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Title: Electrochemically tunable proton coupled electron transfer in Pd–catalyzed benzaldehyde hydrogenation

Abstract

Acid–functionalization of carbon support allows enhancing the electrocatalytic activity of Pd to hydrogenate benzaldehyde to benzyl alcohol in proportion to the concentration of Brønsted acid sites. In contrast, the hydrogenation rate is not affected when H 2 is used as reduction equivalent. The different response to catalyst properties is shown to be caused by differences in the hydrogenation mechanism between the electrochemical and the H 2 induced hydrogenation pathways. Here, the enhancement of the electrocatalytic reduction is realized by the participation of support generated hydronium ions at the perimeter of metal particles.

Authors:
 [1];  [1];  [1];  [2];  [1];  [1];  [2];  [1];  [1];  [1];  [1];  [3];  [4]
  1. Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
  2. TU Munchen, Garching (Germany)
  3. Pacific Northwest National Lab. (PNNL), Richland, WA (United States); TU Munchen, Garching (Germany)
  4. Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Polish Academy of Sciences, Cracow (Poland)
Publication Date:
Research Org.:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1576964
Report Number(s):
PNNL-SA-144918
Journal ID: ISSN 0044-8249
Grant/Contract Number:  
AC05-76RL01830
Resource Type:
Accepted Manuscript
Journal Name:
Angewandte Chemie
Additional Journal Information:
Journal Volume: 132; Journal Issue: 4; Journal ID: ISSN 0044-8249
Publisher:
German Chemical Society
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; carbon modification; acidity of support; nanocatalysts; electrocatalytic hydrogenation; biomass conversion

Citation Formats

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, Lercher, Johannes A., and Derewinski, Miroslaw. Electrochemically tunable proton coupled electron transfer in Pd–catalyzed benzaldehyde hydrogenation. United States: N. p., 2019. Web. doi:10.1002/ange.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, Lercher, Johannes A., & Derewinski, Miroslaw. Electrochemically tunable proton coupled electron transfer in Pd–catalyzed benzaldehyde hydrogenation. United States. doi:10.1002/ange.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, Lercher, Johannes A., and Derewinski, Miroslaw. Mon . "Electrochemically tunable proton coupled electron transfer in Pd–catalyzed benzaldehyde hydrogenation". United States. doi:10.1002/ange.201912241. https://www.osti.gov/servlets/purl/1576964.
@article{osti_1576964,
title = {Electrochemically tunable proton coupled electron transfer in Pd–catalyzed benzaldehyde hydrogenation},
author = {Koh, Katherine and Sanyal, Udishnu and Lee, Mal -Soon and Cheng, Guanhua and Song, Miao and Glezakou, Vassiliki -Alexandra and Liu, Yue and Li, Dongsheng and Rousseau, Roger and Gutiérrez, Oliver Y. and Karkamkar, Abhijeet and Lercher, Johannes A. and Derewinski, Miroslaw},
abstractNote = {Acid–functionalization of carbon support allows enhancing the electrocatalytic activity of Pd to hydrogenate benzaldehyde to benzyl alcohol in proportion to the concentration of Brønsted acid sites. In contrast, the hydrogenation rate is not affected when H 2 is used as reduction equivalent. The different response to catalyst properties is shown to be caused by differences in the hydrogenation mechanism between the electrochemical and the H 2 induced hydrogenation pathways. Here, the enhancement of the electrocatalytic reduction is realized by the participation of support generated hydronium ions at the perimeter of metal particles.},
doi = {10.1002/ange.201912241},
journal = {Angewandte Chemie},
number = 4,
volume = 132,
place = {United States},
year = {2019},
month = {10}
}

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