COOLEFIN · Novel Dinuclear Late Transition Metal Catalysts for CO2/Olefin and CO2/Epoxide/Olefin Copolymerization

Novel Dinuclear Late Transition Metal Catalysts for CO2/Olefin and CO2/Epoxide/Olefin Copolymerization

While anthropogenic carbon dioxide (CO2) emissions present a daunting societal challenge with respect to climate change, concentrated CO2 sources also afford an attractive CO2-recycling opportunity. The electrochemical carbon dioxide reduction reaction (CO2RR) is a catalytic process by which CO2-recycling can be driven via renewably derived electricity, hence affording a pathway toward zero- or low-carbon chemical/fuel feedstocks. Among all the products that can be obtained from the CO2RR, this project was especially interested in the development of electrocatalysts for the production of ethylene. Ethylene is a commodity chemical generated on a massive scale annually (~200 MT/yr globally) with a market value of approximately $250 billion dollar per year. Ethylene refinement from oil plays a major role in the business models of large oil and chemical companies such as Exxon and Dow, where it is a precursor for polymers synthesis and other important chemicals. Current methods for ethylene generation contribute to 0.6% of the annual global carbon dioxide (CO2) generation. Complementary methods for sustainable ethylene production, directly from CO2 as the sole carbon source, are appealing, especially when they benefit from the utilization of renewable electricity. The development of catalytic materials for the efficient conversion of CO2 into ethylene from renewable energy presents an exciting opportunity, but also a challenge for the field of catalysis. CO2RR can facilitate the transformation of CO2 into a range of desirable carbon-containing products through the use of metallic electrodes and renewable electricity. However, the mechanistic landscape of CO2RR is complex and competing proton-coupled electron transfer (PCET) pathways can be operative; the control of product selectivity remains a central issue. To circumvent the use of expensive separation processes that will hamper the large-scale implementation of electrochemical CO2RR, approaches for the rational design of selective catalytic surfaces are needed. To date, copper is the only known metal capable of producing ethylene, from CO2RR with decent selectivity. Bridging homogeneous molecular systems with heterogeneous copper surfaces is a promising approach for the development of new electrodes, combining the advantages of both approaches. The objective of the project is to develop hybrid copper electrodes consisting of molecular organic films and a planar copper electrode to target high selectivity for ethylene.

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