Boosting Hydrogen Release: Optimized C3N4-Supported Palladium Catalysts for Formic Acid Dehydrogenation

Carbon nitride, C3N4, was synthesized through thermal polycondensation of melamine with varying temperature and time conditions. This approach represents a cost-effective, straightforward, and environmentally friendly synthetic method with lower energy consumption to obtain hierarchically structured...

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Detalles Bibliográficos
Autores: Moreno, Antonio, Lobo, L., Martínez Tejada, L.M., Bobadilla, Luis F., Ivanova, Svetlana, Domínguez Leal, María Isabel, Centeno, Miguel Ángel
Tipo de recurso: artículo
Estado:Versión publicada
Fecha de publicación:2025
País:España
Institución:Consejo Superior de Investigaciones Científicas (CSIC)
Repositorio:DIGITAL.CSIC. Repositorio Institucional del CSIC
OAI Identifier:oai:digital.csic.es:10261/406042
Acceso en línea:http://hdl.handle.net/10261/406042
https://api.elsevier.com/content/abstract/scopus_id/105012605746
Access Level:acceso abierto
Palabra clave:CO2 Hydrogenation
Formic acid
Hydrogen economy
Melamine decomposition
Pd/C3N4
Descripción
Sumario:Carbon nitride, C3N4, was synthesized through thermal polycondensation of melamine with varying temperature and time conditions. This approach represents a cost-effective, straightforward, and environmentally friendly synthetic method with lower energy consumption to obtain hierarchically structured carbon nitride. The resulting materials were subjected to comprehensive characterization to analyze their crystalline structure, textural properties, composition, and light absorption characteristics. To evaluate their catalytic potential, the supports were impregnated with different loadings of palladium (1, 5, and 10 wt%) as the active phase and tested in the decomposition of formic acid for hydrogen production in liquid phase at mild conditions. This study revealed that the structure and composition of the C3N4 were highly dependent on the degree of polycondensation, which in turn was influenced by the temperature and the thermal synthesis process. The most promising catalytic performance was achieved with a support prepared by decomposing melamine at 650 °C for 4 h, followed by impregnation with 10 wt% Pd. Furthermore, a mechanistic study was conducted using operando DRIFTS-MS to explore the plausible catalytic pathways for synthesizing formic acid via CO2 hydrogenation using the aforementioned catalyst. This investigation highlights the potential of C3N4 as a support, further demonstrating its versatility in the circular economy of formic acid.