Electrochemically Tunable Proton-Coupled Electron Transfer in Pd-Catalyzed Benzaldehyde Hydrogenation

Katherine Koh, Udishnu Sanyal, Mal Soon Lee, Guanhua Cheng, Miao Song, Vassiliki Alexandra Glezakou, Yue Liu, Dongsheng Li, Roger Rousseau, Oliver Y. Gutiérrez, Abhijeet Karkamkar, Miroslaw Derewinski, Johannes A. Lercher

Research output: Contribution to journalArticle

Abstract

Acid functionalization of a carbon support allows to enhance the electrocatalytic activity of Pd to hydrogenate benzaldehyde to benzyl alcohol proportional to the concentration of Brønsted-acid sites. In contrast, the hydrogenation rate is not affected when H2 is used as a reduction equivalent. The different responses to the catalyst properties are shown to be caused by differences in the hydrogenation mechanism between the electrochemical and the H2-induced hydrogenation pathways. The enhancement of electrocatalytic reduction is realized by the participation of support-generated hydronium ions in the proximity of the metal particles.

Original languageEnglish
JournalAngewandte Chemie - International Edition
DOIs
Publication statusAccepted/In press - Jan 1 2019

Fingerprint

Hydrogenation
Protons
Electrons
Benzyl Alcohol
Acids
Alcohols
Carbon
Metals
Catalysts
Ions
benzaldehyde
hydronium ion

Keywords

  • acidity of support
  • biomass conversion
  • carbon modification
  • electrocatalytic hydrogenation
  • nanocatalysis

ASJC Scopus subject areas

  • Catalysis
  • Chemistry(all)

Cite this

Electrochemically Tunable Proton-Coupled Electron Transfer in Pd-Catalyzed Benzaldehyde Hydrogenation. / Koh, Katherine; Sanyal, Udishnu; Lee, Mal Soon; Cheng, Guanhua; Song, Miao; Glezakou, Vassiliki Alexandra; Liu, Yue; Li, Dongsheng; Rousseau, Roger; Gutiérrez, Oliver Y.; Karkamkar, Abhijeet; Derewinski, Miroslaw; Lercher, Johannes A.

In: Angewandte Chemie - International Edition, 01.01.2019.

Research output: Contribution to journalArticle

Koh, K, Sanyal, U, Lee, MS, Cheng, G, Song, M, Glezakou, VA, Liu, Y, Li, D, Rousseau, R, Gutiérrez, OY, Karkamkar, A, Derewinski, M & Lercher, JA 2019, 'Electrochemically Tunable Proton-Coupled Electron Transfer in Pd-Catalyzed Benzaldehyde Hydrogenation', Angewandte Chemie - International Edition. https://doi.org/10.1002/anie.201912241
Koh, Katherine ; Sanyal, Udishnu ; Lee, Mal Soon ; Cheng, Guanhua ; Song, Miao ; Glezakou, Vassiliki Alexandra ; Liu, Yue ; Li, Dongsheng ; Rousseau, Roger ; Gutiérrez, Oliver Y. ; Karkamkar, Abhijeet ; Derewinski, Miroslaw ; Lercher, Johannes A. / Electrochemically Tunable Proton-Coupled Electron Transfer in Pd-Catalyzed Benzaldehyde Hydrogenation. In: Angewandte Chemie - International Edition. 2019.
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