EFRI DCheM: Chemicals from Renewables Through Green Electrochemistry (ChaRGE)

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This project aims to develop a new approach to distributed chemical manufacturing that combines sustainability, performance, and chemical flexibility. It capitalizes on electrochemistry, a technology that uses electric fields to enhance chemical transformations and open new reaction pathways. The investigators in this project will streamline fermentation and electrochemistry in modular reactor systems to produce high-value chemicals from regional carbon (biomass) and wind/solar energy sources. To this end, they will develop fundamental insights into the electrochemical transformation of intermediates obtained from fermentation, design new catalysts for organic electro-reductions and -oxidations, engineer reactor systems for flexible operation, and synthesize novel high-value monomers. In addition, the copolymerization and chemistry of the obtained monomers will be explored with the intent to access Nylons with performance advantages. Constant feedback among electrochemical experiments, theory, reactor design, polymer engineering, and operations research will yield distributed manufacturing systems where energy management, plant scale and plant location are optimized for maximum expected operating profit under uncertainty in feedstock availability and quality, and in renewable energy supply. The overarching goal of this project is to decarbonize the U.S. chemical industry, evolve the power and chemical industries, advance the American leadership in chemical manufacturing, improve rural economies, and provide unique outreach and training opportunities for building a biomanufacturing workforce. The project is particularly relevant to develop a locally-rooted STEM workforce in the Midwest, with enhanced participation of underrepresented students in STEM education.The project addresses the scientific and technological barriers to the implementation of organic electrosynthesis for the distributed manufacturing of chemicals. The team will design catalysts and reaction pathways for the diversification of biologically-produced cis,cis-muconic acid (MA), a diacid that has recently been elevated to the status of platform chemical due to its unparalleled promise for strategically advancing the bioeconomy. The project will focus on three transformations of industrial importance for which the project will provide environmental and economic benefits: (i) cathodic hydrogenations using water as hydrogen source, (ii) cathodic carbon-carbon coupling using green electrons and, (iii) anodic epoxidations using chloride ions as a mediator. Using green electrons from wind/solar energy and compounds already present in the fermentation broth will create new opportunities for sustainable manufacturing, process intensification, and the cost-effective production of monomers from waste biomass. In addition to adipic acid, a commodity monomer used in the manufacture of Nylon 6,6, the proposed research will provide novel diacids with functionalities that are not readily accessible from petroleum. The outcomes of the project are transformative at multiple levels as (i) it will elucidate the role of the substrate’s molecular structure, ions in solution, pH, the nature and the structure of the electrocatalyst, and the electric field on the conversion of bioproducts; (ii) it will also highlight how species abundant in biomass, namely water and chloride ions, can be efficiently used as a source of hydrogen and as a mediator, respectively, to perform industrially-relevant hydrogenation and epoxidation reactions under ambient conditions; (iii) it will reveal the benefits of electrocatalysis to access new monomers and performance-advantaged bioplastics; and (iv) it will reveal strategies to mitigate the intermittent nature of renewable energy for chemical manufacturing.This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.