Highly efficient immobilized PN3P-pincer iridium catalyst for dehydrogenation of neat formic acid.
In: Applied Catalysis B: Environmental, Jg. 342 (2024-03-01), S. N.PAG
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Zugriff:
Formic acid (FA) has been well recognized as one of the most promising hydrogen carriers. The dehydrogenation of the FA could offer an efficient process to on-demand hydrogen generation with a suitable catalyst. Homogeneous catalysts have demonstrated superior activity and selectivity compared to traditional heterogeneous catalysis. However, the latter is preferred for large-scale applications. By incorporating the homogeneous organometallic complex onto an appropriate support, the unique features of both types of catalysts can be combined and utilized effectively. Herein, we synthesized an immobilized PN3P-Ir pincer catalyst (2) supported onto KCC-1, a 3D fibrous silica nanosphere that exhibits a high surface area and contains a tetracoordinate aluminum site. To reduce the use of volatile additives, the choice of cesium formate (CsO 2 CH) was found to be crucial as at 80–90 °C, CsO 2 CH could act as a reaction medium and serve as basic additive. Remarkable reactivities under neat conditions were achieved with a TOF of 13,290 h-1 and a TON of up to 540,000. The comparative study indicates a significant improvement of 2 from its homogenous counterpart, PN3P-IrH 3 (1). Neat Formic Acid Dehydrogenation: The synthesized immobilized PN3P pincer iridium catalyst (2) showed remarkable reactivity under neat conditions to achieve a TOF of 13,290 h-1 and TON up to 540,000 compared to a homogenous PN3P pincer iridium catalyst (1). Cesium formate (CsO 2 CH) was found to act as a molten matrix and serve as both solvent and basic additive in the formic acid dehydrogenation. The overall study revealed that 2 shows superior activity, selectivity, and stability for the neat formic acid dehydrogenation. [Display omitted] • CsO 2 CH acts as both solvent and basic additive. • The larger negative charge on immobilized PN3P-Ir improves the formic acid dehydrogenation activity. [ABSTRACT FROM AUTHOR]
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Highly efficient immobilized PN3P-pincer iridium catalyst for dehydrogenation of neat formic acid.
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Autor/in / Beteiligte Person: | Alrais, Lujain ; Gholap, Sandeep Suryabhan ; Dutta, Indranil ; Abou-Hamad, Edy ; Chen, Benjamin W.J. ; Zhang, Jia ; Hedhili, Mohamed Nejib ; Basset, Jean-Marie ; Huang, Kuo-Wei |
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Zeitschrift: | Applied Catalysis B: Environmental, Jg. 342 (2024-03-01), S. N.PAG |
Veröffentlichung: | 2024 |
Medientyp: | academicJournal |
ISSN: | 0926-3373 (print) |
DOI: | 10.1016/j.apcatb.2023.123439 |
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