Journal
CHINESE JOURNAL OF CHEMICAL PHYSICS
Volume 27, Issue 5, Pages 541-547Publisher
CHINESE PHYSICAL SOC
DOI: 10.1063/1674-0068/27/05/541-547
Keywords
Differential electrochemical mass spectrometry; Electrochemical in situ infrared spectroscopy; Methanol oxidation; PtRu electrode; Current efficiency
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Funding
- National Natural Science Foundation of China [21273215]
- National Instrumentation Program [2011YQ03012416]
- Major State Basic Research Development Program of China [2010CB923302]
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Methanol oxidation reaction (MOR) at Pt and Pt electrode surface deposited with various amounts of Ru (denoted as PtxRuy, nominal coverage y is 0.17, 0.27, and 0.44 ML) in 0.1 mol/L HClO4+0.5 mol/L MeOH has been studied under potentiostatic conditions by in situ FTIR spectroscopy in attenuated-total-reflection configuration and differential electrochemical mass spectrometry under controlled flow conditions. Results reveal that (1) CO is the only methanol-related adsorbate observed by IR spectroscopy at all the Pt and PtRu electrodes examined at potentials from 0.3 V to 0.6 V (vs. RHE); (ii) at Pt0.56Ru0.44, two IR bands, one from CO adsorbed at Ru islands and the other from COL at Pt substrate are detected, while at other electrodes, only a single band for COL adsorbed at Pt is observed; (iii) MOR activity decreases in the order of Pt0.73Ru0.27>Pt0.56Ru0.44>Pt0.83Ru0.17>Pt; (iv) at 0.5 V, MOR at Pt0.73Ru0.27 reaches a current efficiency of 50% for CO2 production, the turn-over frequency from CH3OH to CO2 is ca. 0.1 molecule/(site.sec). Suggestions for further improving of PtRu catalysts for MOR are provided.
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