Designer Titania-Supported Au-Pd Nanoparticles for Efficient Photocatalytic Hydrogen Production

被引：285

作者：

Su, Ren ^{[1
,2
]}

Tiruvalam, Ramchandra ^{[3
]}

Logsdail, Andrew J. ^{[4
]}

He, Qian ^{[3
]}

Downing, Christopher A. ^{[4
]}

Jensen, Mikkel T. ^{[5
]}

Dimitratos, Nikolaos ^{[4
,6
]}

Kesavan, Lokesh ^{[7
]}

Wells, Peter P. ^{[4
,6
]}

Bechstein, Ralf ^{[1
,2
]}

Jensen, Henrik H. ^{[5
]}

Wendt, Stefan ^{[1
,2
]}

Catlow, C. Richard A. ^{[4
,6
]}

Kiely, Christopher J. ^{[3
]}

Hutchings, Graham J. ^{[6
]}

Besenbacher, Flemming ^{[1
,2
]}

机构：

[1] Aarhus Univ, Interdisciplinary Nanosci Ctr iNANO, DK-8000 Aarhus C, Denmark

[2] Aarhus Univ, Dept Phys & Astron, DK-8000 Aarhus C, Denmark

[3] Lehigh Univ, Dept Mat Sci & Engn, Bethlehem, PA 18015 USA

[4] UCL, Dept Chem, Kathleen Lonsdale Mat Chem, London WC1H 0AJ, England

[5] Aarhus Univ, Dept Chem, DK-8000 Aarhus C, Denmark

[6] Rutherford Appleton Lab, UK Catalysis Hub, Didcot OX11 0FA, Oxon, England

[7] Cardiff Univ, Cardiff Catalysis Inst, Sch Chem, Cardiff CF10 3AT, S Glam, Wales

来源：

ACS NANO | 2014年 / 8卷 / 04期

基金：

英国工程与自然科学研究理事会;

关键词：

photocatalysis; hydrogen evolution; metal nanoparticles; cocatalysts; TiO2; density functional theory; BENZYL ALCOHOL OXIDATION; METAL NANOPARTICLES; VISIBLE-LIGHT; PARTICLE-SIZE; TIO2; SURFACE; EVOLUTION; NANOCLUSTERS; COCATALYST; PEROXIDE;

D O I：

10.1021/nn500963m

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

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, Pd-shell-Au-core nanoparticles immobilized on TiO2 exhibit extremely high quantum efficiencies for H-2 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.

引用

页码：3490 / 3497

页数：8

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