4.8 Article

Re(tBu-bpy)(CO)3Cl Supported on Multi-Walled Carbon Nanotubes Selectively Reduces CO2 in Water

Journal

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 141, Issue 43, Pages 17270-17277

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/jacs.9b08445

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Funding

  1. Internal Research and Technology Development program of the Jet Propulsion Laboratory, California Institute of Technology
  2. National Aeronautics and Space Administration
  3. National Science Foundation Major Research Instrumentation Program [CHE-1338173]
  4. Materials Science and Engineering Program at UC San Diego
  5. 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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