TY - JOUR AU - Chen, Weize AU - Su, Hui AU - Chen, Xiaoping AU - Zheng, Xuan AU - Zou, Zehua AU - Tang, Jing AU - Zhang, Maosheng AU - Wang, Qingxiang AU - Ling, Yun AU - Li, Jian-Feng PY - 2026 TI - Dual-polymer engineered Ni–O–Si interface catalysts for selective and durable electrocatalytic urea synthesis JO - Nano Research SN - 1998-0124 SP - 94908251 VL - 19 IS - 2 AB - Nickel (Ni) is a promising catalyst for electrochemical urea oxidation reactions. However, its strong chemisorption of CO2 and the tendency for uncontrollable structural reconstruction during catalysis have limited the exploration of Ni-based catalysts in electrocatalytic urea synthesis. Herein, we propose a co-modification strategy for Ni-mSiOx using polydopamine (PDA) and polyethyleneimine (PEI) to enable efficient electrocatalytic co-reduction of nitrate and CO2 for urea synthesis. The incorporation of stable Ni–O–Si active sites effectively balanced competing reaction pathways, while dual polymer modification optimized the surface electronic structure, promoted the formation of pyrrolic/pyridinic nitrogen species (ProN/PN, 86.7%), and accelerated C–N coupling kinetics. The resulting PDA/PEI-Ni-mSiOx catalyst achieved a urea production rate of 2513 μg·h−1·mgcat−1, a Faradaic efficiency of 28.6%, and a urea selectivity of 54.2%. Notably, the catalyst retained over 90% of its activity after 39 h of continuous operation, with no observable structural degradation following repeated cycling. This work presents a robust strategy for the rational design of high-performance, durable Ni-based catalysts for urea electrosynthesis and provides mechanistic insights into the structure–activity relationships at polymer–metal oxide interfaces. UR - https://doi.org/10.26599/NR.2025.94908251 DO - 10.26599/NR.2025.94908251