中国科学院机构知识库网格
Chinese Academy of Sciences Institutional Repositories Grid
Photofragmentation Pathways for Gas-Phase Lanthanide Tris(isopropylcyclopentadienyl) Complexes

文献类型:期刊论文

作者Han, Yulun; Kilin, Dmitri S.; May, P. Stanley; Berry, Mary T.
刊名Organometallics
出版日期2016
卷号35期号:20页码:3461-3473
ISSN号0276-7333
产权排序3
英文摘要

Photofragmentation mechanisms of gas-phase lanthanide tris(isopropylcyclopentadienyl) complexes, Ln(iCp)3, were studied through experimental photoionization time-of-flight mass spectrometry (PI-TOF-MS). A DFT-based time-dependent excited-state molecular dynamics (TDESMD) algorithm, under standard approximations, was used to simulate the photofragmentation process. Two competing reaction pathways, intact ligand stripping and ligand cracking within the metal-ligand complex, were hypothesized based on experimental data. It was evident that intramolecular hydrogen, methyl, and isopropyl abstraction play an important role in the ligand-cracking reaction pathway, leading to metal carbide and metal hydrocarbide products. The TDESMD simulations also produced branching reaction pathways for ligand ejection and ligand cracking and further suggested that both pathways are initiated by ligand-to-metal charge transfer. Although the simulations reproduced several of the proposed reactions and several of the products of cracking observed in the PI-TOF mass spectra, differences between the simulation and experimental results suggest specific directions for improvement in the computational model.

WOS关键词OXIDE THIN-FILMS ; ATOMIC LAYER DEPOSITION ; CHEMICAL-VAPOR-DEPOSITION ; STATE MOLECULAR-DYNAMICS ; GATE DIELECTRICS ; PHOTODISSOCIATION ; CYCLOPENTADIENYL ; CHEMISTRY ; PRECURSORS ; DECOMPOSITION
WOS研究方向Chemistry
语种英语
WOS记录号WOS:000386314800008
资助机构South Dakota Governor’s Office of Economic Development and NSF award EPS-0903804 ; South Dakota IDeA Networks of Biomedical Research Excellence NIH 2 P20RR016479
源URL[http://ir.sia.cn/handle/173321/19370]  
专题沈阳自动化研究所_广州中国科学院沈阳自动化研究所分所
通讯作者Berry, Mary T.
作者单位1.Department of Chemistry, University of South Dakota, Vermillion, SD, 57069, United States
2.Shenyang Institute of Automation, Guangzhou, Chinese Academy of Sciences, Guangzhou, 511458, China
3.Department of Chemistry and Biochemistry, North Dakota State University, Fargo, ND, 58108, United States
推荐引用方式
GB/T 7714
Han, Yulun,Kilin, Dmitri S.,May, P. Stanley,et al. Photofragmentation Pathways for Gas-Phase Lanthanide Tris(isopropylcyclopentadienyl) Complexes[J]. Organometallics,2016,35(20):3461-3473.
APA Han, Yulun,Kilin, Dmitri S.,May, P. Stanley,&Berry, Mary T..(2016).Photofragmentation Pathways for Gas-Phase Lanthanide Tris(isopropylcyclopentadienyl) Complexes.Organometallics,35(20),3461-3473.
MLA Han, Yulun,et al."Photofragmentation Pathways for Gas-Phase Lanthanide Tris(isopropylcyclopentadienyl) Complexes".Organometallics 35.20(2016):3461-3473.

入库方式: OAI收割

来源:沈阳自动化研究所

浏览0
下载0
收藏0
其他版本

除非特别说明,本系统中所有内容都受版权保护,并保留所有权利。