title: Ordered gyroidal tantalum oxide photocatalysts: eliminating diffusion limitations and tuning surface barriers.
abstract: In this work we synthesized well-ordered, Ta2O5films with a 3D-interconnected gyroid mesopore architecture with large pore sizes beyond 30 nm and extended crystalline domains through self-assembly of tailor-made triblock-terpolymers. This has effectively eliminated diffusion limitations inherent to previously reported mesoporous photocatalysts and resulted in superior hydrogen evolution with apparent quantum yields of up to 4.6% in the absence of any cocatalyst. We further show that the injection barrier at the solid-liquid interface constitutes a key criterion for photocatalytic performance and can be modified by the choice of the carbon template. This work highlights pore and surface engineering as a promising tool towards high-performance mesoporous catalysts and electrodes for various energy-related applications.
authors.affiliation: Institut für Materialchemie, Technische Universität Wien, Getreidemarkt 9/BC/2, A-1060, Vienna, Austria. dominik.eder@tuwien.ac.at.
authors.forename: Alexey S
authors.initials: AS
authors.lastname: Cherevan
authors.affiliation: Department of Materials Science and Engineering, 330 Bard Hall, Cornell University, Ithaca, NY 14853, USA.
authors.forename: Spencer
authors.initials: S
authors.lastname: Robbins
authors.affiliation: Institut für Materialchemie, Technische Universität Wien, Getreidemarkt 9/BC/2, A-1060, Vienna, Austria. dominik.eder@tuwien.ac.at.
authors.forename: Dennis
authors.initials: D
authors.lastname: Dieterle
authors.affiliation: Institut für Materialchemie, Technische Universität Wien, Getreidemarkt 9/BC/2, A-1060, Vienna, Austria. dominik.eder@tuwien.ac.at.
authors.forename: Paul
authors.initials: P
authors.lastname: Gebhardt
authors.affiliation: Department of Materials Science and Engineering, 330 Bard Hall, Cornell University, Ithaca, NY 14853, USA.
authors.forename: Ulrich
authors.initials: U
authors.lastname: Wiesner
authors.affiliation: Institut für Materialchemie, Technische Universität Wien, Getreidemarkt 9/BC/2, A-1060, Vienna, Austria. dominik.eder@tuwien.ac.at.
authors.forename: Dominik
authors.initials: D
authors.lastname: Eder