abstract
This work unveils a route for a new generation of heterogeneous polyoxometalate (POMs) based catalysts associated to the preparation of hybrid materials as a triad of POMs, mesoporous silica (SBA-15) and microporous MOF structures (MOF-808). The prepared catalyst, PMo12@MOF-808@SBA-15, with the main active center the phosphomolybdic acid (PMo12), was successfully applied for the desulfurization of a multicomponent fuel. Its oxidative catalytic performance showed to be considerable superior to the isolated POM@MOF and able to be recycled for more catalytic cycles without active loss. The higher catalytic performance seems to be directly related with the preparation of a more amorphous MOF structure within the channels of SBA-15, in the presence of active POM guests. An unprecedented tri-hybrid material, PMo12@MOF-808@SBA-15, revealed a notable catalytic performance and robustness to desulfurize a multicomponent model fuel containing approximately 1500 ppm of sulfur. It demonstrated an enhanced activity and recyclability relatively to the parent's composites, PMo12@MOF-808 and PMo12@SBA-15. image
keywords
METAL-ORGANIC FRAMEWORK; MESOPOROUS SILICA; PERFORMANCE; UIO-66; MOF; CO2; HYDRODESULFURIZATION; OXIDESULFURIZATION; POLYOXOMOLYBDATE; SUPPORT
subject category
Chemistry
authors
Fernandes, SC; Leo, P; Santos-Vieira, I; de Castro, B; Cunha-Silva, L; Balula, SS
Groups
Projects
CICECO - Aveiro Institute of Materials (UIDB/50011/2020)
CICECO - Aveiro Institute of Materials (UIDP/50011/2020)
Associated Laboratory CICECO-Aveiro Institute of Materials (LA/P/0006/2020)
acknowledgements
This research work received financial support from Portuguese national funds (FCT/MCTES, Fundacao para a Ciencia e Tecnologia and Ministerio da Ciencia, Tecnologia e Ensino Superior) through through LAQV/REQUIMTE (Ref. UIDP/50006/2020 DOI 10.54499/UIDP/50006/2020; LA/P/0008/2020 DOI 10.54499/LA/P/0008/2020; UIDB/50006/2020 DOI 10.54499/UIDB/50006/2020). This work was partially developed within the scope of the project CICECO-Aveiro Institute of Materials, UIDB/50011/2020, UIDP/50011/2020 & LA/P/0006/2020, financed by national funds through the FCT/MCTES (PIDDAC). The position held by ISV (Ref. [197]_97_ARH-2018) was funded by national funds (OE), through FCT, I. P., in the scope of the framework contract foreseen in the numbers 4, 5 and 6 of article 23 of the Decree-Law 57/2016 of 29 August, changed by Law 57/2017 of 19 July. L. C. S. and S. S. B. thank FCT/MCTES for funding through the Individual Call to Scientific Employment Stimulus (Ref. CEECIND/00793/2018 and Ref. CEECIND/03877/2018, respectively). S. F. thanks FCT/MCTES and ESF (European Social Fund) through POCH (Programa Operacional Capital Humano) for her PhD grants (Refs. PRT/BD/154274/2023). P. L. thanks the Ministry of Universities for grant CAS21/00417.