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Uranyl Salen-Type Complex as Co-catalyst for Electrocatalytic Oxidation of Ethanol

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Abstract

Direct ethanol fuel cells (DEFCs) are considered a viable alternative power source for both stationary and mobile applications. Obstacles to widespread use of DEFCs include the slow kinetics of ethanol electro-oxidation, which has been countered by using Pt-based electrocatalysts. Pt-based electrocatalysts are produced by partially or totally replacing the platinum alloys with other less expensive materials such as transition metal complexes. This study describes the synthesis and characterization of the electrochemical properties of a new uranyl complex, whose molecular structure has been previously elucidated by FTIR, elemental analysis (CHN), and 1H NMR. Its cyclic voltammogram indicates two reversible redox pairs at 0.69/0.56 V (E1/2 = 0.63 V) and 0.85/0.77 V (E1/2 = 0.81 V) vs. RHE, attributed to ligand processes such as two successive oxidations of phenolate to phenoxyl radicals. The use of UO2(3-OMe-t-salcn)H2O as catalyst for ethanol oxidation reaction in acidic media was also investigated via cyclic voltammetry and chronoamperometry. Six PtSn-based catalysts were produced by adjusting the molar ratio of the PtSn:UO2-complex. Direct scanning of the samples indicated that the peak-current density for the 6:1 PtSn/C:[UO2(3-OMe-t-salcn)H2O] catalyst was higher than that for mixed catalysts. Moreover, as compared to the pure PtSn catalyst, 6:1 PtSn/C:[UO2(3-OMe-t-salcn)H2O] exhibited better catalytic activity for ethanol electrooxidation; i.e., it decreased the onset potential during the oxidation of ethanol. Moreover, this catalyst exhibited peak-current densities (j) at 34.53 mA cm−2; i.e., ~ 5.2-fold that of PtSn/C. In addition, chronoamperometry data indicated higher catalytic activity at 0.6 V for PtSn/C:[UO2(3-OMe-t-salcn)H2O]-based catalysts.

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Acknowledgements

The authors would like to acknowledge Programa de Pós-Graduação em Ciência e Tecnologia para Recursos Amazônicos (PPGCTRA–UFAM), Programa de Pós-Graduação em Nanociência, Processos e Materiais Avançados (PPGNPMat–UFSC), Fundação de Amparo à Pesquisa do Estado do Amazonas–FAPEAM (process no. 005/2019), PROPESP/UFAM-CNPq (process no. 041/2016 and 008/2018), Fundação de Amparo à Pesquisa e Inovação do Estado de Santa Catarina–FAPESC (I. V. de F.—Grant no. 21/2021), Coordenação de Aperfeiçoamento de Pessoal de Nível Superior—Brasil (CAPES), and Conselho Nacional de Desenvolvimento Científico–CNPq.

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Authors and Affiliations

  1. Instituto de Ciências Exatas e Tecnologia, Universidade Federal do Amazonas, AM, Itacoatiara, Brazil

    Elizomar Medeiros Barbosa, Kaique Soares Souza, Pedro Henrique Siqueira de Oliveira, Ítalo Santos Costa & Elson Almeida Souza

  2. Departamento de Ciências Exatas e Educação, Universidade Federal de Santa Catarina, Rua João Pessoa 2514, SC, Blumenau, Brazil

    Igor Vinicius de França & José Wilmo da Cruz Jr.

  3. Departamento de Química, Universidade Federal de São Carlos, Rod. Washington Luiz, km 235, São Carlos, SP, Brazil

    Lucas dos Santos Mello & Edward Ralph Dockal

  4. Universidade Federal of Rio de Janeiro – Centro Multidisciplinar UFRJ Macaé – Instituto Multidisciplinar de Química, GEQBio: Grupo de Eletrocatálise, Fotoquímica Inorgânica e Química Bioinorgânica, CEP 27930-560, RJ, Macaé, Brazil

    Paulo José Sousa Maia

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  1. Elizomar Medeiros Barbosa
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Barbosa, E.M., Souza, K.S., de Oliveira, P.S. et al. Uranyl Salen-Type Complex as Co-catalyst for Electrocatalytic Oxidation of Ethanol. Electrocatalysis 13, 91–100 (2022). https://doi.org/10.1007/s12678-021-00697-0

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