Understanding the Role of Metal and Molecular Structure on the Electrocatalytic Hydrogenation of Oxygenated Organic Compounds

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

Research output: Contribution to journalArticlepeer-review

20 Citations (Scopus)


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.

Original languageEnglish
Pages (from-to)9964-9972
Number of pages9
JournalACS Catalysis
Issue number11
Publication statusPublished - Nov 2019


  • H evolution
  • electrocatalytic hydrogenation
  • theoretical thermodynamic descriptors, Sabatier principle

ASJC Scopus subject areas

  • Catalysis
  • Chemistry(all)

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