Implications of Byproduct Chemistry in Nanoparticle Synthesis

Research output: Contribution to journalJournal articleResearchpeer-review

Abstract

Byproducts in metalnanoparticle synthesis can interfere with nanomaterial formation and self-assembly, as well as the perceived nanomaterial properties. Such syntheses go through a complicated series of intermediates, making it difficult to predict byproduct chemistry and challenging to determine experimentally. By a combined experimental and theoretical approach, the formation of organic byproducts is mapped out for the synthesis of gold nanoparticles with Good’s buffer 2-(N-morpholino)ethanesulfonic acid. Comprehensive nuclear magnetic resonance studies supported by mass spectrometry, ultraviolet–visible spectroscopy, and density functional theory reveal a number of previously unidentified byproducts formed by oxidation, C–N bond cleavage,and C–C bond formation. A reaction mechanism involving up to four consecutive oxidations is proposed. Oligomeric products with electronic transitions in the visible range are suggested. This approach can be extended broadly and lead to a more informed synthesis designand material characterization.
Original languageEnglish
JournalJournal of Physical Chemistry C
Volume123
Issue number41
Pages (from-to)25402-25411
Number of pages10
ISSN1932-7447
DOIs
Publication statusPublished - 2019

Cite this

@article{45b2f985c7e943878871d1970ba4ba95,
title = "Implications of Byproduct Chemistry in Nanoparticle Synthesis",
abstract = "Byproducts in metalnanoparticle synthesis can interfere with nanomaterial formation and self-assembly, as well as the perceived nanomaterial properties. Such syntheses go through a complicated series of intermediates, making it difficult to predict byproduct chemistry and challenging to determine experimentally. By a combined experimental and theoretical approach, the formation of organic byproducts is mapped out for the synthesis of gold nanoparticles with Good’s buffer 2-(N-morpholino)ethanesulfonic acid. Comprehensive nuclear magnetic resonance studies supported by mass spectrometry, ultraviolet–visible spectroscopy, and density functional theory reveal a number of previously unidentified byproducts formed by oxidation, C–N bond cleavage,and C–C bond formation. A reaction mechanism involving up to four consecutive oxidations is proposed. Oligomeric products with electronic transitions in the visible range are suggested. This approach can be extended broadly and lead to a more informed synthesis designand material characterization.",
author = "Stappen, {Frederick N.} and Kasper Enemark-Rasmussen and Junor, {Glen P.} and Clausen, {Mads Hartvig} and Jingdong Zhang and Christian Engelbrekt",
year = "2019",
doi = "10.1021/acs.jpcc.9b03193",
language = "English",
volume = "123",
pages = "25402--25411",
journal = "The Journal of Physical Chemistry Part C",
issn = "1932-7447",
publisher = "American Chemical Society",
number = "41",

}

Implications of Byproduct Chemistry in Nanoparticle Synthesis. / Stappen, Frederick N.; Enemark-Rasmussen, Kasper; Junor, Glen P.; Clausen, Mads Hartvig; Zhang, Jingdong; Engelbrekt, Christian.

In: Journal of Physical Chemistry C, Vol. 123, No. 41, 2019, p. 25402-25411.

Research output: Contribution to journalJournal articleResearchpeer-review

TY - JOUR

T1 - Implications of Byproduct Chemistry in Nanoparticle Synthesis

AU - Stappen, Frederick N.

AU - Enemark-Rasmussen, Kasper

AU - Junor, Glen P.

AU - Clausen, Mads Hartvig

AU - Zhang, Jingdong

AU - Engelbrekt, Christian

PY - 2019

Y1 - 2019

N2 - Byproducts in metalnanoparticle synthesis can interfere with nanomaterial formation and self-assembly, as well as the perceived nanomaterial properties. Such syntheses go through a complicated series of intermediates, making it difficult to predict byproduct chemistry and challenging to determine experimentally. By a combined experimental and theoretical approach, the formation of organic byproducts is mapped out for the synthesis of gold nanoparticles with Good’s buffer 2-(N-morpholino)ethanesulfonic acid. Comprehensive nuclear magnetic resonance studies supported by mass spectrometry, ultraviolet–visible spectroscopy, and density functional theory reveal a number of previously unidentified byproducts formed by oxidation, C–N bond cleavage,and C–C bond formation. A reaction mechanism involving up to four consecutive oxidations is proposed. Oligomeric products with electronic transitions in the visible range are suggested. This approach can be extended broadly and lead to a more informed synthesis designand material characterization.

AB - Byproducts in metalnanoparticle synthesis can interfere with nanomaterial formation and self-assembly, as well as the perceived nanomaterial properties. Such syntheses go through a complicated series of intermediates, making it difficult to predict byproduct chemistry and challenging to determine experimentally. By a combined experimental and theoretical approach, the formation of organic byproducts is mapped out for the synthesis of gold nanoparticles with Good’s buffer 2-(N-morpholino)ethanesulfonic acid. Comprehensive nuclear magnetic resonance studies supported by mass spectrometry, ultraviolet–visible spectroscopy, and density functional theory reveal a number of previously unidentified byproducts formed by oxidation, C–N bond cleavage,and C–C bond formation. A reaction mechanism involving up to four consecutive oxidations is proposed. Oligomeric products with electronic transitions in the visible range are suggested. This approach can be extended broadly and lead to a more informed synthesis designand material characterization.

U2 - 10.1021/acs.jpcc.9b03193

DO - 10.1021/acs.jpcc.9b03193

M3 - Journal article

VL - 123

SP - 25402

EP - 25411

JO - The Journal of Physical Chemistry Part C

JF - The Journal of Physical Chemistry Part C

SN - 1932-7447

IS - 41

ER -