Citation: Hao Sun, Jingyao Liu. Carbon-supported CoS₄-C single-atom nanozyme for dramatic improvement in CO₂ electroreduction to HCOOH: A DFT study combined with hybrid solvation model[J]. Chinese Chemical Letters, ;2023, 34(8): 108018. doi: 10.1016/j.cclet.2022.108018 shu

Carbon-supported CoS₄-C single-atom nanozyme for dramatic improvement in CO₂ electroreduction to HCOOH: A DFT study combined with hybrid solvation model

Hao Sun ,
Jingyao Liu ^*,

Institute of Theoretical Chemistry, College of Chemistry, Jilin University, Changchun 130023, China

ljy121@jlu.edu.cn

Received Date: 25 October 2022
Revised Date: 17 November 2022
Accepted Date: 22 November 2022
Available Online: 24 November 2022

Figures(6)

Single-atom nanozymes (SANs) have attracted extensive attention due to their characteristics of both single-atom catalysts (SACs) and enzymes. Using spin-polarized density functional theory (DFT) calculations combined with the hybrid solvation model, this work designed a series of carbon-supported Group Ⅷ transition metals TMS₄-C SANs, similar to the TMS₄ active center of formate dehydrogenase (FADH), aiming to develop highly efficient SANs for CO₂ electroreduction. DFT calculations show that compared with TMN₄-C, TMS₄-C have FADH-like feature, which can selectively reduce CO₂ to formic acid. Particularly, CoS₄-C is the most promising SAN for CO₂ reduction, with a low limiting potential of -0.07 V, which exceeds most reported catalysts. Two descriptors of TMX₄-C (X = N, S) based on intrinsic and electronic structure properties were proposed to shed light on the origin activity of candidates. The findings presented here will provide new insights into the design of novel enzyme-like catalysts for electrochemical CO₂ reduction.
- Single-atom catalysts,
- Nanozymes,
- Electrocatalysis,
- CO₂ reduction,
- Density functional theory
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Carbon-supported CoS4-C single-atom nanozyme for dramatic improvement in CO2 electroreduction to HCOOH: A DFT study combined with hybrid solvation model

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通讯作者: 陈斌, bchen63@163.com

Carbon-supported CoS₄-C single-atom nanozyme for dramatic improvement in CO₂ electroreduction to HCOOH: A DFT study combined with hybrid solvation model