Electroreduction of CO2 on polycrystalline copper: Effect of temperature on product selectivity

作者: Steven T. Ahn , Ismael Abu-Baker , G.Tayhas R. Palmore

DOI: 10.1016/J.CATTOD.2016.09.028

关键词:

摘要: Abstract In this paper, we investigate the effect of temperature on product selectivity for electrochemical reduction carbon dioxide (CO2) polycrystalline copper (Cu). We show that an electrolyte solution can influence several reaction parameters in CO2 (CO2RR), including pH (both local and bulk), concentration dissolved ([CO2]), resistance, rate diffusion reactants to electrode surface, adsorbed intermediates. The working potential was −1.60 V vs. Ag/AgCl allow direct comparison with literature values. Under optimal conditions at 2 °C, faradaic efficiency (FE) converting methane (CH4) a Cu electrocatalyst increases ca. 50% while ethylene (C2H4) decreases 10%. Above room temperature, production hydrogen gas (H2) dominates reaction, reaching >50% FE. major products (i.e., >5% FE) observed all temperatures studied were H2, CH4, C2H4, monoxide, formate, driven by changes [CO2] rather than pH. Our initial goal confirm dependence CO2RR different temperatures. Importantly, discovered varies minimally over range (2 °C 42 °C), contrast corresponding selectivity.

参考文章(40)
Ana Sofia Varela, Matthias Kroschel, Tobias Reier, Peter Strasser, Controlling the selectivity of CO2 electroreduction on copper: The effect of the electrolyte concentration and the importance of the local pH Catalysis Today. ,vol. 260, pp. 8- 13 ,(2016) , 10.1016/J.CATTOD.2015.06.009
Paul T. Anastas, John Charles Warner, Green Chemistry: Theory and Practice ,(1998)
Sujat Sen, Dan Liu, G. Tayhas R. Palmore, Electrochemical reduction of co2 at copper nanofoams ACS Catalysis. ,vol. 4, pp. 3091- 3095 ,(2014) , 10.1021/CS500522G
Masashi Azuma, Kazuhito Hashimoto, Masahiro Hiramoto, Masahiro Watanabe, Tadayoshi Sakata, Electrochemical Reduction of Carbon Dioxide on Various Metal Electrodes in Low‐Temperature Aqueous KHCO 3 Media Journal of The Electrochemical Society. ,vol. 137, pp. 1772- 1778 ,(1990) , 10.1149/1.2086796
David W. DeWulf, Tuo Jin, Allen J. Bard, Electrochemical and Surface Studies of Carbon Dioxide Reduction to Methane and Ethylene at Copper Electrodes in Aqueous Solutions Journal of The Electrochemical Society. ,vol. 136, pp. 1686- 1691 ,(1989) , 10.1149/1.2096993
K. J. P. Schouten, Y. Kwon, C. J. M. van der Ham, Z. Qin, M. T. M. Koper, A new mechanism for the selectivity to C1 and C2 species in the electrochemical reduction of carbon dioxide on copper electrodes Chemical Science. ,vol. 2, pp. 1902- 1909 ,(2011) , 10.1039/C1SC00277E
Allen J Bard, Larry R Faulkner, Henry S White, Electrochemical Methods: Fundamentals and Applications ,(1980)
Chi Shing Wong, Pavel Ya. Tishchenko, Wm. Keith Johnson, Solubility of carbon dioxide in aqueous HCl and NaHCO3 solutions from 278 to 298 K Journal of Chemical & Engineering Data. ,vol. 50, pp. 817- 821 ,(2005) , 10.1021/JE049716Q
John J. Carroll, John D. Slupsky, Alan E. Mather, The Solubility of Carbon Dioxide in Water at Low Pressure Journal of Physical and Chemical Reference Data. ,vol. 20, pp. 1201- 1209 ,(1991) , 10.1063/1.555900
Chung Shou Chen, Albertus D. Handoko, Jane Hui Wan, Liang Ma, Dan Ren, Boon Siang Yeo, Stable and selective electrochemical reduction of carbon dioxide to ethylene on copper mesocrystals Catalysis Science & Technology. ,vol. 5, pp. 161- 168 ,(2015) , 10.1039/C4CY00906A