Synthesis and applications of N-doped carbon supported Pd-based bimetallic nanoparticles by synergistic chemical and thermal modifications of mofs

• Autores: Jordan Santiago Martínez
• Directores de la Tesis: Jaime Mazarío Santa Pau (dir. tes.), Pascual Oña Burgos (dir. tes.), Antonio Eduardo Palomares Gimeno (tut. tes.)
• Lectura: En la Universitat Politècnica de València ( España ) en 2025
• Idioma: inglés
• Tribunal Calificador de la Tesis: Manuel Moliner Marín (presid.), José Solla Gullón (secret.), Montserrat Gómez Simón (voc.)
• Programa de doctorado: Programa de Doctorado en Química Sostenible por la Universidad de Castilla-La Mancha; la Universidad de Extremadura; la Universidad Jaume I de Castellón; la Universitat de València (Estudi General) y la Universitat Politècnica de València
• Calificación: Sobresaliente Cum Laude
• Materias:
  • Química
    • Química inorgánica
      • Metales
      • Estructura de los compuestos inorgánicos
    • Química orgánica
• Enlaces
  • Tesis en acceso abierto en: RiuNet
• Resumen

  • This thesis develops sustainable catalytic processes using advanced heterogeneous catalysts based on the preparation of MOF-derived composites for selective semi-hydrogenation of alkynes and electrochemical water-splitting applications. Precisely, new methods were followed to transform PdIn-MOF into N-doped carbon-supported nanoparticles. First, a combined chemical and thermal treatment afforded the PdIn-QT composite, which has been distinguished by its stability and structural control. The material was thoroughly compared to the material resulting from the traditional direct pyrolysis method. Then, the study demonstrates that the properties of nanoparticles and carbon can be improved by optimizing solvent polarity and the type of amines involved during the chemical transformation.

    Later, after the elaboration of the new PdCo, and PdMn MOF precursors, our newly developed MOF transformation strategy was applied. The resulting PdCo, PdMn, and PdIn-based catalysts were used in the selective hydrogenation of phenylacetylene. They showed excellent selectivity at quantitative conversion levels, with high stability. Among them, PdCo-QT showed excellent activity in continuous gas-phase processes, indicating its potential in industrial applications. Lastly, the first-row transition metal-based materials were tested as electrodes and showed competitive performance against benchmark catalysts in hydrogen and oxygen evolution reactions (HER and OER). Specifically, PdCo-QT showed highly efficient and stable performance, with great potential for sustainable water-splitting applications.

    In conclusion, this study reports on a new family of tunable catalysts suitable for both industrial catalysis and clean energy applications.