Substrate diffusion electrodes allow for the electrochemical hydrogenation of concentrated alkynol substrate feeds
Summary: Electrosynthesis has the potential to revolutionize industrial organic synthesis sustainably and efficiently. However, high cell voltages and low stability often arise due to solubility issues with organic solvents, while protic electrolytes restrict substrate options. We present a three-la...
Saved in:
| Main Authors: | , , , , , , , |
|---|---|
| Format: | Article |
| Language: | English |
| Published: |
Elsevier
2025-02-01
|
| Series: | iScience |
| Subjects: | |
| Online Access: | http://www.sciencedirect.com/science/article/pii/S2589004225000483 |
| Tags: |
Add Tag
No Tags, Be the first to tag this record!
|
| _version_ | 1832586294413230080 |
|---|---|
| author | Jonas Wolf Fatima Shahrour Zafer Acar Kevinjeorjios Pellumbi Julian Tobias Kleinhaus Leon Wickert Ulf-Peter Apfel Daniel Siegmund |
| author_facet | Jonas Wolf Fatima Shahrour Zafer Acar Kevinjeorjios Pellumbi Julian Tobias Kleinhaus Leon Wickert Ulf-Peter Apfel Daniel Siegmund |
| author_sort | Jonas Wolf |
| collection | DOAJ |
| description | Summary: Electrosynthesis has the potential to revolutionize industrial organic synthesis sustainably and efficiently. However, high cell voltages and low stability often arise due to solubility issues with organic solvents, while protic electrolytes restrict substrate options. We present a three-layered electrode design that enables the use of concentrated to neat substrate feeds. This design separates the organic substrate from the aqueous electrolyte using layers with varying porosity and hydrophilicity, ensuring precise reactant transport to the catalyst layer while minimizing substrate and electrolyte crossover. We demonstrate its effectiveness by semi-hydrogenating three alkynols with different hydrophobicities. For the semi-hydrogenation of 3-methyl-1-pentyn-3-ol in pure form, we achieved 65% faradaic efficiency at 80 mA cm−2. Additionally, semi-hydrogenation of neat 2-methyl-3-butyn-2-ol on palladium showed a faradaic efficiency for semi-hydrogenation of 36%, that was stable for 22 h. This design could be pioneering the electrochemical valorization of neat substrates, reducing the need for extensive downstream processing. |
| format | Article |
| id | doaj-art-be44e914ef954f37adea443dd5134372 |
| institution | Kabale University |
| issn | 2589-0042 |
| language | English |
| publishDate | 2025-02-01 |
| publisher | Elsevier |
| record_format | Article |
| series | iScience |
| spelling | doaj-art-be44e914ef954f37adea443dd51343722025-01-26T05:04:35ZengElsevieriScience2589-00422025-02-01282111789Substrate diffusion electrodes allow for the electrochemical hydrogenation of concentrated alkynol substrate feedsJonas Wolf0Fatima Shahrour1Zafer Acar2Kevinjeorjios Pellumbi3Julian Tobias Kleinhaus4Leon Wickert5Ulf-Peter Apfel6Daniel Siegmund7Department of Electrocatalysis, Fraunhofer Institute for Environmental, Safety and Energy Technology UMSICHT, 46047 Oberhausen, GermanyDepartment of Electrocatalysis, Fraunhofer Institute for Environmental, Safety and Energy Technology UMSICHT, 46047 Oberhausen, GermanyDepartment of Electrocatalysis, Fraunhofer Institute for Environmental, Safety and Energy Technology UMSICHT, 46047 Oberhausen, GermanyDepartment of Electrocatalysis, Fraunhofer Institute for Environmental, Safety and Energy Technology UMSICHT, 46047 Oberhausen, GermanyTechnical Electrochemistry, Faculty of Chemistry and Biochemistry, Ruhr University Bochum, 44801 Bochum, GermanyTechnical Electrochemistry, Faculty of Chemistry and Biochemistry, Ruhr University Bochum, 44801 Bochum, GermanyDepartment of Electrocatalysis, Fraunhofer Institute for Environmental, Safety and Energy Technology UMSICHT, 46047 Oberhausen, Germany; Technical Electrochemistry, Faculty of Chemistry