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

^*Corresponding author for this work

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

81 Scopus citations

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
State	Published - 20 Jan 2020
Externally published	Yes

Keywords

acidity of support
biomass conversion
carbon modification
electrocatalytic hydrogenation
nanocatalysis

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10.1002/anie.201912241

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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

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title = "Electrochemically Tunable Proton-Coupled Electron Transfer in Pd-Catalyzed Benzaldehyde Hydrogenation",

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.",

keywords = "acidity of support, biomass conversion, carbon modification, electrocatalytic hydrogenation, nanocatalysis",

author = "Katherine Koh and Udishnu Sanyal and Lee, \{Mal Soon\} and Guanhua Cheng and Miao Song and Glezakou, \{Vassiliki Alexandra\} and Yue Liu and Dongsheng Li and Roger Rousseau and Guti{\'e}rrez, \{Oliver Y.\} and Abhijeet Karkamkar and Miroslaw Derewinski and Lercher, \{Johannes A.\}",

note = "Publisher Copyright: {\textcopyright} 2020 The Authors. Published by Wiley-VCH Verlag GmbH \& Co. KGaA.",

year = "2020",

month = jan,

day = "20",

doi = "10.1002/anie.201912241",

language = "英语",

volume = "59",

pages = "1501--1505",

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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

TY - JOUR

T1 - Electrochemically Tunable Proton-Coupled Electron Transfer in Pd-Catalyzed Benzaldehyde Hydrogenation

AU - Koh, Katherine

AU - Sanyal, Udishnu

AU - Lee, Mal Soon

AU - Cheng, Guanhua

AU - Song, Miao

AU - Glezakou, Vassiliki Alexandra

AU - Liu, Yue

AU - Li, Dongsheng

AU - Rousseau, Roger

AU - Gutiérrez, Oliver Y.

AU - Karkamkar, Abhijeet

AU - Derewinski, Miroslaw

AU - Lercher, Johannes A.

PY - 2020/1/20

Y1 - 2020/1/20

N2 - 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.

AB - 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.

KW - acidity of support

KW - biomass conversion

KW - carbon modification

KW - electrocatalytic hydrogenation

KW - nanocatalysis

UR - https://www.scopus.com/pages/publications/85076411293

U2 - 10.1002/anie.201912241

DO - 10.1002/anie.201912241

M3 - 文章

C2 - 31634416

AN - SCOPUS:85076411293

SN - 1433-7851

VL - 59

SP - 1501

EP - 1505

JO - Angewandte Chemie - International Edition

JF - Angewandte Chemie - International Edition

IS - 4

ER -

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

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