NSF-DFG Echem: Electrochemical pyrrolidone synthesis: an integrated experimental and theoretical investigation of the electrochemical amination of levulinic acid (ElectroPyr)

• Applicant: Professorin Dr. Regina Palkovits
• Subject Area: Technical Chemistry
• Term: since 2021
• Project identifier: Deutsche Forschungsgemeinschaft (DFG) - Project number 459861727

The proposed research relates to the electrochemical synthesis of pyrrolidones based on levulinic acid, a promising platform chemical available based on lignocellulosic biomass. Pyrrolidones are important intermediates for pharmaceutical products, solvents and polymers. Today, pyrrolidone production proceeds via acetylene as substrate to yield -butyrolactone followed by gas-phase amidation with ammonia and, in case of vinyl-pyrrolidone as target for PVP production, further Reppe vinylation again with acetylene. Recent studies demonstrate feasibility of a chemo-catalytic amination of levulinic acid, while an electrochemical pyrrolidone synthesis via such a pathway has, to the best of our knowledge, not been demonstrated yet. In general electrochemistry enables milder reaction conditions compared to chemocatalysis and provides the potential to integrate renewable electrical energy into chemical value chains. In case of the proposed pyrrolidone synthesis, high hydrogen pressure can be avoided and potentially aqueous electrolytes facilitate an integration along the biorefinery value chain. Despite the high potential and rising interest in science and industry, the fundamental understanding of electrochemical transformations remains limited. In case of the chemocatalytic biomass valorization, targeted theoretical and experimental investigations regarding the formation and further transformation of platform molecules such as levulinic acid enabled distinct advance in the fundamental understanding and served as strong base for the design of feasible biorefinery concepts. Examples on prior work include studies by the applicants on the chemocatalytic reduction of levulic acid, the amination of alcohols, and the electrochemical conversion of biogenic acids . Accordingly, we herein aim for an integrated experimental and theoretical investigation of the electrochemical amination of levulinic acid. The Sautet group will focus on first-principles simulations of the electrocatalytic surface reaction aiming for a comprehensive mechanistic understanding together with insight into factors controlling catalytic surface reactivity of the electrocatalyst. The Palkovits group will experimentally investigate the transformation with emphasis on the influence of electrocatalyst and process parameters.

• DFG Programme: Research Grants
• International Connection: USA
• Partner Organisation: National Science Foundation (NSF)
• Cooperation Partner: Professor Dr. Philippe Sautet