Speciation and activity of carbon based single atom heterogeneous catalysts for advanced synthetic processes

Identifier:  TDX:3411

Handle: https://hdl.handle.net/20.500.11797/TDX3411

Authors:  Fako, Edvin

Abstract:
Heterogeneous catalysts are the tool of choice in chemical industry as they are central to more economically and energy efficient processes. Metal catalysts dispersed into single atoms on an inert support offer ultimate atom economy and surface to volume ratio of the active phase, and carbon based support have show great potential as single atom heterogeneous catalyst supports. Carbon-based materials have proven to be one of the most significant catalyst supports over the last decades. Their high versatility in terms of porosity, coordination environments, and tailoring possibilities make carbon-based materials ideal for metal dispersion. SAHCs bring synergy between homogeneous and heterogeneous catalysis, as they have spatially isolated metal atoms entrapped in a support acting as a ligand, thus providing uniform and well-defined active sites resembling coordination environments of homogeneous catalysts while keeping the exemplary reusability of state-of-the-art heterogeneous catalysts. Several examples of high-performance single atom systems have revolutionized the approach to of catalyst design for different chemical processes on which society depends: from chemical transformations such as cross-couplings to selective semihydrogenations and acetylene hydrochlorination. The exceptional performance of SAHCs can be traced to distinct dynamic behavior and speciation was rationalized by Density functional theory simulations.