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†

Ting Wang,

‡^ab Li Xia,‡^a Jia-Jia Yang,‡^c Huanbo Wang,^d Wei-Hai Fang,^c Hongyu Chen,

^a Dianping Tang,

^e Abdullah M. Asiri,

^f Yonglan Luo,

*^a Ganglong Cui

*^c and Xuping Sun

*^ab

Author affiliations

* Corresponding authors

^a Chemical Synthesis and Pollution Control, Key Laboratory of Sichuan Province, School of Chemistry and Chemical Engineering, China West Normal University, Nanchong 637002, Sichuan, China
E-mail: luoylcwnu@hotmail.com

^b Institute of Fundamental and Frontier Sciences, University of Electronic Science and Technology of China, Chengdu 610054, Sichuan, China
E-mail: xpsun@uestc.edu.cn

^c College of Chemistry, Beijing Normal University, Beijing 100875, China
E-mail: ganglong.cui@bnu.edu.cn

^d School of Environment and Resource, Southwest University of Science and Technology, Mianyang 621010, Sichuan, China

^e 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

^f Chemistry Department, Faculty of Science & Center of Excellence for Advanced Materials Research, King Abdulaziz University, P.O. Box 80203, Jeddah 21589, Saudi Arabia

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–CO groups contribute more greatly to the NRR compared with the C–O group.

Chemical Communications

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

Abstract

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

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