Development and understanding of cobaloxime activity through electrochemical molecular catalyst screening

Literature Information

Publication Date 2014-02-06
DOI 10.1039/C4CP00453A
Impact Factor 3.676
Authors

David W. Wakerley, Erwin Reisner


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Abstract

Electrochemical molecular catalyst screening (EMoCS) has been developed. This technique allows fast analysis and identification of homogeneous catalytic species through tandem catalyst assembly and electrochemistry. EMoCS has been used to study molecular proton reduction catalysts made from earth abundant materials to improve their viability for water splitting systems. The efficacy of EMoCS is proven through investigation of cobaloxime proton reduction activity with respect to the axial ligand in aqueous solution. Over 20 axial ligands were analysed, allowing rapid identification of the most active catalysts. Structure–activity relationships showed that more electron donating pyridine ligands result in enhanced catalytic currents due to the formation of a more basic Co–H species. The EMoCS results were validated by isolating and assaying the most electroactive cobaloximes identified during screening. The most active catalyst, [CoIIICl(dimethyl glyoximato)2(4-methoxypyridine)], showed high electro- and photoactivity in both anaerobic and aerobic conditions in pH neutral aqueous solution.

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Source Journal

Physical Chemistry Chemical Physics

Physical Chemistry Chemical Physics
CiteScore: 5.5
Self-citation Rate: 10.3%
Articles per Year: 3036

Physical Chemistry Chemical Physics (PCCP) is an international journal co-owned by 19 physical chemistry and physics societies from around the world. This journal publishes original, cutting-edge research in physical chemistry, chemical physics and biophysical chemistry. To be suitable for publication in PCCP, articles must include significant innovation and/or insight into physical chemistry; this is the most important criterion that reviewers and Editors will judge against when evaluating submissions. The journal has a broad scope and welcomes contributions spanning experiment, theory, computation and data science. Topical coverage includes spectroscopy, dynamics, kinetics, statistical mechanics, thermodynamics, electrochemistry, catalysis, surface science, quantum mechanics, quantum computing and machine learning. Interdisciplinary research areas such as polymers and soft matter, materials, nanoscience, energy, surfaces/interfaces, and biophysical chemistry are welcomed if they demonstrate significant innovation and/or insight into physical chemistry. Joined experimental/theoretical studies are particularly appreciated when complementary and based on up-to-date approaches.

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