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Effect of mass transport on the electrochemical oxidation of alcohols over electrodeposited film and carbon-supported Pt electrodes

Effect of mass transport on the electrochemical oxidation of alcohols over electrodeposited film and carbon-supported Pt electrodes
Effect of mass transport on the electrochemical oxidation of alcohols over electrodeposited film and carbon-supported Pt electrodes

Electrochemical oxidation of four different alcohol molecules (methanol, ethanol, n-butanol and 2-butanol) at electrodeposited Pt film and carbon-supported Pt catalyst film electrodes, as well as the effect of mass transport on the oxidation reaction, has been studied systematically using the rotating disk electrode (RDE) technique. It was shown that oxidation current decreased with an increase in the rotation rate (ω) for all alcohols studied over electrodeposited Pt film electrodes. In contrast, the oxidation current was found to increase with an increase in the ω for Pt/C in ethanol and n-butanol-containing solutions. The decrease was found to be nearly reversible for ethanol and n-butanol at the electrodeposited Pt film electrode ruling out the possibility of intermediate COads poisoning being the sole cause of the decrease and was attributed to the formation of soluble intermediate species which diffuse away from the electrode at higher ω. In contrast, an increase in the current with an increase in ω for the carbon supported catalyst may suggest that the increase in residence time of the soluble species within the catalyst layer, results in further oxidation of these species. Furthermore, the reversibility of the peak current on decreasing the ω could indicate that the surface state has not significantly changed due to the sluggish reaction kinetics of ethanol and n-butanol.

Butanol, Direct alcohol fuel cells, Electro-oxidation, Ethanol, Methanol, Platinum, Rotating disk electrode (RDE)
1022-5528
1-14
Puthiyapura, Vinod Kumar
4787348f-d97a-4288-a9a7-b0c61866f823
Lin, Wen Feng
f8c1c1b5-1bef-41e7-959e-d80429abd13c
Russell, Andrea E.
b6b7c748-efc1-4d5d-8a7a-8e4b69396169
Brett, Dan J.L.
652e18b5-dad8-4dc4-bed4-9810052ad27b
Hardacre, Christopher
0715f59a-c82e-4844-a9f8-6a06fb36320f
Puthiyapura, Vinod Kumar
4787348f-d97a-4288-a9a7-b0c61866f823
Lin, Wen Feng
f8c1c1b5-1bef-41e7-959e-d80429abd13c
Russell, Andrea E.
b6b7c748-efc1-4d5d-8a7a-8e4b69396169
Brett, Dan J.L.
652e18b5-dad8-4dc4-bed4-9810052ad27b
Hardacre, Christopher
0715f59a-c82e-4844-a9f8-6a06fb36320f

Puthiyapura, Vinod Kumar, Lin, Wen Feng, Russell, Andrea E., Brett, Dan J.L. and Hardacre, Christopher (2018) Effect of mass transport on the electrochemical oxidation of alcohols over electrodeposited film and carbon-supported Pt electrodes. Topics in Catalysis, 1-14. (doi:10.1007/s11244-018-0893-6).

Record type: Article

Abstract

Electrochemical oxidation of four different alcohol molecules (methanol, ethanol, n-butanol and 2-butanol) at electrodeposited Pt film and carbon-supported Pt catalyst film electrodes, as well as the effect of mass transport on the oxidation reaction, has been studied systematically using the rotating disk electrode (RDE) technique. It was shown that oxidation current decreased with an increase in the rotation rate (ω) for all alcohols studied over electrodeposited Pt film electrodes. In contrast, the oxidation current was found to increase with an increase in the ω for Pt/C in ethanol and n-butanol-containing solutions. The decrease was found to be nearly reversible for ethanol and n-butanol at the electrodeposited Pt film electrode ruling out the possibility of intermediate COads poisoning being the sole cause of the decrease and was attributed to the formation of soluble intermediate species which diffuse away from the electrode at higher ω. In contrast, an increase in the current with an increase in ω for the carbon supported catalyst may suggest that the increase in residence time of the soluble species within the catalyst layer, results in further oxidation of these species. Furthermore, the reversibility of the peak current on decreasing the ω could indicate that the surface state has not significantly changed due to the sluggish reaction kinetics of ethanol and n-butanol.

Text s11244-018-0893-6 - Version of Record
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Accepted/In Press date: 19 January 2018
e-pub ahead of print date: 19 January 2018
Keywords: Butanol, Direct alcohol fuel cells, Electro-oxidation, Ethanol, Methanol, Platinum, Rotating disk electrode (RDE)

Identifiers

Local EPrints ID: 417438
URI: https://eprints.soton.ac.uk/id/eprint/417438
ISSN: 1022-5528
PURE UUID: ae0046b7-0871-4db1-b63c-7f37af2476da
ORCID for Andrea E. Russell: ORCID iD orcid.org/0000-0002-8382-6443

Catalogue record

Date deposited: 31 Jan 2018 17:30
Last modified: 06 Jun 2018 12:58

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Contributors

Author: Vinod Kumar Puthiyapura
Author: Wen Feng Lin
Author: Dan J.L. Brett
Author: Christopher Hardacre

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