CH-π interaction boosts photocatalytic CO2 reduction activity of a molecular cobalt catalyst anchored on carbon nitride

Jia Wei Wang; Marcos Gil-Sepulcre; Hai Hua Huang; Eduardo Solano; Yan Fei Mu; Antoni Llobet; Gangfeng Ouyang

doi:10.1016/j.xcrp.2021.100681

CH-π interaction boosts photocatalytic CO₂ reduction activity of a molecular cobalt catalyst anchored on carbon nitride

Jia Wei Wang, Marcos Gil-Sepulcre, Hai Hua Huang, Eduardo Solano, Yan Fei Mu, Antoni Llobet^*, Gangfeng Ouyang

^*Autor corresponent d’aquest treball

Departament de Química

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22 Cites (Scopus)

Resum

The construction of efficient noble-metal-free systems for visible-light-driven CO₂ reduction still remains a key challenge. Here, we report an efficient molecular hybrid system composed of a Co-PYN5 catalyst that contains a pyrene functionality that anchors on g-C₃N₄ dye surface via CH-π interactions. This hybrid material achieves high turnover numbers (TONs) and turnover frequencies (TOFs) for visible light reduction of CO₂ to CO of 533 and 95 h⁻¹ that are within the best reported up to now. The improved performance is rationalized in terms of the electronic coupling that takes place with the π system of the pyrene group with both the g-C₃N₄ surface and the Co-pyridyl moiety of the catalysts.

Idioma original	Anglès
Número d’article	100681
Revista	Cell Reports Physical Science
Volum	2
Número	12
DOIs	https://doi.org/10.1016/j.xcrp.2021.100681
Estat de la publicació	Publicada - 22 de des. 2021

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10.1016/j.xcrp.2021.100681

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Link to publication in Scopus

CCDC 2011002: Experimental Crystal Structure Determination
Wang, J.-W. (Creador), Gil-Sepulcre, M. (Col·laborador), Huang, H.-H. (Col·laborador), Solano, E. (Col·laborador), Mu, Y.-F. (Col·laborador), Llobet, A. (Col·laborador) & Ouyang, G. (Col·laborador), Cambridge Crystallographic Data Centre, 20 de juny 2022
DOI: 10.5517/ccdc.csd.cc25hm1c, http://www.ccdc.cam.ac.uk/services/structure_request?id=doi:10.5517/ccdc.csd.cc25hm1c&sid=DataCite
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title = "CH-π interaction boosts photocatalytic CO2 reduction activity of a molecular cobalt catalyst anchored on carbon nitride",

abstract = "The construction of efficient noble-metal-free systems for visible-light-driven CO2 reduction still remains a key challenge. Here, we report an efficient molecular hybrid system composed of a Co-PYN5 catalyst that contains a pyrene functionality that anchors on g-C3N4 dye surface via CH-π interactions. This hybrid material achieves high turnover numbers (TONs) and turnover frequencies (TOFs) for visible light reduction of CO2 to CO of 533 and 95 h−1 that are within the best reported up to now. The improved performance is rationalized in terms of the electronic coupling that takes place with the π system of the pyrene group with both the g-C3N4 surface and the Co-pyridyl moiety of the catalysts.",

keywords = "carbon nitride, CH-π interactions, CO reduction, cobalt complexes, noble-metal-free photocatalysis, solar fuels",

author = "Wang, {Jia Wei} and Marcos Gil-Sepulcre and Huang, {Hai Hua} and Eduardo Solano and Mu, {Yan Fei} and Antoni Llobet and Gangfeng Ouyang",

note = "Publisher Copyright: {\textcopyright} 2021 The Author(s)",

year = "2021",

month = dec,

day = "22",

doi = "10.1016/j.xcrp.2021.100681",

language = "English",

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TY - JOUR

T1 - CH-π interaction boosts photocatalytic CO2 reduction activity of a molecular cobalt catalyst anchored on carbon nitride

AU - Wang, Jia Wei

AU - Gil-Sepulcre, Marcos

AU - Huang, Hai Hua

AU - Solano, Eduardo

AU - Mu, Yan Fei

AU - Llobet, Antoni

AU - Ouyang, Gangfeng

PY - 2021/12/22

Y1 - 2021/12/22

N2 - The construction of efficient noble-metal-free systems for visible-light-driven CO2 reduction still remains a key challenge. Here, we report an efficient molecular hybrid system composed of a Co-PYN5 catalyst that contains a pyrene functionality that anchors on g-C3N4 dye surface via CH-π interactions. This hybrid material achieves high turnover numbers (TONs) and turnover frequencies (TOFs) for visible light reduction of CO2 to CO of 533 and 95 h−1 that are within the best reported up to now. The improved performance is rationalized in terms of the electronic coupling that takes place with the π system of the pyrene group with both the g-C3N4 surface and the Co-pyridyl moiety of the catalysts.

AB - The construction of efficient noble-metal-free systems for visible-light-driven CO2 reduction still remains a key challenge. Here, we report an efficient molecular hybrid system composed of a Co-PYN5 catalyst that contains a pyrene functionality that anchors on g-C3N4 dye surface via CH-π interactions. This hybrid material achieves high turnover numbers (TONs) and turnover frequencies (TOFs) for visible light reduction of CO2 to CO of 533 and 95 h−1 that are within the best reported up to now. The improved performance is rationalized in terms of the electronic coupling that takes place with the π system of the pyrene group with both the g-C3N4 surface and the Co-pyridyl moiety of the catalysts.

KW - carbon nitride

KW - CH-π interactions

KW - CO reduction

KW - cobalt complexes

KW - noble-metal-free photocatalysis

KW - solar fuels

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U2 - 10.1016/j.xcrp.2021.100681

DO - 10.1016/j.xcrp.2021.100681

M3 - Article

AN - SCOPUS:85121637653

SN - 2666-3864

VL - 2

JO - Cell Reports Physical Science

JF - Cell Reports Physical Science

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M1 - 100681

ER -

CH-π interaction boosts photocatalytic CO2 reduction activity of a molecular cobalt catalyst anchored on carbon nitride

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CCDC 2011002: Experimental Crystal Structure Determination

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CH-π interaction boosts photocatalytic CO₂ reduction activity of a molecular cobalt catalyst anchored on carbon nitride