The H-D-isotope effect of heavy water affecting ligand-mediated nanoparticle formation in SANS and NMR experiments

被引:1
作者
Krauss, Sebastian W. [1 ]
Eckardt, Mirco [1 ]
Will, Johannes [2 ]
Spiecker, Erdmann [2 ]
Siegel, Renee [3 ,4 ]
Dulle, Martin [5 ]
Schweins, Ralf [6 ]
Pauw, Brian [7 ]
Senker, Juergen [3 ,4 ]
Zobel, Mirijam [8 ]
机构
[1] Univ Bayreuth, Dept Chem, Univ Str 30, D-9544 Bayreuth, Germany
[2] Friedrich Alexander Univ Erlangen Nurnberg, Inst Micro & Nanostruct Res Ctr Nanoanal, IZNF, Cauerstr 3, D-91058 Erlangen, Germany
[3] Univ Bayreuth, CInorgan Chem III, Univ Str 30, D-95447 Bayreuth, Germany
[4] Univ Bayreuth, Northern Bavarian NMR Ctr, Univ Str 30, D-95447 Bayreuth, Germany
[5] Forschungszentrum Julich Gmbh, Neutron Scattering & Biol Matter, DJCNS1IBI8, Wilhelm Johnen Str, D-52428 Julich, Germany
[6] Institut Laue Langevin, DS LSS, 71 Ave Martyrs, F-38000 Grenoble, France
[7] Bundesanstalt Mat & Prufung BAM, Unter Eichen 87, D-12205 Berlin, Germany
[8] Rhein Westfal TH Aachen, Institute Crystallog, Jagerstr 17-19, D-52066 Aachen, Germany
关键词
METAL COMPLEXATION KINETICS; X-RAY; CDS NANOPARTICLES; SURFACE; NANOCRYSTALS; SIZE; PROTONATION; SHELL; EDTA;
D O I
10.1039/d3nr02419a
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
An isotopic effect of normal (H2O) vs. heavy water (D2O) is well known to fundamentally affect the structure and chemical properties of proteins, for instance. Here, we correlate the results from small angle X-ray and neutron scattering (SAXS, SANS) with high-resolution scanning transmission electron microscopy to track the evolution of CdS nanoparticle size and crystallinity from aqueous solution in the presence of the organic ligand ethylenediaminetetraacetate (EDTA) at room temperature in both H2O and D2O. We provide evidence via SANS experiments that exchanging H2O with D2O impacts nanoparticle formation by changing the equilibria and dynamics of EDTA clusters in solution as investigated by nuclear magnetic resonance analysis. The colloidal stability of the CdS nanoparticles, covered by a layer of [Cd(EDTA)]2- complexes, is significantly reduced in D2O despite the strong stabilizing effect of EDTA in suspensions of normal water. Hence, conclusions about nanoparticle formation mechanisms from D2O solutions reveal limited transferability to reactions in normal water due to isotopic effects, which thus need to be discussed for contrast match experiments. Changing from H2O to D2O in CdS nanoparticle formation creates an isotopic effect impacting particle formation. SANS and NMR reveal different complex building constants with the EDTA ligand and how these affect colloidal stability too.
引用
收藏
页码:16413 / 16424
页数:12
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