Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 137, Issue 14, Pages 4701-4708Publisher
AMER CHEMICAL SOC
DOI: 10.1021/ja511890h
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Funding
- Stanford University
- Hellman Foundation
- NSF [CHE-1266401]
- Stanford Office of Technology
- Direct For Mathematical & Physical Scien [1266401] Funding Source: National Science Foundation
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Electrochemical reduction of CO2 to formate (HCO2-) powered by renewable electricity is a possible carbon-negative alternative to synthesizing formate from fossil fuels. This process is energetically inefficient because >1 V of overpotential is required for CO2 reduction to HCO2- on the metals currently used as cathodic catalysts. Pd reduces CO2 to HCO2- with no overpotential, but this activity has previously been limited to low synthesis rates and plagued by an unidentified deactivation pathway. Here we show that Pd nanoparticles dispersed on a carbon support reach high mass activities (50-80 mA HCO2- synthesis per mg Pd) when driven by less than 200 mV of overpotential in aqueous bicarbonate solutions. Electrokinetic measurements are consistent with a mechanism in which the rate-determining step is the addition of electrochemically generated surface adsorbed hydrogen to CO2 (i.e., electrohydrogenation). The electrodes deactivate over the course of several hours because of a minor pathway that forms CO. Activity is recovered, however, by removing CO with brief air exposure.
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