Highly Efficient Photocatalytic Reduction of CO2 to CO by In Situ Formation of a Hybrid Catalytic System Based on Molecular Iron Quaterpyridine Covalently Linked to Carbon Nitride

Yue Wei; Lingjing Chen; Huan Chen; Lirong Cai; Guiping Tan; Yongfu Qiu; Quanjun Xiang; Gui Chen; Tai-Chu Lau; Marc Robert

doi:10.1002/anie.202116832

Highly Efficient Photocatalytic Reduction of CO₂ to CO by In Situ Formation of a Hybrid Catalytic System Based on Molecular Iron Quaterpyridine Covalently Linked to Carbon Nitride

Yue Wei
, Lingjing Chen
, Huan Chen
, Lirong Cai
, Guiping Tan
, Yongfu Qiu
, Quanjun Xiang
, Gui Chen^*
, Tai-Chu Lau^*
, Marc Robert^*

^*Corresponding author for this work

Department of Chemistry

Research output: Journal Publications and Reviews › RGC 21 - Publication in refereed journal › peer-review

107 Citations (Scopus)

Abstract

Efficient and selective photocatalytic CO₂ reduction was obtained within a hybrid system that is formed in situ via a Schiff base condensation between a molecular iron quaterpyridine complex bearing an aldehyde function and carbon nitride. Irradiation (blue LED) of an CH₃CN solution containing 1,3-dimethyl-2-phenyl-2,3-dihydro-1H-benzo[d]imidazole (BIH), triethylamine (TEA), Feqpy-BA (qpy-BA=4-([2,2′:6′,2′′:6′′,2′′′-quaterpyridin]-4-yl)benzaldehyde) and C₃N₄ resulted in CO evolution with a turnover number of 2554 and 95 % selectivity. This hybrid catalytic system unlocks covalent linkage of molecular catalysts with semiconductor photosensitizers via Schiff base reaction for high-efficiency photocatalytic reduction of CO₂, opening a pathway for diverse photocatalysis.

Original language	English
Article number	e202116832
Journal	Angewandte Chemie - International Edition
Volume	61
Issue number	11
Online published	5 Jan 2022
DOIs	https://doi.org/10.1002/anie.202116832
Publication status	Published - 7 Mar 2022

Funding

This research was funded by the National Natural Science Foundation of China (21975043), Guangdong Basic and Applied Basic Research Foundation, the NSFC/RGC joint research scheme (N_CityU115/18) and the City University of Hong Kong (9229038). Partial financial support from the Institut Universitaire de France (IUF) is also gratefully acknowledged.

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

SDG 13 Climate Action

Research Keywords

Carbon Nitride
CO2 Reduction
Fe Quaterpyridine
Photocatalysis
Schiff Base Reaction

RGC Funding Information

RGC-funded

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10.1002/anie.202116832

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Wei, Y., Chen, L., Chen, H., Cai, L., Tan, G., Qiu, Y., Xiang, Q., Chen, G., Lau, T.-C., & Robert, M. (2022). Highly Efficient Photocatalytic Reduction of CO₂ to CO by In Situ Formation of a Hybrid Catalytic System Based on Molecular Iron Quaterpyridine Covalently Linked to Carbon Nitride. Angewandte Chemie - International Edition, 61(11), Article e202116832. https://doi.org/10.1002/anie.202116832

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title = "Highly Efficient Photocatalytic Reduction of CO2 to CO by In Situ Formation of a Hybrid Catalytic System Based on Molecular Iron Quaterpyridine Covalently Linked to Carbon Nitride",

abstract = "Efficient and selective photocatalytic CO2 reduction was obtained within a hybrid system that is formed in situ via a Schiff base condensation between a molecular iron quaterpyridine complex bearing an aldehyde function and carbon nitride. Irradiation (blue LED) of an CH3CN solution containing 1,3-dimethyl-2-phenyl-2,3-dihydro-1H-benzo[d]imidazole (BIH), triethylamine (TEA), Feqpy-BA (qpy-BA=4-([2,2′:6′,2′′:6′′,2′′′-quaterpyridin]-4-yl)benzaldehyde) and C3N4 resulted in CO evolution with a turnover number of 2554 and 95 \% selectivity. This hybrid catalytic system unlocks covalent linkage of molecular catalysts with semiconductor photosensitizers via Schiff base reaction for high-efficiency photocatalytic reduction of CO2, opening a pathway for diverse photocatalysis.",

keywords = "Carbon Nitride, CO2 Reduction, Fe Quaterpyridine, Photocatalysis, Schiff Base Reaction",

author = "Yue Wei and Lingjing Chen and Huan Chen and Lirong Cai and Guiping Tan and Yongfu Qiu and Quanjun Xiang and Gui Chen and Tai-Chu Lau and Marc Robert",

year = "2022",

month = mar,

day = "7",

doi = "10.1002/anie.202116832",

language = "English",

volume = "61",

journal = "Angewandte Chemie - International Edition",

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Wei, Y, Chen, L, Chen, H, Cai, L, Tan, G, Qiu, Y, Xiang, Q, Chen, G, Lau, T-C & Robert, M 2022, 'Highly Efficient Photocatalytic Reduction of CO₂ to CO by In Situ Formation of a Hybrid Catalytic System Based on Molecular Iron Quaterpyridine Covalently Linked to Carbon Nitride', Angewandte Chemie - International Edition, vol. 61, no. 11, e202116832. https://doi.org/10.1002/anie.202116832

Highly Efficient Photocatalytic Reduction of CO₂ to CO by In Situ Formation of a Hybrid Catalytic System Based on Molecular Iron Quaterpyridine Covalently Linked to Carbon Nitride. / Wei, Yue; Chen, Lingjing; Chen, Huan et al.
In: Angewandte Chemie - International Edition, Vol. 61, No. 11, e202116832, 07.03.2022.

