CO2 Reduction Selective for C≥2 Products on Polycrystalline Copper with N-Substituted Pyridinium Additives
نویسندگان
چکیده
Electrocatalytic CO2 reduction to generate multicarbon products is of interest for applications in artificial photosynthetic schemes. This is a particularly attractive goal for CO2 reduction by copper electrodes, where a broad range of hydrocarbon products can be generated but where selectivity for C-C coupled products relative to CH4 and H2 remains an impediment. Herein we report a simple yet highly selective catalytic system for CO2 reduction to C≥2 hydrocarbons on a polycrystalline Cu electrode in bicarbonate aqueous solution that uses N-substituted pyridinium additives. Selectivities of 70-80% for C2 and C3 products with a hydrocarbon ratio of C≥2/CH4 significantly greater than 100 have been observed with several additives. 13C-labeling studies verify CO2 to be the sole carbon source in the C≥2 hydrocarbons produced. Upon electroreduction, the N-substituted pyridinium additives lead to film deposition on the Cu electrode, identified in one case as the reductive coupling product of N-arylpyridinium. Product selectivity can also be tuned from C≥2 species to H2 (∼90%) while suppressing methane with certain N-heterocyclic additives.
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© 2018 Macmillan Publishers Limited, part of Springer Nature. All rights reserved. 1Rowland Institute, Harvard University, Cambridge, MA, USA. 2SUNCAT Center for Interface Science and Catalysis, Department of Chemical Engineering, Stanford University, Stanford, CA, USA. 3Center for Nanoscale Systems, Harvard University, Cambridge, MA, USA. 4Harvard John A. Paulson School of Engineering and Appl...
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عنوان ژورنال:
دوره 3 شماره
صفحات -
تاریخ انتشار 2017