Date of Completion

7-10-2018

Embargo Period

7-10-2018

Keywords

Mesoporous materials; Manganese oxide; Oxidative dehydrogenation; Aniline Coupling; sp2-sp3 coupling; Cobalt sulphoselenide; Hydrogen evolution reaction

Major Advisor

Prof. Steven L. Suib

Associate Advisor

Prof. Alfredo Angeles-Boza

Associate Advisor

Prof. Gaël Ung

Field of Study

Chemistry

Degree

Doctor of Philosophy

Open Access

Open Access

Abstract

This thesis includes five chapters. The 1st Chapter provides a brief introduction of mesoporous materials and heterogeneous catalysis. Chapter 2 describes the coupling of anilines to azo dyes in the presence of mesoporous manganese oxide materials. In Chapter 3 an extension of the applicability of mesoporous manganese oxide catalysts to cross dehydrogenative coupling of N-Aryltetrahydroisoquinolines (sp3 C-H) with indoles (sp2 C-H) is discussed. Moreover, in Chapter 4 the applicability of mesoporous cobalt sulfoselenide system was studied for producing hydrogen from water under electro-catalytic conditions. Finally, in Chapter 5, the future perspectives of the development of mesoporous materials has been discussed to extend their applicability to performing complicated chemical reactions.

Since the past few decades, intense research is ongoing for development of alternatives to fossil fuels and petroleum products. To curb the menace of global warming, the development of green chemical pathways is also a recent focus. These green chemical methodologies are intended to repel traditional pathways that often involve the use or production of toxic elements, environmentally unfriendly protocols, and non-reusable techniques. Therefore, to develop green chemical pathways for reactions, systems are designed using earth-abundant but non-toxic elements. Moreover, these reusable protocols are preferred to be operable under atmospheric conditions, and without any additives. These fundamentals of ‘green chemistry’, interested me in understanding the surface chemistry and further the applications of mesoporous metal oxides and sulfides such as manganese oxides and cobalt sulfides.

In this thesis, the importance of different catalytic processes, their operational procedures, and fundamental details have been depicted. We have identified the active sites responsible for the excellent activity of reported transformations. Detailed investigation of the surface chemistry of these heterogeneous catalytic processes is expected to facilitate the understanding and further the advancement of rather complicated procedures. Computational calculations were performed in all cases to support our experimental findings. These non-toxic, additive free catalytic protocols discussed here showed excellent reusability and environmentally benign waste (water) generation, which abides by the rules of Green Chemistry.

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