Highly Selective Conversion Of CO2 To C2H6 On Graphene Modified ...

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Nanoscale

Highly selective conversion of CO2 to C2H6 on graphene modified chlorophyll Cu through multi-electron process for artificial photosynthesis†

Check for updates Tongshun Wu, ORCID logo *a Cheng Zhu, ORCID logo b Dongxue Han,ac Zhenhui Kang ORCID logo *b and Li Niuac Author affiliations

* Corresponding authors

a Centre for Advanced Analytical Science, c/o School of Chemistry and Chemical Engineering, Guangzhou University, Guangzhou 510006, P.R. China E-mail: [email protected]

b Jiangsu Key Laboratory for Carbon-Based Functional Materials & Devices, Institute of Functional Nano & Soft Materials (FUNSOM), Soochow University, 199 Ren'ai Road, Suzhou, Jiangsu, PR China E-mail: [email protected]

c State Key Laboratory of Electroanalytical Chemistry, c/o Engineering Laboratory for Modern Analytical Techniques, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, Changchun 130022, Jilin, China

Abstract

Artificial photosynthesis is a promising strategy for converting carbon dioxide into hydrocarbon fuels through solar energy as it is clean, economical and environmentally friendly. Herein, we developed a selective and stable photocatalyst for CO2 photocatalytic reduction into C2H6 through a multi-electron transfer pathway without the external sacrificial regents. The core component of this composite catalyst was extracted from a silkworm excrement and modified to make chlorophyll Cu (Chl-Cu), which contained a porphyrin structure as an antenna for light absorption and a Cu cation as an active centre. We found that C2 hydrocarbons such as C2H2, C2H4, and C2H6 tended to generate on chlorophyll-a/graphene. After substituting Mg2+ with Cu2+ cations in the centre of the porphyrin and modifying with graphene, only C2H6 was detected in the 18 hours reaction. This photocatalyst presented an outstanding activity and selectivity for the photocatalytic CO2 reduction (CO2RR) with a C2H6 yield rate at 68.23 μmol m−2 h−1 under visible light irradiation and an apparent quantum efficiency of 1.26% at 420 nm. In this system, the porphyrin rings were excited to produce electron–hole pairs by light. The photo-induced holes oxidized water to produce oxygen while graphene worked as an adsorption centre and electron acceptor for the CO2 reduction.

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Article information

DOI https://doi.org/10.1039/C9NR07824J Article type Paper Submitted 11 Sep 2019 Accepted 12 Nov 2019 First published 12 Nov 2019

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Nanoscale, 2019,11, 22980-22988 BibTex EndNote MEDLINE ProCite ReferenceManager RefWorks RIS

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Highly selective conversion of CO2 to C2H6 on graphene modified chlorophyll Cu through multi-electron process for artificial photosynthesis

T. Wu, C. Zhu, D. Han, Z. Kang and L. Niu, Nanoscale, 2019, 11, 22980 DOI: 10.1039/C9NR07824J

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