Electrocatalytic N2-to-NH3 conversion using oxygen-doped graphene: experimental and theoretical studies

Ting Wang; Li Xia; Jia-Jia Yang; Huanbo Wang; Wei-Hai Fang; Hongyu Chen; Dianping Tang; Abdullah M Asiri; Yonglan Luo; Ganglong Cui; Xuping Sun

doi:10.1039/c9cc01999e

Electrocatalytic N₂-to-NH₃ conversion using oxygen-doped graphene: experimental and theoretical studies

Chem Commun (Camb). 2019 Jul 4;55(52):7502-7505. doi: 10.1039/c9cc01999e. Epub 2019 Jun 12.

Authors

Ting Wang¹, Li Xia², Jia-Jia Yang³, Huanbo Wang⁴, Wei-Hai Fang³, Hongyu Chen², Dianping Tang⁵, Abdullah M Asiri⁶, Yonglan Luo², Ganglong Cui³, Xuping Sun¹

Affiliations

¹ Chemical Synthesis and Pollution Control, Key Laboratory of Sichuan Province, School of Chemistry and Chemical Engineering, China West Normal University, Nanchong 637002, Sichuan, China. luoylcwnu@hotmail.com and Institute of Fundamental and Frontier Sciences, University of Electronic Science and Technology of China, Chengdu 610054, Sichuan, China. xpsun@uestc.edu.cn.
² Chemical Synthesis and Pollution Control, Key Laboratory of Sichuan Province, School of Chemistry and Chemical Engineering, China West Normal University, Nanchong 637002, Sichuan, China. luoylcwnu@hotmail.com.
³ College of Chemistry, Beijing Normal University, Beijing 100875, China. ganglong.cui@bnu.edu.cn.
⁴ School of Environment and Resource, Southwest University of Science and Technology, Mianyang 621010, Sichuan, China.
⁵ Key Laboratory for Analytical Science of Food Safety and Biology (MOE & Fujian Province), State Key Laboratory of Photocatalysis on Energy and Environment, Department of Chemistry, Fuzhou University, Fuzhou 350108, Fujian, 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.

PMID: 31187806
DOI: 10.1039/c9cc01999e

Abstract

Oxygen-doped graphene (O-G) derived from sodium gluconate is identified as a promising candidate to effectively catalyze ambient electrohydrogenation of N₂ to NH₃. Electrochemical tests on O-G in 0.1 M HCl suggest a large NH₃ yield of 21.3 μg h^-1 mg_cat.^-1 and a high faradaic efficiency of 12.6% at -0.55 and -0.45 V vs. reversible hydrogen electrode, respectively, with strong electrochemical and structural stability in 0.1 M HCl. Density functional theory calculations reveal the NRR catalytic mechanism and suggest that both the C[double bond, length as m-dash]O and O-C[double bond, length as m-dash]O groups contribute more greatly to the NRR compared with the C-O group.