Enhanced Electrochemical Hydrogenation of Benzaldehyde to Benzyl Alcohol on Pd@Ni-MOF by Modifying the Adsorption Configuration
Gong, Li (Universitat de Barcelona)
Zhang, Chao Yue (Institut de Recerca en Energia de Catalunya)
Li, Junshan (Chengdu University. Institute for Advanced Study)
Montaña-Mora, Guillem (Universitat de Barcelona)
Botifoll, Marc (Institut Català de Nanociència i Nanotecnologia)
Guo, Tiezhu (Xi'an Jiaotong University. School of Electronic Science and Engineering)
Arbiol i Cobos, Jordi (Institut Català de Nanociència i Nanotecnologia)
Zhou, Jin Yuan (Lanzhou University. School of Physical Science & Technology)
Kallio, Tanja (Aalto University School of Chemical Engineering. Department of Chemistry and Materials Science)
Martínez-Alanis, Paulina R. (Institut de Recerca en Energia de Catalunya)
Cabot i Codina, Andreu (Institut de Recerca en Energia de Catalunya)

Date:	2024
Abstract:	Electrocatalytic hydrogenation (ECH) approaches under ambient temperature and pressure offer significant potential advantages over thermal hydrogenation processes but require highly active and efficient hydrogenation electrocatalysts. The performance of such hydrogenation electrocatalysts strongly depends not only on the active phase but also on the architecture and surface chemistry of the support material. Herein, Pd nanoparticles supported on a nickel metal-organic framework (MOF), Ni-MOF-74, are prepared, and their activity toward the ECH of benzaldehyde (BZH) in a 3 M acetate (pH 5. 2) aqueous electrolyte is explored. An outstanding ECH rate up to 283 μmol cm h with a Faradaic efficiency (FE) of 76% is reached. Besides, higher FEs of up to 96% are achieved using a step-function voltage. Materials Studio and density functional theory calculations show these outstanding performances to be associated with the Ni-MOF support that promotes H-bond formation, facilitates water desorption, and induces favorable tilted BZH adsorption on the surface of the Pd nanoparticles. In this configuration, BZH is bonded to the Pd surface by the carbonyl group rather than through the aromatic ring, thus reducing the energy barriers of the elemental reaction steps and increasing the overall reaction efficiency.
Grants:	Agencia Estatal de Investigación PID2022-136883OB-C22 European Commission 801342 Agència de Gestió d'Ajuts Universitaris i de Recerca 2021/SGR-00457 Agència de Gestió d'Ajuts Universitaris i de Recerca 2021/SGR-1581 Agencia Estatal de Investigación PID2020-116093RB-C43 Agencia Estatal de Investigación CEX2021-001214-S Agència de Gestió d'Ajuts Universitaris i de Recerca 2020/FI-00103
Rights:	Aquest material està protegit per drets d'autor i/o drets afins. Podeu utilitzar aquest material en funció del que permet la legislació de drets d'autor i drets afins d'aplicació al vostre cas. Per a d'altres usos heu d'obtenir permís del(s) titular(s) de drets.
Language:	Anglès
Document:	Article ; recerca ; Versió sotmesa a revisió
Subject:	Electrochemical hydrogenation ; Metal-organic-framework ; Palladium ; Benzaldehyde ; Benzyl alcohol
Published in:	ACS applied materials & interfaces, Vol. 16, Issue 6 (February 2024) , p. 6948-6957, ISSN 1944-8252

DOI: 10.1021/acsami.3c13920

Preprint 40 p, 3.0 MB

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Research literature > UAB research groups literature > Research Centres and Groups (research output) > Experimental sciences > Catalan Institute of Nanoscience and Nanotechnology (ICN2)
Articles > Research articles
Articles > Published articles