Proceedings of nanoGe Fall Meeting19 (NFM19)
DOI: https://doi.org/10.29363/nanoge.nfm.2019.024
Publication date: 18th July 2019
Cu is the only monometallic catalyst capable to electroreduce CO2 beyond CO and produce a large variety of fuels and valuable chemicals (hydrocarbons and alcohols). However, the reaction presents low selectivity and mainly competes with the hydrogen evolution reaction, thus affecting the efficiency of the overall process. Fundamental work on well-ordered electrified interfaces, i.e. involving Cu single crystalline electrodes (Cu(hkl)), is pivotal to understand the CO2RR mechanism because both specific active site and electrolyte controls the selectivity of the reaction. [1][2]
In the present communication, we have systematically investigated Cu(111) and Cu(100) single crystalline electrodes in contact with phosphate buffer solutions and in a wide range of pH (from pH 1.5 to 12.5). Phosphate is known to adsorb specifically on Cu electrodes. [3][4] Here, we show that the anion adsorption is strongly dependent on the geometry of the active site, as well as on the bulk solution pH. In parallel, we have saturated the different buffer solutions with CO (key intermediate of the CO2RR on Cu), aiming to compare how the interfacial properties of Cu(hkl) would be affected or modified under reaction conditions. Furthermore, we attempt to assess a few fundamental aspects that highly influence the CO electroreduction, such as pH effect, specific anion adsorption and/or the stability of the surface under reductive conditions. Figure 1 shows the voltammetric response of Cu(100) (Fig. 1A) and Cu(111) (Fig. 1B) in contact with a 0.1M phosphate buffer neutral solution and recorded at 50mV/s. The quasi-reversible peak recorded on both surfaces (red solid line) corresponds to the phosphate displacement by CO, and its potential position is sensitive to the active site. The enlargement of the cathodic scan towards the CO reduction (black dashed line) modifies this voltammetric feature, showing the potential dependence of the interfacial processes on Cu(hkl).
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