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DOE OSTI · 2914180

Efficient electrocatalytic valorization of chlorinated organic water pollutant to ethylene

Abstract

Electrochemistry can provide an efficient and sustainable way to treat environmental waters polluted by chlorinated organic compounds. However, the electrochemical valorization of 1,2-dichloroethane (DCA) is currently challenged by the lack of a catalyst that can selectively convert DCA in aqueous solutions into ethylene. Here, in this work, we report a catalyst comprising cobalt phthalocyanine molecules assembled on multiwalled carbon nanotubes that can electrochemically decompose aqueous DCA with high current and energy efficiencies. Ethylene is produced at high rates with unprecedented ~100% Faradaic efficiency across wide electrode potential and reactant concentration ranges. Kinetic studies and density functional theory calculations reveal that the rate-determining step is the first C–Cl bond breaking, which does not involve protons—a key mechanistic feature that enables cobalt phthalocyanine/carbon nanotube to efficiently catalyse DCA dechlorination and suppress the hydrogen evolution reaction. The nanotubular structure of the catalyst enables us to shape it into a flow-through electrified membrane, which we have used to demonstrate >95% DCA removal from simulated water samples with environmentally relevant DCA and electrolyte concentrations.

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BibTeXRIS

Choi, Chungseok [Yale Univ., New Haven, CT (United States)] (ORCID:0000000191691393), Wang, Xiaoxiong [Yale Univ., New Haven, CT (United States)], Kwon, Soonho [California Institute of Technology (CalTech), Pasadena, CA (United States)], Hart, James L. [Cornell Univ., Ithaca, NY (United States)], Rooney, Conor L. [Yale Univ., New Haven, CT (United States)], Harmon, Nia J. [Yale Univ., New Haven, CT (United States)], Sam, Quynh P. [Cornell Univ., Ithaca, NY (United States)], Cha, Judy J. [Yale Univ., New Haven, CT (United States); Cornell Univ., Ithaca, NY (United States)] (ORCID:0000000263462814), Goddard III, William A. [California Institute of Technology (CalTech), Pasadena, CA (United States)] (ORCID:0000000300975716), Elimelech, Menachem [Yale Univ., New Haven, CT (United States)] (ORCID:0000000341861563), Wang, Hailiang [Yale Univ., New Haven, CT (United States)] (ORCID:0000000344092034). 2022-12-19. Efficient electrocatalytic valorization of chlorinated organic water pollutant to ethylene. https://doi.org/10.1038/s41565-022-01277-z

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