A hybrid artificial photosynthesis system with molecular catalysts covalently linked onto TiO2 as electron relay for efficient photocatalytic hydrogen evolution

doi:10.1016/j.jmst.2019.12.028

Abstract

Abstract:

Efficient charge carrier transfer from light harvesters to catalysts greatly determines the photocatalytic activity in an artificial photosynthesis (AP) system for solar hydrogen evolution. In this study, an AP system composed of xanthene dye as light harvester and cobaloxime molecular complex as catalyst, with TiO₂ as electron relay, was designed for photocatalytic hydrogen evolution under visible light (λ > 420 nm). It was demonstrated that with cobaloxime molecule covalently linked onto the TiO₂ electron relay, the resulting hybrid AP system exhibited much increased photocatalytic activity as compared to that without TiO₂. The greatly increased photocatalytic activity should be due to the efficient electron transfer from xanthene dye as light harvester and cobaloxime molecular complex as catalyst, shuttled by the TiO₂ electron relay, for the following water reduction reaction. The present study demonstrates a facile and feasible strategy to guide the design of high performance AP systems through the electron relay shuttled and promoted charge transfer process.

Key words: Artificial photosynthesis, Molecular catalysts, Electron relay, Photocatalytic hydrogen evolution

Jie Zhang, Gehong Zhang, Jing Zhang. A hybrid artificial photosynthesis system with molecular catalysts covalently linked onto TiO₂ as electron relay for efficient photocatalytic hydrogen evolution[J]. J. Mater. Sci. Technol., 2020, 50: 147-152.

Figures/Tables 5

Fig. 1. Molecular structures of (a) xanthene dyes and (b) CoP, (c) ESI-MS spectrum of CoP, (d) FTIR spectra of CoP and CoP covalently linked TiO2 (CoP/TiO2), (e) UV-vis absorption spectra of CoP solution before and after covalent linking to TiO2, (f) photocatalytic activity for hydrogen evolution from different hybrid AP systems under visible light (>420?nm). TiO2/CoP or TiO2: 10?mg, FL: 5?mg, CoP: 0.03?mg.

Fig. 2. Photocatalytic activities of different hybrid systems for hydrogen evolution: (a) TiO2/CoP: 10?mg, xanthene dyes: 0.15?mmol, i.e., FL: 5?mg, RB: 15.3?mg, EY: 9.7?mg; (b) TiO2/CoP or TiO2: 10?mg, CoP: 0.03?mg, EY: 9.7?mg; (c) TiO2/CoP: 5?mg, EY: 4.85-19.4?mg; (d) TiO2/CoP: 2-15?mg, EY: 9.7?mg.

Fig. 3. (a) UV-vis spectra of the solutions in the EY/TiO2/CoP system with 10?mg of TiO2/CoP and 9.7?mg of EY under visible light irradiation for photocatalytic hydrogen evolution for different times; (b) time courses of photocatalytic hydrogen evolution in the EY/TiO2/CoP system with 10?mg of TiO2/CoP and 9.7?mg of EY, and readdition of TiO2/CoP (10?mg) and then EY (9.7?mg) to the system after irradiation for 12?h.

Fig. 4. (a) Cyclic voltammetry (CV) measurement of CoP in DMF/acetonitrile (1/1) solution containing 0.1?M tetrabutylammonium hexafluorophosphate (TBAPF6), with and without trifluoroacetic acid (TFA); (b) initial hydrogen evolution rates depending on the concentrations of CoP under visible light irradiation. EY: 5?mg.

Fig. 5. Proposed catalysis mechanism of the EY/TiO2/CoP system for photocatalytic hydrogen evolution.

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A hybrid artificial photosynthesis system with molecular catalysts covalently linked onto TiO₂ as electron relay for efficient photocatalytic hydrogen evolution

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