Two-Dimensional Transition Metal-Hexaaminobenzene Monolayer Single-Atom Catalyst for Electrocatalytic Carbon Dioxide Reduction

Electrocatalytic reduction of CO<sub>2</sub> to valuable fuels and chemicals can not only alleviate the energy crisis but also improve the atmospheric environment. The key is to develop electrocatalysts that are extremely stable, efficient, selective, and reasonably priced. In this study...

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Main Authors: Xianshi Zeng, Zongxing Tu, Yanli Yuan, Luliang Liao, Chuncai Xiao, Yufeng Wen, Kai Xiong
Format: Article
Language:English
Published: MDPI AG 2022-11-01
Series:Nanomaterials
Subjects:
Online Access:https://www.mdpi.com/2079-4991/12/22/4005
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author Xianshi Zeng
Zongxing Tu
Yanli Yuan
Luliang Liao
Chuncai Xiao
Yufeng Wen
Kai Xiong
author_facet Xianshi Zeng
Zongxing Tu
Yanli Yuan
Luliang Liao
Chuncai Xiao
Yufeng Wen
Kai Xiong
author_sort Xianshi Zeng
collection DOAJ
description Electrocatalytic reduction of CO<sub>2</sub> to valuable fuels and chemicals can not only alleviate the energy crisis but also improve the atmospheric environment. The key is to develop electrocatalysts that are extremely stable, efficient, selective, and reasonably priced. In this study, spin-polarized density function theory (DFT) calculations were used to comprehensively examine the catalytic efficacy of transition metal-hexaaminobenzene (TM-HAB) monolayers as single-atom catalysts for the electroreduction of CO<sub>2</sub>. In the modified two-dimensional TM-HAB monolayer, our findings demonstrate that the binding of individual metal atoms to HAB can be strong enough for the atoms to be evenly disseminated and immobilized. In light of the conflicting hydrogen evolution processes, TM-HAB effectively inhibits hydrogen evolution. CH<sub>4</sub> dominates the reduction byproducts of Sc, Ti, V, Cr, and Cu. HCOOH makes up the majority of Zn’s reduction products. Co’s primary reduction products are CH<sub>3</sub>OH and CH<sub>4</sub>, whereas Mn and Fe’s primary reduction products are HCHO, CH<sub>3</sub>OH, and CH<sub>4</sub>. Among these, the Ti-HAB reduction products have a 1.14 eV limiting potential and a 1.31 V overpotential. The other monolayers have relatively low overpotentials between 0.01 V and 0.7 V; therefore, we predict that TM-HAB monolayers will exhibit strong catalytic activity in the electrocatalytic reduction of CO<sub>2</sub>, making them promising electrocatalysts for CO<sub>2</sub> reduction.
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spelling doaj.art-55dc3188af8943a582fa817bad3125ff2023-11-24T09:28:08ZengMDPI AGNanomaterials2079-49912022-11-011222400510.3390/nano12224005Two-Dimensional Transition Metal-Hexaaminobenzene Monolayer Single-Atom Catalyst for Electrocatalytic Carbon Dioxide ReductionXianshi Zeng0Zongxing Tu1Yanli Yuan2Luliang Liao3Chuncai Xiao4Yufeng Wen5Kai Xiong6Institute for Advanced Study, School of Physics and Materials Science, Nanchang University, Nanchang 330031, ChinaSchool of Chemistry and Chemical Engineering, Nanchang University, Nanchang 330031, ChinaSchool of Chemistry and Chemical Engineering, Nanchang University, Nanchang 330031, ChinaInstitute for Advanced Study, School of Physics and Materials Science, Nanchang University, Nanchang 330031, ChinaSchool of Mechanical and Electrical Engineering, Xinyu University, Xinyu 338004, ChinaSchool of Mathematical Sciences and Physics, Jinggangshan University, Ji’an 343009, ChinaMaterials Genome Institute, National Center for International Research on Photoelectric and Energy Materials, School of Materials and Energy, Yunnan University, Kunming 650091, ChinaElectrocatalytic reduction of CO<sub>2</sub> to valuable fuels and chemicals can not only alleviate the energy crisis but also improve the atmospheric environment. The key is to develop electrocatalysts that are extremely stable, efficient, selective, and reasonably priced. In this study, spin-polarized density function theory (DFT) calculations were used to comprehensively examine the catalytic efficacy of transition metal-hexaaminobenzene (TM-HAB) monolayers as single-atom catalysts for the electroreduction of CO<sub>2</sub>. In the modified two-dimensional TM-HAB monolayer, our findings demonstrate that the binding of individual metal atoms to HAB can be strong enough for the atoms to be evenly disseminated and immobilized. In light of the conflicting hydrogen evolution processes, TM-HAB effectively inhibits hydrogen evolution. CH<sub>4</sub> dominates the reduction byproducts of Sc, Ti, V, Cr, and Cu. HCOOH makes up the majority of Zn’s reduction products. Co’s primary reduction products are CH<sub>3</sub>OH and CH<sub>4</sub>, whereas Mn and Fe’s primary reduction products are HCHO, CH<sub>3</sub>OH, and CH<sub>4</sub>. Among these, the Ti-HAB reduction products have a 1.14 eV limiting potential and a 1.31 V overpotential. The other monolayers have relatively low overpotentials between 0.01 V and 0.7 V; therefore, we predict that TM-HAB monolayers will exhibit strong catalytic activity in the electrocatalytic reduction of CO<sub>2</sub>, making them promising electrocatalysts for CO<sub>2</sub> reduction.https://www.mdpi.com/2079-4991/12/22/4005CO<sub>2</sub> reduction reactionelectro-catalysissingle-atom catalyststwo-dimensional materialstransition metal-hexaaminobenzenedensity functional theory (DFT) calculations
spellingShingle Xianshi Zeng
Zongxing Tu
Yanli Yuan
Luliang Liao
Chuncai Xiao
Yufeng Wen
Kai Xiong
Two-Dimensional Transition Metal-Hexaaminobenzene Monolayer Single-Atom Catalyst for Electrocatalytic Carbon Dioxide Reduction
Nanomaterials
CO<sub>2</sub> reduction reaction
electro-catalysis
single-atom catalysts
two-dimensional materials
transition metal-hexaaminobenzene
density functional theory (DFT) calculations
title Two-Dimensional Transition Metal-Hexaaminobenzene Monolayer Single-Atom Catalyst for Electrocatalytic Carbon Dioxide Reduction
title_full Two-Dimensional Transition Metal-Hexaaminobenzene Monolayer Single-Atom Catalyst for Electrocatalytic Carbon Dioxide Reduction
title_fullStr Two-Dimensional Transition Metal-Hexaaminobenzene Monolayer Single-Atom Catalyst for Electrocatalytic Carbon Dioxide Reduction
title_full_unstemmed Two-Dimensional Transition Metal-Hexaaminobenzene Monolayer Single-Atom Catalyst for Electrocatalytic Carbon Dioxide Reduction
title_short Two-Dimensional Transition Metal-Hexaaminobenzene Monolayer Single-Atom Catalyst for Electrocatalytic Carbon Dioxide Reduction
title_sort two dimensional transition metal hexaaminobenzene monolayer single atom catalyst for electrocatalytic carbon dioxide reduction
topic CO<sub>2</sub> reduction reaction
electro-catalysis
single-atom catalysts
two-dimensional materials
transition metal-hexaaminobenzene
density functional theory (DFT) calculations
url https://www.mdpi.com/2079-4991/12/22/4005
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