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.

doi:10.1002/anie.201912241

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 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.

Authors:

Koh, Katherine ^[1];

^[1];

^[1]; Cheng, Guanhua ^[2]; Song, Miao ^[1];

^[1]; Liu, Yue ^[2];

^[1];

^[1]; Derewinski, Miroslaw ^[3];

^[4]

Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Technische Univ. Munchen, Garching (Germany)
Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Polish Academy of Sciences (Poland)
Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Technische Univ. Munchen, Garching (Germany)

Publication Date:: Mon Oct 21 00:00:00 EDT 2019

Research Org.:: Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Sponsoring Org.:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences, and Biosciences Division; German Research Foundation (DFG)

OSTI Identifier:: 1614995

Report Number(s):: PNNL-SA-150488
Journal ID: ISSN 1433-7851

Grant/Contract Number:: AC05-76RL01830

Resource Type:: Accepted Manuscript

Journal Name:: Angewandte Chemie (International Edition)

Additional Journal Information:: Journal Name: Angewandte Chemie (International Edition); Journal Volume: 59; Journal Issue: 4; Journal ID: ISSN 1433-7851

Publisher:: Wiley

Country of Publication:: United States

Language:: English

Subject:: 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; acidity of support; biomass conversion; carbon modification; electrocatalytic hydrogenation; nanocatalysis

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, Derewinski, Miroslaw, and Lercher, Johannes A. Electrochemically Tunable Proton-Coupled Electron Transfer in Pd-Catalyzed Benzaldehyde Hydrogenation.  United States: N. p., 2019. 
Web.  doi:10.1002/anie.201912241.

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                    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.  United States.  https://doi.org/10.1002/anie.201912241

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                    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, and Lercher, Johannes A. Mon .  
"Electrochemically Tunable Proton-Coupled Electron Transfer in Pd-Catalyzed Benzaldehyde Hydrogenation".  United States.  https://doi.org/10.1002/anie.201912241.  https://www.osti.gov/servlets/purl/1614995.

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@article{osti_1614995,

  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 Derewinski, Miroslaw and Lercher, Johannes A.},

  abstractNote = {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.},

  doi          = {10.1002/anie.201912241},

  journal      = {Angewandte Chemie (International Edition)},

  number       = 4,

  volume       = 59,

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

Abstract

Citation Formats

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Some aspects of the surface chemistry of carbon blacks and other carbons journal, January 1994

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Some aspects of the surface chemistry of carbon blacks and other carbons
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