IHEP OpenIR  > 院士
A Quasi-relativistic Density Functional Theory Study of the Actinyl(VI, V) (An = U, Np, Pu) Complexes with a Six-Membered Macrocycle Containing Pyrrole, Pyridine, and Furan Subunits
Lan JH(蓝建慧); Wang CZ(王聪芝); Wu QY(吴群燕); Feng YX(冯一潇); Zhao YL(赵宇亮); Chai ZF(柴之芳); Shi WQ(石伟群); Lan, JH; Wang, CZ; Wu, QY; Wang, SA; Feng, YX; Zhao, YL; Chai, ZF; Shi, WQ
2015
Source PublicationJOURNAL OF PHYSICAL CHEMISTRY A
ISSN1089-5639
Volume119Issue:34Pages:9178-9188
Corresponding Author石伟群
SubtypeArticle
AbstractActinyl(VI, V) (An = U, Np and Pu) complexes of the recently reported hybrid macrocycle, cyclo[1]furan[1]pyridine[4]pyrrole (denoted as H4L), have been studied using density functional theory in combination with the small-core scalar-relativistic effective core potentials and corresponding (14s13p10d8f6g)/[ 10s9p5d4f3g] basis sets in the segmented contraction scheme. On the basis of our calculations, the pyrrole nitrogen atoms that possess the shortest An-L bonds and strongest basicity are the main donor atoms that contribute to the formation of actinyl(VI, V) complexes. The natural population analysis (NPA) suggests higher ligand-to-actinyl charge transfer in the actinyl(VI) complexes than in their actinyl(V) analogues, which account for the higher decomposition energies of the former. A significant actinide-to-ligand spin density delocalization in the uranyl(V) and neptunyl(V) complexes was observed owing to the redistribution of spin density caused by complexation. A thermodynamic analysis indicates that the formation of the actinyl(VI, V) complexes are exothermic reactions in CH2Cl2 solvent, where the uranyl cations show the highest selectivity. In aqueous solution containing chloride ions, for complexing with macrocycle H4L, the plutonyl(VI) and uranyl(V) cations possess the highest selectivity among actinyl(VI) and (V) cations, respectively. This work can shed light on the design of macrocycle complexes for actinide recognition and extraction in the future.
Subject AreaChemistry; Physics
DOI10.1021/acs.jpca.5b06370
Indexed BySCI ; ADS ; EI ; CA
Language英语
WOS Research AreaChemistry, Physical ; Physics, Atomic, Molecular & Chemical
WOS SubjectChemistry ; Physics
WOS IDWOS:000360415400024
ADS Bibcode2015JPCA..119.9178L
ADS URLhttps://ui.adsabs.harvard.edu/abs/2015JPCA..119.9178L
ADS CITATIONShttps://ui.adsabs.harvard.edu/abs/2015JPCA..119.9178L/citations
Citation statistics
Cited Times:7 [ADS]
Document Type期刊论文
Identifierhttp://ir.ihep.ac.cn/handle/311005/228641
Collection院士
多学科研究中心
Recommended Citation
GB/T 7714
Lan JH,Wang CZ,Wu QY,et al. A Quasi-relativistic Density Functional Theory Study of the Actinyl(VI, V) (An = U, Np, Pu) Complexes with a Six-Membered Macrocycle Containing Pyrrole, Pyridine, and Furan Subunits[J]. JOURNAL OF PHYSICAL CHEMISTRY A,2015,119(34):9178-9188.
APA 蓝建慧.,王聪芝.,吴群燕.,冯一潇.,赵宇亮.,...&Shi, WQ.(2015).A Quasi-relativistic Density Functional Theory Study of the Actinyl(VI, V) (An = U, Np, Pu) Complexes with a Six-Membered Macrocycle Containing Pyrrole, Pyridine, and Furan Subunits.JOURNAL OF PHYSICAL CHEMISTRY A,119(34),9178-9188.
MLA 蓝建慧,et al."A Quasi-relativistic Density Functional Theory Study of the Actinyl(VI, V) (An = U, Np, Pu) Complexes with a Six-Membered Macrocycle Containing Pyrrole, Pyridine, and Furan Subunits".JOURNAL OF PHYSICAL CHEMISTRY A 119.34(2015):9178-9188.
Files in This Item:
File Name/Size DocType Version Access License
586.pdf(2055KB)期刊论文作者接受稿限制开放CC BY-NC-SAApplication Full Text
Related Services
Recommend this item
Bookmark
Usage statistics
Export to Endnote
Google Scholar
Similar articles in Google Scholar
[蓝建慧]'s Articles
[王聪芝]'s Articles
[吴群燕]'s Articles
Baidu academic
Similar articles in Baidu academic
[蓝建慧]'s Articles
[王聪芝]'s Articles
[吴群燕]'s Articles
Bing Scholar
Similar articles in Bing Scholar
[蓝建慧]'s Articles
[王聪芝]'s Articles
[吴群燕]'s Articles
Terms of Use
No data!
Social Bookmark/Share
All comments (0)
No comment.
 

Items in the repository are protected by copyright, with all rights reserved, unless otherwise indicated.