A theoretical simulation on the catalytic oxidation of CO on Pt/graphene

作者：Tang, Yanan; Yang, Zongxian^*; Dai, Xianqi

来源：Physical Chemistry Chemical Physics, 2012, 14(48): 16566-16572.

DOI：10.1039/c2cp41441d

• ENHANCED ELECTROCATALYTIC ACTIVITY
• TOTAL-ENERGY CALCULATIONS
• ELASTIC BAND METHOD
• CARBON NANOTUBES
• METAL ATOMS
• GRAPHENE
• NANOSTRUCTURES
• IMPURITIES
• REDUCTION
• CLUSTER

The catalytic oxidation of CO on Pt/X-graphene (X = "pri" for pristine-or "SV" for defective-graphene with a single vacancy) is investigated using the first-principles method based on density functional theory. In contrast to a Pt atom on pristine graphene, a vacancy defect in graphene strongly stabilizes a single Pt adatom and makes the Pt adatom more positively charged, which helps to weaken the CO adsorption and facilitates the O-2 adsorption, thus enhancing the activity for CO oxidation and alleviating the CO poisoning of the platinum catalysts. The CO oxidation reaction on Pt/SV-graphene has a low energy barrier (0.58 eV) by the Langmuir-Hinshelwood (LH) reaction (CO + O-2 -> OOCO -> CO2 + O-ads) which is followed by the Eley-Rideal (ER) reaction with an energy barrier of 0.59 eV (CO + O-ads -> CO2). The results validate the reactivity of catalysts on the atomic-scale and initiate a clue for fabricating carbon-based catalysts with low cost and high activity.

• 出版日期2012
• 单位河南师范大学