Electrochemical reforming of ethanol with acetate Co-Production on nickel cobalt selenide nanoparticles

The energy efficiency of water electrolysis is limited by the sluggish reaction kinetics of the anodic oxygen evolution reaction (OER). To overcome this limitation, OER can be replaced by a less demanding oxidation reaction, which in the ideal scenario could be even used to generate additional valua...

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Detalles Bibliográficos
Autores: Li, Junshan|||0000-0002-1482-1972, Wang, Xiang, Xing, Congcong|||0000-0001-7674-6720, Li, Luming, Mu, Shijia, Han, Xu|||0000-0001-8319-8830, He, Ren|||0000-0003-3712-5539, Liang, Zhifu, Martínez-Alanis, Paulina R.|||0000-0003-3675-4472, Yi, Yunan, Wu, Qianbao|||0000-0003-3236-8582, Pan, Huiyan, Arbiol i Cobos, Jordi|||0000-0002-0695-1726, Cui, Chunhua|||0000-0002-2774-1576, Zhang, Yu|||0000-0002-0332-0013, Cabot i Codina, Andreu|||0000-0002-7533-3251
Tipo de recurso: artículo
Fecha de publicación:2022
País:España
Institución:Universitat Autònoma de Barcelona
Repositorio:Dipòsit Digital de Documents de la UAB
Idioma:inglés
OAI Identifier:oai:ddd.uab.cat:270833
Acceso en línea:https://ddd.uab.cat/record/270833
https://dx.doi.org/urn:doi:10.1016/j.cej.2022.135817
Access Level:acceso abierto
Palabra clave:Electrocatalysis
Ethanol reforming
Hydrogen production
Selenide nanoparticle
Acetate
Descripción
Sumario:The energy efficiency of water electrolysis is limited by the sluggish reaction kinetics of the anodic oxygen evolution reaction (OER). To overcome this limitation, OER can be replaced by a less demanding oxidation reaction, which in the ideal scenario could be even used to generate additional valuable chemicals. Herein, we focus on the electrochemical reforming of ethanol in alkaline media to generate hydrogen at a Pt cathode and acetate as a co-product at a NiCoSe anode. We first detail the solution synthesis of a series of NiCoSe electrocatalysts. By adjusting the Ni/Co ratio, the electrocatalytic activity and selectivity for the production of acetate from ethanol are optimized. Best performances are obtained at low substitutions of Ni by Co in the cubic NiSe phase. Density function theory reveals that the Co substitution can effectively enhance the ethanol adsorption and decrease the energy barrier for its first step dehydrogenation during its conversion to acetate. However, we experimentally observe that too large amounts of Co decrease the ethanol-to-acetate Faradaic efficiency from values above 90% to just 50 %. At the optimized composition, the NiCoSe electrode delivers a stable chronoamperometry current density of up to 45 mA cm, corresponding to 1.2 A g, in a 1 M KOH + 1 M ethanol solution, with a high ethanol-to-acetate Faradaic efficiency of 82.2% at a relatively low potential, 1.50 V vs. RHE, and with an acetate production rate of 0.34 mmol cm-2 h-1.