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 |
|---|---|
| Journal | Angewandte Chemie - International Edition |
| DOIs | |
| Publication status | Accepted/In press - Jan 1 2019 |
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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 journal › Article
}
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 - 2019/1/1
Y1 - 2019/1/1
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 - http://www.scopus.com/inward/record.url?scp=85076411293&partnerID=8YFLogxK
UR - http://www.scopus.com/inward/citedby.url?scp=85076411293&partnerID=8YFLogxK
U2 - 10.1002/anie.201912241
DO - 10.1002/anie.201912241
M3 - Article
AN - SCOPUS:85076411293
JO - Angewandte Chemie - International Edition
JF - Angewandte Chemie - International Edition
SN - 1433-7851
ER -