Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 141, Issue 43, Pages 17270-17277Publisher
AMER CHEMICAL SOC
DOI: 10.1021/jacs.9b08445
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Funding
- Internal Research and Technology Development program of the Jet Propulsion Laboratory, California Institute of Technology
- National Aeronautics and Space Administration
- National Science Foundation Major Research Instrumentation Program [CHE-1338173]
- Materials Science and Engineering Program at UC San Diego
- IARPA [2018-18071700005]
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The selective electrochemical reduction of CO2 to CO in water by a Re(tBu-bpy)(CO)(3)Cl catalyst incorporated into multi-walled carbon nanotubes (MWCNT) was investigated. Current densities of similar to 4 mA/cm(2) and selectivities (FECO) of 99% were achieved at -0.56 V vs RHE in CO2-saturated aqueous KHCO3 solutions. The Re(tBu-bpy)(CO)(3)Cl catalyst has been widely studied as a homogeneous catalyst in organic solvents. Supporting Re(tBu-bpy)(CO)(3)Cl on MVVCNTs increases current densities, decreases overpotential, retains selectivity for reduction of CO2 to CO, and allows operation in water at pH = 7.3 compared to the molecular catalyst in acetonitrile solution. The Re/MWCNT electrocatalysts achieve TON > 5600 and TOF > 1.6 s(-1). This electrocatalyst material is efficient, robust, simple to prepare, and scalable.
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