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Efficient transformation of biomass to value-added chemicals and high-energy density fuels is pivotal for a more sustainable economy and carbon-neutral society. In this framework, developing potential cascade chemical processes using functionalised heterogeneous catalysts is essential because of their versatile roles towards viable biomass valorisation. Advances in materials science and catalysis have provided several innovative strategies for the design of new appealing catalytic materials with well-defined structures and special characteristics. Promising catalytic materials that have paved the way for exciting scientific breakthroughs in biomass upgrading are carbon materials, metal-organic frameworks, solid phase ionic liquids, and magnetic iron oxides. These fascinating catalysts offer unique possibilities to accommodate adequate amounts of acid-base and redox functional species, hence enabling various biomass conversion reactions in a one-pot way. This review therefore aims to provide a comprehensive account of the most significant advances in the development of functionalised heterogeneous catalysts for efficient biomass upgrading. In addition, this review highlights important progress ensued in tailoring the immobilisation of desirable functional groups on particular sites of the above-listed materials, while critically discussing the role of consequent properties on cascade reactions as well as on other vital processes within the bio-refinery. Current challenges and future opportunities towards a rational design of novel functionalised heterogeneous catalysts for sustainable biomass valorisation are also emphasized. ispartof: Chemical Society Reviews vol:47 issue:22 pages:8349-8402 ispartof: location:England status: published

In the last 5 years, reductive catalytic fractionation of lignocellulose biomass has emerged as a promising biorefinery concept that combines biomass fractionation with the preservation of chemical functionality in its products. Although significant efforts have been made in optimizing this technology on lab scale, the implementation on a larger (pilot) scale is still in its infancy. In our own search for the scale-up potential of this technology, we faced several fundamental and technical research questions that, to this day, remain unanswered. These fundamental questions are related to four main aspects of RCF, the lignocellulose feedstock, the operating pressure, the redox catalyst, and the solvent. In order to inspire future multidisciplinary research in the RCF community, these scale-up challenges are presented and discussed via multiple angles combining chemical process hurdles with more technical aspects, such as reactor design and process consequences.