Please use this identifier to cite or link to this item: doi:10.22028/D291-28987
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Title: Ordered Mesoporous TiO2 Gyroids: Effects of Pore Architecture and Nb-Doping on Photocatalytic Hydrogen Evolution under UV and Visible Irradiation
Author(s): Dörr, Tobias Sebastian
Deilmann, Leonie
Haselmann, Greta
Cherevan, Alexey
Zhang, Peng
Blaha, Peter
de Oliveira, Peter William
Kraus, Tobias
Eder, Dominik
Language: English
Title: Advanced energy materials
Volume: 8
Issue: 36
Publisher/Platform: Wiley-VCH
Year of Publication: 2018
Publikation type: Journal Article
Abstract: Pure and Nb‐doped TiO2 photocatalysts with highly ordered alternating gyroid architecture and well‐controllable mesopore size of 15 nm via co‐assembly of a poly(isoprene)‐block‐poly(styrene)‐block‐poly(ethylene oxide) block copolymer are synthesized. A combined effort by electron microscopy, X‐ray scattering, photoluminescence, X‐ray photoelectron spectroscopy, Raman spectroscopy, and density functional theory simulations reveals that the addition of small amounts of Nb results in the substitution of Ti4+ with isolated Nb5+ species that introduces inter‐bandgap states, while at high concentrations, Nb prefers to cluster forming shallow trap states within the conduction band minimum of TiO2. The gyroidal photocatalysts are remarkably active toward hydrogen evolution under UV and visible light due to the open 3D network, where large mesopores ensure efficient pore diffusion and high photon harvesting. The gyroids yield unprecedented high evolution rates beyond 1000 µmol h−1 (per 10 mg catalyst), outperforming even the benchmark P25‐TiO2 more than fivefold. Under UV light, the Nb‐doping reduces the activity due to the introduction of charge recombination centers, while the activity in the visible triple upon incorporation is owed to a more efficient absorption due to inter‐bandgap states. This unique pore architecture may further offer hitherto undiscovered optical benefits to photocatalysis, related to chiral and metamaterial‐like behavior, which will stimulate further studies focusing on novel light–matter interactions.
DOI of the first publication: 10.1002/aenm.201802566
URL of the first publication: https://onlinelibrary.wiley.com/doi/full/10.1002/aenm.201802566
Link to this record: hdl:20.500.11880/27933
http://dx.doi.org/10.22028/D291-28987
ISSN: 1614-6840
1614-6832
Date of registration: 27-Sep-2019
Faculty: NT - Naturwissenschaftlich- Technische Fakultät
Department: NT - Chemie
Professorship: NT - Prof. Dr. Tobias Kraus
Collections:UniBib – Die Universitätsbibliographie

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