Lattice-Engineered Nickel Oxide for Electrocatalytic Urea Recycling with Near-Unity N 2 Selectivity

作者：Zhe Chen, Jili Li, Ya Li, Ya Li, Xudong Liu, Tao Jiang, Wei Du, Shengshuo Xu, Xiangchen Hu, Can Lei, Yaming Hao, Ran Wang, Xueting Cao, Yi Yu, Yefei Li, Yefei Li, Zhipan Liu, Ming Gong, Xuejing Yang · 发表于：Journal of the American Chemical Society · 年份：2026 · DOI：10.1021/jacs.5c13017 · 被引用次数：4 · 研究领域：Ammonia Synthesis and Nitrogen Reduction、Electrocatalysts for Energy Conversion、CO2 Reduction Techniques and Catalysts

Circulating nitrogen is crucial to the sustainability of our living system. Urea is a central form of nitrogen species that sustains our food supply, but its natural abundance in fertilizing effluent and human metabolite demands circulating technology back to innocuous dinitrogen (N 2 ), while it would otherwise pollute the environment. Electrochemical urea reforming can fragment the urea molecule into N 2 and dihydrogen (H 2 ) using renewable electricity, and N 2 can be formed directly via oxidative intramolecular N–N coupling on catalytic surfaces. However, this reforming technology remains elusive due to the low N 2 selectivity. Herein, we uncovered a urea oxidation pathway that selectively splits urea into N 2, driven by nickel oxide (NiO) lattices with adjacent Ni sites. The double-ended urea coordination on NiO facilitates intramolecular N–N coupling and suppresses C–N cleavage toward undesired overoxidation products. Further lattice engineering via Al substitution creates the optimal performance of near-unity N 2 selectivity toward N-based products and a 1 order of magnitude higher N 2 production rate compared to those of most reported catalysts. The electrochemical urea reforming devices can effectively split urea into N 2 and H 2 using both synthetic urea and artificial urine, reviving this technology as a bridge of sustainable energy and environmental treatment toward the water–energy–food nexus.