Connection of Ru nanoparticles with rich defects enables the enhanced electrochemical reduction of nitrogen

Xingrui Tang; Xiuquan Tian; Li Zhou; Fan Yang; Rong He; Xu Zhao; Wenkun Zhu

doi:10.1039/d2cp00340f

Connection of Ru nanoparticles with rich defects enables the enhanced electrochemical reduction of nitrogen

Phys Chem Chem Phys. 2022 May 18;24(19):11491-11495. doi: 10.1039/d2cp00340f.

Authors

Xingrui Tang¹, Xiuquan Tian¹, Li Zhou¹, Fan Yang¹, Rong He¹, Xu Zhao², Wenkun Zhu¹

Affiliations

¹ State Key Laboratory of Environment-friendly Energy Materials, National Co-innovation Center for Nuclear Waste Disposal and Environmental Safety, Sichuan Co-Innovation Center for New Energetic Materials, Nuclear Waste and Environmental Safety Key Laboratory of Defense, School of National Defence Science & Technology, Southwest University of Science and Technology, Mianyang, 621010, Sichuan, China. zhuwenkun@swust.edu.cn.
² Key Laboratory of Material Chemistry for Energy Conversion and Storage (Ministry of Education), Hubei Key Laboratory of Material Chemistry and Service Failure, School of Chemistry and Chemical Engineering, Huazhong University of Science and Technology, Wuhan, Hubei, 430074, P. R. China. zhaoxu91@hust.edu.cn.

PMID: 35531769
DOI: 10.1039/d2cp00340f

Abstract

The electrochemical reduction of N₂ into NH₃ under ambient conditions is an attractive topic in the chemical industry, but the chemical inertness of N₂ and the competing hydrogen evolution reaction hamper the activity and selectivity of this reaction. Herein, we connected Ru nanocrystals through a facile annealing process, which constructed intraparticle grain boundaries and stacking faults in the connection regions to enhance the N₂ reduction reaction. The connected Ru nanoparticles exhibited an enhanced yield rate and faradaic efficiency for NH₃ production. At -0.1 V versus RHE, the connected Ru nanoparticles exhibited a maximum yield rate of 29.3 μg cm^-2 h^-1 (148.0 μg mg_cat^-1 h^-1) for NH₃ production with a faradaic efficiency of 7.0%. Mechanistic study revealed that the promotion of the electrochemical reduction of N₂ over connected Ru nanoparticles could be attributed to the decreased work function and facilitated electron transfer, which originated from the abundant defects in the connection region.