Sustainable pathways to bio-based amines via the 'hydrogen borrowing' strategy

Abstract

The reduction of society’s dependence on fossil fuels and a gradual shift towards the use of renewables is of prime importance. Despite the considerable efforts that have been made to the introduction of novel catalytic methodologies that convert renewable resources to fuels or bio-based platform chemicals, the development of systematic strategies for the synthesis of amines - centrally important compounds in the bulk and fine chemical industry - from renewables, especially via waste-free catalytic routes, has not received due attention yet. This thesis outlines ample possibilities of using a variety of biomass sources for the synthesis of the high-value chemicals demonstrating the potential of renewable feedstocks as viable replacements for currently used fossil fuels. More specifically, it discloses the development of novel catalytic methods that enable the formation of value-added amines from readily available aliphatic and aromatic alcohol intermediates generated by the catalytic conversion of renewable resources such as lignocellulose. In order to design sustainable catalytic protocols two key strategies, namely ‘hydrogen borrowing’ and ‘cross-coupling’, have been applied to provide the target high-value products with exceptional selectivity and in-line with the principals of green chemistry. The present work attempts the first steps on a ‘high road’ to profitability from lignin and contributes to the development of fully sustainable and economically viable lignocellulosic biorefineries.