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Chapter 3. Sustainable Hydrocarbon Fuels by Recycling CO2 with Renewable/Nuclear Energy 63 fuels would exceed world demand for chlorine by many orders of magnitude. Therefore, due to the toxicity of chlorine, oxygen would be the preferred anode product from a seawater electrolysis cell. Since the anode potential for oxygen evolution is lower than that of chlorine evolution, the cell must be operated with an anode potential within a range above the oxygen evolution potential and below the chlorine potential. Therefore, new anode materials such as Mo- and W-doped MnO2 are being developed to achieve high anodic efficiency [111]. However, it may be unnecessary to deal with seawater in an electrolysis cell since obtaining pure water by desalination adds only a negligible cost to the fuel production process, as discussed in section 3.2.1. Related to alkaline electrolysis is the co-electrolysis of H2O and CO2 using aqueous carbonate or bicarbonate electrolyte [16, 115-123]. The CO2 can be supplied by being bubbled in or dissolved in the aqueous media, or supplied from the gas phase to a gas diffusion electrode. The majority of research in aqueous co-electrolysis of CO2 and H2O has focused on improving current efficiency (product selectivity) at a given potential rather than maximizing energy efficiency (for lower operating cost) or current density (for lower capital cost). The CO2 and H2O are electrocatalytically reduced to products such as HCOOH, CO, CH4, C2H4, and higher hydrocarbons and alcohols, depending on the cathode composition and cell parameters. For example, copper electrodes were found to selectively produce methane, methanol and other hydrocarbons over just H2 and CO, whereas Au and Ag selectively produce CO [115, 116, 119]. The cathode reaction for methanol is as follows: CO2(aq) + 6 H+ + 6 e– CH3OH(l) + H2O(l) Cu and Ag metal electrodes have shown low durability due to accumulation of carbon particles during CO2 reduction [124-126]. Metal alloy cathodes were shown to have increased durability and inhibit poisoning over pure metals [127, 128]. Reactivation of the electrodes by briefly pulsing an anodic current has also been explored [128-131]. Electrodes made of transition metal complexes [120, 132], e.g. phthalocyanine–Co/Ni, are able to coordinate the CO2 molecule and electrocatalytically reduce it with high selectivity (but not high efficiency). Though they have lower durability, their promise lies in being less expensive than pure metals. Because the solubility of carbon dioxide in water (~0.036 M at STP) is low, rate limitation from mass transport of CO2 to the surface results in limiting current densities of –10 to –20 mA/cm2 under 1 atm CO2 [133, 134]. Electrolyzing bicarbonate, which has a higher solubility (~1 M) than CO2, has not been found to enhance the reaction rate. Gas diffusion electrodes enable higher current densities. Centi et al [122, 123] reported the production of CO and small fractions of various long-chain C5+ hydrocarbons at a gas diffusion electrode. However, they used an electrode with expensive Pt and Pd nanoclusters, and found the maximum product selectivity was at the low current density of –20 mA/cm2.PDF Image | Electrolysis of CO2 and H2O
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