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. 2022 Sep 6;7(37):33156-33166.
doi: 10.1021/acsomega.2c03388. eCollection 2022 Sep 20.

Electronic Properties and Electrocatalytic Water Splitting Activity for Precious-Metal-Adsorbed Silicene with Nonmetal Doping

Wen-Zhong Li  1 , Yao He  1 , Yong Mao  2 , Kai Xiong  2
Affiliations

Electronic Properties and Electrocatalytic Water Splitting Activity for Precious-Metal-Adsorbed Silicene with Nonmetal Doping

Wen-Zhong Li et al. ACS Omega. .

Abstract

Since nonmetal (NM)-doped two-dimensional (2D) materials can effectively modulate their physical properties and chemical activities, they have received a lot of attention from researchers. Therefore, the stability, electronic properties, and electrocatalytic water splitting activity of precious-metal (PM)-adsorbed silicene doped with two NM atoms are investigated based on density functional theory (DFT) in this paper. The results show that NM doping can effectively improve the stability of PM-adsorbed silicene and exhibit rich electronic properties. Meanwhile, by comparing the free energies of the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) intermediates of 15 more stable NM-doped systems, it can be concluded that the electrocatalytic water splitting activity of the NM-doped systems is more influenced by the temperature. Moreover, the Si-S2-Ir-doped system exhibits good HER performance when the temperature is 300 K, while the Si-N2-Pt-doped system shows excellent OER activity. Our theoretical study shows that NM doping can effectively promote the stability and electrocatalytic water splitting of PM-adsorbed silicene, which can help in the application of silicene in electrocatalytic water splitting.

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Conflict of interest statement

The authors declare no competing financial interest.

Figures

Figure 1
Figure 1
Geometrical structure of silicene-supported PMs with doped NMs.
Figure 2
Figure 2
Schematic diagram of stability strength for silicene-supported PMs with doped NMs.
Figure 3
Figure 3
ELF of Si–O2–Ru, Si–O2–Rh, Si–N2–Os, Si–O2–Os, Si–P2–Os, Si–S2–Os, Si–Se2–Os, Si–N2–Ir, and Si–O2–Ir.
Figure 4
Figure 4
ELF of Si–P2–Ir, Si–S2–Ir, Si–Se2–Ir, Si–N2–Pt, Si–O2–Pt, and Si–Se2–Pt.
Figure 5
Figure 5
TDOS of Si–O2–Ru, Si–O2–Rh, Si–N2–Os, Si–O2–Os, Si–P2–Os, Si–S2–Os, Si–Se2–Os, Si–N2–Ir, and Si–O2–Ir.
Figure 6
Figure 6
TDOS of Si–P2–Ir, Si–S2–Ir, Si–Se2–Ir, Si–N2–Pt, Si–O2–Pt, and Si–Se2–Pt.
Figure 7
Figure 7
Free-energy changes of HER intermediates (*H) at temperatures between 200 and 600 K.
Figure 8
Figure 8
Free-energy diagram of HER intermediates (*H) at 300 K.
Figure 9
Figure 9
Linear fit between HER intermediates’ free-energy changes (ΔG*H) and HER intermediates’ adsorption energy (Eads-*H).
Figure 10
Figure 10
Limiting reaction barrier (ΔGRDS) of the OER at temperatures between 200 and 600 K.
Figure 11
Figure 11
Free-energy diagram at 1.23 eV for the OER over NM-doped systems at 300 K. The two circles represent the RDS.
See this image and copyright information in PMC

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