Enhanced electrocatalytic N2-to-NH3 fixation by ZrS2 nanofibers with a sulfur vacancy

Tong Xu; Dongwei Ma; Tingshuai Li; Luchao Yue; Yongsong Luo; Siyu Lu; Xifeng Shi; Abdullah M Asiri; Chun Yang; Xuping Sun

doi:10.1039/d0cc05917j

Enhanced electrocatalytic N₂-to-NH₃ fixation by ZrS₂ nanofibers with a sulfur vacancy

Chem Commun (Camb). 2020 Nov 12;56(90):14031-14034. doi: 10.1039/d0cc05917j.

Authors

Tong Xu¹, Dongwei Ma², Tingshuai Li³, Luchao Yue³, Yongsong Luo³, Siyu Lu⁴, Xifeng Shi⁵, Abdullah M Asiri⁶, Chun Yang⁷, Xuping Sun³

Affiliations

¹ College of Chemistry and Materials Science, Sichuan Normal University, Chengdu 610068, China. chunyang@sicnu.edu.cn and Institute of Fundamental and Frontier Sciences, University of Electronic Science and Technology of China, Chengdu 610054, Sichuan, China. xpsun@uestc.edu.cn.
² Key Laboratory for Special Functional Materials of Ministry of Education, and School of Materials Science and Engineering, Henan University, Kaifeng 475004, Henan, China.
³ Institute of Fundamental and Frontier Sciences, University of Electronic Science and Technology of China, Chengdu 610054, Sichuan, China. xpsun@uestc.edu.cn.
⁴ Green Catalysis Center, and College of Chemistry, Zhengzhou University, Zhengzhou 450001, Henan, China.
⁵ College of Chemistry, Chemical Engineering and Materials Science, Shandong Normal University, Jinan 250014, Shandong, China.
⁶ Chemistry Department, Faculty of Science & Center of Excellence for Advanced Materials Research, King Abdulaziz University, P.O. Box 80203, Jeddah 21589, Saudi Arabia.
⁷ College of Chemistry and Materials Science, Sichuan Normal University, Chengdu 610068, China. chunyang@sicnu.edu.cn.

PMID: 33099589
DOI: 10.1039/d0cc05917j

Abstract

Industrially, large-scale NH3 production is achieved by the Haber-Bosch process, which operates under harsh reaction conditions with abundant energy consumption and CO2 emission. Electrochemical N2 reduction is an eco-friendly and energy-saving method for artificial N2 to NH3 fixation under ambient reaction conditions. Herein, we demonstrate that ZrS2 nanofibers with a sulfur vacancy (ZrS2 NF-Vs) behave as an efficient electrocatalyst for ambient N2 reduction to NH3 with excellent selectivity. In 0.1 M HCl, this ZrS2 NF-Vs catalyst attains a large NH3 yield of 30.72 μg h-1 mgcat.-1 and a high faradaic efficiency of 10.33% at -0.35 V and -0.30 V vs. reversible hydrogen electrode, respectively. It also shows high electrochemical and structural stability. The density functional theory calculations reveal that the introduction of Vs facilitates the adsorption and activation of N2 molecules.