Exploring novel catalytic transformations of bioalcohols and mechanistic studies using Ru-PNP complexes

Zhenwei Ni

Research output: Book/ReportPh.D. thesis

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Abstract

The large-scale development and supply of renewable, clean, and green energy to fulfill the needs of our society is an important task in the context of a green transition. The study of biomassrelated alcohols plays an essential role in new energy exploration. In this thesis, three projects on the transformations of bioalcohols by using homogeneous catalyzed processes in presence of pincer PNP complexes, which are both valuable in academia and industry, are discussed.
Of these results, I disclosed an unprecedented reaction pathway for ethanol upgrading that leads to the production of secondary alcohols rather than the typical primary alcohols, employing Ru-PNP complexes as the catalyst under mild reaction conditions. Interestingly, the selectivity of the reaction pathway between secondary and primary alcohols was modulated by simply tuning the bulkiness of peripheral ligand substituents on the ancillary phosphine units. The novelty of the findings will open new horizons in ethanol valorization to deliver innovative catalytic solutions and new technologies under mild conditions.
Continuing my ethanol journey, I studied the effect of solvents with different polarities on the acceptorless dehydrogenative coupling of ethanol, achieving high conversion and yield. Experimental guidelines were given for the selection of such dual-organic phase catalytic systems in acceptorless dehydrogenation.
The last inspiration was gained in the alcohol transfer hydrogenation project that I initially worked on as a collaborator. I applied this idea to glycerol, which possesses three hydroxyl groups and can make more chemical changes, and the transfer hydrogenation or dehydrogenation performed by it has not been much studied in academia, thus leaving me more room for manipulation.
In conclusion, this thesis contributes to enlarging current knowledge about catalytic processes for ethanol and glycerol valorization, explaining relevant parameters for their conversions, and presenting new routes for the optimization of the homogeneous catalytic system.
Original languageEnglish
PublisherDTU Chemistry
Number of pages259
Publication statusPublished - 2022

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