P-Doped graphene toward enhanced electrocatalytic N2 reduction

Tongwei Wu; Xinyi Li; Xiaojuan Zhu; Shiyong Mou; Yonglan Luo; Xifeng Shi; Abdullah M. Asiri; Yanning Zhang; Baozhan Zheng; Haitao Zhao; Xuping Sun

doi:10.1039/C9CC09179C

P-Doped graphene toward enhanced electrocatalytic N₂ reduction†

Tongwei Wu,‡^a Xinyi Li,

‡^b Xiaojuan Zhu,^c Shiyong Mou,^a Yonglan Luo,

^c Xifeng Shi,^d Abdullah M. Asiri,

^e Yanning Zhang,

^a Baozhan Zheng,

*^f Haitao Zhao*^g and Xuping Sun

*^a

Author affiliations

* Corresponding authors

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

^b State Key Laboratory of Oral Diseases, Department of Orthodontics, West China Hospital of Stomatology, Sichuan University, Chengdu 610041, Sichuan, China

^c Chemical Synthesis and Pollution Control Key Laboratory of Sichuan Province, College of Chemistry and Chemical Engineering, China West Normal University, Nanchong 637002, Sichuan, China

^d College of Chemistry, Chemical Engineering and Materials Science, Shandong Normal University, Jinan 250014, Shandong, China

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

^f College of Chemistry, Sichuan University, Chengdu 610064, Sichuan, China
E-mail: zhengbaozhan@scu.edu.cn

^g Department of Mechanical Engineering, Massachusetts Institute of Technology, Cambridge, Massachusetts 02139, USA
E-mail: haitaoz@mit.edu

Abstract

Catalysts for the N₂ reduction reaction (NRR) are at the heart of key alternative technology to the Haber–Bosch process for NH₃ synthesis, and are expected to optimize the interplay between efficiency, activity and selectivity. Here, we report our recent finding that P-doped graphene shows superior NRR performances in aqueous media at present, with a remarkably large NH₃ yield of 32.33 μg h⁻¹ mg_cat.⁻¹ and a high faradaic efficiency of 20.82% at −0.65 V vs. reversible hydrogen electrode. The mechanism is clarified by density functional theory calculations.

Chemical Communications

P-Doped graphene toward enhanced electrocatalytic N₂ reduction†

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P-Doped graphene toward enhanced electrocatalytic N₂ reduction

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