Boosting electrocatalytic N2 reduction by MnO2 with oxygen vacancies

Ling Zhang; Xiao-Ying Xie; Huanbo Wang; Lei Ji; Ya Zhang; Hongyu Chen; Tingshuai Li; Yonglan Luo; Ganglong Cui; Xuping Sun

doi:10.1039/C9CC00936A

Boosting electrocatalytic N₂ reduction by MnO₂ with oxygen vacancies†

Ling Zhang,‡^a Xiao-Ying Xie,‡^b Huanbo Wang,^c Lei Ji,^a Ya Zhang,^a Hongyu Chen,

^ad Tingshuai Li,^e Yonglan Luo,

*^d Ganglong Cui

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

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

^d 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

^e School of Materials and Energy, University of Electronic Science and Technology of China, Chengdu 611731, Sichuan, China

Abstract

Here, we demonstrate the experimental verification of utilizing a MnO₂ with oxygen vacancies (MnO_x) nanowire array for high-performance and durable electrocatalytic reduction at neutral pH. Such MnO_x nanoarray obtains a high rate of NH₃ formation (1.63 × 10⁻¹⁰ mol cm⁻² s⁻¹) and a high Faradaic efficiency of 11.40%, which are much higher than those of its pristine MnO₂ counterpart (2.3 × 10⁻¹¹ mol cm⁻² s⁻¹; 1.96%). Density functional theory calculations demonstrate that the enhancement of N₂ adsorption on the MnO_x surface is due to stronger electronic interaction between the N₂ molecule and the Mn_6c atoms as a result of the oxygen vacancy. This work opens up a new avenue to explore oxygen nonstoichiometry toward the rational design of N₂-fixing electrocatalysts with boosted performance for applications.

Chemical Communications

Boosting electrocatalytic N₂ reduction by MnO₂ with oxygen vacancies†

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