Campus Units

Chemistry, Ames Laboratory

Document Type

Article

Publication Version

Published Version

Publication Date

9-13-2012

Journal or Book Title

Journal of Physical Chemistry Letters

Volume

3

Issue

19

First Page

2798

Last Page

2802

DOI

10.1021/jz301309d

Abstract

Photocatalytic conversion of biomass is a potentially transformative concept in renewable energy. Dehydrogenation and hydrogenolysis of biomass-derived alcohols can produce renewable fuels such as H 2 and hydrocarbons, respectively. We have successfully used semiconductor-metal heterostructures for sunlight-driven dehydrogenation and hydrogenolysis of benzyl alcohol. The heterostructure composition dictates activity, product distribution, and turnovers. A few metal (M = Pt, Pd) islands on the semiconductor (SC) surface significantly enhance activity and selectivity and also greatly stabilize the SC against photoinduced etching and degradation. Under selected conditions, CdS-Pt favors dehydrogenation (H 2) over hydrogenolysis (toluene) 8:1, whereas CdS 0.4Se 0.6-Pd favors hydrogenolysis over dehydrogenation 3:1. Photochemically generated, surface-adsorbed hydrogen is useful in tandem catalysis, for example, via transfer hydrogenation. We expect this work will lead to new paradigms for sunlight-driven conversions of biomass-relevant substrates.

Comments

Reprinted (adapted) with permission from Journal of Physical Chemistry Letters 3 (2012): 2798, doi:10.1021/jz301309d. Copyright 2012 American Chemical Society.

Copyright Owner

American Chemical Society

Language

en

File Format

application/pdf

Included in

Chemistry Commons

Share

COinS