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:
-
- Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
- TU Munchen, Garching (Germany)
- Pacific Northwest National Lab. (PNNL), Richland, WA (United States); TU Munchen, Garching (Germany)
- Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Polish Academy of Sciences, Cracow (Poland)
- Publication Date:
- Research Org.:
- Pacific Northwest National Laboratory (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. https://doi.org/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. https://doi.org/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 = {Mon Oct 21 00:00:00 EDT 2019},
month = {Mon Oct 21 00:00:00 EDT 2019}
}
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