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
SN - 1932-7447
VL - 123
SP - 25402
EP - 25411
JO - Journal of Physical Chemistry C
JF - Journal of Physical Chemistry C
IS - 41
ER -