Double-single-atom MoCu-embedded porous carbons boost the electrocatalytic N2 reduction reaction

Zhiya Han; Chenbao Lu; Senhe Huang; Xinyu Chai; Zhenying Chen; Xintong Li; Jilong Wang; Jingshun Zhang; Boxu Feng; Sheng Han; Rongbin Li

doi:10.1039/d3dt02813e

Double-single-atom MoCu-embedded porous carbons boost the electrocatalytic N₂ reduction reaction

Dalton Trans. 2023 Nov 14;52(44):16217-16223. doi: 10.1039/d3dt02813e.

Authors

Zhiya Han¹, Chenbao Lu², Senhe Huang², Xinyu Chai², Zhenying Chen², Xintong Li³, Jilong Wang³, Jingshun Zhang³, Boxu Feng², Sheng Han⁴, Rongbin Li¹

Affiliations

¹ School of Materials, Shanghai Dianji University, No. 300 Shuihua Road, Shanghai, 200245, China. zhiyahan@outlook.com.
² The meso-Entropy Matter Lab, State Key Laboratory of Metal Matrix Composites, School of Chemistry and Chemical Engineering, Frontiers Science Center for Transformative Molecules, Shanghai Jiao Tong University, No. 800 Dongchuan Road, Shanghai, 200240, China. boxufeng@sjtu.edu.cn.
³ Department of Chemistry, Shanghai Key Laboratory of Green Chemistry and Chemical Process, East China Normal University, No. 3663 Zhongshan North Road, Shanghai, 200062, China. 52194300056@stu.ecnu.edu.cn.
⁴ School of Chemical and Environmental Engineering, Shanghai Institute of Technology, No. 100 Haiquan Road, Shanghai, 201418, China. hansheng654321@sina.com.

PMID: 37850569
DOI: 10.1039/d3dt02813e

Abstract

NH₃ is an essential ingredient of chemical, fertilizer, and energy storage products. Industrial nitrogen fixation consumes an enormous amount of energy, which is counter to the concept of carbon neutrality, hence eNRR ought to be implemented as a clean alternative. Herein, we propose a double-single-atom MoCu-embedded porous carbon material derived from uio-66 (MoCu@C) by plasma-enhanced chemical vapor deposition (PECVD) to boost eNRR capabilities, with an NH₃ yield rate of 52.4 μg h^-1 g_cat.^-1 and a faradaic efficiency (FE) of 27.4%. Advanced XANES shows that the Mo active site receives electrons from Cu, modifies the electronic structure of the Mo active site and enhances N₂ adsorption activation. The invention of rational MoCu double-single-atom materials and the utilization of effective eNRR approaches furnish the necessary building blocks for the fundamental study and practical application of Mo-based materials.