First Row Transition Metal Catalyzed (De)hydrogenation Reactions

Waiba, Satyadeep (2022) First Row Transition Metal Catalyzed (De)hydrogenation Reactions. PhD thesis, Indian Institute of Science Education and Research Kolkata.

Text (PhD thesis of Satyadeep Waiba (17RS026)) 17RS026.pdf - Submitted Version Restricted to Repository staff only Download (22MB)

Abstract

Synthetic chemistry has played a pivotal role in the betterment of humankind and has been an integral part of developing pharmaceuticals, agrochemicals, medicinal sciences, and functional materials. Contemporary research has focused on creating sustainable and environmentally benign methodologies moving forward in a similar path. This global emphasis has motivated chemists to explore greener approaches using readily available feedstocks and catalysts. Contextually, transition metal-catalyzed cross dehydrogenative coupling (CDC); namely, borrowing hydrogenation (BH) and acceptorless dehydrogenative coupling (ADC), has transpired as an attractive methodology for generating molecular complexity via C-C or C-heteroatom bond formations. The CDC approach is highly beneficial as readily available materials can be used for functionalization, avoiding functional group manipulations. At the same time, it is environmentally harmless as only water and in case of ADC, hydrogen are produced as by-products. Additionally, the latter also has the potential to be used as a clean energy source. The CDC reactions have been thoroughly explored with various precious transition metal catalysts in the past years. However, in terms of sustainability, replacing these precious metals with less toxic and more abundant base metal (3d) catalysts is highly alluring and, at the same time, challenging. In this regard, manganese can be an excellent candidate for replacing the higher congeners. It is the 3rd most abundant transition metal (after iron and titanium), less toxic, less expensive, and frequently encountered in various biological systems. This thesis's main aim will be to explore manganese complexes for various hydrogenations and dehydrogenations reactions. The main focus will be on constructing various carbon–carbon and carbon–heteroatom bonds via the CDC approach using different manganese complexes.

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