Research output: Journal Publications and Reviews › RGC 21 - Publication in refereed journal › peer-review

TY - JOUR

T1 - Highly Efficient Photocatalytic Reduction of CO2 to CO by In Situ Formation of a Hybrid Catalytic System Based on Molecular Iron Quaterpyridine Covalently Linked to Carbon Nitride

AU - Wei, Yue

AU - Chen, Lingjing

AU - Chen, Huan

AU - Cai, Lirong

AU - Tan, Guiping

AU - Qiu, Yongfu

AU - Xiang, Quanjun

AU - Chen, Gui

AU - Lau, Tai-Chu

AU - Robert, Marc

PY - 2022/3/7

Y1 - 2022/3/7

N2 - Efficient and selective photocatalytic CO2 reduction was obtained within a hybrid system that is formed in situ via a Schiff base condensation between a molecular iron quaterpyridine complex bearing an aldehyde function and carbon nitride. Irradiation (blue LED) of an CH3CN solution containing 1,3-dimethyl-2-phenyl-2,3-dihydro-1H-benzo[d]imidazole (BIH), triethylamine (TEA), Feqpy-BA (qpy-BA=4-([2,2′:6′,2′′:6′′,2′′′-quaterpyridin]-4-yl)benzaldehyde) and C3N4 resulted in CO evolution with a turnover number of 2554 and 95 % selectivity. This hybrid catalytic system unlocks covalent linkage of molecular catalysts with semiconductor photosensitizers via Schiff base reaction for high-efficiency photocatalytic reduction of CO2, opening a pathway for diverse photocatalysis.

AB - Efficient and selective photocatalytic CO2 reduction was obtained within a hybrid system that is formed in situ via a Schiff base condensation between a molecular iron quaterpyridine complex bearing an aldehyde function and carbon nitride. Irradiation (blue LED) of an CH3CN solution containing 1,3-dimethyl-2-phenyl-2,3-dihydro-1H-benzo[d]imidazole (BIH), triethylamine (TEA), Feqpy-BA (qpy-BA=4-([2,2′:6′,2′′:6′′,2′′′-quaterpyridin]-4-yl)benzaldehyde) and C3N4 resulted in CO evolution with a turnover number of 2554 and 95 % selectivity. This hybrid catalytic system unlocks covalent linkage of molecular catalysts with semiconductor photosensitizers via Schiff base reaction for high-efficiency photocatalytic reduction of CO2, opening a pathway for diverse photocatalysis.

KW - Carbon Nitride

KW - CO2 Reduction

KW - Fe Quaterpyridine

KW - Photocatalysis

KW - Schiff Base Reaction

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U2 - 10.1002/anie.202116832

DO - 10.1002/anie.202116832

M3 - RGC 21 - Publication in refereed journal

SN - 1433-7851

VL - 61

JO - Angewandte Chemie - International Edition

JF - Angewandte Chemie - International Edition

IS - 11

M1 - e202116832

ER -

Highly Efficient Photocatalytic Reduction of CO₂ to CO by In Situ Formation of a Hybrid Catalytic System Based on Molecular Iron Quaterpyridine Covalently Linked to Carbon Nitride

Abstract

Funding

UN SDGs

Research Keywords

RGC Funding Information

Access Output

Other Access Options

Permanent Link

Other Files and Links

Fingerprint

DON_RMG: Solid-supported Catalysts for Carbon Dioxide Reduction - RMGS

NSFC: Bioinspired Molecular Systems for Catalytic CO2 Reduction Based on Earth-abundant Metal Complexes

Cite this

Highly Efficient Photocatalytic Reduction of CO2 to CO by In Situ Formation of a Hybrid Catalytic System Based on Molecular Iron Quaterpyridine Covalently Linked to Carbon Nitride

Abstract

Funding

UN SDGs

Research Keywords

RGC Funding Information

Access Output

Other Access Options

Permanent Link

Other Files and Links

Fingerprint

Projects

DON_RMG: Solid-supported Catalysts for Carbon Dioxide Reduction - RMGS

NSFC: Bioinspired Molecular Systems for Catalytic CO2 Reduction Based on Earth-abundant Metal Complexes

Cite this

Highly Efficient Photocatalytic Reduction of CO₂ to CO by In Situ Formation of a Hybrid Catalytic System Based on Molecular Iron Quaterpyridine Covalently Linked to Carbon Nitride