Windle, CD; Wieczorek, A; Xiong, L; Sachs, M; Bozal-Ginesta, C; Cha, H; Cockcroft, JK; ... Tang, J; + view all Windle, CD; Wieczorek, A; Xiong, L; Sachs, M; Bozal-Ginesta, C; Cha, H; Cockcroft, JK; Durrant, J; Tang, J; - view fewer (2020) Covalent grafting of molecular catalysts on C₄NₓH_{y} as robust, efficient and well-defined photocatalysts for solar fuel synthesis. Chemical Science 10.1039/d0sc02986f. (In press).

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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 C₄NₓH_{y} to form noble metal-free photocatalysts for H2 production. The hybrids produce H_{2} 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.

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