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Effective Photocatalytic Hydrogen Evolution by Cascadal Carrier Transfer in the Reverse Direction.

ABSTRACT: Visible-light-responsive photocatalysts used in the highly efficient hydrogen production exhibit several disadvantages such as photocorrosion and fast recombination. Because of the potential important applications of such catalysts, it is crucial that a simple, effective solution is developed. In this respect, in this study, we combined SiC (? modification) and TiO₂ with CdS to overcome the challenges of photocorrosion and fast recombination of CdS. Notably, we found that when irradiated with visible light, CdS was excited, and the excited electrons moved to the conduction band of TiO₂, thereby increasing the efficiency of charge separation. In addition, by moving the holes generated on CdS to the valence band of SiC, in the opposite direction of TiO₂, photocorrosion and fast recombination were prevented. As a result, in the sulfide solution, the CdS/SiC composite catalyst exhibited 4.3 times higher hydrogen generation ability than pure CdS. Moreover, this effect was enhanced with the addition of TiO₂, giving 10.8 times higher hydrogen generation ability for the CdS/SiC/TiO₂ catalyst. Notably, the most efficient catalyst, which was obtained by depositing Pt as a cocatalyst, exhibited 1.09 mmol g^-1 h^-1 hydrogen generation ability and an apparent quantum yield of 24.8%. Because water reduction proceeded on the TiO₂ surface and oxidative sulfide decomposition proceeded on the SiC surface, the exposure of CdS to the solution was unnecessary, and X-ray photoelectron spectroscopy confirmed that photocorrosion was successfully suppressed. Thus, we believe that the effective composite photocatalyst construction method presented herein can also be applied to other visible-light-responsive powder photocatalysts having the same disadvantages as CdS, thereby improving the efficiency of such catalysts.

SUBMITTER: Nagakawa H

PROVIDER: S-EPMC6645024 | biostudies-literature | 2018 Oct

REPOSITORIES: biostudies-literature

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Effective Photocatalytic Hydrogen Evolution by Cascadal Carrier Transfer in the Reverse Direction.

Nagakawa Haruki H Ochiai Tsuyoshi T Takekuma Yuya Y Konuma Seiji S Nagata Morio M

ACS omega 20181008 10

Visible-light-responsive photocatalysts used in the highly efficient hydrogen production exhibit several disadvantages such as photocorrosion and fast recombination. Because of the potential important applications of such catalysts, it is crucial that a simple, effective solution is developed. In this respect, in this study, we combined SiC (β modification) and TiO<sub>2</sub> with CdS to overcome the challenges of photocorrosion and fast recombination of CdS. Notably, we found that when irradia ...[more]

PMID: 31458002

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Project description:Semiconducting polymers are versatile materials for solar energy conversion and have gained popularity as photocatalysts for sunlight-driven hydrogen production. Organic polymers often contain residual metal impurities such as palladium (Pd) clusters that are formed during the polymerization reaction, and there is increasing evidence for a catalytic role of such metal clusters in polymer photocatalysts. Using transient and operando optical spectroscopy on nanoparticles of F8BT, P3HT, and the dibenzo[b,d]thiophene sulfone homopolymer P10, we demonstrate how differences in the time scale of electron transfer to Pd clusters translate into hydrogen evolution activity optima at different residual Pd concentrations. For F8BT nanoparticles with common Pd concentrations of >1000 ppm (>0.1 wt %), we find that residual Pd clusters quench photogenerated excitons via energy and electron transfer on the femto-nanosecond time scale, thus outcompeting reductive quenching. We spectroscopically identify reduced Pd clusters in our F8BT nanoparticles from the microsecond time scale onward and show that the predominant location of long-lived electrons gradually shifts to the F8BT polymer when the Pd content is lowered. While a low yield of long-lived electrons limits the hydrogen evolution activity of F8BT, P10 exhibits a substantially higher hydrogen evolution activity, which we demonstrate results from higher yields of long-lived electrons due to more efficient reductive quenching. Surprisingly, and despite the higher performance of P10, long-lived electrons reside on the P10 polymer rather than on the Pd clusters in P10 particles, even at very high Pd concentrations of 27000 ppm (2.7 wt %). In contrast, long-lived electrons in F8BT already reside on Pd clusters before the typical time scale of hydrogen evolution. This comparison shows that P10 exhibits efficient reductive quenching but slow electron transfer to residual Pd clusters, whereas the opposite is the case for F8BT. These findings suggest that the development of even more efficient polymer photocatalysts must target materials that combine both rapid reductive quenching and rapid charge transfer to a metal-based cocatalyst.

Dataset Information

Effective Photocatalytic Hydrogen Evolution by Cascadal Carrier Transfer in the Reverse Direction.

Publications

Effective Photocatalytic Hydrogen Evolution by Cascadal Carrier Transfer in the Reverse Direction.

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