Issue 28, 2019

Single molybdenum center supported on N-doped black phosphorus as an efficient electrocatalyst for nitrogen fixation

Abstract

Ammonia (NH3) is one of the most significant industrial chemical products due to its wide applications in various fields. However, the production of NH3 from the electrochemical nitrogen (N2) reduction reaction (NRR) under ambient conditions is one of the most important issues that remain challenging for chemists. Herein, the candidacy of a series of molybdenum (Mo)-based single-atom catalysts (SACs) supported on N-doped black phosphorus (BP) as the electrocatalyst for the NRR has been evaluated by means of density functional theory (DFT) calculations. In particular, Mo1N3 has been found to chemically adsorb N2, and it exhibits the highest catalytic activity toward the NRR with an ultralow overpotential of 0.02 V via the associative distal mechanism, indicative of catalyzing the NRR under ambient conditions. Additionally, Mo1N3 shows the fast removal of the produced NH3 with a free energy uphill of only 0.56 eV and good stability of NRR intermediates. Moreover, the Mo-based SACs were demonstrated to be more selective to the NRR over the competing hydrogen evolution reaction (HER) process. These excellent features render Mo1N3 on BP as a compelling highly efficient and durable catalyst for electrochemical N2 fixation. Our results provide a rational paradigm for catalytic nitrogen fixation by SACs in two-dimensional (2D) materials under ambient conditions.

Graphical abstract: Single molybdenum center supported on N-doped black phosphorus as an efficient electrocatalyst for nitrogen fixation

Supplementary files

Article information

Article type
Paper
Submitted
25 mar 2019
Accepted
25 jun 2019
First published
26 jun 2019

Nanoscale, 2019,11, 13600-13611

Single molybdenum center supported on N-doped black phosphorus as an efficient electrocatalyst for nitrogen fixation

P. Ou, X. Zhou, F. Meng, C. Chen, Y. Chen and J. Song, Nanoscale, 2019, 11, 13600 DOI: 10.1039/C9NR02586C

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