Understanding the role of metal and molecular structure on the electrocatalytic hydrogenation of oxygenated organic compounds

Lopez-Ruiz, Juan A.; Andrews, Evan M.; Akhade, Sneha A.; Lee, Mal Soon; Koh, Katherine; Sanyal, Udishnu; Yuk, Simuck F.; Karkamkar, Abhijeet J.; Derewinski, Miroslaw A.; Holladay, Johnathan E.; Glezakou, Vassiliki-Alexandra; Rousseau, Roger J.; Gutierrez-Tinoco, Oliver Y.; Holladay, Jamelyn D.

doi:10.1021/acscatal.9b02921

Title: Understanding the role of metal and molecular structure on the electrocatalytic hydrogenation of oxygenated organic compounds

Journal Article · Thu Sep 19 00:00:00 EDT 2019 · ACS Catalysis

DOI:https://doi.org/10.1021/acscatal.9b02921· OSTI ID:1576758

^[1]; Andrews, Evan M. ^[1]; Akhade, Sneha A. ^[2];

^[1]; Koh, Katherine ^[1]; Sanyal, Udishnu ^[1]; Yuk, Simuck F. ^[1];

^[1]; Derewinski, Miroslaw A. ^[3]; Holladay, Johnathan E. ^[1];

^[1]; Rousseau, Roger J. ^[1];

^[1]; Holladay, Jamelyn D. ^[1]

BATTELLE (PACIFIC NW LAB)
LAWRENCE LIVERMORE
VISITORS

Electrocatalytic hydrogenation is increasingly studied as an alternative to integrate the use of recycled carbon feedstocks with renewable energy sources. However, the abundant empiric observations available have not been correlated with fundamental properties of substrates and catalysts. In this study, we investigated electrocatalytic hydrogenation of a homologues series of carboxylic acids, ketones, phenolics, and aldehydes on a variety of metals (Pd, Rh, Ru, Cu, Ni, Zn, and Co). We found that the rates of carbonyl reduction in aldehydes correlate with the corresponding binding energies between the aldehydes and the metals according to the Sabatier principle. That is, the highest rates are obtained at intermediate binding energies. The rates of H2 evolution that occur in parallel to hydrogenation also correlate with the H-metal binding energies, following the same volcano-type behavior. Within the boundaries of this model (e.g., compounds reactive at room temperature and without important steric effects over the carbonyl group), the reported correlations help to explain the complex trends derived from the experimental observations, allowing for the correlation of rates with binding energies and the differentiation of mechanistic routes.

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Research Organization:: Pacific Northwest National Lab. (PNNL), Richland, WA (United States)

Sponsoring Organization:: USDOE National Nuclear Security Administration (NNSA); USDOE Laboratory Directed Research and Development (LDRD) Program

DOE Contract Number:: AC05-76RL01830; AC52-07NA27344

OSTI ID:: 1576758

Report Number(s):: PNNL-SA-145115

Journal Information:: ACS Catalysis, Vol. 9, Issue 11

Country of Publication:: United States

Language:: English

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