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Broadband and strong visible-light-absorbing cuprous sensitizers for boosting photosynthesis
Rational construction of broadband and strong visible-light-absorbing (BSVLA) earth-abundant complexes is of great importance for efficient and sustainable solar energy utilization. Herein, we explore a universal Cu(I) center to couple with multiple strong visible-light-absorbing antennas to break t...
Autores principales: | , , , , , |
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Formato: | Online Artículo Texto |
Lenguaje: | English |
Publicado: |
National Academy of Sciences
2022
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Materias: | |
Acceso en línea: | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9897433/ https://www.ncbi.nlm.nih.gov/pubmed/36469783 http://dx.doi.org/10.1073/pnas.2213479119 |
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author | Chen, Kai-Kai Qin, Chao-Chao Ding, Meng-Jie Guo, Song Lu, Tong-Bu Zhang, Zhi-Ming |
author_facet | Chen, Kai-Kai Qin, Chao-Chao Ding, Meng-Jie Guo, Song Lu, Tong-Bu Zhang, Zhi-Ming |
author_sort | Chen, Kai-Kai |
collection | PubMed |
description | Rational construction of broadband and strong visible-light-absorbing (BSVLA) earth-abundant complexes is of great importance for efficient and sustainable solar energy utilization. Herein, we explore a universal Cu(I) center to couple with multiple strong visible-light-absorbing antennas to break the energy level limitations of the current noble-metal complexes, resulting in the BSVLA nonprecious complex (Cu-3). Systematic investigations demonstrate that double “ping-pong” energy-transfer processes in Cu-3 involving resonance energy transfer and Dexter mechanism enable a BSVLA between 430 and 620 nm and an antenna-localized long-lived triplet state for efficient intermolecular electron/energy transfer. Impressively, Cu-3 exhibited an outstanding performance for both energy- and electron-transfer reactions. Pseudo-first-order rate constant of photooxidation of 1,5-dihydroxynaphthalene with Cu-3 can achieve a record value of 190.8 × 10(−)(3) min(−)(1) among the molecular catalytic systems, over 30 times higher than that with a noble-metal photosensitizer (PS) [Ru(bpy)(3)](2+). These findings pave the way to develop BSVLA earth-abundant PSs for boosting photosynthesis. |
format | Online Article Text |
id | pubmed-9897433 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2022 |
publisher | National Academy of Sciences |
record_format | MEDLINE/PubMed |
spelling | pubmed-98974332023-06-05 Broadband and strong visible-light-absorbing cuprous sensitizers for boosting photosynthesis Chen, Kai-Kai Qin, Chao-Chao Ding, Meng-Jie Guo, Song Lu, Tong-Bu Zhang, Zhi-Ming Proc Natl Acad Sci U S A Physical Sciences Rational construction of broadband and strong visible-light-absorbing (BSVLA) earth-abundant complexes is of great importance for efficient and sustainable solar energy utilization. Herein, we explore a universal Cu(I) center to couple with multiple strong visible-light-absorbing antennas to break the energy level limitations of the current noble-metal complexes, resulting in the BSVLA nonprecious complex (Cu-3). Systematic investigations demonstrate that double “ping-pong” energy-transfer processes in Cu-3 involving resonance energy transfer and Dexter mechanism enable a BSVLA between 430 and 620 nm and an antenna-localized long-lived triplet state for efficient intermolecular electron/energy transfer. Impressively, Cu-3 exhibited an outstanding performance for both energy- and electron-transfer reactions. Pseudo-first-order rate constant of photooxidation of 1,5-dihydroxynaphthalene with Cu-3 can achieve a record value of 190.8 × 10(−)(3) min(−)(1) among the molecular catalytic systems, over 30 times higher than that with a noble-metal photosensitizer (PS) [Ru(bpy)(3)](2+). These findings pave the way to develop BSVLA earth-abundant PSs for boosting photosynthesis. National Academy of Sciences 2022-12-05 2022-12-13 /pmc/articles/PMC9897433/ /pubmed/36469783 http://dx.doi.org/10.1073/pnas.2213479119 Text en Copyright © 2022 the Author(s). Published by PNAS. https://creativecommons.org/licenses/by-nc-nd/4.0/This article is distributed under Creative Commons Attribution-NonCommercial-NoDerivatives License 4.0 (CC BY-NC-ND). (https://creativecommons.org/licenses/by-nc-nd/4.0/) |
spellingShingle | Physical Sciences Chen, Kai-Kai Qin, Chao-Chao Ding, Meng-Jie Guo, Song Lu, Tong-Bu Zhang, Zhi-Ming Broadband and strong visible-light-absorbing cuprous sensitizers for boosting photosynthesis |
title | Broadband and strong visible-light-absorbing cuprous sensitizers for boosting photosynthesis |
title_full | Broadband and strong visible-light-absorbing cuprous sensitizers for boosting photosynthesis |
title_fullStr | Broadband and strong visible-light-absorbing cuprous sensitizers for boosting photosynthesis |
title_full_unstemmed | Broadband and strong visible-light-absorbing cuprous sensitizers for boosting photosynthesis |
title_short | Broadband and strong visible-light-absorbing cuprous sensitizers for boosting photosynthesis |
title_sort | broadband and strong visible-light-absorbing cuprous sensitizers for boosting photosynthesis |
topic | Physical Sciences |
url | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9897433/ https://www.ncbi.nlm.nih.gov/pubmed/36469783 http://dx.doi.org/10.1073/pnas.2213479119 |
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