文章基本信息

标题：Reversible catalytic dehydrogenation of alcohols for energy storage
本地全文：下载
作者：Peter J. Bonitatibus ; Sumit Chakraborty ; Mark D. Doherty 等
期刊名称：Proceedings of the National Academy of Sciences
印刷版ISSN：0027-8424
电子版ISSN：1091-6490
出版年度：2015
卷号：112
期号：6
页码：1687-1692
DOI：10.1073/pnas.1420199112
语种：English
出版社：The National Academy of Sciences of the United States of America
摘要：SignificanceCatalytic hydrogenation and dehydrogenation reactions are extremely important in organic chemistry and recently for energy storage in the form of chemical bonds. Although catalysts are known which catalyze both reactions, the rates and conditions required for the two are frequently very different due to the differences associated with the bonds to be activated (C-H/O-H/N-H and C = O/C = N/H-H). The use of a bifunctional catalyst would substantially simplify the design of processes related to energy storage. In this work, organometallic complexes of iron and iridium are shown to act as catalysts for reversible dehydrogenation of alcohols to carbonyl compounds. This finding opens a pathway to the development of catalysts for direct reversible electrochemical dehydrogenation of organic fuels in energy generation and storage reactions. Reversibility of a dehydrogenation/hydrogenation catalytic reaction has been an elusive target for homogeneous catalysis. In this report, reversible acceptorless dehydrogenation of secondary alcohols and diols on iron pincer complexes and reversible oxidative dehydrogenation of primary alcohols/reduction of aldehydes with separate transfer of protons and electrons on iridium complexes are shown. This reactivity suggests a strategy for the development of reversible fuel cell electrocatalysts for partial oxidation (dehydrogenation) of hydroxyl-containing fuels.
关键词：catalysis ; energy storage ; reversibility ; hydrogenation ; dehydrogenation