Journal
ACS OMEGA
Volume 4, Issue 8, Pages 13454-13464Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsomega.9b01741
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Funding
- CSIRHRD Project [01(2921/18EMR-II)]
- DST-Inspire [IF160353]
- CUK
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Ruthenium-containing tetraphenylporphyrin (Ru-TPP) molecule was prepared, and the structural elucidation was confirmed using H-1 nuclear magnetic resonance (NMR), CHN, and mass spectral analyses. The incorporation of ruthenium ion into the cavities of the macromolecule was confirmed from the disappearance of the H-1 NMR signal, characteristic of the N-H bond (-2.72 ppm in TPP). The CHN and mass spectral analyses of the ligand and metallomacromolecules are consistent with the theoretically calculated values. The homogeneous Ru-TPP macromolecule is grafted on the surface of aminosilane-, diaminosilane-, and iodosilane-functionalized SBA-15 molecular sieves. The successful grafting of Ru-TPP on functionalized mesoporous molecular sieve materials was evident from low-angle powder X-ray diffraction, C-13 magic angle spinning NMR, and scanning electron microscopy-energy-dispersive X-ray analyses. The resultant homogeneous and heterogenized Ru-TPP catalysts were used for the utilization of carbon dioxide (CO2) under moderate reaction conditions. The homogeneous Ru-TPP catalyst showed first-order kinetics with respect to epoxide with the exclusive formation of cyclic carbonate (about 98%) and an activation energy of 16.07 kg/mol, which is much lower than some of the reported catalysts. Ru-TPP grafted on aminosilane-and iodosilane-functionalized materials showed better catalytic activity (above 90% conversion and 83-96% cyclic carbonate selectivity) and reusability for the chosen reaction.
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