Effects of Periodic Pore Ordering on Photocatalytic Hydrogen Generation with Mesoporous Semiconductor Oxides

Crystalline and 3D continuous mesoporous quaternary CsTaWO6 semiconductors are prepared with different degrees of long‐range periodic order and local order, respectively, to investigate the influence of periodic pore order on the photocatalytic performance in hydrogen evolution of mesoporous photoca...

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Main Authors: Tobias Weller, Jana Timm, Leonie Deilmann, Tobias S. Doerr, Christopher Greve, Alexey S. Cherevan, Peter A. Beaucage, Ulrich B. Wiesner, Eva M. Herzig, Dominik Eder, Roland Marschall
Format: Article
Language:English
Published: Wiley-VCH 2023-06-01
Series:Small Structures
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Online Access:https://doi.org/10.1002/sstr.202200184
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author Tobias Weller
Jana Timm
Leonie Deilmann
Tobias S. Doerr
Christopher Greve
Alexey S. Cherevan
Peter A. Beaucage
Ulrich B. Wiesner
Eva M. Herzig
Dominik Eder
Roland Marschall
author_facet Tobias Weller
Jana Timm
Leonie Deilmann
Tobias S. Doerr
Christopher Greve
Alexey S. Cherevan
Peter A. Beaucage
Ulrich B. Wiesner
Eva M. Herzig
Dominik Eder
Roland Marschall
author_sort Tobias Weller
collection DOAJ
description Crystalline and 3D continuous mesoporous quaternary CsTaWO6 semiconductors are prepared with different degrees of long‐range periodic order and local order, respectively, to investigate the influence of periodic pore order on the photocatalytic performance in hydrogen evolution of mesoporous photocatalysts. The degree of long‐range order of the mesopores is changed by modifying the ratio between metal precursors and soft polymer template poly(isoprene‐b‐styrene‐b‐ethylene oxide) (PI‐b‐PS‐b‐PEO; ISO) in the sol–gel synthesis. Long‐range periodic order is found to have no appreciable advantage compared with an only locally ordered continuous pore system. On the contrary, nonperiodically ordered mesopores result in higher activity toward photocatalytic hydrogen evolution, even with slightly smaller pore diameter and lower cumulative pore volume. Most importantly, it is shown that pore connectivity and heterogeneous pore systems in mesoporous photocatalysts play a major role for hydrogen evolution when other parameters are confirmed to be not rate limiting.
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spelling doaj.art-f7465fe4e3bb4b2d9eb9b34af7fd24a12023-07-26T01:40:18ZengWiley-VCHSmall Structures2688-40622023-06-0146n/an/a10.1002/sstr.202200184Effects of Periodic Pore Ordering on Photocatalytic Hydrogen Generation with Mesoporous Semiconductor OxidesTobias Weller0Jana Timm1Leonie Deilmann2Tobias S. Doerr3Christopher Greve4Alexey S. Cherevan5Peter A. Beaucage6Ulrich B. Wiesner7Eva M. Herzig8Dominik Eder9Roland Marschall10Institute of Physical Chemistry Justus-Liebig-University Giessen 35392 Giessen GermanyDepartment of Chemistry University of Bayreuth 95447 Bayreuth GermanyInstitut für Materialchemie Technische Universität Wien 1060 Vienna AustriaINM—Leibniz Institute for New Materials Campus D2 2 66123 Saarbrücken GermanyInstitute of Physics Dynamics and Structure Formation—Herzig Group University of Bayreuth 95447 Bayreuth GermanyInstitut für Materialchemie Technische Universität Wien 1060 Vienna AustriaMaterials Science and Engineering Cornell University 14853 Ithaca NY USAMaterials Science and Engineering Cornell University 14853 Ithaca NY USAInstitute of Physics Dynamics and Structure Formation—Herzig Group University of Bayreuth 95447 Bayreuth GermanyInstitut für Materialchemie Technische Universität Wien 1060 Vienna AustriaInstitute of Physical Chemistry Justus-Liebig-University Giessen 35392 Giessen GermanyCrystalline and 3D continuous mesoporous quaternary CsTaWO6 semiconductors are prepared with different degrees of long‐range periodic order and local order, respectively, to investigate the influence of periodic pore order on the photocatalytic performance in hydrogen evolution of mesoporous photocatalysts. The degree of long‐range order of the mesopores is changed by modifying the ratio between metal precursors and soft polymer template poly(isoprene‐b‐styrene‐b‐ethylene oxide) (PI‐b‐PS‐b‐PEO; ISO) in the sol–gel synthesis. Long‐range periodic order is found to have no appreciable advantage compared with an only locally ordered continuous pore system. On the contrary, nonperiodically ordered mesopores result in higher activity toward photocatalytic hydrogen evolution, even with slightly smaller pore diameter and lower cumulative pore volume. Most importantly, it is shown that pore connectivity and heterogeneous pore systems in mesoporous photocatalysts play a major role for hydrogen evolution when other parameters are confirmed to be not rate limiting.https://doi.org/10.1002/sstr.202200184hydrogen evolution reactionsmesoporesphotocatalysispore orderingscanning isotherms
spellingShingle Tobias Weller
Jana Timm
Leonie Deilmann
Tobias S. Doerr
Christopher Greve
Alexey S. Cherevan
Peter A. Beaucage
Ulrich B. Wiesner
Eva M. Herzig
Dominik Eder
Roland Marschall
Effects of Periodic Pore Ordering on Photocatalytic Hydrogen Generation with Mesoporous Semiconductor Oxides
Small Structures
hydrogen evolution reactions
mesopores
photocatalysis
pore ordering
scanning isotherms
title Effects of Periodic Pore Ordering on Photocatalytic Hydrogen Generation with Mesoporous Semiconductor Oxides
title_full Effects of Periodic Pore Ordering on Photocatalytic Hydrogen Generation with Mesoporous Semiconductor Oxides
title_fullStr Effects of Periodic Pore Ordering on Photocatalytic Hydrogen Generation with Mesoporous Semiconductor Oxides
title_full_unstemmed Effects of Periodic Pore Ordering on Photocatalytic Hydrogen Generation with Mesoporous Semiconductor Oxides
title_short Effects of Periodic Pore Ordering on Photocatalytic Hydrogen Generation with Mesoporous Semiconductor Oxides
title_sort effects of periodic pore ordering on photocatalytic hydrogen generation with mesoporous semiconductor oxides
topic hydrogen evolution reactions
mesopores
photocatalysis
pore ordering
scanning isotherms
url https://doi.org/10.1002/sstr.202200184
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