Photoelectrochemical alcohols oxidation over polymeric carbon nitride photoanodes with simultaneous H 2 production.

Autor: Karjule N; Department of Chemistry and Ilse Katz Institute for Nanoscale Science and Technology, Ben-Gurion University of the Negev Beer-Sheva 8410501 Israel mennysh@bgu.ac.il., Phatake RS; Department of Chemistry and Ilse Katz Institute for Nanoscale Science and Technology, Ben-Gurion University of the Negev Beer-Sheva 8410501 Israel mennysh@bgu.ac.il., Barzilai S; Department of Chemistry, Nuclear Research Centre-Negev P.O. Box 9001 Beer-Sheva 84910 Israel., Mondal B; Department of Chemistry and Ilse Katz Institute for Nanoscale Science and Technology, Ben-Gurion University of the Negev Beer-Sheva 8410501 Israel mennysh@bgu.ac.il., Azoulay A; Department of Chemistry and Ilse Katz Institute for Nanoscale Science and Technology, Ben-Gurion University of the Negev Beer-Sheva 8410501 Israel mennysh@bgu.ac.il., Shames AI; Department of Physics, Ben-Gurion University of the Negev Beer-Sheva 8410501 Israel., Volokh M; Department of Chemistry and Ilse Katz Institute for Nanoscale Science and Technology, Ben-Gurion University of the Negev Beer-Sheva 8410501 Israel mennysh@bgu.ac.il., Albero J; Instituto Universitario de Tecnología Química (ITQ), Consejo Superior de Investigaciones, Científicas (CSIC), Universitat Politècnica de València (UPV) Avda. de Los Narajos s/n Valencia 46022 Spain., García H; Instituto Universitario de Tecnología Química (ITQ), Consejo Superior de Investigaciones, Científicas (CSIC), Universitat Politècnica de València (UPV) Avda. de Los Narajos s/n Valencia 46022 Spain., Shalom M; Department of Chemistry and Ilse Katz Institute for Nanoscale Science and Technology, Ben-Gurion University of the Negev Beer-Sheva 8410501 Israel mennysh@bgu.ac.il.
Jazyk: angličtina
Zdroj: Journal of materials chemistry. A [J Mater Chem A Mater] 2022 Jul 25; Vol. 10 (31), pp. 16585-16594. Date of Electronic Publication: 2022 Jul 25 (Print Publication: 2022).
DOI: 10.1039/d2ta03660f
Abstrakt: The photoelectrochemical oxidation of organic molecules into valuable chemicals is a promising technology, but its development is hampered by the poor stability of photoanodic materials in aqueous solutions, low faradaic efficiency, low product selectivity, and a narrow working pH range. Here, we demonstrate the synthesis of value-added aldehydes and carboxylic acids with clean hydrogen (H 2 ) production in water using a photoelectrochemical cell based solely on polymeric carbon nitride (CN) as the photoanode. Isotope labeling measurements and DFT calculations reveal a preferential adsorption of benzyl alcohol and molecular oxygen to the CN layer, enabling fast proton abstraction and oxygen reduction, which leads to the synthesis of an aldehyde at the first step. Further oxidation affords the corresponding acid. The CN photoanode exhibits excellent stability (>40 h) and activity for the oxidation of a wide range of substituted benzyl alcohols with high yield, selectivity (up to 99%), and faradaic efficiency (>90%).
Competing Interests: There are no conflicts to declare.
(This journal is © The Royal Society of Chemistry.)
Databáze: MEDLINE
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