Boosting Electrochemical Urea Synthesis via Cooperative Electroreduction Through the Parallel Reduction
Yalan Zhang, Jie Hu, Huike Zhou, Yingpeng Zhang, Zebin Yu, Qiang Wei, Wenrong Xiong, Lijun Chen, Zhigang Yu, Jiahao Yang, Wei Liu, Hu Du, Jinying Xu, Sunlin Chi, Aiying Wang, Xianchuan Xie
Abstract
Abstract Despite recent achievements in the co‐reduction electrosynthesis of urea from nitrogen wastes and CO 2 , the selectivity and yield of the products remain fairly average because of the competition of the NITRR, CO 2 RR, and HER. Here, a strategy involving FeNC catalysts disperse with oxygen‐vacancy‐rich CeO 2 (FeNC‐Ce) is illustrated, in which the reversible hydrogenation of defects, and bimetallic catalytic centers enable spontaneous switching between the reduction paths of NO 3 − and CO 2 . The FeNC‐Ce electrocatalyst exhibits an extremely high urea yield and Faraday efficiency (FE) of 20969.2 µg mg −1 h −1 and 89.3%, respectively, which is highly superior to most reported values (maximum urea yield of 200–2300 µg mg −1 h −1 , FE max of 11.5%–83.4%). The study findings, rationalize by in situ spectroscopy and theoretical calculations, are rooted in the evolution of dynamic NITRR and CO 2 RR co‐reduction involving protons, alleviating the overwhelming single‐system reduction of reactants and thereby minimizing the formation of by‐products.