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

Angew Chem Int Ed Engl. 2022 Mar 7;61(11):e202116832. doi: 10.1002/anie.202116832. Epub 2022 Jan 25.

Authors

Yue Wei^{1

2}, Lingjing Chen¹, Huan Chen¹, Lirong Cai¹, Guiping Tan¹, Yongfu Qiu¹, Quanjun Xiang², Gui Chen¹, Tai-Chu Lau³, Marc Robert⁴

Affiliations

¹ School of Environment and Civil Engineering, Dongguan University of Technology, Dongguan, 523808, Guangdong, P.R. China.
² State Key Laboratory of Electronic Thin Film and Integrated Devices, School of Electronic Science and Engineering, University of Electronic Science and Technology of China, Chengdu, 611731, P.R. China.
³ Department of Chemistry, City University of Hong Kong, Kowloon, 999077, Hong Kong, P.R. China.
⁴ Université de Paris, Laboratoire d'Electrochimie Moléculaire, CNRS, F-75006 Paris, France, Institut Universitaire de France (IUF), 75005, Paris, France.

PMID: 34986281
DOI: 10.1002/anie.202116832

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 CH₃ CN 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 C₃ N₄ 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: CO2 Reduction; Carbon Nitride; Fe Quaterpyridine; Photocatalysis; Schiff Base Reaction.

Abstract

Grants and funding