Theory-Guide Design of Integrative Catalytic Pairs for Urea Synthesis from Nitrate and Carbon Dioxide

作者：Qiwen Su, Shucheng Yang, Shiyao Shang, Song Liu, Dongxu Jiao, Yuwei Yan, Xueshi Song, Ke Chu, Jingxiang Zhao · 发表于：ACS Nano · 年份：2025 · DOI：10.1021/acsnano.5c01909 · 被引用次数：26 · 研究领域：Ammonia Synthesis and Nitrogen Reduction、Carbon dioxide utilization in catalysis、Catalytic Processes in Materials Science

Electrochemical coreduction of carbon dioxide and nitrate offers a sustainable pathway to synthesize value-added urea from greenhouse gas and nitrogen-containing waste; however, challenges remain in designing efficient catalysts. Based on the concept of “integrative catalytic pairs (ICPs)”, a catalyst for urea synthesis is designed by introducing heteroatoms (B and C) into M–N–C, where a single transition metal is dispersed on N-doped carbon material. Using a two-step theoretical screening strategy, Ni–N 3 B is identified as a promising catalyst for urea synthesis, with a low limiting potential (−0.43 V) and a small kinetic barrier for C–N coupling (0.74 eV) due to the electronic regulation effects and the synergy of Ni and B function for enhancing NO 3 – activation and facilitating C–N coupling between gaseous CO 2 and *NH intermediate. Under the guidance of these theoretical results, our further experimental validation demonstrates that the synthesized Ni–N 3 B catalyst achieves a Faradaic efficiency of 51.92% and a urea yield rate of 32.30 mmol h –1 g –1 at −0.6 V vs RHE. Our work not only identifies an efficient urea synthesis catalyst without relying on trial-and-error methods but also inspires further exploration of ICPs-based catalysts in electrocatalysis.