Molecular catalyst coordinatively bonded to organic semiconductors for selective light-driven CO2 reduction in water

The selective photoreduction of CO2 in aqueous media based on earth-abundant elements only, is today a challenging topic. Here we present the anchoring of discrete molecular catalysts on organic polymeric semiconductors via covalent bonding, generating molecular hybrid materials with well-defined ac...

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Authors: Wang, Jia-Wei, Zhao, Fengyi, Velasco, Lucia, Sauvan, Maxime, Moonshiram, Dooshaye, Salati, Martina, Luo, Zhi-Mei, He, Sheng, Jin, Tao, Mu, Yan-Fei, Mehmed Z., Ertem, Lian, Tianquan, Llobet, Antoni
Format: article
Status:Published version
Publication Date:2024
Country:España
Institution:Varias* (Consorci de Biblioteques Universitáries de Catalunya, Centre de Serveis Científics i Acadèmics de Catalunya)
Repository:Recercat. Dipósit de la Recerca de Catalunya
OAI Identifier:oai:recercat.cat:2072/537990
Online Access:http://hdl.handle.net/2072/537990
https://doi.org/10.1038/s41467-024-54026-2
Access Level:Open access
Keyword:Química
54 - Química
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spelling Molecular catalyst coordinatively bonded to organic semiconductors for selective light-driven CO2 reduction in waterWang, Jia-WeiZhao, FengyiVelasco, LuciaSauvan, MaximeMoonshiram, DooshayeSalati, MartinaLuo, Zhi-MeiHe, ShengJin, TaoMu, Yan-FeiMehmed Z., ErtemLian, TianquanLlobet, AntoniQuímica54 - QuímicaThe selective photoreduction of CO2 in aqueous media based on earth-abundant elements only, is today a challenging topic. Here we present the anchoring of discrete molecular catalysts on organic polymeric semiconductors via covalent bonding, generating molecular hybrid materials with well-defined active sites for CO2 photoreduction, exclusively to CO in purely aqueous media. The molecular catalysts are based on aryl substituted Co phthalocyanines that can be coordinated by dangling pyridyl attached to a polymeric covalent triazine framework that acts as a light absorber. This generates a molecular hybrid material that efficiently and selectively achieves the photoreduction of CO2 to CO in KHCO3 aqueous buffer, giving high yields in the range of 22 mmol g−1 (458 μmol g−1 h−1) and turnover numbers above 550 in 48 h, with no deactivation and no detectable H2. The electron transfer mechanism for the activation of the catalyst is proposed based on the combined results from time-resolved fluorescence spectroscopy, in situ spectroscopies and quantum chemical calculations.Springer Nature2024info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersion14 p.application/pdfhttp://hdl.handle.net/2072/537990https://doi.org/10.1038/s41467-024-54026-2RECERCAT (Dipòsit de la Recerca de Catalunya)reponame:Recercat. Dipósit de la Recerca de Catalunyainstname:Varias* (Consorci de Biblioteques Universitáries de Catalunya, Centre de Serveis Científics i Acadèmics de Catalunya)InglésEuropean Union’s Horizon 2020 research and innovation programme, under Grant Agreement No 101006839 (H2020 Research Innovation Actions 2020-2024 “CONDOR”)Guangdong Basic Research Center of Excellence for Functional Molecular Engineering (31000-42080002 866)PhD grant from Communidad de Grant (PIPF-2022/ECO-2580)Spanish Ministerio de Ciencia, Innovacion y Universidades grants (PID2019−111086RA-I00, PID2022−143013OB-I00, CNS2023−145046), oriented project to the ecological transition and the digital transition (TED2021-132757B-I00), PIE grant from CSIC-ICMM (20226AT001) and the Ramon y Cajal Fellowship (RYC2020-029863-I)Ministerio de Ciencia e Innovación (MICINN), the European Union, and Universitat Rovira i Virgili for the financial support through grants PID2019-111617RB-I00 and PRE2020-093789U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Solar Photochemistry Program under Award Number (DOE DE-SC0008798)MICINN through project PID2022-140143OB-I00, Generalitat the Catalunya for the project 2017 SGR 1631, the Severo Ochoa Excellence Accreditation 2020−2023 (CEX2019-000925-S, MCI/AEI)U.S. Department of Energy (DOE), Office of Science, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences & Biosciences, under Contract no. DE-SC0012704.Creative Commons Attribution-NonCommercial-NoDerivatives 4.0 International Licenseinfo:eu-repo/semantics/openAccessoai:recercat.cat:2072/5379902026-05-29T05:05:01Z
dc.title.none.fl_str_mv Molecular catalyst coordinatively bonded to organic semiconductors for selective light-driven CO2 reduction in water
title Molecular catalyst coordinatively bonded to organic semiconductors for selective light-driven CO2 reduction in water
spellingShingle Molecular catalyst coordinatively bonded to organic semiconductors for selective light-driven CO2 reduction in water
Wang, Jia-Wei
Química
54 - Química
title_short Molecular catalyst coordinatively bonded to organic semiconductors for selective light-driven CO2 reduction in water
title_full Molecular catalyst coordinatively bonded to organic semiconductors for selective light-driven CO2 reduction in water
