期刊
ENERGY & ENVIRONMENTAL SCIENCE
卷 13, 期 3, 页码 917-927出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/c9ee02783a
关键词
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资金
- RBI at Georgia Tech
Electrocatalytic hydrogenation (ECH) provides a green route to upgrade oxygenated bio-oil under mild conditions, but is still challenged with the issues of low working current density (<60 mA cm(-2)) and low faradaic efficiency (usually 20-60%) that seriously hinder its practical applications. Herein, we present a dual-catalyst electrochemical route that achieves extremely high faradaic efficiency (>99% for many chemicals) and high working current density (up to 800 mA cm(-2)) in the hydrogenation of model bio-oil compounds. More importantly, efficient deoxygenation to alkanes, often thought to be very difficult in conventional ECH, was achieved in the aqueous electrolysis. The dual-catalyst system consists of a suspended noble-metal catalyst and soluble polyoxometalate (POM). The theoretical calculations indicate that the POM functions as a superacid, changing the common hydrogenation route to a carbocation mechanism and resulting in effective electrolytic deoxygenation of oxygenates. Because no current flows through the catalyst, even a non-conductive catalyst can be used, which provides a great opportunity for extension to general applications.
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