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甲醇在Pt-Co(111)/C表面吸附和分解的量子化学研究

, PP. 263-269

Keywords: 甲醇,Pt-Co(111)/C表面,密度泛函理论,电子结构,过渡态

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Abstract:

采用密度泛函理论和周期平板模型相结合的方法,对CH3OH分子在Pt-Co(111)/C表面top、fcc、hcp和bridge位的9种吸附模型进行了构型优化、能量计算,结果表明fcc-Pt2Co位是较有利的吸附位.Co掺杂后整个体系的态密度略向低能方向移动,费米能级的位置发生了右移导带增宽,表明掺杂后的Pt/C具有更强的氧化能力.考虑催化剂抗中毒性能时发现CO在Pt-Co(111)/C表面的吸附能比相应各位置上甲醇的吸附能均要低,说明Pt-Co(111)/C确实具有较好的抗CO中毒化能力;甲醇在Pt-Co(111)/C表面的解离过程也发现该催化剂使得甲醇催化氧化反应的进行比在气相中断裂H—O键所需要的能量降低了296.0kJ/mol,说明在Pt-Co(111)/C面反应较容易发生,因此碳负载Pt-Co合金是催化氧化甲醇较好的催化剂.

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