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Title: Efficient Conversion of CO2 to CO Using Tin and Other Inexpensive and Easily Prepared Post-Transition Metal Catalysts

Abstract

The development of affordable electrocatalysts that can drive the reduction of CO2 to CO with high selectivity, efficiency, and large current densities is a critical step on the path to production of liquid carbon-based fuels. In this work, we show that inexpensive triflate salts of Sn2+, Pb2+, Bi3+, and Sb3+ can be used as precursors for the electrodeposition of CO2 reduction cathode materials from MeCN solutions, providing a general and facile electrodeposition strategy, which streamlines catalyst synthesis. The ability of these four platforms to drive the formation of CO from CO2 in the presence of [BMIM]OTf was probed. The electrochemically prepared Sn and Bi catalysts proved to be highly active, selective, and robust platforms for CO evolution, with partial current densities of jCO = 5-8 mA/cm2 at applied overpotentials of η < 250 mV. By contrast, the electrodeposited Pb and Sb catalysts do not promote rapid CO generation with the same level of selectivity. The Pb material is only ~10% as active as the Sn and Bi systems at an applied potential of E = -1.95 V and is rapidly passivated during catalysis. The Sb-comprised cathode material shows no activity for conversion of CO2 to CO under analogous conditions. Whenmore » taken together, this work demonstrates that 1,3-dialkylimidazoliums can promote CO production, but only when used in combination with an appropriately chosen electrocatalyst material. More broadly, these results suggest that the interactions between CO2, the imidazolium promoter, and the cathode surface are all critical to the observed catalysis.« less

Authors:
 [1];  [1];  [1];  [1];  [1]
+ Show Author Affiliations
  1. Univ. of Delaware, Newark, DE (United States). Dept. of Chemistry and Biochemistry
Publication Date:
Research Org.:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1265435
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
Journal of the American Chemical Society
Additional Journal Information:
Journal Volume: 137; Journal Issue: 15; Journal ID: ISSN 0002-7863
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Medina-Ramos, Jonnathan, Pupillo, Rachel C., Keane, Thomas P., DiMeglio, John L., and Rosenthal, Joel. Efficient Conversion of CO2 to CO Using Tin and Other Inexpensive and Easily Prepared Post-Transition Metal Catalysts. United States: N. p., 2015. Web. doi:10.1021/ja5121088.
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Medina-Ramos, Jonnathan, Pupillo, Rachel C., Keane, Thomas P., DiMeglio, John L., & Rosenthal, Joel. Efficient Conversion of CO2 to CO Using Tin and Other Inexpensive and Easily Prepared Post-Transition Metal Catalysts. United States. https://doi.org/10.1021/ja5121088
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Medina-Ramos, Jonnathan, Pupillo, Rachel C., Keane, Thomas P., DiMeglio, John L., and Rosenthal, Joel. Thu . "Efficient Conversion of CO2 to CO Using Tin and Other Inexpensive and Easily Prepared Post-Transition Metal Catalysts". United States. https://doi.org/10.1021/ja5121088. https://www.osti.gov/servlets/purl/1265435.
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@article{osti_1265435,
title = {Efficient Conversion of CO2 to CO Using Tin and Other Inexpensive and Easily Prepared Post-Transition Metal Catalysts},
author = {Medina-Ramos, Jonnathan and Pupillo, Rachel C. and Keane, Thomas P. and DiMeglio, John L. and Rosenthal, Joel},
abstractNote = {The development of affordable electrocatalysts that can drive the reduction of CO2 to CO with high selectivity, efficiency, and large current densities is a critical step on the path to production of liquid carbon-based fuels. In this work, we show that inexpensive triflate salts of Sn2+, Pb2+, Bi3+, and Sb3+ can be used as precursors for the electrodeposition of CO2 reduction cathode materials from MeCN solutions, providing a general and facile electrodeposition strategy, which streamlines catalyst synthesis. The ability of these four platforms to drive the formation of CO from CO2 in the presence of [BMIM]OTf was probed. The electrochemically prepared Sn and Bi catalysts proved to be highly active, selective, and robust platforms for CO evolution, with partial current densities of jCO = 5-8 mA/cm2 at applied overpotentials of η < 250 mV. By contrast, the electrodeposited Pb and Sb catalysts do not promote rapid CO generation with the same level of selectivity. The Pb material is only ~10% as active as the Sn and Bi systems at an applied potential of E = -1.95 V and is rapidly passivated during catalysis. The Sb-comprised cathode material shows no activity for conversion of CO2 to CO under analogous conditions. When taken together, this work demonstrates that 1,3-dialkylimidazoliums can promote CO production, but only when used in combination with an appropriately chosen electrocatalyst material. More broadly, these results suggest that the interactions between CO2, the imidazolium promoter, and the cathode surface are all critical to the observed catalysis.},
doi = {10.1021/ja5121088},
journal = {Journal of the American Chemical Society},
number = 15,
volume = 137,
place = {United States},
year = {Thu Feb 19 00:00:00 EST 2015},
month = {Thu Feb 19 00:00:00 EST 2015}
}
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