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Electrochemical de-alloying synthesis of porous AuTiCeOx/NC cyclohexene hydrogenation SPE membrane electrode by combination method

  • Yueming Shang,
  • Yunhao Feng,
  • Liangming Duan,
  • Xudong Li,
  • Huaihang Fan,
  • Shaqin Wang,
  • Xinying Zhuang,
  • Bin Yang

摘要

High-performance hydrogenation catalysts are crucial for integrating hydrogen production and storage in organic/water systems, as well as for CO2 electrocatalytic reduction reactions. In this study, ion beam sputtering, coupled electrochemical de-alloying, and hot pressing have been employed to fabricate an SPE membrane electrode containing porous AuTiCeOx/NC. Characterization techniques were utilized to analyze and discuss the phase composition, surface morphology, components, exposed crystal faces, and their relationship with the catalytic efficiency and reaction stability of the Au-based SPE membrane electrode during the hydrogenation of cyclohexene. The results revealed that the membrane electrode carrier is composed of hexagonal phase C3N4, the Au-based catalyst possesses tetragonal Au2Ti and face-centered cubic Au phases, and Ce exists as amorphous ceria at the grain boundary; electrochemical de-alloying treatment yielded uniform elemental distribution and mesopores with an average pore size of < 10 nm; the binding energy of Au's 4f reduced by 0.17 eV, the Au–Au distance decreased the interplanar spacings of Au2Ti {112} and {103} shrank by approximately 6.8% and 5.8%, respectively, and a new high-index surface (105) emerged; the cyclohexane generation rate and the current efficiency in the hydrogenation reaction of cyclohexene increased by 7.92% and 14.14% respectively.