Probing Solvent-Ligand Interactions in Colloidal Nanocrystals by the NMR Line Broadening

被引：126

作者：

De Roo, Jonathan ^{[1
,2
]}

Yazdani, Nuri ^{[3
]}

Drijvers, Emile ^{[1
,4
]}

Lauria, Alessandro ^{[5
]}

Maes, Jorick ^{[1
,4
]}

Owen, Jonathan S. ^{[2
]}

Van Driessche, Isabel ^{[1
]}

Niederberger, Markus ^{[5
]}

Wood, Vanessa ^{[3
]}

Martins, Jose C. ^{[6
]}

Infante, Ivan ^{[7
,8
]}

Hens, Zeger ^{[1
,4
]}

机构：

[1] Univ Ghent, Dept Chem, B-9000 Ghent, Belgium

[2] Columbia Univ, Dept Chem, New York, NY 10027 USA

[3] Swiss Fed Inst Technol, Dept Informat Technol & Elect Engn, CH-8092 Zurich, Switzerland

[4] Univ Ghent, Ctr Nano & Biophoton, B-9000 Ghent, Belgium

[5] Swiss Fed Inst Technol, Lab Multifunct Mat, Dept Mat, Vladimir Prelog Weg 5, CH-8093 Zurich, Switzerland

[6] Univ Ghent, Dept Organ & Macromol Chem, B-9000 Ghent, Belgium

[7] Vrije Univ Amsterdam, Dept Theoret Chem, NL-1081 HV Amsterdam, Netherlands

[8] Vrije Univ Amsterdam, ACMM, NL-1081 HV Amsterdam, Netherlands

来源：

CHEMISTRY OF MATERIALS | 2018年 / 30卷 / 15期

基金：

欧盟地平线“2020”;

关键词：

METAL-SELENIDE NANOCRYSTALS; PBS QUANTUM DOTS; OXIDE NANOCRYSTALS; SURFACE-CHEMISTRY; SIZE; NANOPARTICLES; SUPERLATTICES; EXCHANGE; BINDING; NANOMATERIALS;

D O I：

10.1021/acs.chemmater.8b02523

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：

Although solvent-ligand interactions play a major role in nanocrystal synthesis, dispersion formulation, and assembly, there is currently no direct method to study this. Here we examine the broadening of H-1 NMR resonances associated with bound ligands and turn this poorly understood descriptor into a tool to assess solvent-ligand interactions. We show that the line broadening has both a homogeneous and a heterogeneous component. The former is nanocrystal-size dependent, and the latter results from solvent-ligand interactions. Our model is supported by experimental and theoretical evidence that correlates broad NMR lines with poor ligand solvation. This correlation is found across a wide range of solvents, extending from water to hexane, for both hydrophobic and hydrophilic ligand types, and for a multitude of oxide, sulfide, and selenide nanocrystals. Our findings thus put forward NMR line-shape analysis as an indispensable tool to form, investigate, and manipulate nanocolloids.

引用

页码：5485 / 5492

页数：8

共 35 条

[31] Amino Acid-Based Stabilization of Oxide Nanocrystals in Polar Media: From Insight in Ligand Exchange to Solution 1H NMR Probing of Short-Chained Adsorbates
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[32] Molecular and ionic diffusion in aqueous - deep eutectic solvent mixtures: probing inter-molecular interactions using PFG NMR (vol 17, pg 15297, 2015)
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Ahmed, Essa I.
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Harris, Robert C.
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[33] Probing anion-p interactions of metallacycles with the π-acidic ligand 3,6-bis(2-pyridyl)-1,2,4,5-tetrazine (bptz) by NMR spectroscopy
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[34] Direct probing of sorbent-solvent interactions for amylose tris(3,5-dimethylphenylcarbamate) using infrared spectroscopy, X-ray diffraction, solid-state NMR, and DFT modeling
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Zvinevich, Yury
Hillhouse, Hugh W.
Thomson, Kendall T.
Wang, Nien-Hwa Linda
Franses, Elias I.
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[35] A HIGH-RESOLUTION SOLID-STATE NA-23 NMR-STUDY OF SODIUM COMPLEXES WITH SOLVENTS, SMALL LIGAND MOLECULES, AND IONOPHORES - NA-23 CHEMICAL-SHIFTS AS MEANS FOR IDENTIFICATION AND CHARACTERIZATION OF ION ION, ION SOLVENT, AND ION LIGAND INTERACTIONS
TABETA, R
AIDA, M
SAITO, H
BULLETIN OF THE CHEMICAL SOCIETY OF JAPAN, 1986, 59 (06) : 1957 - 1966

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