Issue 33, 2022

Single boron modulated graphdiyne nanosheets for efficient electrochemical nitrogen fixation: a first-principles study

Abstract

The electroreduction of dinitrogen (N2) is a promising alternative approach for ammonia synthesis under mild conditions. In this work, metal-free electrocatalysts using a single boron atom doped into a graphdiyne (GDY) monolayer are fabricated for N2 fixation and conversion to NH3. The NRR electrochemical mechanism has been examined by density functional theory (DFT) calculations. Our calculations revealed that configuration B(S3)@GDY fabricated using a single boron substituting the diacetylene carbon atom exhibits superior catalytic activity in the nitrogen reduction reaction. The preferred distal pathway of the NRR has an extremely low limiting potential of only 0.27 V. In addition, boron atom doping in GDY results in a small band gap (0.24 eV for B(S3)@GDY) and redistribution of the electron density. The electron deficient boron atom is largely positively charged, and thus plays a crucial role in the activation of the N[triple bond, length as m-dash]N bond. Moreover, the competing HER is effectively suppressed. This work provides an efficient metal-free single atom electrocatalyst for the NRR based on a 2D graphdiyne monolayer.

Graphical abstract: Single boron modulated graphdiyne nanosheets for efficient electrochemical nitrogen fixation: a first-principles study

Supplementary files

Article information

Article type
Paper
Submitted
13 Apr 2022
Accepted
23 Jun 2022
First published
24 Jun 2022

Phys. Chem. Chem. Phys., 2022,24, 19817-19826

Single boron modulated graphdiyne nanosheets for efficient electrochemical nitrogen fixation: a first-principles study

C. Fu, Y. Li and H. Wei, Phys. Chem. Chem. Phys., 2022, 24, 19817 DOI: 10.1039/D2CP01711C

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