Influence of the catalyst surface chemistry on the electrochemical self-coupling of biomass-derived benzaldehyde into hydrobenzoin
Gong, Li (Universitat de Barcelona)
Zhao, Shiling (Lanzhou University of Technology)
Yu, Jing (Institut Català de Nanociència i Nanotecnologia)
Li, Junshan (Chengdu University)
Arbiol i Cobos, Jordi (Institut Català de Nanociència i Nanotecnologia)
Kallio, Tanja (Aalto University School of Chemical Engineering)
Calcabrini, Mariano (IST Austria)
Martínez-Alanis, Paulina R. (Institut de Recerca en Energia de Catalunya)
Ibáñez, Maria (IST Austria)
Cabot i Codina, Andreu (Institut de Recerca en Energia de Catalunya)

Data:	2024
Resum:	The electroreduction of biomass-derived benzaldehyde (BZH) provides a potentially cost-effective route to produce benzyl alcohol (BA). This reaction competes with the electrochemical self-coupling of BZH to hydrobenzoin (HDB), which holds significance as a biofuel. Herein, we demonstrate the selectivity towards one or the other product strongly depends on the surface chemistry of the catalyst, specifically on its ability to adsorb hydrogen, as showcased with Cu2S electrocatalysts. We particularly analyze the effect of surface ligands, oleylamine (OAm), on the selective conversion of BZH to BA or HDB. The effect of the electrode potential, electrolyte pH, and temperature are studied. Results indicate that bare Cu2S exhibits higher selectivity towards BA, while OAm-capped Cu2S promotes HDB formation. This difference is explained by the competing adsorption of protons and BZH. During the BZH electrochemical conversion, electrons first transfer to the C in the C[double bond, length as m-dash]O group to form a ketyl radical. Then the radical either couples with surrounding H+ to form BA or self-couple to produce HDB, depending on the H+ availability that is affected by the electrocatalyst surface properties. The presence of OAm inhibits the H adsorption on the electrode surface therefore reducing the formation of high-energy state Had and its combination with ketyl radicals to form BA. Instead, the presence of OAm promotes the outer sphere reaction for obtaining HDB.
Ajuts:	Agència de Gestió d'Ajuts Universitaris i de Recerca 2021/SGR-00457 Agencia Estatal de Investigación PID2020-116093RB-C43 Agencia Estatal de Investigación CEX2021-001214-S
Drets:	Aquest document està subjecte a una llicència d'ús Creative Commons. Es permet la reproducció total o parcial, la distribució, la comunicació pública de l'obra i la creació d'obres derivades, sempre que no sigui amb finalitats comercials, i sempre que es reconegui l'autoria de l'obra original.
Llengua:	Anglès
Document:	Article ; recerca ; Versió publicada
Publicat a:	Energy Advances, Vol. 3, Issue 9 (September 2024) , p. 2287-2294, ISSN 2753-1457

DOI: 10.1039/d4ya00334a

8 p, 1.4 MB

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