title_fullStr Molecular catalyst coordinatively bonded to organic semiconductors for selective light-driven CO2 reduction in water
title_full_unstemmed Molecular catalyst coordinatively bonded to organic semiconductors for selective light-driven CO2 reduction in water
title_sort Molecular catalyst coordinatively bonded to organic semiconductors for selective light-driven CO2 reduction in water
dc.creator.none.fl_str_mv Wang, Jia-Wei
Zhao, Fengyi
Velasco, Lucia
Sauvan, Maxime
Moonshiram, Dooshaye
Salati, Martina
Luo, Zhi-Mei
He, Sheng
Jin, Tao
Mu, Yan-Fei
Mehmed Z., Ertem
Lian, Tianquan
Llobet, Antoni
author Wang, Jia-Wei
author_facet Wang, Jia-Wei
Zhao, Fengyi
Velasco, Lucia
Sauvan, Maxime
Moonshiram, Dooshaye
Salati, Martina
Luo, Zhi-Mei
He, Sheng
Jin, Tao
Mu, Yan-Fei
Mehmed Z., Ertem
Lian, Tianquan
Llobet, Antoni
author_role author
author2 Zhao, Fengyi
Velasco, Lucia
Sauvan, Maxime
Moonshiram, Dooshaye
Salati, Martina
Luo, Zhi-Mei
He, Sheng
Jin, Tao
Mu, Yan-Fei
Mehmed Z., Ertem
Lian, Tianquan
Llobet, Antoni
author2_role author
author
author
author
author
author
author
author
author
author
author
author
dc.subject.none.fl_str_mv Química
54 - Química
topic Química
54 - Química
description The selective photoreduction of CO2 in aqueous media based on earth-abundant elements only, is today a challenging topic. Here we present the anchoring of discrete molecular catalysts on organic polymeric semiconductors via covalent bonding, generating molecular hybrid materials with well-defined active sites for CO2 photoreduction, exclusively to CO in purely aqueous media. The molecular catalysts are based on aryl substituted Co phthalocyanines that can be coordinated by dangling pyridyl attached to a polymeric covalent triazine framework that acts as a light absorber. This generates a molecular hybrid material that efficiently and selectively achieves the photoreduction of CO2 to CO in KHCO3 aqueous buffer, giving high yields in the range of 22 mmol g−1 (458 μmol g−1 h−1) and turnover numbers above 550 in 48 h, with no deactivation and no detectable H2. The electron transfer mechanism for the activation of the catalyst is proposed based on the combined results from time-resolved fluorescence spectroscopy, in situ spectroscopies and quantum chemical calculations.
publishDate 2024
dc.date.none.fl_str_mv 2024
dc.type.none.fl_str_mv info:eu-repo/semantics/article
info:eu-repo/semantics/publishedVersion
format article
status_str publishedVersion
dc.identifier.none.fl_str_mv http://hdl.handle.net/2072/537990
https://doi.org/10.1038/s41467-024-54026-2
url http://hdl.handle.net/2072/537990
https://doi.org/10.1038/s41467-024-54026-2
dc.language.none.fl_str_mv Inglés
language_invalid_str_mv Inglés
dc.relation.none.fl_str_mv European Union’s Horizon 2020 research and innovation programme, under Grant Agreement No 101006839 (H2020 Research Innovation Actions 2020-2024 “CONDOR”)
Guangdong Basic Research Center of Excellence for Functional Molecular Engineering (31000-42080002 866)
PhD grant from Communidad de Grant (PIPF-2022/ECO-2580)
Spanish Ministerio de Ciencia, Innovacion y Universidades grants (PID2019−111086RA-I00, PID2022−143013OB-I00, CNS2023−145046), oriented project to the ecological transition and the digital transition (TED2021-132757B-I00), PIE grant from CSIC-ICMM (20226AT001) and the Ramon y Cajal Fellowship (RYC2020-029863-I)
Ministerio de Ciencia e Innovación (MICINN), the European Union, and Universitat Rovira i Virgili for the financial support through grants PID2019-111617RB-I00 and PRE2020-093789
U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Solar Photochemistry Program under Award Number (DOE DE-SC0008798)
MICINN through project PID2022-140143OB-I00, Generalitat the Catalunya for the project 2017 SGR 1631, the Severo Ochoa Excellence Accreditation 2020−2023 (CEX2019-000925-S, MCI/AEI)
U.S. Department of Energy (DOE), Office of Science, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences & Biosciences, under Contract no. DE-SC0012704.
dc.rights.none.fl_str_mv Creative Commons Attribution-NonCommercial-NoDerivatives 4.0 International License
info:eu-repo/semantics/openAccess
rights_invalid_str_mv Creative Commons Attribution-NonCommercial-NoDerivatives 4.0 International License
eu_rights_str_mv openAccess
dc.format.none.fl_str_mv 14 p.
application/pdf
dc.publisher.none.fl_str_mv Springer Nature
publisher.none.fl_str_mv Springer Nature
dc.source.none.fl_str_mv RECERCAT (Dipòsit de la Recerca de Catalunya)
reponame:Recercat. Dipósit de la Recerca de Catalunya
instname:Varias* (Consorci de Biblioteques Universitáries de Catalunya, Centre de Serveis Científics i Acadèmics de Catalunya)
instname_str Varias* (Consorci de Biblioteques Universitáries de Catalunya, Centre de Serveis Científics i Acadèmics de Catalunya)
reponame_str Recercat. Dipósit de la Recerca de Catalunya
collection Recercat. Dipósit de la Recerca de Catalunya
repository.name.fl_str_mv
repository.mail.fl_str_mv
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score 15.812455

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