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Catalysts 2021, 11, x FOR PEER REVIEW 10 of Catalysts 2021, 11, 482 10 of 19 Figure 7. Chronoamperometry responses (a), partial FEs (b), productivities of gas (c) and liquid (d) products for Cu-06 catalyst with ~ 4 mg cm−2 and 0.44 mg cm−2 (30% of Nafion) tested in 1 M Figure 7. Chronoamperometry responses (a), partial FEs (b), productivities of gas (c) and liquid KHCO aqueouselectrolyteat−1.5Vvs.Ag/AgCl−.2 −2 (d) prod3ucts for Cu-06 catalyst with ~ 4 mg cm and 0.44 mg cm (30% of Nafion) tested in 1 M KHCO3 aqueous electrolyte at −1.5 V vs. Ag/AgCl. 2.3.4. Effect of Nafion and Electrolyte Concentration The results obtained with the Cu-06 catalyst deposited in the GDE with a variation In particular, higher FEs (Figure 7b) are observed towards CO2 reduction produc of the Nafion concentration in ink (from 15%wt to 45%wt) are discussed in the following. with the lower catalyst loading case (0.44 mg cm−2), which are reflected in an increase In the light of the better CO2R performance [38] and less favoured H2 production [39] the productivity of CO and formate, but also in the generation of other liquid produc with solutions of low KHCO3 concentration, a more diluted electrolyte was employed at Ttheisresftaogre,obf ythceowmoprka.riKnngotwhiensgetvhatlueeasch, cfoanctcolrupsliaoynssacraonlebien dthreawacntivaibtyoauntdthperoadcuticvtsity. In t distribution of the reduction process, it was found to−2be reasonable to use an intermediate regard, Cu-06 GDE loaded with 0.44 mg Cu cm and tested at −1.5 V vs. Ag/AgCl was t catalyst loading of 2 mg cm−2 to carry out the tests at the same applied potential (−1.5 V most active electrode towards formate production, as well as it was the only case whe vs. Ag/AgCl) and in a 0.1 M KHCO3 electrolyte. In the case of Nafion at 45%wt, a production of different C1 to C3 products like methanol, ethanol, acetone, 1- and 2-prop slightly lower current density was recorded (−2.1 mA cm−2) than for the other cases nol and propa−n2al were visible, as sh−o2wn in Figure 7d. Two hypotheses have been a (−2.25 mA cm at 30%wt, −3.5 mA cm at 15%wt), as it could be expected if a decrease vanced concerning the better results obtained with a lower catalyst loading: on the o in the number of exposed active sites is prevalent due to the high Nafion content. These hraensudl,tsthaegrreeawctitahnrtecdeinfftustsuiodniestothwatadrdems othnestractteidvaensoitpetsim(anl bdi,ncdoernlsoeaqduinegnitnlyt,htehreancgoeunter d between 11%wt and 20%wt [40], by which an optimal balance between ionic conductivity, fusion of the products) may be promoted by reducing the catalyst-layer thickness; mor pH, available active sites and electrons conductivity can be found. over, a lower catalyst loading may lead to a lower increase of the local pH, which tran The results of FEs and productivities are displayed in Figure 8. Switching to a lower lates in a reduced formation of (bi)carbonate species, as it will be discussed in Section 2 catholyte concentration and a lower Nafion content than the previous tests led to unex- pected data. A higher FE to CO than to H2 was obtained with 15%wt Nafion. A consid- 2.3.4. Effect of Nafion and Electrolyte Concentration eration of the relative ratio of CO and formate should be done. Indeed, the increasing of NafiTonheloraedsinuglttsoo3b0%tawinteadndwthitehnthoe45C%uw-0t6seceamtasltyosftavdoeuprothsietefodrminattehaenGd DCE awlciothoalsvariati 2+ (i.e., ethanol, 1- and 2-propanol) production over the CO. Thus, it is clear that the Nafion of the Nafion concentration in ink (from 15%wt to 45%wt) are discussed in the followin content has a role in altering the course of the CO2 reduction reaction under this conditions. In the light of the better CO2R performance [38] and less favoured H2 production [39] wi Its interaction with the catalyst nanoparticles probably contributes to decreasing the energy solutions of low KHCO3 concentration, a more diluted electrolyte was employed at t barrier of the RDS: *CO + *H → *CHO and the barrier to the coupling of *CO intermediate, stage of the work. Knowing that each factor plays a role in the activity and products di promoting more reduced products. tribution of the reduction process, it was found to be reasonable to use an intermedia For an efficient CO2 reduction, an optimal balance needs to be searched among −2 cathtaeleylsetctlroadctiinvge soufr2famcegarcema, thteoiocnaircrycoonudtucthtievityesatnsdathtehehysdarmopehailpicp/lhieydrpopohteonbtiical (−1.5 properties of the catalyst layer [41]. The study of the effect of the ionomer content was vs. Ag/AgCl) and in a 0.1 M KHCO3 electrolyte. In the case of Nafion at 45%wt, a slight lower current density was recorded (−2.1 mA cm−2) than for the other cases (−2.25 mA c at 30%wt, −3.5 mA cm−2 at 15%wt), as it could be expected if a decrease in the number exposed active sites is prevalent due to the high Nafion content. These results agree wi recent studies that demonstrated an optimal binder loading in the range between 11% i t h h d n i . o t h m o t wPDF Image | Gas Diffusion Electrode Systems for the Electro CO2 Conversion
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