Hostname: page-component-8448b6f56d-jr42d Total loading time: 0 Render date: 2024-04-18T10:57:40.148Z Has data issue: false hasContentIssue false
  • English
  • Français

Composite copper oxide–copper bromide films for the selective electroreduction of carbon dioxide

Published online by Cambridge University Press:  20 April 2017

Norma R. de Tacconi ,
Wilaiwan Chanmanee ,
Brian H. Dennis  and
Krishnan Rajeshwar Open the ORCID record for Krishnan Rajeshwar [Opens in a new window]
Norma R. de Tacconi*
Affiliation:
Department of Chemistry & Biochemistry, The University of Texas at Arlington, Arlington, Texas 76019-0065
Wilaiwan Chanmanee
Affiliation:
Department of Mechanical & Aerospace Engineering, The University of Texas at Arlington, Arlington, Texas 76019-0018
Brian H. Dennis
Affiliation:
Department of Mechanical & Aerospace Engineering, The University of Texas at Arlington, Arlington, Texas 76019-0018
Krishnan Rajeshwar*
Affiliation:
Department of Chemistry & Biochemistry, The University of Texas at Arlington, Arlington, Texas 76019-0065
*
a) Address all correspondence to these authors. e-mail: ntacconi@uta.edu
b) e-mail: rajeshwar@uta.edu
Get access

Abstract

Composite copper oxide–copper bromide films were electrodeposited on gas diffusion layer (GDL) supports under controlled potential from aqueous copper salt solutions in the presence of a complexing/surfactant agent such as lactate. The solution pH was adjusted to target simultaneous deposition of cubic nanostructures composed of copper, oxygen, and bromine elements. The film composition and morphology were carefully tuned for enhanced electrochemical conversion of CO2 to hydrocarbons. Hydrocarbon products, predominantly ethylene and minor amounts of methane, ethane, and propylene were observed along with inevitable H2 co-generation. Importantly, CO gas was not detected during CO2 electrolyses. Low temperatures (3–5 °C) enhanced the conversion of CO intermediate to C2H4. The durability and electroactivity of these composite films were maintained for extended periods (up to 10 h) of CO2 electrolysis by periodic in situ application of anodic pulses to regenerate the cathode surface.

Keywords

electrochemical synthesiselectrodepositionenergy generation
Type
Articles
Information
Journal of Materials Research , Volume 32 , Issue 9 , 15 May 2017 , pp. 1727 - 1734
Check for updates
Copyright
Copyright © Materials Research Society 2017 

Access options

Get access to the full version of this content by using one of the access options below. (Log in options will check for institutional or personal access. Content may require purchase if you do not have access.)

