Role of Adsorbed Water on Charge Carrier Dynamics in Photoexcited TiO.

J Phys Chem C Nanomater Interfaces

Laboratory of Inorganic Materials Chemistry, Department of Chemical Engineering and Chemistry, Eindhoven University of Technology, P.O. Box 513, 5600MB Eindhoven, The Netherlands.

Published: April 2017

Overall photocatalytic water splitting is one of the most sought after processes for sustainable solar-to-chemical energy conversion. The efficiency of this process strongly depends on charge carrier recombination and interaction with surface adsorbates at different time scales. Here, we investigated how hydration of TiO P25 affects dynamics of photogenerated electrons at the millisecond to minute time scale characteristic for chemical reactions. We used rapid scan diffuse-reflectance infrared Fourier transform spectroscopy (DRIFTS). The decay of photogenerated electron absorption was substantially slower in the presence of associated water. For hydrated samples, the charge carrier recombination rates followed an Arrhenius-type behavior in the temperature range of 273-423 K; these became temperature-independent when the material was dehydrated at temperatures above 423 K or cooled below 273 K. A DFT+ analysis revealed that hydrogen bonding with adsorbed water stabilizes surface-trapped holes at anatase TiO(101) facet and lowers the barriers for hole migration. Hence, hole mobility should be higher in the hydrated material than in the dehydrated system. This demonstrates that adsorbed associated water can efficiently stabilize photogenerated charge carriers in nanocrystalline TiO and suppress their recombination at the time scale up to minutes.

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http://www.ncbi.nlm.nih.gov/pmc/articles/PMC5388900PMC
http://dx.doi.org/10.1021/acs.jpcc.7b00472DOI Listing

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