selectivity. Herein, we report a hierarchical nanoporous Ag,Ni-codoped Cu (np Ag,Ni-Cu) catalyst that exhibits a high NH 3 Faradaic efficiency of 98.5% with an attractive NH 3 yield rate of 41.1 mg h –1 mg cat –1 at −0.2 V vs RHE for the NO 3 – RR. Density functional theory calculations and molecular dynamics simulations suggest that the excellent performance of np Ag,Ni-Cu results from a trimetallic synergistic effect and nanopore enrichment/confinement effect, in which the codoping of Ni and Ag into Cu can enhance NO 3 – adsorption, prevent *NO 2 desorption, and suppress the hydrogen evolution reaction, while nanopores can promote NO 3 – accumulation on the internal surface of nanopores and confine the reaction intermediates within the nanopores for a deeper NO 3 – electroreduction.