High-Performance Electrochemical NO Reduction into NH3 by MoS2 Nanosheet

Longcheng Zhang; Jie Liang; Yuanyuan Wang; Ting Mou; Yiting Lin; Luchao Yue; Tingshuai Li; Qian Liu; Yonglan Luo; Na Li; Bo Tang; Yang Liu; Shuyan Gao; Abdulmohsen Ali Alshehri; Xiaodong Guo; Dongwei Ma; Xuping Sun

doi:10.1002/anie.202110879

High-Performance Electrochemical NO Reduction into NH₃ by MoS₂ Nanosheet

Angew Chem Int Ed Engl. 2021 Nov 22;60(48):25263-25268. doi: 10.1002/anie.202110879. Epub 2021 Oct 27.

Authors

Longcheng Zhang^{1

2}, Jie Liang¹, Yuanyuan Wang³, Ting Mou¹, Yiting Lin¹, Luchao Yue^{1

2}, Tingshuai Li¹, Qian Liu⁴, Yonglan Luo⁴, Na Li⁵, Bo Tang⁵, Yang Liu⁶, Shuyan Gao⁶, Abdulmohsen Ali Alshehri⁷, Xiaodong Guo², Dongwei Ma³, Xuping Sun¹

Affiliations

¹ Institute of Fundamental and Frontier Sciences, University of Electronic Science and Technology of China, Chengdu, 610054, Sichuan, China.
² School of Chemical Engineering, Sichuan University, Chengdu, 610065, Sichuan, China.
³ Key Laboratory for Special Functional Materials of Ministry of Education, and School of Materials Science and Engineering, Henan University, Kaifeng, 475004, Henan, China.
⁴ Institute for Advanced Study, Chengdu University, Chengdu, 610106, Sichuan, China.
⁵ College of Chemistry, Chemical Engineering and Materials Science, Shandong Normal University, Jinan, 250014, Shandong, China.
⁶ School of Materials Science and Engineering, Henan Normal University, Xinxiang, 453007, Henan, China.
⁷ Chemistry Department, Faculty of Science, King Abdulaziz University, P.O. Box 80203, Jeddah, 21589, Saudi Arabia.

PMID: 34519397
DOI: 10.1002/anie.202110879

Abstract

Electrochemical reduction of NO not only offers an attractive alternative to the Haber-Bosch process for ambient NH₃ production but mitigates the human-caused unbalance of nitrogen cycle. Herein, we report that MoS₂ nanosheet on graphite felt (MoS₂ /GF) acts as an efficient and robust 3D electrocatalyst for NO-to-NH₃ conversion. In acidic electrolyte, such MoS₂ /GF attains a maximal Faradaic efficiency of 76.6 % and a large NH₃ yield of up to 99.6 μmol cm^-2 h^-1 . Using MoS₂ nanosheet-loaded carbon paper as the cathode, a proof-of-concept device of Zn-NO battery was assembled to deliver a discharge power density of 1.04 mW cm^-2 and an NH₃ yield of 411.8 μg h^-1 mg_cat. ^-1 . Calculations reveal that the positively charged Mo-edge sites facilitate NO adsorption/activation via an acceptance-donation mechanism and disfavor the binding of protons and the coupling of N-N bond.

Keywords: MoS2; NH3 synthesis; NO reduction reaction; density functional theory; electrocatalysis.