Cooperative CO2-to-ethanol conversion via enriched intermediates

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Cooperative CO2-to-ethanol conversion via enriched intermediates ( cooperative-co2-to-ethanol-conversion-via-enriched-intermedi )

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Articles ab Nature Catalysis 40 20 0 –0.4 c 25 20 15 10 5 0 –0.4 FeTPP[Cl]/Cu Cu 150 100 50 0 –0.4 CEEethanol This work Ref.17 Ref.20 Ref.19 Ref.11 Ref.15 Ref.18 FeTPP[Cl]/Cu Cu e 0.8 0.4 0.0 40 20 0 –0.5 –0.6 E (V versus RHE) –0.8 –0.9 –0.5 –0.6 –0.7 –0.8 –0.9 E (V versus RHE) –0.6 E (V versus RHE) –0.8 –0.9 100 jethanol –0.7 FeTPP[Cl]/Cu Cu –0.5 –0.4 –0.6 –0.8 10 30 –0.7 d Onset potential 1.0 0.9 η 45 FEethanol FEethanol (%) i (A) CEEethanol (%) FEethanol (%) jethanol (mA cm–2) 0 3 6 9 12 Time (h) Fig. 3 | CO2-to-ethanol conversion performance. a–c, Ethanol FE (a), partial current density (b) and half-cell CEE (c) over applied potentials of the FeTPP[Cl]/Cu and Cu catalysts. jethanol is the ethanol partial current density normalized by geometric area. The error bars represent 1 s.d. on the basis of three independent samples. The experiments were carried out in a GDE-based flow cell using 1 M KHCO3 as the electrolyte. d, Comparison of the onset potential, overpotential (η), FE, ethanol partial current density and half-cell CEE of the FeTPP[Cl]/Cu catalyst with those of state-of-the-art Cu-based catalysts. Only reports with a total current density >10 ma cm−2 were compared. e, Extended electrosynthesis of ethanol using the FeTPP[Cl]/Cu catalyst in a MEa system using 0.1 M KHCO3 as the anolyte. i, total current. The full-cell voltage was gradually increased from 3 V to 3.7 V and kept constant over the course of electrolysis. overpotential, FE, partial current density and half-cell CEE (Fig. 3d and Supplementary Table 1). The CO2-to-ethanol activity normal- ized to the electrochemical surface area was also one order of mag- nitude higher than that in previous reports (Supplementary Table 1), in part benefitting from the flow cell we used herein. The use of neutral electrolyte circumvented the carbonate formation issue encountered in CO2RR electrolysers using alkaline electrolytes42. We further integrated the CO2 reduction and H2O oxidation reactions in a system employing a membrane electrode assembly (MEA; Supplementary Fig. 15) to carry out the full electrosynthesis of ethanol from CO2 and water via the reaction: We observed a decrease of ethanol selectivity after the initial 12 h (Supplementary Fig. 16), which we attributed to the mass loss of the FeTPP[Cl] molecules on the Cu substrate (Supplementary Note 2 and Supplementary Figs. 17 and 18). Nevertheless, we observed no structural damage of the FeTPP[Cl] molecules (such as decompo- sition to nanoparticles) following electrolysis when we studied the catalyst using ultraviolet-visible absorption and X-ray absorption spectroscopies (Supplementary Fig. 18). Mechanistic investigations. To investigate the origins of the improved ethanol selectivity of FeTPP[Cl]/Cu, we reported the combined FE of major C2 products (ethanoland ethylene) against applied potential (Fig. 4a). We found that the combined C2 FE for the FeTPP[Cl]/Cu catalyst was higher than that for the pure Cu elec- trode. Further analysis of the product distribution (Supplementary Fig. 19) indicated that the C2 selectivity increased mainly at the expense of CO. We further compared the ratio of ethanol FE to ethylene FE. We found that, across the entire applied potential range, the FeTPP[Cl]/Cu electrode favoured ethanol over ethylene o 2CO2 þ3H2O!C2H5OHþ3O2 E 1⁄41:14 ð1Þ We operated the system for an initial 12 h at a full-cell voltage of 3.7 V. The system delivered a stable current of 0.6 A and an average ethanol FE of 41% (Fig. 3e). Thus, we obtained a full-cell EE (see Methods for calculation details) of 13%. This value is reported with- out the benefit of ohmic resistance (iR) corrections. 78 NATurE CATALYSiS | VOL 3 | JanUarY 2020 | 75–82 | www.nature.com/natcatal 20 1.2 1.1 10 15

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