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Synergetic Boron-Dopants and Boron-Induce Oxygen Vacancies in MnO2 Nanosheets to Promote Electrocatalytic Nitrogen Reduction

Abstract

Development of highly efficient and durable electrocatalysts for the nitrogen reduction reaction (NRR) is of paramount significance for NH3 electrosynthesis. Herein, we reported an effective B-doping strategy for the structural engineering of MnO2 toward the NRR through the combined experimental and theoretical studies. Introducing B-dopants into MnO2 nanosheets was found to create abundant O-vacancies which cooperated with B-dopants to promote the conductivity and enhance the intrinsic NRR activity of MnO2. The developed B-doped MnO2 nanosheets grown on carbon cloth (B-MnO2/CC) exhibited a significantly enhanced NRR performance with an NH3 yield of 54.2 μg h−1 mg−1 (-0.4 V) and a Faradaic efficiency of 16.8% (-0.2 V), which was among the best Mn-based NRR catalysts so far. Density functional theory calculations further revealed the synergetic role of B-dopant and O-vacancy in inducing asymmetrical charge distribution, which could activate the neighbor Mn atoms to facilitate the stabilization of the key intermediate *N2H on MnO2, leading to the reduced reaction energy barrier and enhanced intrinsic NRR activity.

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Article information


Submitted
06 Jan 2020
Accepted
11 Feb 2020
First published
11 Feb 2020

J. Mater. Chem. A, 2020, Accepted Manuscript
Article type
Paper

Synergetic Boron-Dopants and Boron-Induce Oxygen Vacancies in MnO2 Nanosheets to Promote Electrocatalytic Nitrogen Reduction

K. Chu, Y. Liu, Y. Chen and Q. Li, J. Mater. Chem. A, 2020, Accepted Manuscript , DOI: 10.1039/D0TA00220H

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