Issue 39, 2019

Computational screening of transition-metal single atom doped C9N4 monolayers as efficient electrocatalysts for water splitting

Abstract

The search for high efficiency and low-cost catalysts for the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) is vital to overall water splitting. In this work, on the basis of first-principles calculations, we screened a series of late transition metal atoms supported on a C9N4 monolayer (TM@C9N4, where TM represents Mn, Fe, Co, Ni, Cu, Ru, Rh, Pd, Ir, and Pt) as electrocatalysts for both the HER and OER. Our results demonstrate that the TM atoms can be bonded with the nitrogen atoms around the hole to form stable structures, and the bonded TM atoms are stable against diffusion. Co@C9N4 exhibits high catalytic activity toward the HER. In particular, the N active sites in the Co@C9N4, Ni@C9N4, and Pt@C9N4 systems demonstrate relatively high performance for the HER. However, Co@C9N4 and Pt@C9N4 exhibit low OER activities with large overpotentials. Among the ten cases of TM@C9N4 considered here, only Ni@C9N4 performs as a promising bifunctional electrocatalyst with N and Ni atoms as catalytic active sites for the HER and OER, with a calculated hydrogen adsorption Gibbs free energy (ΔGH*) of −0.04 eV and an OER overpotential (ηOER) of 0.31 V. The results demonstrate that TM@C9N4 is a promising single-atom catalytic system, which can be used as the non-noble metal bifunctional electrocatalyst for overall water splitting.

Graphical abstract: Computational screening of transition-metal single atom doped C9N4 monolayers as efficient electrocatalysts for water splitting

Supplementary files

Article information

Article type
Paper
Submitted
15 Jūl. 2019
Accepted
03 Sept. 2019
First published
09 Sept. 2019

Nanoscale, 2019,11, 18169-18175

Author version available

Computational screening of transition-metal single atom doped C9N4 monolayers as efficient electrocatalysts for water splitting

Y. Zhou, G. Gao, J. Kang, W. Chu and L. Wang, Nanoscale, 2019, 11, 18169 DOI: 10.1039/C9NR05991A

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