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

Abstract

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

Authors:
 [1];  [2];  [3];  [1];  [1];  [4];  [1];  [5];  [1]
+ Show Author Affiliations
  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:
Research Org.:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS); Energy Frontier Research Centers (EFRC) (United States). Fluid Interface Reactions, Structures and Transport Center (FIRST)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1302937
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
ACS Catalysis
Additional Journal Information:
Journal Volume: 6; Journal Issue: 9; Journal ID: ISSN 2155-5435
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
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

Citation Formats

Zhang, Zhiyong, Chi, Miaofang, Veith, Gabriel M., Zhang, Pengfei, Lutterman, Daniel A., Rosenthal, Joel, Overbury, Steven H., Dai, Sheng, and Zhu, Huiyuan. Rational Design of Bi Nanoparticles for Efficient Electrochemical CO2 Reduction: The Elucidation of Size and Surface Condition Effects. United States: N. p., 2016. Web. doi:10.1021/acscatal.6b01297.
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Zhang, Zhiyong, Chi, Miaofang, Veith, Gabriel M., Zhang, Pengfei, Lutterman, Daniel A., Rosenthal, Joel, Overbury, Steven H., Dai, Sheng, & Zhu, Huiyuan. Rational Design of Bi Nanoparticles for Efficient Electrochemical CO2 Reduction: The Elucidation of Size and Surface Condition Effects. United States. https://doi.org/10.1021/acscatal.6b01297
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Zhang, Zhiyong, Chi, Miaofang, Veith, Gabriel M., Zhang, Pengfei, Lutterman, Daniel A., Rosenthal, Joel, Overbury, Steven H., Dai, Sheng, and Zhu, Huiyuan. Mon . "Rational Design of Bi Nanoparticles for Efficient Electrochemical CO2 Reduction: The Elucidation of Size and Surface Condition Effects". United States. https://doi.org/10.1021/acscatal.6b01297. https://www.osti.gov/servlets/purl/1302937.
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@article{osti_1302937,
title = {Rational Design of Bi Nanoparticles for Efficient Electrochemical CO2 Reduction: The Elucidation of Size and Surface Condition Effects},
author = {Zhang, Zhiyong and Chi, Miaofang and Veith, Gabriel M. and Zhang, Pengfei and Lutterman, Daniel A. and Rosenthal, Joel and Overbury, Steven H. and Dai, Sheng and Zhu, Huiyuan},
abstractNote = {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 and paves the way for understanding the CO2 electrochemical reduction mechanism in nonaqueous media.},
doi = {10.1021/acscatal.6b01297},
journal = {ACS Catalysis},
number = 9,
volume = 6,
place = {United States},
year = {Mon Aug 08 00:00:00 EDT 2016},
month = {Mon Aug 08 00:00:00 EDT 2016}
}
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https://doi.org/10.1021/acscatal.6b01297
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