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Double Hydroxide Nanocatalysts for Urea Electrooxidation Engineered toward Environmentally Benign Products.
Yang, Yuwei; Yuwono, Jodie A; Whittaker, Todd; Ibáñez, Marc Manyé; Wang, Bingliang; Kim, Changmin; Borisevich, Albina Y; Chua, Stephanie; Prada, Jhair Pena; Wang, Xichu; Autran, Pierre-Olivier; Unocic, Raymond R; Dai, Liming; Holewinski, Adam; Bedford, Nicholas M.
Afiliación
  • Yang Y; School of Chemical Engineering, University of New South Wales, Sydney, NSW, 2052, Australia.
  • Yuwono JA; Australian Research Council Centre of Excellence in Carbon Science and Innovation, University of New South Wales, Sydney, NSW, 2052, Australia.
  • Whittaker T; School of Chemical Engineering, The University of Adelaide, Adelaide, SA, 5005, Australia.
  • Ibáñez MM; Department of Chemical and Biological Engineering, University of Colorado, Boulder, CO, 80309, USA.
  • Wang B; Renewable and Sustainable Energy Institute, University of Colorado, Boulder, CO, 80309, USA.
  • Kim C; Department of Chemical and Biological Engineering, University of Colorado, Boulder, CO, 80309, USA.
  • Borisevich AY; Renewable and Sustainable Energy Institute, University of Colorado, Boulder, CO, 80309, USA.
  • Chua S; School of Chemical Engineering, University of New South Wales, Sydney, NSW, 2052, Australia.
  • Prada JP; Australian Carbon Materials Centre (A-CMC), University of New South Wales, Sydney, NSW, 2052, Australia.
  • Wang X; School of Chemical Engineering, University of New South Wales, Sydney, NSW, 2052, Australia.
  • Autran PO; Australian Carbon Materials Centre (A-CMC), University of New South Wales, Sydney, NSW, 2052, Australia.
  • Unocic RR; Center for Nanophase Materials Sciences, Oak Ridge National Laboratory, Oak Ridge, TN, 37831, USA.
  • Dai L; School of Chemical Engineering, University of New South Wales, Sydney, NSW, 2052, Australia.
  • Holewinski A; School of Chemical Engineering, University of New South Wales, Sydney, NSW, 2052, Australia.
  • Bedford NM; School of Chemical Engineering, University of New South Wales, Sydney, NSW, 2052, Australia.
Adv Mater ; 36(35): e2403187, 2024 Aug.
Article en En | MEDLINE | ID: mdl-39003619
ABSTRACT
Recent advancements in the electrochemical urea oxidation reaction (UOR) present promising avenues for wastewater remediation and energy recovery. Despite progress toward optimized efficiency, hurdles persist in steering oxidation products away from environmentally unfriendly products, mostly due to a lack of understanding of structure-selectivity relationships. In this study, the UOR performance of Ni and Cu double hydroxides, which show marked differences in their reactivity and selectivity is evaluated. CuCo hydroxides predominantly produce N2, reaching a current density of 20 mA cmgeo -2 at 1.04 V - 250 mV less than NiCo hydroxides that generate nitrogen oxides. A collection of in-situ spectroscopies and scattering experiments reveal a unique in situ generated Cu(2-x)+-OO-• active sites in CuCo, which initiates nucleophilic substitution of NH2 from the amide, leading to N-N coupling between *NH on Co and Cu. In contrast, the formation of nitrogen oxides on NiCo is primarily attributed to the presence of high-valence Ni3+ and Ni4+, which facilitates N-H activation. This process, in conjunction with the excessive accumulation of OH- ions on Jahn-Teller (JT) distorted Co sites, leads to the generation of NO2 - as the primary product. This work underscores the importance of catalyst composition and structural engineering in tailoring innocuous UOR products.
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Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: Adv Mater Asunto de la revista: BIOFISICA / QUIMICA Año: 2024 Tipo del documento: Article País de afiliación: Australia Pais de publicación: Alemania
Texto completo
Añadir a Mi BVS
Imprimir
XML
PubMed Links
Buscar en Google

Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: Adv Mater Asunto de la revista: BIOFISICA / QUIMICA Año: 2024 Tipo del documento: Article País de afiliación: Australia Pais de publicación: Alemania