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Covalent grafting of molecular catalysts on C3NxHy as robust, efficient and well-defined photocatalysts for solar fuel synthesis

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Abstract

The covalent attachment of molecules to 2D materials is an emerging area as strong covalent chemistry offers new hybrid properties and greater mechanical stability compared with nanoparticles. A nickel bis-aminothiophenol catalyst was grafted onto a range of 2D carbon nitrides (C3NxHy) to form noble metal-free photocatalysts for H2 production. The hybrids produce H2 beyond 8 days with turnover numbers reaching 1360 based on nickel, a more than 3 fold higher durability than reported molecular catalyst-carbon nitride mixtures, and under longer wavelengths (>475 nm). Time-resolved spectroscopy reveals sub-microsecond electron transfer to the grafted catalyst, six orders of magnitude faster compared with similar reports of non-grafted catalysts. The photoelectrons on the catalyst have a ca. 1000 times longer half-time (7 ms) compared with bare carbon nitride (10 μs). The grafting strategy operates across a range of molecular catalyst-carbon nitride combinations, thus paving the way for robust efficient photocatalysts based on low-cost tunable components.

Graphical abstract: Covalent grafting of molecular catalysts on C3NxHy as robust, efficient and well-defined photocatalysts for solar fuel synthesis

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Article information


Submitted
27 May 2020
Accepted
24 Jul 2020
First published
24 Jul 2020

This article is Open Access
All publication charges for this article have been paid for by the Royal Society of Chemistry

Chem. Sci., 2020, Advance Article
Article type
Edge Article

Covalent grafting of molecular catalysts on C3NxHy as robust, efficient and well-defined photocatalysts for solar fuel synthesis

C. D. Windle, A. Wieczorek, L. Xiong, M. Sachs, C. Bozal-Ginesta, H. Cha, J. K. Cockcroft, J. Durrant and J. Tang, Chem. Sci., 2020, Advance Article , DOI: 10.1039/D0SC02986F

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