A theoretical simulation on the catalytic oxidation of CO on Pt/graphene.
A theoretical simulation on the catalytic oxidation of CO on Pt/graphene.
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DOI：
10.1039/c2cp41441d
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发表时间：
2012-11
期刊：
影响因子：
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通讯作者：
Yanan Tang;Zongxian Yang;X. Dai
中科院分区：
文献类型：
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作者：
Yanan Tang;Zongxian Yang;X. Dai
用基于密度泛函理论的第一性原理方法研究了CO在铂/X-石墨烯上的催化氧化反应。与原始石墨烯上的铂原子相比，石墨烯中的空位缺陷强烈地稳定了单个铂吸附原子，使铂吸附原子更带正电，有助于削弱CO吸附，促进O(2)吸附，从而提高了CO氧化活性，缓解了铂催化剂的CO中毒。在铂/SV-石墨烯上的CO氧化反应具有较低的能垒(0.58eV)，该反应是通过朗缪尔-辛谢尔伍德(L H)反应(CO+O(2)→OOCO→CO(2)+O(ADS)+O(ADS))进行的，然后是Eley-RIdeal(ER)反应，能垒为0.59eV(CO+O(ADS)→CO(2))。这些结果验证了催化剂在原子尺度上的反应活性，为制备低成本、高活性的碳基催化剂提供了线索。
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 → CO(2) + O(ads)) which is followed by the Eley-Rideal (ER) reaction with an energy barrier of 0.59 eV (CO + O(ads)→ CO(2)). 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.