and Biochemistry, Ruhr University Bochum, 44801 Bochum, Germany; Corresponding authorDepartment of Electrocatalysis, Fraunhofer Institute for Environmental, Safety and Energy Technology UMSICHT, 46047 Oberhausen, Germany; Technical Electrochemistry, Faculty of Chemistry and Biochemistry, Ruhr University Bochum, 44801 Bochum, Germany; Corresponding authorSummary: Electrosynthesis has the potential to revolutionize industrial organic synthesis sustainably and efficiently. However, high cell voltages and low stability often arise due to solubility issues with organic solvents, while protic electrolytes restrict substrate options. We present a three-layered electrode design that enables the use of concentrated to neat substrate feeds. This design separates the organic substrate from the aqueous electrolyte using layers with varying porosity and hydrophilicity, ensuring precise reactant transport to the catalyst layer while minimizing substrate and electrolyte crossover. We demonstrate its effectiveness by semi-hydrogenating three alkynols with different hydrophobicities. For the semi-hydrogenation of 3-methyl-1-pentyn-3-ol in pure form, we achieved 65% faradaic efficiency at 80 mA cm−2. Additionally, semi-hydrogenation of neat 2-methyl-3-butyn-2-ol on palladium showed a faradaic efficiency for semi-hydrogenation of 36%, that was stable for 22 h. This design could be pioneering the electrochemical valorization of neat substrates, reducing the need for extensive downstream processing.http://www.sciencedirect.com/science/article/pii/S2589004225000483Chemical engineeringElectrochemistryEngineering |
| spellingShingle | Jonas Wolf Fatima Shahrour Zafer Acar Kevinjeorjios Pellumbi Julian Tobias Kleinhaus Leon Wickert Ulf-Peter Apfel Daniel Siegmund Substrate diffusion electrodes allow for the electrochemical hydrogenation of concentrated alkynol substrate feeds iScience Chemical engineering Electrochemistry Engineering |
| title | Substrate diffusion electrodes allow for the electrochemical hydrogenation of concentrated alkynol substrate feeds |
| title_full | Substrate diffusion electrodes allow for the electrochemical hydrogenation of concentrated alkynol substrate feeds |
| title_fullStr | Substrate diffusion electrodes allow for the electrochemical hydrogenation of concentrated alkynol substrate feeds |
| title_full_unstemmed | Substrate diffusion electrodes allow for the electrochemical hydrogenation of concentrated alkynol substrate feeds |
| title_short | Substrate diffusion electrodes allow for the electrochemical hydrogenation of concentrated alkynol substrate feeds |
| title_sort | substrate diffusion electrodes allow for the electrochemical hydrogenation of concentrated alkynol substrate feeds |
| topic | Chemical engineering Electrochemistry Engineering |
| url | http://www.sciencedirect.com/science/article/pii/S2589004225000483 |
| work_keys_str_mv | AT jonaswolf substratediffusionelectrodesallowfortheelectrochemicalhydrogenationofconcentratedalkynolsubstratefeeds AT fatimashahrour substratediffusionelectrodesallowfortheelectrochemicalhydrogenationofconcentratedalkynolsubstratefeeds AT zaferacar substratediffusionelectrodesallowfortheelectrochemicalhydrogenationofconcentratedalkynolsubstratefeeds AT kevinjeorjiospellumbi substratediffusionelectrodesallowfortheelectrochemicalhydrogenationofconcentratedalkynolsubstratefeeds AT juliantobiaskleinhaus substratediffusionelectrodesallowfortheelectrochemicalhydrogenationofconcentratedalkynolsubstratefeeds AT leonwickert substratediffusionelectrodesallowfortheelectrochemicalhydrogenationofconcentratedalkynolsubstratefeeds AT ulfpeterapfel substratediffusionelectrodesallowfortheelectrochemicalhydrogenationofconcentratedalkynolsubstratefeeds AT danielsiegmund substratediffusionelectrodesallowfortheelectrochemicalhydrogenationofconcentratedalkynolsubstratefeeds |