Abstract:Generating
syngas (H
2
and CO mixture) from electrochemically
reduced CO
2
in an aqueous solution is one of the sustainable
strategies utilizing atmospheric CO
2
in value-added products.
However, a conventional single-component metal catalyst, such as Ag,
Au, or Zn, exhibits potential-dependent CO
2
reduction selectivity,
which could result in temporal variation of syngas composition and
limit its use in large-scale ele… Show more
“…Recently, a number of catalysts, including cadmium sulfoselenide nanorods, 16 Cu-enriched Au, 15 silver nanowire/ carbon sheet composites, 19 and silver diphosphide nanocrystals, 20 have been demonstrated as active catalysts for ECR syngas formation. However, ECR technologies are still far from being economically completive.…”
Producing syngas from electrochemical reduction of CO 2 by renewable energy offers an opportunity to reduce CO 2 emissions and provide chemicals and fuels. Herein, we report the careful manipulation of the reduction treatment to synthesize copper nanowire arrays (Cu NAs). By thermal oxidation, copper oxide nanowires were grown on a Cu mesh. Then, thermal reduction and electrochemical reduction were used to reduce copper oxide to Cu with the morphologic features largely preserved. The derived Cu NAs are cost-effective electrocatalysts capable of reducing CO 2 and H 2 O for tunable syngas production. It is demonstrated that syngas, the mixture of H 2 and CO, could be attained with a wide range of compositions (from 1:2 to 3:1) from CO 2 reduction and H 2 O reduction on these Cu NAs in aqueous solutions. In addition, Cu NAs show a high current density, 4 mA/cm 2 , at a low potential, −0.5 V, with a high syngas faradaic efficiency of over 70%. This approach explores a new method that sheds light on tuning the syngas composition from the electrochemical CO 2 reduction by Cu-based catalysts.
“…Recently, a number of catalysts, including cadmium sulfoselenide nanorods, 16 Cu-enriched Au, 15 silver nanowire/ carbon sheet composites, 19 and silver diphosphide nanocrystals, 20 have been demonstrated as active catalysts for ECR syngas formation. However, ECR technologies are still far from being economically completive.…”
Producing syngas from electrochemical reduction of CO 2 by renewable energy offers an opportunity to reduce CO 2 emissions and provide chemicals and fuels. Herein, we report the careful manipulation of the reduction treatment to synthesize copper nanowire arrays (Cu NAs). By thermal oxidation, copper oxide nanowires were grown on a Cu mesh. Then, thermal reduction and electrochemical reduction were used to reduce copper oxide to Cu with the morphologic features largely preserved. The derived Cu NAs are cost-effective electrocatalysts capable of reducing CO 2 and H 2 O for tunable syngas production. It is demonstrated that syngas, the mixture of H 2 and CO, could be attained with a wide range of compositions (from 1:2 to 3:1) from CO 2 reduction and H 2 O reduction on these Cu NAs in aqueous solutions. In addition, Cu NAs show a high current density, 4 mA/cm 2 , at a low potential, −0.5 V, with a high syngas faradaic efficiency of over 70%. This approach explores a new method that sheds light on tuning the syngas composition from the electrochemical CO 2 reduction by Cu-based catalysts.
