Journal
ACS CATALYSIS
Volume 4, Issue 10, Pages 3621-3629Publisher
AMER CHEMICAL SOC
DOI: 10.1021/cs500628m
Keywords
PtRh nanoclusters; methanol oxidation; mass activity; activation energy; durability
Categories
Funding
- Board of Research in Nuclear Sciences (BRNS), Department of Atomic Energy (DAE), Govt. of India, under Basic Sciences program [2009/37/29/BRNS]
- SCSVMV University
- CSIR, New Delhi [09/1104(0001)/2013-EMR-I]
- Operational Program Research and Development for Innovations-European Regional Development Fund of the Ministry of Education, Youth and Sports of the Czech Republic [CZ.1.05/2.1.00/03.0058]
- Operational Program Education for Competitiveness-European Social Fund of the Ministry of Education, Youth and Sports of the Czech Republic [CZ.1.07/2.3.00/30.0004]
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The supportless PtRh nanoclusters (Pt3Rh NC) were prepared using formic acid reductant. High-resolution transmission electron microscopy (HRTEM) showed individual particle sizes less than 7 nm, and energy-dispersive X-ray (EDX) analysis confirmed a 3:1 ratio of Pt and Rh. The as-prepared Pt3Rh NC exhibited an improved activity and durability toward electrocatalytic oxidation of methanol (MOR) and possesses greater CO tolerance than conventional PtRu and other Pt-based MOR catalysts. For comparison, the Vulcan carbon supported (Pt3Rh NC/VC) catalyst was prepared under identical conditions and used for MOR. The supportless Pt3Rh NC catalyst possessed mass activity of 1392.5 mA mg(-1) with an I-f/I-b ratio of 2.61, which is nearly 3-fold higher than the Pt3Rh NC/VC and also comparable to the benchmark MOR catalysts. The surface poisoning rate was found to be relatively smaller compared to the standard PtRu/C catalysts (delta = 0.0044% s(-1)). The activation energy for MOR was found to be 22.5 kJ mol(-1). The durability study for 4000 potential cycles in an acidic solution showed that nearly 78% of mass activity has been retained. The supportless Pt3Rh NC has much improved activity and stability compared to both Pt3Rh NC/VC and standard PtRu MOR catalysts. Therefore, the supportless Pt3Rh NC could be seen as a potential electrocatalyst for methanol oxidation due to high activity, enhanced stability, and diminished poisoning of the Pt surface, which is stabilized in the presence of Rh in nanocluster morphology.
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