dftstudyofdifferencecausedbycatalystsupportsinptandpdcatalysisofoxygenreductionreaction
文献类型：期刊论文
| 作者 | XIA MeiRong2; ZHANG Jie2; SHAO ZhiGang1; Sun CaiXin2; LI Li2; WEI ZiDong2; ZHANG Yi2; QI XueQiang2 |
| 刊名 | scienceinchinaseriesbchemistry
 |
| 出版日期 | 2009-01-01 |
| 卷号 | 52期号:5页码:571 |
| ISSN号 | 1006-9291 |
| 英文摘要 | Based on an experimental phenomenon that catalytic activity of Pt and Pd for oxygen reduction reaction (ORR) changes with catalyst supports from C to TiO2, density function theory (DFT) was used to elucidate the cause behind the difference in catalysis caused by catalyst supports. First, factors closely associated with the first electron transfer of the ORR were assessed in the light of quantum chemistry. Then intermediate (atomic oxygen, O) adsorption strength on the catalyst surface was calculated. The results show that, in terms of minimum energy difference, the best orbital symmetry match, and the maximum orbital overlap, TiO2 does bring about a very positive effect on catalysts Pd/TiO2 for the first electron transfer of the ORR. Especially, TiO2 remarkably expands the space size of Pd/TiO2 HOMO orbital and improves orbital overlap of Pd/TiO2 HOMO and O-2 LUMO. The analysis of deformation density and partial density of state shows that the strong interaction between Pt and Ti leads to a strong adsorption of intermediate O on Pt/TiO2, but the strong interaction between Pd and surface O causes positive net charge of Pd and a weak adsorption of intermediate O on Pd/TiO2. Thus, the ORR can proceed more smoothly on Pd/TiO2 than Pt/TiO2 in every respect of maximum orbital overlap and rate delay by intermediate O. The research also discloses that several factors lead to less activity of TiO2-supported Pt and Pd catalysts than the C-supported ones for the ORR. These factors include the poor dispersion of Pt and Pd particles on TiO2, poor electric conduction of TiO2 carrier itself, and bigger energy difference between HOMO of TiO2-carried metallic catalysts and LUMO of O-2 molecule due to electrons deeply embedded in the semiconductor TiO2 carrier. |
| 语种 | 英语 |
| 源URL | [http://cas-ir.dicp.ac.cn/handle/321008/174385]  |
| 专题 | 大连化学物理研究所_中国科学院大连化学物理研究所 |
| 作者单位 | 1.中国科学院大连化学物理研究所 2.重庆大学 |
| 推荐引用方式 GB/T 7714 | XIA MeiRong,ZHANG Jie,SHAO ZhiGang,et al. dftstudyofdifferencecausedbycatalystsupportsinptandpdcatalysisofoxygenreductionreaction[J]. scienceinchinaseriesbchemistry,2009,52(5):571. |
| APA | XIA MeiRong.,ZHANG Jie.,SHAO ZhiGang.,Sun CaiXin.,LI Li.,...&QI XueQiang.(2009).dftstudyofdifferencecausedbycatalystsupportsinptandpdcatalysisofoxygenreductionreaction.scienceinchinaseriesbchemistry,52(5),571. |
| MLA | XIA MeiRong,et al."dftstudyofdifferencecausedbycatalystsupportsinptandpdcatalysisofoxygenreductionreaction".scienceinchinaseriesbchemistry 52.5(2009):571. |
入库方式： OAI收割
来源：大连化学物理研究所
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