Issue 5, 2020

Transition metal-tetracyanoquinodimethane monolayers as single-atom catalysts for the electrocatalytic nitrogen reduction reaction

Abstract

Converting earth-abundant nitrogen into value-added chemical ammonia is a significant yet challenging topic. The electrocatalytic nitrogen reduction reaction (NRR), compared with the conventional Haber–Bosch process, is an energy-saving and environmentally friendly approach. Finding electrocatalysts which can activate nitrogen effectively and exhibit high selectivity and stability for the electrocatalytic NRR is a major task. Single-atom catalysts can act as a good solution. In this work, by means of first-principles density functional theory, molecular dynamics calculations, and a two-step screening process, we have studied 17 transition metal single atoms supported on tetracyanoquinodimethane monolayers (TM-TCNQ), and among them, Sc-TCNQ and Ti-TCNQ are found to be excellent candidates for NRR electrocatalysts. N2 adsorption and activation are effective due to the ‘acceptance–donation’ mechanism and suitable electronic structure of TM-TCNQ. The Gibbs free energy diagram shows that Sc-TCNQ and Ti-TCNQ exhibit a low NRR overpotential of 0.33 and 0.22 V, respectively, through an enzymatic-consecutive mixed pathway. In addition, the selectivity of the NRR over the HER and stability of the Sc-/Ti-TCNQ monolayers are also validated. This work opens a new avenue for designing novel single-atom catalysts for the NRR as well as other catalytic applications.

Graphical abstract: Transition metal-tetracyanoquinodimethane monolayers as single-atom catalysts for the electrocatalytic nitrogen reduction reaction

Supplementary files

Article information

Article type
Paper
Submitted
26 may. 2020
Accepted
01 jul. 2020
First published
02 jul. 2020
This article is Open Access
Creative Commons BY-NC license

Mater. Adv., 2020,1, 1285-1292

Transition metal-tetracyanoquinodimethane monolayers as single-atom catalysts for the electrocatalytic nitrogen reduction reaction

Y. Ying, K. Fan, X. Luo, J. Qiao and H. Huang, Mater. Adv., 2020, 1, 1285 DOI: 10.1039/D0MA00348D

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