High-Pressure Effects on Hofmann-Type Clathrates: Promoted Release and Restricted Insertion of Guest Molecules

Li, Qui1; Sha, Xiaojing3; Li, Shourui5; Wang, Kai2; Quan, Zewei1; Meng, Yue4; Zou, Bo2

2017-06-15

10.1021/acs.jpclett.7b01057

Journal of Physical Chemistry Letters   影响因子和分区

1948-7185

The search for effective methods to accurately control host guest relationship is the central theme of host guest chemistry. In this work, high pressure successfully promotes guest release in the Hofmann-type clathrate of [Ni(NH3)(2)Ni-(CN)(4)]center dot 2C(6)H(6) (Ni-Bz) and restricts guest insertion into Ni(NH3)(2)Ni(CN)(4) (Ni-Ni). Because of the weak host guest interactions of Ni-Bz, external force gradually removes guest benzene from the host framework, leading to puckered layers. Further theoretical calculations reveal the positive pressure contribution to breaking the energy barrier between Ni-Bz and Ni Ni, explaining guest release from an energy standpoint. Inversely, guest insertion is restricted in the synthesized host of Ni Ni because of the steric hindrance effect at high pressure. This study not only reveals structural effects on host guest behaviors but also proves the role of pressure in controlling host guest interactions. This unique observation is also crucial for the further application of host guest materials in sustained and intelligent drug release, molecular separation, and transportation.

SCI ; EI

英语

NI期刊

第一

DOE Office of Science[DE-AC02-06CH11357]

Chemistry ; Science & Technology - Other Topics ; Materials Science ; Physics

Chemistry, Physical ; Nanoscience & Nanotechnology ; Materials Science, Multidisciplinary ; Physics, Atomic, Molecular & Chemical

WOS:000403741800033

AMER CHEMICAL SOC

20172503796147

Binary alloys ; Controlled drug delivery ; Drug interactions ; Dyes ; Hydrates ; Materials handling ; Targeted drug delivery

Medicine and Pharmacology:461.6 ; Chemical Agents and Basic Industrial Chemicals:803

Web of Science

1.South Univ Sci & Technol China, Dept Chem, Shenzhen 518055, Peoples R China
2.Jilin Univ, State Key Lab Superhard Mat, Changchun 130012, Peoples R China
3.Beijing Inst Aeronaut Mat, Mat Genome Ctr, Beijing 100095, Peoples R China
4.CIW, Geophys Lab, HPCAT, Argonne, IL 60439 USA
5.China Acad Engn Phys, Inst Fluid Phys, Natl Key Lab Shock Wave & Detonat Phys, Mianyang 621900, Peoples R China

Li, Qui,Sha, Xiaojing,Li, Shourui,et al. High-Pressure Effects on Hofmann-Type Clathrates: Promoted Release and Restricted Insertion of Guest Molecules[J]. Journal of Physical Chemistry Letters,2017,8(12):2745-2750.

Li, Qui.,Sha, Xiaojing.,Li, Shourui.,Wang, Kai.,Quan, Zewei.,...&Zou, Bo.(2017).High-Pressure Effects on Hofmann-Type Clathrates: Promoted Release and Restricted Insertion of Guest Molecules.Journal of Physical Chemistry Letters,8(12),2745-2750.

Li, Qui,et al."High-Pressure Effects on Hofmann-Type Clathrates: Promoted Release and Restricted Insertion of Guest Molecules".Journal of Physical Chemistry Letters 8.12(2017):2745-2750.