Hou Tong, Wei Tianran, Wu Yeyu, Zhang Lang, Ding Junyang, Liu Qian, Feng Ligang, Liu Xijun
State Key Laboratory of Featured Metal Materials and Life-cycle Safety for Composite Structures, Guangxi Key Laboratory of Processing for Non-ferrous Metals and Featured Materials, School of Resources, Environment and Materials, Guangxi University, Nanning 530004, China.
Education Department of Guangxi Zhuang Autonomous Region, Key Laboratory of Applied Analytical Chemistry, Guangxi Collaborative Innovation Center for Chemistry and Engineering of Forest Products, Guangxi Key Laboratory of Chemistry and Engineering of Forest Products, Key Laboratory of Chemistry and Engineering of Forest Products, State Ethnic Affairs Commission, School of Chemistry and Chemical Engineering, Guangxi Minzu University, Nanning 530006, China.
J Colloid Interface Sci. 2024 Nov 15;674:834-840. doi: 10.1016/j.jcis.2024.06.217. Epub 2024 Jun 27.
Urea electrosynthesis has appeared to meet the nitrogen cycle and carbon neutrality with energy-saving features. Copper can co-electrocatalyze among CO and nitrogen species to generate urea, however developing effective electrocatalysts is still an obstacle. Here, we developed a nitrogen-doped porous carbon loaded with FeCu clusters that convert CO and NO into urea, with the highest Faradaic efficiency of 39.8 % and yield rate of 1024.6 μg h mg, under optimized ambient conditions, exceeding that at the Fe or Cu homogeneous sites. Furthermore, a favorable CN coupling pathway originates from *NHCO and *NHCONO two intermediates with lower free energy barriers on FeCu dual active sites are verified through in-situ Fourier transform infrared spectroscopy and theoretical calculations. This research might provide deep insights into coupling mechanisms and investigation of efficient catalysts for green urea production.
尿素电合成似乎符合氮循环和碳中性的要求，并具有节能特性。铜可以在一氧化碳和含氮物种之间进行共电催化以生成尿素，然而，开发有效的电催化剂仍然是一个障碍。在此，我们开发了一种负载有铁铜簇的氮掺杂多孔碳，其在优化的环境条件下将一氧化碳和一氧化氮转化为尿素，法拉第效率最高可达39.8%，产率为1024.6 μg h mg，超过了铁或铜均相位点的相应值。此外，通过原位傅里叶变换红外光谱和理论计算证实，一种有利的碳氮偶联途径源自铁铜双活性位点上具有较低自由能垒的NHCO和NHCONO这两种中间体。这项研究可能为绿色尿素生产的偶联机制和高效催化剂的研究提供深刻见解。
