Selective Alcohol Dehydrogenation and Hydrogenolysis with Semiconductor-Metal Photocatalysts: Toward Solar-to-Chemical Energy Conversion of Biomass-Relevant Substrates

Thumbnail Image
Supplemental Files
Date
2012-09-13
Authors
Nelson, Nicholas
Vela, Javier
Major Professor
Advisor
Committee Member
Journal Title
Journal ISSN
Volume Title
Publisher
Authors
Person
Person
Research Projects
Organizational Units
Organizational Unit
Organizational Unit
Journal Issue
Is Version Of
Versions
Series
Department
Ames National LaboratoryChemistry
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.

Description
Keywords
Citation
DOI
Subject Categories
Copyright
Sun Jan 01 00:00:00 UTC 2012
Collections