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Chemisorption of Atomically Precise 42-Carbon Graphene Quantum Dots on Metal Oxide Films Greatly Accelerates Interfacial Electron Transfer
[Image: see text] Graphene quantum dots (GQDs) are emerging as environmentally friendly, low-cost, and highly tunable building blocks in solar energy conversion architectures, such as solar (fuel) cells. Specifically, GQDs constitute a promising alternative for organometallic dyes in sensitized oxid...
Autores principales: | , , , , , , , |
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Formato: | Online Artículo Texto |
Lenguaje: | English |
Publicado: |
American Chemical
Society
2019
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Acceso en línea: | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC6727373/ https://www.ncbi.nlm.nih.gov/pubmed/30848919 http://dx.doi.org/10.1021/acs.jpclett.9b00399 |
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author | Han, Peng Hou, Ian Cheng-Yi Lu, Hao Wang, Xiao-Ye Müllen, Klaus Bonn, Mischa Narita, Akimitsu Cánovas, Enrique |
author_facet | Han, Peng Hou, Ian Cheng-Yi Lu, Hao Wang, Xiao-Ye Müllen, Klaus Bonn, Mischa Narita, Akimitsu Cánovas, Enrique |
author_sort | Han, Peng |
collection | PubMed |
description | [Image: see text] Graphene quantum dots (GQDs) are emerging as environmentally friendly, low-cost, and highly tunable building blocks in solar energy conversion architectures, such as solar (fuel) cells. Specifically, GQDs constitute a promising alternative for organometallic dyes in sensitized oxide systems. Current sensitized solar cells employing atomically precise GQDs are based on physisorbed sensitizers, with typically limited efficiencies. Chemisorption has been pointed out as a solution to boost photoconversion efficiencies, by allowing improved control over sensitizer surface coverage and sensitizer-oxide coupling strength. Here, employing time-resolved THz spectroscopy, we demonstrate that chemisorption of atomically precise C42-GQDs (hexa-peri-hexabenzocoronene derivatives consisting of 42 sp(2) carbon atoms) onto mesoporous metal oxides, enabled by their functionalization with a carboxylate group, enhances electron transfer (ET) rates by almost 2 orders of magnitude when compared with physisorbed sensitizers. Density functional theory (DFT) calculations, absorption spectroscopy and valence band X-ray photoelectron spectroscopy reveal that the enhanced ET rates can be traced to stronger donor–acceptor coupling strength enabled by chemisorption. |
format | Online Article Text |
id | pubmed-6727373 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2019 |
publisher | American Chemical
Society |
record_format | MEDLINE/PubMed |
spelling | pubmed-67273732019-09-06 Chemisorption of Atomically Precise 42-Carbon Graphene Quantum Dots on Metal Oxide Films Greatly Accelerates Interfacial Electron Transfer Han, Peng Hou, Ian Cheng-Yi Lu, Hao Wang, Xiao-Ye Müllen, Klaus Bonn, Mischa Narita, Akimitsu Cánovas, Enrique J Phys Chem Lett [Image: see text] Graphene quantum dots (GQDs) are emerging as environmentally friendly, low-cost, and highly tunable building blocks in solar energy conversion architectures, such as solar (fuel) cells. Specifically, GQDs constitute a promising alternative for organometallic dyes in sensitized oxide systems. Current sensitized solar cells employing atomically precise GQDs are based on physisorbed sensitizers, with typically limited efficiencies. Chemisorption has been pointed out as a solution to boost photoconversion efficiencies, by allowing improved control over sensitizer surface coverage and sensitizer-oxide coupling strength. Here, employing time-resolved THz spectroscopy, we demonstrate that chemisorption of atomically precise C42-GQDs (hexa-peri-hexabenzocoronene derivatives consisting of 42 sp(2) carbon atoms) onto mesoporous metal oxides, enabled by their functionalization with a carboxylate group, enhances electron transfer (ET) rates by almost 2 orders of magnitude when compared with physisorbed sensitizers. Density functional theory (DFT) calculations, absorption spectroscopy and valence band X-ray photoelectron spectroscopy reveal that the enhanced ET rates can be traced to stronger donor–acceptor coupling strength enabled by chemisorption. American Chemical Society 2019-03-08 2019-04-04 /pmc/articles/PMC6727373/ /pubmed/30848919 http://dx.doi.org/10.1021/acs.jpclett.9b00399 Text en Copyright © 2019 American Chemical Society This is an open access article published under a Creative Commons Attribution (CC-BY) License (http://pubs.acs.org/page/policy/authorchoice_ccby_termsofuse.html) , which permits unrestricted use, distribution and reproduction in any medium, provided the author and source are cited. |
spellingShingle | Han, Peng Hou, Ian Cheng-Yi Lu, Hao Wang, Xiao-Ye Müllen, Klaus Bonn, Mischa Narita, Akimitsu Cánovas, Enrique Chemisorption of Atomically Precise 42-Carbon Graphene Quantum Dots on Metal Oxide Films Greatly Accelerates Interfacial Electron Transfer |
title | Chemisorption of Atomically Precise 42-Carbon Graphene
Quantum Dots on Metal Oxide Films Greatly Accelerates Interfacial
Electron Transfer |
title_full | Chemisorption of Atomically Precise 42-Carbon Graphene
Quantum Dots on Metal Oxide Films Greatly Accelerates Interfacial
Electron Transfer |
title_fullStr | Chemisorption of Atomically Precise 42-Carbon Graphene
Quantum Dots on Metal Oxide Films Greatly Accelerates Interfacial
Electron Transfer |
title_full_unstemmed | Chemisorption of Atomically Precise 42-Carbon Graphene
Quantum Dots on Metal Oxide Films Greatly Accelerates Interfacial
Electron Transfer |
title_short | Chemisorption of Atomically Precise 42-Carbon Graphene
Quantum Dots on Metal Oxide Films Greatly Accelerates Interfacial
Electron Transfer |
title_sort | chemisorption of atomically precise 42-carbon graphene
quantum dots on metal oxide films greatly accelerates interfacial
electron transfer |
url | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC6727373/ https://www.ncbi.nlm.nih.gov/pubmed/30848919 http://dx.doi.org/10.1021/acs.jpclett.9b00399 |
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