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Title: Rotating Disk Slurry Au Electrodeposition at Unsupported Carbon Vulcan XC-72 and Ce 3+ Impregnation for Ethanol Oxidation in Alkaline Media

Abstract

A robust electrodeposition method consisting of the rotating disk slurry electrode (RoDSE) technique to obtain Au nanoparticles highly dispersed on a conductive carbonaceous support, i.e., Vulcan XC-72R, for ethanol electrooxidation reaction in alkaline media was developed. Ceria was used as a cocatalyst using a Ce(III)-EDTA impregnation method in order to enhance the catalytic activity and improve the catalyst’s overall stability. Furthermore, the RoDSE method used to obtain highly dispersed Au nanoparticles does not require the use of a reducing agent or stabilizing agent, and the noble-metal loading was controlled by the addition and tuning of the metal precursor concentration. Inductively coupled plasma and thermogravimetric analysis indicated that the Au loading in the catalyst was 9 %. We determined the particle size and characteristic Au fcc crystal facets by X-ray diffraction. The morphology of the catalyst was also investigated using electron microscopy techniques. In addition, X-ray absorption spectroscopy was used to corroborate the presence and identify the oxidation state of Ce in the system and to observe if there are any electronic interactions within the 8 % Au/CeO x/C system. Cyclic voltammetry of electrodeposited 9 % Au/C and Ce-promoted 8 % Au/C showed a higher catalytic current density for ethanol oxidationmore » when compared with commercially available catalysts (20 % Au/C) of a higher precious metal loading. Additionally, we report a higher stability toward the ethanol electrooxidation process, which was corroborated by 1 mV/s linear sweep voltammetry and chronoamperometric studies.« less

Authors:
 [1];  [1];  [2];  [2];  [2];  [1];  [1]
  1. Univ. of Puerto Rico, San Juan, PR (United States). Dept. of Chemistry
  2. Brookhaven National Lab. (BNL), Upton, NY (United States). Chemistry Dept.
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1366354
Report Number(s):
BNL-113992-2017-JA
Journal ID: ISSN 1868-2529; R&D Project: CO009; KC0302010
Grant/Contract Number:  
SC00112704; AC02-98CH10886
Resource Type:
Accepted Manuscript
Journal Name:
Electrocatalysis
Additional Journal Information:
Journal Volume: 8; Journal Issue: 2; Journal ID: ISSN 1868-2529
Publisher:
Springer
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 36 MATERIALS SCIENCE; Au nanoparticles; ceria; nanomaterials; ethanol oxidation; RoDSE

Citation Formats

Betancourt, Luis E., Guzman-Blas, Rolando, Luo, Si, Stacchiola, Dario J., Senanayake, Sanjaya D., Guinel, Maxime, and Cabrera, Carlos R. Rotating Disk Slurry Au Electrodeposition at Unsupported Carbon Vulcan XC-72 and Ce3+ Impregnation for Ethanol Oxidation in Alkaline Media. United States: N. p., 2016. Web. doi:10.1007/s12678-016-0342-x.
Betancourt, Luis E., Guzman-Blas, Rolando, Luo, Si, Stacchiola, Dario J., Senanayake, Sanjaya D., Guinel, Maxime, & Cabrera, Carlos R. Rotating Disk Slurry Au Electrodeposition at Unsupported Carbon Vulcan XC-72 and Ce3+ Impregnation for Ethanol Oxidation in Alkaline Media. United States. doi:10.1007/s12678-016-0342-x.
Betancourt, Luis E., Guzman-Blas, Rolando, Luo, Si, Stacchiola, Dario J., Senanayake, Sanjaya D., Guinel, Maxime, and Cabrera, Carlos R. Sat . "Rotating Disk Slurry Au Electrodeposition at Unsupported Carbon Vulcan XC-72 and Ce3+ Impregnation for Ethanol Oxidation in Alkaline Media". United States. doi:10.1007/s12678-016-0342-x. https://www.osti.gov/servlets/purl/1366354.
@article{osti_1366354,
title = {Rotating Disk Slurry Au Electrodeposition at Unsupported Carbon Vulcan XC-72 and Ce3+ Impregnation for Ethanol Oxidation in Alkaline Media},
author = {Betancourt, Luis E. and Guzman-Blas, Rolando and Luo, Si and Stacchiola, Dario J. and Senanayake, Sanjaya D. and Guinel, Maxime and Cabrera, Carlos R.},
abstractNote = {A robust electrodeposition method consisting of the rotating disk slurry electrode (RoDSE) technique to obtain Au nanoparticles highly dispersed on a conductive carbonaceous support, i.e., Vulcan XC-72R, for ethanol electrooxidation reaction in alkaline media was developed. Ceria was used as a cocatalyst using a Ce(III)-EDTA impregnation method in order to enhance the catalytic activity and improve the catalyst’s overall stability. Furthermore, the RoDSE method used to obtain highly dispersed Au nanoparticles does not require the use of a reducing agent or stabilizing agent, and the noble-metal loading was controlled by the addition and tuning of the metal precursor concentration. Inductively coupled plasma and thermogravimetric analysis indicated that the Au loading in the catalyst was 9 %. We determined the particle size and characteristic Au fcc crystal facets by X-ray diffraction. The morphology of the catalyst was also investigated using electron microscopy techniques. In addition, X-ray absorption spectroscopy was used to corroborate the presence and identify the oxidation state of Ce in the system and to observe if there are any electronic interactions within the 8 % Au/CeOx/C system. Cyclic voltammetry of electrodeposited 9 % Au/C and Ce-promoted 8 % Au/C showed a higher catalytic current density for ethanol oxidation when compared with commercially available catalysts (20 % Au/C) of a higher precious metal loading. Additionally, we report a higher stability toward the ethanol electrooxidation process, which was corroborated by 1 mV/s linear sweep voltammetry and chronoamperometric studies.},
doi = {10.1007/s12678-016-0342-x},
journal = {Electrocatalysis},
number = 2,
volume = 8,
place = {United States},
year = {2016},
month = {11}
}

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