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Computational Screening of 3 d Transition Metal Atoms Anchored on Defective Graphene for Efficient Electrocatalytic N 2 Fixation
Author(s) -
Song Wei,
Xie Kun,
Guo Yongliang,
Fu Ling,
He Chaozheng
Publication year - 2021
Publication title -
chemphyschem
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 1.016
H-Index - 140
eISSN - 1439-7641
pISSN - 1439-4235
DOI - 10.1002/cphc.202100257
Subject(s) - density functional theory , graphene , transition metal , electrochemistry , catalysis , chemistry , crystal (programming language) , materials science , nanotechnology , computational chemistry , chemical physics , electrode , biochemistry , computer science , programming language
The synthesis of ammonia (NH 3 ) through the electrochemical reduction of molecular nitrogen (N 2 ) is a promising strategy for significantly reducing energy consumption compared to traditional industrial processes. Herein, we report the design of a series of monovacancy and divacancy defective graphenes decorated with single 3d transition metal atoms (TM@MVG and TM@DVG; TM=Sc−Zn) as electrocatalysts for the nitrogen‐reduction reaction (NRR) aided by density functional theory (DFT) calculations. By comparing energies for N 2 adsorption as well as the free energies associated with *N 2 activation and *N 2 H formation, we successfully identified V@MVG, with the lowest potential of −0.63 V, to be an effective catalytic substrate for the NRR in an enzymatic mechanism. Electronic properties, including Bader charges, charge density differences, partial densities of states, and crystal orbital Hamilton populations, are further analyzed in detail. We believe that these results help to explain recent observations in this field and provide guidance for the exploration of efficient electrocatalysts for the NRR.