What is it about?
Reported herein are molecular insights into cationic mononuclear ruthenium carboxylates ([Ru(OCOR)]+) as prototypical catalysts for the hydrogenation of CAs. The substrate-derived coordinated carboxylate was found to function initially as a proton acceptor for the heterolytic cleavage of dihydrogen, and subsequently also as an acceptor for the hydride from [Ru–H]þ, which was generated in the first step. That is why we call the catalytic system "CA self-induced hydrogenation of CAs".
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Why is it important?
CAs are ubiquitous in bio-renewable and petrochemical sources of carbon. Hydrogenation of CAs to yield alcohols produces water as the only byproduct, and thus represents a possible next generation, sustainable method for the production of these alternative energy carriers/platform chemicals on a large scale. These fundamental molecular insights are expected to significantly benefit the future development of metal carboxylate-catalyzed hydrogenation processes of bio-renewable resources. CAs are also accessible by CO2 transformation, thus representing a useful way for contributing carbon neutral/recyclable society and SDGs.
Perspectives
The discovery should be further applicable to other homogeneous hydrogenation catalysts based on both base- and precious metals, as well as both low- and high-valent metal species. In fact, (PPP)Co(II) and (PPP)Ru(II) catalysts are proposed by in silico calculations to use similar [M(OCOR)]+ species for hydrogenation of CAs. (PP)Re(V) also seems to be adopting a [Re(OCOR)Hn]+ structure as catalytically active species (Sci. Rep. 2017)!
Professor Susumu SAITO
Nagoya Univ
Read the Original
This page is a summary of: Cationic mononuclear ruthenium carboxylates as catalyst prototypes for self-induced hydrogenation of carboxylic acids, Nature Communications, August 2015, Nature,
DOI: 10.1038/ncomms9140.
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