journal article·2023

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

Sebastian W. Krauss, Mirco Eckardt, Johannes Will, Erdmann Spiecker, Renée Siegel, Martin Dulle, Ralf Schweins, Brian Pauw, Jürgen Senker, Mirijam Zobel

Nanoscale· Volume 15· Issue 40
Publisher page

Abstract

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.
Source: europepmc · Quality: candidate unverified · Source record ↗

Research context

OpenAlex topics: Quantum Dots Synthesis And Properties · Chalcogenide Semiconductor Thin Films · Spectroscopy and Quantum Chemical Studies

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

Department of Chemistry, University of Bayreuth, Universitätsstr. 30, 95447 Bayreuth, Germany

Institute of Micro- and Nanostructure Research & Center for Nanoanalysis and Electron Microscopy (CENEM), Friedrich-Alexander-Universität Erlangen-Nürnberg, IZNF, Cauerstraße 3, 91058 Erlangen, Germany

Inorganic Chemistry III and Northern Bavarian NMR Centre, University of Bayreuth, Universitätsstr. 30, 95447 Bayreuth, Germany

JCNS-1/IBI-8: Neutron Scattering and Biological Matter, Forschungszentrum Jülich Gmbh, Wilhelm-Johnen-Straße, 52428 Jülich, Germany

Institut Laue-Langevin, DS/LSS, 71 Avenue des Martyrs, Grenoble 38000, France

Bundesanstalt für Materialforschung und -prüfung (BAM), Unter den Eichen 87, 12205 Berlin, Germany

Institute of Crystallography, RWTH Aachen University, Jägerstr. 17-19, 52066 Aachen, Germany

Funding

Horizon 2020 · Fonds der Chemischen Industrie · Elitenetzwerk Bayern · Deutsche Forschungsgemeinschaft

References (49)

Show source-provided references
1. Peng · Nature · 2000 · 404 · 5910.1038/35003535 ↗
2. Aldana · J. Am. Chem. Soc. · 2005 · 127 · 249610.1021/ja047000+ ↗
3. Zobel · J. Nanopart. Res. · 2015 · 1710.1007/s11051-015-3006-5 ↗
4. Green · J. Mater. Chem. C · 2020 · 8 · 1206810.1039/D0TC03252B ↗
5. Hayden · Adv. Mater. · 2005 · 17 · 70110.1002/adma.200401235 ↗
6. Voss · J. Appl. Phys. · 2004 · 96 · 581910.1063/1.1804244 ↗
7. Bullen · Langmuir · 2006 · 22 · 300710.1021/la051898e ↗
8. Alivisatos · Science · 1996 · 271 · 93310.1126/science.271.5251.933 ↗
9. Kozhevnikova · Russ. J. Gen. Chem. · 2010 · 80 · 39110.1134/S1070363210030035 ↗
10. Schiener · Nanoscale · 2015 · 7 · 1132810.1039/C5NR01602A ↗
11. A.Magerl
12. Koehler · Chem. Commun. · 2009 · 486210.1039/b909447d ↗
13. Sudmeier · Inorg. Chem. · 1966 · 5 · 104710.1021/ic50040a021 ↗
14. Diroll · Nano Lett. · 2015 · 15 · 800810.1021/acs.nanolett.5b04011 ↗
15. Schindler · Langmuir · 2015 · 31 · 1013010.1021/acs.langmuir.5b02198 ↗
16. Winslow · ACS Mater. Lett. · 2019 · 1 · 20910.1021/acsmaterialslett.9b00200 ↗
17. Stadmiller · Protein Sci. · 2018 · 27 · 171010.1002/pro.3477 ↗
18. Carl · Colloid Polym. Sci. · 2020 · 298 · 66310.1007/s00396-019-04596-1 ↗
19. Taube · J. Am. Chem. Soc. · 1960 · 82 · 52410.1021/ja01488a005 ↗
20. Lazzarini · J. Inorg. Nucl. Chem. · 1980 · 42 · 95310.1016/0022-1902(80)80381-2 ↗
21. Wang · J. Phys. Chem. C · 2009 · 113 · 1797910.1021/jp907642b ↗
22. Ojea-Jiménez · J. Phys. Chem. C · 2010 · 114 · 180010.1021/jp9091305 ↗
23. Fritzinger · J. Am. Chem. Soc. · 2010 · 132 · 1019510.1021/ja104351q ↗
24. Hanrahan · J. Am. Chem. Soc. · 2019 · 141 · 1553210.1021/jacs.9b05509 ↗
25. Piveteau · ACS Cent. Sci. · 2018 · 4 · 111310.1021/acscentsci.8b00196 ↗
26. Cotrait · Acta Crystallogr., Sect. B: Struct. Crystallogr. Cryst. Chem. · 1972 · 28 · 78110.1107/S056774087200319X ↗
27. Masadeh · Phys. Rev. B: Condens. Matter Mater. Phys. · 2007 · 76 · 11541310.1103/PhysRevB.76.115413 ↗
28. Hens · Chem. Mater. · 2013 · 25 · 121110.1021/cm303361s ↗
29. De Roo · Chem. Mater. · 2018 · 30 · 548510.1021/acs.chemmater.8b02523 ↗
30. Ladizhansky · J. Phys. Chem. B · 2000 · 104 · 193910.1021/jp993071x ↗
31. Polyakova · Crystallogr. Rep. · 2001 · 46 · 4010.1134/1.1343124 ↗
32. Kurihara · J. Phys. Chem. Lett. · 2017 · 8 · 255510.1021/acs.jpclett.7b00909 ↗
33. Eichele · Inorg. Chem. · 2002 · 33 · 276610.1021/ic00091a017 ↗
34. van Leeuwen · J. Phys. Chem. A · 2007 · 111 · 211510.1021/jp0673009 ↗
35. Zhu · Solid State Commun. · 2006 · 137 · 50310.1016/j.ssc.2005.12.026 ↗
36. van Leeuwen · Environ. Sci. Technol. · 2009 · 43 · 8810.1021/es802185h ↗
37. Kuznetsova · Inorg. Mater. · 2015 · 51 · 21510.1134/S0020168515020119 ↗
38. Rubinson · Anal. Methods · 2017 · 9 · 274410.1039/C7AY00669A ↗
39. Sawyer · J. Am. Chem. Soc. · 1963 · 85 · 239010.1021/ja00899a011 ↗
40. Thomä · Rev. Sci. Instrum. · 2019 · 90 · 04390510.1063/1.5093714 ↗
41. Wright · J. Synchrotron Radiat. · 2017 · 24 · 50610.1107/S1600577517000157 ↗
42. Juhás · J. Appl. Crystallogr. · 2013 · 46 · 56010.1107/S0021889813005190 ↗
43. Farrow · J. Phys.: Condens. Matter · 2007 · 19 · 335219
44. Yang · Phys. Chem. Chem. Phys. · 2013 · 15 · 848010.1039/c3cp00111c ↗
45. M.Polyanskiy , Refrective Index Database, https://refractiveindex.info/
46. Smales · J. Instrum. · 2021 · 16 · P0603410.1088/1748-0221/16/06/P06034 ↗
47. Filik · J. Appl. Crystallogr. · 2017 · 50 · 95910.1107/S1600576717004708 ↗
48. Basham · J. Synchrotron Radiat. · 2015 · 22 · 85310.1107/S1600577515002283 ↗
49. Bressler · J. Appl. Crystallogr. · 2015 · 48 · 96210.1107/S1600576715007347 ↗