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20 Chapter 4. Non-Aqueous PEC System 4.2 Fundamental Electrochemistry and Materials Technology 4.2.1 Cathode Reaction: CO2 Reduction via Dimerization/Disproportionation 4.2.1.1 Homogeneous Catalysis: Mn(mesbpy) Earlier reports from the Kubiak group (cf. Ratiff et al., 1986–1988; Lewis, 1993) describe a solid-state p-GaP semiconductor PEC device with Ni3-cluster electrocatalyst for the CO2 splitting to CO and O2. A prototype electrochemical device for the CO2 splitting would consist of a cathode chamber with a molecular CO2 reduction catalyst, an anode chamber for oxygen production, and an ion selective membrane in between. The catalyst will selectively disproportionate CO2 to CO and carbonate (CO32-), of which the CO32- will pass through the membrane and be oxidized at the anode to provide O2. Thus both CO and oxygen will be produced by this device. Figure 4.2: Electrochemical CO2 reduction by Mn(mesbpy) catalyst with Lewis acids and with weak Brønsted acids (Adapted with permission from Sampson & Kubiak, 2016). A recent investigation of the catalyst Mn(mesbpy)(CO)3Cl and its catalytic reactivity with Lewis acids (Sampson & Kubiak, 2016) provides a recent illustration of the operating principles necessary for the development of a molecular catalyst for non-aqueous CO2 reduction to CO and carbonate. Here, conversion of CO2 to CO and carbonate occurs in the presence of a Lewis acid Mg(OTf)2 at room temperature with the lowest overpotential (η) ever reported for molecular CO2 reduction electrocatalysts (η= 0.30–0.45 V). Formation of CO and carbonate proceeds via the desired reductivedisproportionationofCO2 (2CO2+2e– −−→COandCO32-). Thiscatalystoperates in dry acetonitrile at –1.60 V vs. Fc+/0 with a Faradaic efficiency of 98 ± 2% and a turnover number (TON) of 36 after 6 hours of electrolysis. The formation of CO, CO32- and HCO32- wasPDF Image | ISRU Challenge Production of O2 and Fuel from CO2
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