Electron Transfer Catalysis for Strong Bond and Greenhouse Gas Activation

Biswas, Amit (2025) Electron Transfer Catalysis for Strong Bond and Greenhouse Gas Activation. PhD thesis, Indian Institute of Science Education and Research Kolkata.

Text (PhD thesis of Amit Biswas (19RS059)) 19RS059.pdf - Submitted Version Restricted to Repository staff only Download (20MB)

Abstract

The research works presented in this PhD thesis entitled “Electron Transfer Catalysis for Strong Bond and Greenhouse Gas Activation” discusses the utilization of polycyclic odd alternant hydrocarbon phenalenyl (PLY) and bis(borondifluoride)-8-imidazodipyrromethene (BOIMPY) systems in designing efficient mechano-redox catalysts and photo-redox catalysts for various organic transformations (including gas activation) taking advantage of the energetically accessible non-bonding molecular orbital (NBMO) under the mechanochemical condition as a metal-free catalyst for PLY and bonding and anti-bonding orbital (ABMO)under photochemical condition for BOIMPY as a metal-free catalysis. This thesis is divided into three chapters. The first is “Introduction”, which discusses a general overview of electron transfer catalysis and its application in organic chemistry. The later section describes the properties of phenalenyl-based molecules and BOIMPY-based molecules with the early approaches, giving a logical explanation for designing a phenalenyl-based and BOIMPY-based catalytic system. The second chapter, “Results and Discussion”, is subdivided into three sections that describe the dissertation work carried out during the PhD tenure. Section 2.1 describes the mechanochemical generation of phenalenyl-based dianion species supported by detailed spectroscopic studies and its application in the development of redox catalysis for C-C cross-coupling reactions such as direct C-H arylation with heteroarenes, arenes, polyarene under solvent-free solid state without using any transition metal. Section 2.2 discusses the discovery of new multi-photoinduced electron transfer catalysis ideas using BOIMPY as a metal-free photoredox catalyst and its application for various inert bond activations such as C-F, C-Cl and arenes. In section 2.3, a highly efficient, one-catalyst can activate both CO2 and N2O under photochemical conditions. Utilizing greenhouse gases, we have successfully developed a range of organic transformation reactions, including the reductive mono-carboxylation of arenes with CO2 and the reductive dihydroxylation of arenes using N2O. In the 2.4 section, the synthesis of polyesters from olefins through the activation of both CO2 and N2O. We synthesized bulk polymer using a two-spot reaction involving CO2 and N2O. The third chapter consists of the “Experimental Section”, which describes in detail all the experimental procedures for Chapter 2. This section includes all the synthetic and characterization data for all the compounds discussed in this thesis.

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