Footnotes

Contributing Editor: Edson Roberto Leite

References

REFERENCES

Online Source: Climate Change: Vital Signs of the Planet: Evidence. Available at: http://climate.nasa.gov/evidence, Climate change: how do we know? (downloaded February 2017).Google Scholar
Hori, Y.: Electrochemical CO2 reduction on metal electrodes. In Modern Aspects of Electrochemistry, Vol. 42, Vayenas, C.G., White, R.E., and Gamboa-Aldeco, M.E., eds. (Springer, New York, 2008); pp. 89−189.CrossRefGoogle Scholar
Oloman, C. and Li, H.: Electrochemical processing of carbon dioxide. ChemSusChem 1, 385 (2008).CrossRefGoogle ScholarPubMed
Hori, Y., Takahashi, I., Koga, O., and Hoshi, N.: Selective formation of C2 compounds from electrochemical reduction of CO2 at a series of copper single crystal electrodes. J. Phys. Chem. B 106, 15 (2002).CrossRefGoogle Scholar
Li, C.W. and Kanan, M.W.: CO2 reduction at low overpotential on Cu electrodes resulting from the reduction of thick Cu2O films. J. Am. Chem. Soc. 134, 7231 (2012).CrossRefGoogle ScholarPubMed
Kas, R., Kortlever, R., Milbrat, A., Koper, M.T.M., Mul, G., and Baltrusaitis, J.: Electrochemical CO2 reduction on Cu2O-derived copper nanoparticles: Controlling the catalytic selectivity of hydrocarbons. Phys. Chem. Chem. Phys. 16, 12194 (2014).CrossRefGoogle ScholarPubMed
Kim, D., Lee, S., Ocon, J.D., Jeong, B., Lee, J.K., and Lee, J.: Insights into an autonomously formed oxygen-evacuated Cu2O electrode for the selective production of C2H4 from CO2 . Phys. Chem. Chem. Phys. 17, 824 (2015).CrossRefGoogle ScholarPubMed
Chen, C.S., Handoko, A.D., Wan, J.H., Ma, L., Ren, D., and Yeo, B.S.: Stable and selective electrochemical reduction of carbon dioxide to ethylene on copper mesocrystals. Catal. Sci. Technol. 5, 161 (2015).CrossRefGoogle Scholar
Hori, Y., Murata, A., Takahashi, R., and Suzuki, S.: Electroreduction of CO to CH4 and C2H4 at a copper electrode in aqueous solutions at ambient temperature and pressure. J. Am. Chem. Soc. 109, 5023 (1987).CrossRefGoogle Scholar
DeWulf, D.W., Jin, T., and Bard, A.J.: Electrochemical and surface studies of carbon dioxide reduction to methane and ethylene at copper electrodes in aqueous solutions. J. Electrochem. Soc. 136, 1686 (1989).CrossRefGoogle Scholar
Wasmus, S., Cattaneo, E., and Vielstich, W.: Reduction of carbon dioxide to methane and ethene—an on-line MS study with rotating electrodes. Electrochim. Acta 35, 771 (1990).CrossRefGoogle Scholar
Batista, E.A. and Temperini, M.L.A.: Spectroscopic evidences of the presence of hydrogenated species on the surface of copper during CO2 electroreduction at low cathodic potentials. J. Electroanal. Chem. 629, 158 (2009).CrossRefGoogle Scholar
Cook, R.L., MacDuff, R.C., and Sammells, A.F.: High rate gas phase CO2 reduction to ethylene and methane using gas diffusion electrodes. J. Electrochem. Soc. 137, 607 (1990).CrossRefGoogle Scholar
Roberts, F.S., Kuhl, K.P., and Nilsson, A.: High selectivity for ethylene from carbon dioxide reduction over copper nanocube electrocatalysts. Angew. Chem., Int. Ed. 54, 5179 (2015).CrossRefGoogle ScholarPubMed
Reske, R., Mistry, H., Behafarid, F., Roldan Cuenya, B., and Strasser, P.: Particle size effects in the catalytic electroreduction of CO2 on Cu nanoparticles. J. Am. Chem. Soc. 136, 6978 (2014).CrossRefGoogle ScholarPubMed
Mistry, H., Varela, A.S., Bonifacio, C.S., Zegkinoglou, I., Sinev, I., Choi, Y-W., Kisslinger, K., Stach, E.A., Yang, J.C., Strasser, P., and Roldan Cuenya, B.: Corrigendum: Highly selective plasma-activated copper catalysts for carbon dioxide reduction to ethylene. Nat. Commun. 7, 12123 (2016).CrossRefGoogle Scholar
Roldan Cuenya, B. and Behafarid, F.: Nanocatalysis: Size- and shape-dependent chemisorption and catalytic reactivity. Surf. Sci. Rep. 70, 135 (2015).CrossRefGoogle Scholar
Homayuni, H., Chanmanee, W., de Tacconi, N.R., Dennis, B.H., and Rajeshwar, K.: Continuous flow photoelectrochemical reactor for solar conversion of carbon dioxide to alcohols. J. Electrochem. Soc. 162, E115 (2015).CrossRefGoogle Scholar
Ghadimkhani, G., de Tacconi, N.R., Chanmanee, W., Janaky, C., and Rajeshwar, K.: Efficient solar photoelectrosynthesis of methanol from carbon dioxide using hybrid CuO–Cu2O semiconductor nanorod arrays. Chem. Commun. 49, 1297 (2013).CrossRefGoogle ScholarPubMed
Rajeshwar, K., de Tacconi, N.R., Chanmanee, W., and Janaky, C.: Tailoring copper oxide semiconductor nanorod arrays for photoelectrochemical reduction of carbon dioxide to methanol. ChemPhysChem 14, 2251 (2013).CrossRefGoogle Scholar
Ferreira de Brito, J., Araujo, A.R., Rajeshwar, K., and Boldrin Zanoni, M.V.: Photoelectrochemical reduction of CO2 on Cu/Cu2O films: Product distribution and pH effects. Chem. Eng. J. 264, 302 (2015).CrossRefGoogle Scholar
Hursan, D., Kormanyos, A., Rajeshwar, K., and Janaky, C.: Polyaniline films photoelectrochemically reduce CO2 to alcohols. Chem. Commun. 52, 8858 (2016).CrossRefGoogle ScholarPubMed
Janaky, C., Hursán, D., Endrődi, B., Chanmanee, W., Roy, D., Liu, D., de Tacconi, N.R., Dennis, B.H., and Rajeshwar, K.: Electro- and photoreduction of carbon dioxide: The twain shall meet at copper oxide/copper interfaces. ACS Energy Lett. 1, 332 (2016).CrossRefGoogle Scholar
Kecsenovity, E., Endrodi, B., Papa, Z., Hernadi, K., Rajeshwar, K., and Janaky, C.: Decoration of ultralong carbon nanotubes with Cu2O nanocrystals: A hybrid platform for enhanced photoelectrochemical CO2 reduction. J. Mater. Chem. A. 4, 3139 (2016).CrossRefGoogle Scholar
Golden, T.D., Shumsky, M.G., Zhou, Y., VanderWerf, R.A., Van Leeuwen, R.A., and Switzer, J.A.: Electrochemical deposition of copper(I) oxide films. Chem. Mater. 8, 2499 (1996).CrossRefGoogle Scholar
Wang, L., de Tacconi, N.R., Chenthamarakshan, C., Rajeshwar, K., and Tao, M.: Electrodeposited copper oxide films: Effect of bath pH on grain orientation and orientation-dependent interfacial behavior. Thin Solid Films 515, 3090 (2007).CrossRefGoogle Scholar
Wu, S., Yin, Z., He, Q., Huang, X., Zhou, X., and Zhang, H.: Electrochemical deposition of semiconductor oxides on reduced graphene oxide-based flexible, transparent, and conductive electrodes. J. Phys. Chem. C 114, 11816 (2010).CrossRefGoogle Scholar
de Tacconi, N.R., Chanmanee, W., Rajeshwar, K., and Dennis, B.H.: Photoelectrochemical devices, methods, and systems with a cupric oxide/cuprous oxide coated electrode. U.S. Patent Pending. Serial Number: 15/111,621.Google Scholar
Ogura, K.: Electrochemical reduction of carbon dioxide to ethylene: Mechanistic approach. J. CO2 Util. 1, 43 (2013).CrossRefGoogle Scholar
Supplementary material: File

De Tacconi supplementary material

De Tacconi supplementary material

Download De Tacconi supplementary material(File)
File 759.1 KB