Citation: Chenxu Zhao, Menghui Xi, Jinrong Huo, Chaozheng He, Ling Fu. Computational design of BC₃N₂ based single atom catalyst for dramatic activation of inert CO₂ and CH₄ gasses into CH₃COOH with ultralow CH₄ dissociation barrier[J]. Chinese Chemical Letters, ;2023, 34(1): 107213. doi: 10.1016/j.cclet.2022.02.018 shu

Computational design of BC₃N₂ based single atom catalyst for dramatic activation of inert CO₂ and CH₄ gasses into CH₃COOH with ultralow CH₄ dissociation barrier

Chenxu Zhao ^a ,
Menghui Xi ^a ,
Jinrong Huo ^b ,
Chaozheng He ^{a, *,} ,
Ling Fu ^{c, *,}

a.
Institute of Environment and Energy Catalysis, School of Materials Science and Chemical Engineering, Xi'an Technological University, Xi'an 710021, China
b.
School of Sciences, Xi'an Technological University, Xi'an 710021, China
c.
College of Resources and Environmental Engineering, Tianshui Normal University, Tianshui 741001, China

hecz2019@xatu.edu.cn

ful263@nenu.edu.cn

Received Date: 16 January 2022
Revised Date: 5 February 2022
Accepted Date: 9 February 2022
Available Online: 14 February 2022

Figures(6)

The production of CH₃COOH from CO₂ and CH₄ has stimulated much interest due to the high energy density of C2 species. Various kinds of catalysts have been developed while the high dissociation barrier of CH₄ and low selectivity still hinders the efficiency of the reaction. We have herein proposed a novel catalyst with single metals loaded on 2D BC₃N₂ substrate (M@2D-BC₃N₂) based on density functional theory. Among numerous candidates, Pt@2D-BC₃N₂ possesses the most favorable reactivity with an ultralow barrier of CH₄ splitting (0.26 eV), which is due to the efficient capture ability of CH₄ on Pt site. Besides, the selectivity for CH₃COOH is also very high, which mainly stems from the unique electronic properties of molecules and substrate: The degenerated states, including s, p_x, p_y and p_z, in CO₂ reflects the existence of delocalized π bonds between C and O. This can interact with states of Pt(s), Pt(p_z), Pt(d_xz), Pt(d_yz), and Pt(z²) in Pt@2D-BC₃N₂. The kinetics model also proves that our system can promote CH₃COOH production via simply increasing the temperature or the coverage of CH₄ and CO₂. Our results provide a reasonable illustration in clarifying mechanism and propose promising candidates with high reactivity for further study.
- Density functional theory,
- CO₂/CH₄ coactivation,
- 2D BC₃N₂ substrate,
- CH₃COOH production
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Computational design of BC3N2 based single atom catalyst for dramatic activation of inert CO2 and CH4 gasses into CH3COOH with ultralow CH4 dissociation barrier

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通讯作者: 陈斌, bchen63@163.com

Computational design of BC₃N₂ based single atom catalyst for dramatic activation of inert CO₂ and CH₄ gasses into CH₃COOH with ultralow CH₄ dissociation barrier