“…A commonly employed 0.5 M KHCO 3 aqueous electrolyte solution saturated with CO 2 (pH = 7.5) was used as catholyte. 21,24,26,29 The fluidic characteristics of the employed cell design allowed to recirculate the catholyte solution (flow rate of 20 ml/min), while the CO 2 gas was directly injected through the macroporous 3D Cu-Ag…”
Section: Electrochemical Reduction Of Comentioning
confidence: 99%
“…In this regard, dendritic structures are of particular interest and were targeted in this study. Besides numerous examples of Ag based materials for CO 2 RR to CO, such as nanoplates, 20 nanoporous material and nanoparticles, [21][22][23][24][25] nanowires, 26,27 nanoclusters 28 and porous foams, 29 , dendritic structures offer large active surface areas paired with facile and non-expensive synthetization. [30][31][32] In this regard, we selected the electrodeposition method to deposit the Ag catalyst.…”
The present study outlines the important steps to bring electrochemical conversion of carbon dioxide (CO 2) closer to commercial viability by using a large-scale metallic foam electrode as highly conductive catalyst scaffold. Due to its versatility, it was possible to specifically tailor three-dimensional copper foam through coating with silver dendrite catalysts by electrodeposition. The requirements of high yield CO 2 conversion to carbon monoxide (CO) were met by tuning the deposition parameters towards a homogeneous coverage of the copper foam with nanosized dendrites, which additionally featured crystallographic surface orientations favoring CO production. The presented results evidence that Ag dendrites, owing a high density of planes with stepped (220) surface sites, paired with the superior active surface area of the copper foam can significantly foster the CO productivity. In a continuous flow-cell reactor setup , CO faradaic efficiencies reaching from 85 % to 96 % for a wide range of low applied cathode potentials (< 1.0 V RHE) along with high CO current densities up to 27 mA/cm 2 were achieved, far outperforming other tested scaffold materials. Overall, this research provides new strategic guidelines for the fabrication of efficient and versatile cathodes for CO 2 conversion compatible with large-scale integrated prototype devices.
“…25 A number of researchers have demonstrated that Ag promotes CO evolution in both aqueous and non-aqueous systems with varying electrokinetics that are largely influenced by the surface morphology and nature of electrolyte adsorption at the electrode-electrolyte interface. 25,26,27 It has also been shown that oxide derived nanostructured Ag materials exhibit excellent ability to convert CO2 to CO with selectivities exceeding 80%.…”
The use of renewable electricity to synthesize high energy and high value chemicals via reduction of CO2 is an attractive strategy for renewable energy storage. Improving our understanding of how heterogeneous CO2 reduction electrocatalysts function is important to designing efficient systems for conversion of CO2 into commodity chemicals such as CO and HCO2H. Both Ag- and Sn-based materials have been previously considered as CO2 reduction catalysts and offer distinct CO2RR selectivities. In this work, we have considered electrodeposited composite film electrodes prepared from electroplating baths with varying ratios of Ag+ and Sn2+ triflates to understand how the performance of such composite materials varies as a function of composition. XPS analysis confirms that for each composite film electrodes, Ag existed in the metallic (Ag0) state, while the Sn was mainly oxidized (Sn2+/4+). The AgSn composite film electrodes studied herein are therefore best considered as AgSnOx cathodes with varying ratios of Ag0:Sn2+/4+. These systems were assessed as CO2RR electrocatalysts and were found to promote the 2e–/2H+ reductions to deliver CO and HCOOH with fast kinetics and high efficiencies from electrolyte solutions containing the protic organic cation [DBU–H]+. While Sn-rich composite films showed poor selectivities for CO versus HCO2H, a significant increase in CO versus HCO2H selectivity (up to 99%) is achieved for composite film electrodes in which the Ag content ranged from 25 - 75%. By tuning the ratio of Ag0 to SnOx we prepared composite film cathode materials that support quantitative current efficiencies for generation of CO with geometric current densities approaching 30 mA/cm2 at applied overpotentials that are less than 750 mV were realized. Additionally, electrochemical impedance spectroscopy (EIS) coupled with analysis of the distribution of relaxation times (DRT) was used to better understand factors important to the composites’ activity under CO2RR conditions. Probing the dynamics with DRT analysis revealed that multiple processes relating to both adsorption and diffusion-controlled events are important to the activity of the electrocatalysts considered in this work. The collection of electroanalytical investigations suggest that synergistic interactions between Ag and SnOx give rise to porous films that support enhanced CO2RR kinetics and that mixing of Ag with SnOx enhances the efficacy of adsorption and stabilization of reduced CO2 intermediates and [DBU–H]+ cations to facilitate CO evolution at the cathode/electrolyte interface.
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