Issue 8, 2020

Single-atom transition metals supported on black phosphorene for electrochemical nitrogen reduction

Abstract

The electrochemical nitrogen reduction reaction (NRR) is one of the most promising routes to produce ammonia under mild conditions. Black phosphorene (BP) has attracted wide attention as an NRR electrocatalyst owing to its high Fermi level and unique electronic structure. However, the low intrinsic activity of surface sites greatly restricts its application in the electrochemical NRR. In this work, we theoretically designed a series of single-atom transition metals anchored on the BP surface with MP3 (M = Fe, Mn, Cr, Mo, W, V and Nb) active sites for the NRR via density functional theory (DFT) calculations. By taking stability, activity and selectivity into consideration, the single-atom W-anchored BP was selected as a promising candidate for the NRR. The energy-favorable enzymatic pathway on W@BP (W atoms adsorb on the surface of BP) and the hybrid pathway on W–BP (W atoms substitute the surface P atoms of BP) have reaction onset potentials of 0.46 and 0.42 V, respectively, indicating that the single-atom W-anchored BP shows high activity towards the NRR. This high performance originates from the WP3 active sites, which act as an electron adaptor to activate N2 by donating electrons, thereby greatly regulating the charge transfer between BP and the reaction intermediates. This study proposes a promising active catalyst and provides theoretical guidance to construct BP-supported transition metal single-atom electrocatalysts for the NRR.

Graphical abstract: Single-atom transition metals supported on black phosphorene for electrochemical nitrogen reduction

Supplementary files

Article information

Article type
Paper
Submitted
25 Oct 2019
Accepted
07 Jan 2020
First published
07 Jan 2020

Nanoscale, 2020,12, 4903-4908

Single-atom transition metals supported on black phosphorene for electrochemical nitrogen reduction

K. Liu, J. Fu, L. Zhu, X. Zhang, H. Li, H. Liu, J. Hu and M. Liu, Nanoscale, 2020, 12, 4903 DOI: 10.1039/C9NR09117C

To request permission to reproduce material from this article, please go to the Copyright Clearance Center request page.

If you are an author contributing to an RSC publication, you do not need to request permission provided correct acknowledgement is given.

If you are the author of this article, you do not need to request permission to reproduce figures and diagrams provided correct acknowledgement is given. If you want to reproduce the whole article in a third-party publication (excluding your thesis/dissertation for which permission is not required) please go to the Copyright Clearance Center request page.

Read more about how to correctly acknowledge RSC content.

Social activity

Spotlight

Advertisements