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Designer Titania-supported Au–Pd nanoparticles for efficient photocatalytic hydrogen production

Designer Titania-supported Au–Pd nanoparticles for efficient photocatalytic hydrogen production
Designer Titania-supported Au–Pd nanoparticles for efficient photocatalytic hydrogen production
Photocatalytic hydrogen evolution may provide one of the solutions to the shift to a sustainable energy society, but the quantum efficiency of the process still needs to be improved. Precise control of the composition and structure of the metal nanoparticle cocatalysts is essential, and we show that fine-tuning the Au–Pd nanoparticle structure modifies the electronic properties of the cocatalyst significantly. Specifically, Pdshell–Aucore nanoparticles immobilized on TiO2 exhibit extremely high quantum efficiencies for H2 production using a wide range of alcohols, implying that chemical byproducts from the biorefinery industry can be used as feedstocks. In addition, the excellent recyclability of our photocatalyst material indicates a high potential in industrial applications. We demonstrate that this particular elemental segregation provides optimal positioning of the unoccupied d-orbital states, which results in an enhanced utilization of the photoexcited electrons in redox reactions. We consider that the enhanced activity observed on TiO2 is generic in nature and can be transferred to other narrow band gap semiconductor supports for visible light photocatalysis.
1936-0851
3490-3497
Su, Ren
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Tiruvalam, Ramchandra
15711553-ec07-48d1-8fd1-db5055e0a4cf
Logsdail, Andrew J.
2b65adf3-96a6-4e24-92cc-7025b89db7b6
He, Qian
9983d6cf-fa90-4e7f-874c-17342aa4eeac
Downing, Christopher A.
4519511c-d889-43bb-b6de-0644b5c193d5
Jensen, Mikkel T.
71953271-4997-4988-a99b-84d5c9d53b72
Dimitratos, Nikolaos
a4385576-4a05-478b-8389-460bfb43412b
Kesavan, Lokesh
2c529199-5e03-4c7f-98c1-06ab931b924c
Wells, Peter P.
bc4fdc2d-a490-41bf-86cc-400edecf2266
Bechstein, Ralf
4ee6f6ee-15d4-438f-8f62-f2ffad1079a5
Jensen, Henrik H.
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Wendt, Stefan
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Catlow, C. Richard A.
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Kiely, Christopher J.
431afe51-dda4-44fb-a889-8f0e95a1b902
Hutchings, Graham J.
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Besenbacher, Flemming
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Su, Ren
39ea4c22-e001-45f1-89f8-31c4e056a3b8
Tiruvalam, Ramchandra
15711553-ec07-48d1-8fd1-db5055e0a4cf
Logsdail, Andrew J.
2b65adf3-96a6-4e24-92cc-7025b89db7b6
He, Qian
9983d6cf-fa90-4e7f-874c-17342aa4eeac
Downing, Christopher A.
4519511c-d889-43bb-b6de-0644b5c193d5
Jensen, Mikkel T.
71953271-4997-4988-a99b-84d5c9d53b72
Dimitratos, Nikolaos
a4385576-4a05-478b-8389-460bfb43412b
Kesavan, Lokesh
2c529199-5e03-4c7f-98c1-06ab931b924c
Wells, Peter P.
bc4fdc2d-a490-41bf-86cc-400edecf2266
Bechstein, Ralf
4ee6f6ee-15d4-438f-8f62-f2ffad1079a5
Jensen, Henrik H.
9d197e11-dd45-46bf-be73-e65698e17941
Wendt, Stefan
11637be1-627f-44c7-940f-e255df37bbf5
Catlow, C. Richard A.
50b88125-9415-4b37-9146-af6783e42510
Kiely, Christopher J.
431afe51-dda4-44fb-a889-8f0e95a1b902
Hutchings, Graham J.
efab6909-c2f0-4992-a188-10b761075311
Besenbacher, Flemming
18a324f2-03aa-4096-981e-14682dab1db4

Su, Ren, Tiruvalam, Ramchandra, Logsdail, Andrew J., He, Qian, Downing, Christopher A., Jensen, Mikkel T., Dimitratos, Nikolaos, Kesavan, Lokesh, Wells, Peter P., Bechstein, Ralf, Jensen, Henrik H., Wendt, Stefan, Catlow, C. Richard A., Kiely, Christopher J., Hutchings, Graham J. and Besenbacher, Flemming (2014) Designer Titania-supported Au–Pd nanoparticles for efficient photocatalytic hydrogen production. ACS Nano, 8 (4), 3490-3497. (doi:10.1021/nn500963m).

Record type: Article

Abstract

Photocatalytic hydrogen evolution may provide one of the solutions to the shift to a sustainable energy society, but the quantum efficiency of the process still needs to be improved. Precise control of the composition and structure of the metal nanoparticle cocatalysts is essential, and we show that fine-tuning the Au–Pd nanoparticle structure modifies the electronic properties of the cocatalyst significantly. Specifically, Pdshell–Aucore nanoparticles immobilized on TiO2 exhibit extremely high quantum efficiencies for H2 production using a wide range of alcohols, implying that chemical byproducts from the biorefinery industry can be used as feedstocks. In addition, the excellent recyclability of our photocatalyst material indicates a high potential in industrial applications. We demonstrate that this particular elemental segregation provides optimal positioning of the unoccupied d-orbital states, which results in an enhanced utilization of the photoexcited electrons in redox reactions. We consider that the enhanced activity observed on TiO2 is generic in nature and can be transferred to other narrow band gap semiconductor supports for visible light photocatalysis.

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More information

Accepted/In Press date: 7 March 2014
e-pub ahead of print date: 7 March 2014
Published date: 22 April 2014
Organisations: Organic Chemistry: SCF

Identifiers

Local EPrints ID: 400601
URI: http://eprints.soton.ac.uk/id/eprint/400601
ISSN: 1936-0851
PURE UUID: 1c6ade8f-3356-40b3-a1ae-a720c8609270
ORCID for Peter P. Wells: ORCID iD orcid.org/0000-0002-0859-9172

Catalogue record

Date deposited: 20 Sep 2016 08:54
Last modified: 15 Mar 2024 03:24

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Contributors

Author: Ren Su
Author: Ramchandra Tiruvalam
Author: Andrew J. Logsdail
Author: Qian He
Author: Christopher A. Downing
Author: Mikkel T. Jensen
Author: Nikolaos Dimitratos
Author: Lokesh Kesavan
Author: Peter P. Wells ORCID iD
Author: Ralf Bechstein
Author: Henrik H. Jensen
Author: Stefan Wendt
Author: C. Richard A. Catlow
Author: Christopher J. Kiely
Author: Graham J. Hutchings
Author: Flemming Besenbacher

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