一氧化碳分子在Pt/t-ZrO<sub>2</sub>(101)表面的吸附性质

引用本文: 满梅玲, 陆春海, 陈文凯, 李奕, 章永凡. 一氧化碳分子在Pt/t-ZrO₂(101)表面的吸附性质[J]. 物理化学学报, 2012, 28(01): 51-57. doi: 10.3866/PKU.WHXB20122851 shu

Citation: MAN Mei-Ling, LU Chun-Hai, CHEN Wen-Kai, LI Yi, ZHANG Yong-Fan. Adsorption Properties of CO Molecules on Pt/t-ZrO₂(101) Surfaces[J]. Acta Physico-Chimica Sinica, 2012, 28(01): 51-57. doi: 10.3866/PKU.WHXB20122851 shu

一氧化碳分子在Pt/t-ZrO₂(101)表面的吸附性质

基金项目:
国家自然科学基金(90922022) (90922022)

福建省高等学校新世纪优秀人才计划(HX2006-103)资助项目 (HX2006-103)

摘要: 运用广义梯度密度泛函理论(GGA-PW91)结合周期平板模型方法, 研究了CO分子在完整与Pt 负载的四方ZrO₂(101)表面的吸附行为. 结果表明: 表面第二层第二氧位和表面第二桥位分别为CO分子和Pt 原子在完整ZrO₂(101)表面的稳定吸附位, 且覆盖度为0.25 ML (monolayer)时均为稳定吸附构型, 吸附能分别为56.2和352.7 kJ·mol^-1. CO分子在负载表面的稳定吸附模式为C-end吸附, 吸附能为323.8 kJ·mol^-1. 考察了CO分子在负载表面吸附前后的振动频率、态密度和轨道电荷布居分析, 并与CO分子和Pt 原子在ZrO₂表面的结果进行比较. 结果表明, C端吸附CO分子键长为0.1161 nm, 与自由的和吸附在ZrO₂表面后的CO相应值(0.1141和0.1136 nm)相比伸长. 吸附后C―O键伸缩振动频率为2018 cm^-1, 与自由CO分子相比发生红移; 吸附后CO带部分正电荷, 电子转移以Pt 5d→CO 2π的π反馈机理占主导地位.

关键词:

English

Adsorption Properties of CO Molecules on Pt/t-ZrO₂(101) Surfaces

1.
1. State Key Laboratory Breeding Base of Photocatalysis, Department of Chemistry, Fuzhou University, Fuzhou 350002, P. R. China;
2. College of Nuclear Technology and Automation Engineering, Chengdu University of Technology, Chengdu 610059, P. R. China
Received Date: 25 August 2011
Available Online: 29 December 2011
Fund Project:
国家自然科学基金(90922022)

福建省高等学校新世纪优秀人才计划(HX2006-103)资助项目

Abstract: We studied the adsorption of CO molecules on perfect and Pt-adsorbed t-ZrO₂(101) surfaces using a periodic slab model by PW91 of generalized gradient approximation (GGA) within the framework of density functional theory. The results indicated that the second sub-surface oxygen and the second bridge sites are the most stable adsorbed sites for CO and Pt on the ZrO₂(101) surface, respectively. When the coverage is 0.25 ML (monolayer) the most stable models were obtained with adsorption energies of 56.2 and 352.7 kJ·mol^-1. The most stable model of CO adsorbed on the Pt/t-ZrO₂(101) surface was obtained by C-end adsorption with an adsorption energy of 323.8 kJ·mol^-1. We considered vibrational frequency calculations, density of states and the Mulliken population of the adsorption systems before and after adsorption and these were compared for CO and Pt adsorption onto the ZrO₂ surface. The results indicate that the C―O bond length of 0.1161 nm after adsorption at the C-end is elongated compared with the 0.1141 and 0.1136 nm of free and adsorbed on ZrO₂. The vibrational frequency of CO at 2018 cm^-1 is red-shifted compared with free CO. CO has some positive charge after adsorption and charge transfer is predominantly by the π back-donation bonding mechanism of the Pt 5d→CO 2π orbital.

Key words:

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沈阳化工大学材料科学与工程学院沈阳 110142

一氧化碳分子在Pt/t-ZrO₂(101)表面的吸附性质

English

Adsorption Properties of CO Molecules on Pt/t-ZrO₂(101) Surfaces

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一氧化碳分子在Pt/t-ZrO2(101)表面的吸附性质

English

Adsorption Properties of CO Molecules on Pt/t-ZrO2(101) Surfaces

CCS Chemistry：嵌段共聚物自组装成 “三明治”二维有机材料，实现纳米级压力传感功能

CCS Chemistry：颜徐州、鲍哲南： 你的皮肤可能是一片SPMs

CCS Chemistry：工作高效不疲劳，只须让催化剂动起来

CCS Chemistry：静电组装导向聚合- 聚电解质纳米凝胶量化制备新策略

CCS Chemistry：金黄色葡萄球菌醛基脱氢酶是如何识别特异性底物的？

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通讯作者: 陈斌, bchen63@163.com

中国化学会秘书处

一氧化碳分子在Pt/t-ZrO₂(101)表面的吸附性质

Adsorption Properties of CO Molecules on Pt/t-ZrO₂(101) Surfaces

CCS Chemistry：颜徐州、鲍哲南：你的皮肤可能是一片SPMs