CO2 Reduction Selective for C≥2 Products
on Polycrystalline Copper with N‑Substituted Pyridinium
Additives
Version 3 2017-08-23, 04:20
Version 2 2017-07-21, 20:29
Version 1 2017-07-21, 19:46
Posted on 2017-08-23 - 04:20
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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Han, Zhiji; Kortlever, Ruud; Chen, Hsiang-Yun; Peters, Jonas C.; Agapie, Theodor (2017). CO2 Reduction Selective for C≥2 Products
on Polycrystalline Copper with N‑Substituted Pyridinium
Additives. ACS Publications. Collection. https://doi.org/10.1021/acscentsci.7b00180
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AUTHORS (5)
ZH
Zhiji Han
RK
Ruud Kortlever
HC
Hsiang-Yun Chen
JP
Jonas C. Peters
TA
Theodor Agapie