天津大学Bin Zhang研究小组报道了，利用碳载体增强传质和金属载体相互作用，促进低浓度一氧化氮电还原制氨的活化。相关论文发表在2024年4月1日出版的《美国化学会杂志》上。

电化学一氧化氮NO还原反应(NORR)是一种很有前途的氮循环调控和氨合成方法。由于NO浓度较低，且NO在溶液中的溶解度较差，因此传质限制是一个严重但容易被忽视的问题。在这项工作中，团队制备了在Cu纳米线阵列(定义为Cu@Cu/C NWAs)上生长的多孔碳负载超细Cu团簇用于低浓度的NORR。

在-0.1 V Vs可逆氢电极(RHE)条件下，Cu@Cu/C NWAs在- 0.1 V条件下具有较高的法拉第效率(93.0%)和氨的产率(1180.5 μg h^-1 cm^-2)，远远优于Cu NWAs和其他报道的类似条件下的性能。多孔碳载体的构建可以有效降低NO的扩散动力学，促进NO的覆盖，从而实现后续的高效转化。

此外，与纯Cu NWAs相比，超细Cu NWAs与碳载体之间良好的金属-载体相互作用增强了NO的吸附，降低了*HNO形成的屏障。总体而言，在低NO浓度下，Cu@Cu/C NWAs可以充分加强整个NORR。

附 ：英文原文

Title: Carbon Support Enhanced Mass Transfer and Metal–Support Interaction Promoted Activation for Low-Concentrated Nitric Oxide Electroreduction to Ammonia

Author: Jinying Meng, Chuanqi Cheng, Yuting Wang, Yifu Yu, Bin Zhang

Issue&Volume: April 1, 2024

Abstract: The electrochemical NO reduction reaction (NORR) is a promising approach for both nitrogen cycle regulation and ammonia synthesis. Due to the relatively low concentration of the NO source and poor solubility of NO in solution, mass transfer limitation is a serious but easily overlooked issue. In this work, porous carbon-supported ultrafine Cu clusters grown on Cu nanowire arrays (defined as Cu@Cu/C NWAs) are prepared for low-concentration NORR. A high Faradaic efficiency (93.0%) and yield rate (1180.5 μg h–1 cm–2) of ammonia are realized on Cu@Cu/C NWAs at 0.1 V vs a reversible hydrogen electrode (RHE), which are far superior to those of Cu NWAs and other reported performances under similar conditions. The construction of a porous carbon support can effectively decrease the NO diffusion kinetics and promote NO coverage for subsequent highly effective conversion. Moreover, the favorable metal–support interaction between ultrafine Cu clusters and carbon support enhances the adsorption of NO and decreases the barrier for *HNO formation in comparison with that of pure Cu NWAs. Overall, the whole NORR can be fully strengthened on Cu@Cu/C NWAs at low NO concentrations.

DOI: 10.1021/jacs.4c00898

Source: https://pubs.acs.org/doi/abs/10.1021/jacs.4c00898