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This content will become publicly available on August 8, 2017

Title: Rational Design of Bi Nanoparticles for Efficient Electrochemical CO2 Reduction: The Elucidation of Size and Surface Condition Effects

Here we report an efficient electrochemical conversion of CO2 to CO on surface-activated bismuth nanoparticles (NPs) in acetonitrile (MeCN) under ambient conditions, with the assistance of 1-butyl-3-methylimidazolium trifluoromethanesulfonate ([bmim][OTf]). Through the comparison between electrodeposited Bi films (Bi-ED) and different types of Bi NPs, we, for the first time, demonstrate the effects of catalyst’s size and surface condition on organic phase electrochemical CO2 reduction. Our study reveals that the surface inhibiting layer (hydrophobic surfactants and Bi3+ species) formed during the synthesis and purification process hinders the CO2 reduction, leading to a 20% drop in Faradaic efficiency for CO evolution (FECO). Bi particle size showed a significant effect on FECO when the surface of Bi was air-oxidized, but this effect of size on FECO became negligible on surface-activated Bi NPs. After the surface activation (hydrazine treatment) that effectively removed the native inhibiting layer, activated 36-nm Bi NPs exhibited an almost-quantitative conversion of CO2 to CO (96.1% FECO), and a mass activity for CO evolution (MACO) of 15.6 mA mg–1, which is three-fold higher than the conventional Bi-ED, at ₋2.0 V (vs Ag/AgCl). Ultimately, this work elucidates the importance of the surface activation for an efficient electrochemical CO2 conversion on metal NPs andmore » paves the way for understanding the CO2 electrochemical reduction mechanism in nonaqueous media.« less
 [1] ;  [2] ;  [3] ;  [1] ;  [1] ;  [4] ;  [1] ;  [5] ;  [1]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical Sciences Division
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Science (CNMS)
  3. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science & Technology Division
  4. Univ. of Delaware, Newark, DE (United States). Dept. of Chemistry and Biochemistry
  5. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical Sciences Division; Univ. of Tennessee, Knoxville, TN (United States). Dept. of Chemistry
Publication Date:
OSTI Identifier:
Grant/Contract Number:
Accepted Manuscript
Journal Name:
ACS Catalysis
Additional Journal Information:
Journal Volume: 6; Journal Issue: 9; Journal ID: ISSN 2155-5435
American Chemical Society
Research Org:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 36 MATERIALS SCIENCE; 30 DIRECT ENERGY CONVERSION Keywords: bismuth nanoparticle; CO; electrochemical CO2 reduction; ionic liquid; surface activation