Cargando…

Monolayer Fullerene Networks as Photocatalysts for Overall Water Splitting

[Image: see text] Photocatalytic water splitting can produce hydrogen in an environmentally friendly way and provide alternative energy sources to reduce global carbon emissions. Recently, monolayer fullerene networks have been successfully synthesized [Hou et al. Nature2022, 606, 507], offering new...

Descripción completa

Detalles Bibliográficos
Autor principal: Peng, Bo
Formato: Online Artículo Texto
Lenguaje:English
Publicado: American Chemical Society 2022
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9634807/
https://www.ncbi.nlm.nih.gov/pubmed/36260929
http://dx.doi.org/10.1021/jacs.2c08054
_version_ 1784824577976696832
author Peng, Bo
author_facet Peng, Bo
author_sort Peng, Bo
collection PubMed
description [Image: see text] Photocatalytic water splitting can produce hydrogen in an environmentally friendly way and provide alternative energy sources to reduce global carbon emissions. Recently, monolayer fullerene networks have been successfully synthesized [Hou et al. Nature2022, 606, 507], offering new material candidates for photocatalysis because of their large surface area with abundant active sites, feasibility to be combined with other 2D materials to form heterojunctions, and the C(60) cages for potential hydrogen storage. However, efficient photocatalysts need a combination of a suitable band gap and appropriate positions of the band edges with sufficient driving force for water splitting. In this study, I employ semilocal density functional theory and hybrid functional calculations to investigate the electronic structures of monolayer fullerene networks. I find that only the weakly screened hybrid functional, combined with time-dependent Hartree–Fock calculations to include the exciton binding energy, can reproduce the experimentally obtained optical band gap of monolayer C(60). All the phases of monolayer fullerene networks have suitable band gaps with high carrier mobility and appropriate band edges to thermodynamically drive overall water splitting. In addition, the optical properties of monolayer C(60) are studied, and different phases of fullerene networks exhibit distinct absorption and recombination behavior, providing unique advantages either as an electron acceptor or as an electron donor in photocatalysis.
format Online
Article
Text
id pubmed-9634807
institution National Center for Biotechnology Information
language English
publishDate 2022
publisher American Chemical Society
record_format MEDLINE/PubMed
spelling pubmed-96348072022-11-05 Monolayer Fullerene Networks as Photocatalysts for Overall Water Splitting Peng, Bo J Am Chem Soc [Image: see text] Photocatalytic water splitting can produce hydrogen in an environmentally friendly way and provide alternative energy sources to reduce global carbon emissions. Recently, monolayer fullerene networks have been successfully synthesized [Hou et al. Nature2022, 606, 507], offering new material candidates for photocatalysis because of their large surface area with abundant active sites, feasibility to be combined with other 2D materials to form heterojunctions, and the C(60) cages for potential hydrogen storage. However, efficient photocatalysts need a combination of a suitable band gap and appropriate positions of the band edges with sufficient driving force for water splitting. In this study, I employ semilocal density functional theory and hybrid functional calculations to investigate the electronic structures of monolayer fullerene networks. I find that only the weakly screened hybrid functional, combined with time-dependent Hartree–Fock calculations to include the exciton binding energy, can reproduce the experimentally obtained optical band gap of monolayer C(60). All the phases of monolayer fullerene networks have suitable band gaps with high carrier mobility and appropriate band edges to thermodynamically drive overall water splitting. In addition, the optical properties of monolayer C(60) are studied, and different phases of fullerene networks exhibit distinct absorption and recombination behavior, providing unique advantages either as an electron acceptor or as an electron donor in photocatalysis. American Chemical Society 2022-10-19 2022-11-02 /pmc/articles/PMC9634807/ /pubmed/36260929 http://dx.doi.org/10.1021/jacs.2c08054 Text en © 2022 The Author. Published by American Chemical Society https://creativecommons.org/licenses/by/4.0/Permits the broadest form of re-use including for commercial purposes, provided that author attribution and integrity are maintained (https://creativecommons.org/licenses/by/4.0/).
spellingShingle Peng, Bo
Monolayer Fullerene Networks as Photocatalysts for Overall Water Splitting
title Monolayer Fullerene Networks as Photocatalysts for Overall Water Splitting
title_full Monolayer Fullerene Networks as Photocatalysts for Overall Water Splitting
title_fullStr Monolayer Fullerene Networks as Photocatalysts for Overall Water Splitting
title_full_unstemmed Monolayer Fullerene Networks as Photocatalysts for Overall Water Splitting
title_short Monolayer Fullerene Networks as Photocatalysts for Overall Water Splitting
title_sort monolayer fullerene networks as photocatalysts for overall water splitting
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9634807/
https://www.ncbi.nlm.nih.gov/pubmed/36260929
http://dx.doi.org/10.1021/jacs.2c08054
work_keys_str_mv AT pengbo monolayerfullerenenetworksasphotocatalystsforoverallwatersplitting