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

doi:10.1002/anie.201912241

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

Pacific Northwest National Laboratory

Research output: Contribution to journal › Article › peer-review

7 Citations (Scopus)

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 language	English
Pages (from-to)	1501-1505
Number of pages	5
Journal	Angewandte Chemie - International Edition
Volume	59
Issue number	4
DOIs	https://doi.org/10.1002/anie.201912241
Publication status	Published - Jan 20 2020

Keywords

acidity of support
biomass conversion
carbon modification
electrocatalytic hydrogenation
nanocatalysis

ASJC Scopus subject areas

Catalysis
Chemistry(all)

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Koh, K., Sanyal, U., Lee, M. S., Cheng, G., Song, M., Glezakou, V. A., Liu, Y., Li, D., Rousseau, R., Gutiérrez, O. Y., Karkamkar, A., Derewinski, M., & Lercher, J. A. (2020). Electrochemically Tunable Proton-Coupled Electron Transfer in Pd-Catalyzed Benzaldehyde Hydrogenation. Angewandte Chemie - International Edition, 59(4), 1501-1505. https://doi.org/10.1002/anie.201912241

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, Vol. 59, No. 4, 20.01.2020, p. 1501-1505.

Research output: Contribution to journal › Article › peer-review

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 2020, 'Electrochemically Tunable Proton-Coupled Electron Transfer in Pd-Catalyzed Benzaldehyde Hydrogenation', Angewandte Chemie - International Edition, vol. 59, no. 4, pp. 1501-1505. 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. 2020 ; Vol. 59, No. 4. pp. 1501-1505.

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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 Br{\o}nsted-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.",

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