19F Magic Angle Spinning NMR Spectroscopy and Density Functional Theory Calculations of Fluorosubstituted Tryptophans: Integrating Experiment and Theory for Accurate Determination of Chemical Shift Tensors

被引：30

作者：

Lu, Manman ^{[1
,2
]}

Sarkar, Sucharita ^{[1
,2
]}

Wang, Mingzhang ^{[1
,2
]}

Kraus, Jodi ^{[1
]}

Fritz, Matthew ^{[1
]}

Quinn, Caitlin M. ^{[1
]}

Bai, Shi ^{[1
]}

Holmes, Sean T. ^{[1
]}

Dybowski, Cecil ^{[1
]}

Yap, Glenn P. A. ^{[1
]}

Struppe, Jochem ^{[4
]}

Sergeyev, Ivan V. ^{[4
]}

Maas, Werner ^{[4
]}

Gronenborn, Angela M. ^{[2
,3
]}

Polenova, Tatyana ^{[1
]}

机构：

[1] Univ Delaware, Dept Chem & Biochem, Newark, DC 19716 USA

[2] Univ Pittsburgh, Sch Med, Pittsburgh Ctr HIV Prot Interact, 1051 Biomed Sci Tower 3501 Fifth Ave, Pittsburgh, PA 15261 USA

[3] Univ Pittsburgh, Sch Med, Dept Struct Biol, 3501 Fifth Ave, Pittsburgh, PA 15261 USA

[4] Bruker Biospin Corp, 15 Fortune Dr, Billerica, MA 01821 USA

来源：

JOURNAL OF PHYSICAL CHEMISTRY B | 2018年 / 122卷 / 23期

基金：

美国国家卫生研究院; 美国国家科学基金会;

关键词：

SOLID-STATE NMR; CRYSTAL-STRUCTURE; PROTEIN-STRUCTURE; SHIELDING TENSOR; FLUORINE; PREDICTION; PARAMETERS; PROTOCOL; BINDING; PROBE;

D O I：

10.1021/acs.jpcb.8b00377

中图分类号：

O64 [物理化学（理论化学）、化学物理学];

学科分类号：

070304 ; 081704 ;

摘要：

The F-19 chemical shift is a sensitive NMR probe of structure and electronic environment in organic and biological molecules. In this report, we examine chemical shift parameters of 4F-, 5F-, 6F-, and 7F-substituted crystalline tryptophan by magic angle spinning (MAS) solid-state NMR spectroscopy and density functional theory. Significant narrowing of the 19F lines was observed under fast MAS conditions, at spinning frequencies above 50 kHz. The parameters characterizing the 19F chemical shift tensor are sensitive to the position of the fluorine in the aromatic ring and, to a lesser extent, the chirality of the molecule. Accurate calculations of F-19 magnetic shielding tensors require the PBEO functional with a 50% admixture of a Hartree Fock exchange term, as well as taking account of the local crystal symmetry. The methodology developed will be beneficial for 19F based MAS NMR structural analysis of proteins and protein assemblies.

引用

页码：6148 / 6155

页数：8

共 30 条

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