TY - JOUR
T1 - Polymer-Mediated Particle Coarsening within Hollow Silica Shell Nanoreactors
AU - Jibril, Liban
AU - Cheng, Matthew
AU - Wahl, Carolin B.
AU - Dravid, Vinayak P.
AU - Mirkin, Chad A.
N1 - Funding Information:
The project described was supported by the Sherman Fairchild Foundation, Inc., Toyota Research Institute, Inc., and the Air Force Office of Scientific Research award FA9550-17-1-0348. L.J. was supported by the National Science Foundation through the National Science Foundation Graduate Research Fellowship Program under Grant No. DGE-1842165. Any opinions, findings, and conclusions or recommendations expressed in this material are those of the authors and do not necessarily reflect the views of the National Science Foundation. This work utilized the EPIC, Bio-Cryo, and Keck II facilities of Northwestern University's NUANCE Center, which has received support from the Soft and Hybrid Nanotechnology Experimental (SHyNE) resource (NSF ECCS-1542205), the MRSEC program (NSF DMR-1121262) at the Materials Research Center The International Institute for Nanotechnology (IIN), the Keck Foundation and the State of Illinois through the IIN. This work also utilized the Northwestern University Quantitative Bioelement Imaging Center (QBIC) and Reactor Engineering and Catalyst Testing (REACT) core facilities. The authors would like to acknowledge Drs. Kun He, Neil Schweitzer and Selim Alayoglu for experimental advice and helpful discussion.
Funding Information:
The project described was supported by the Sherman Fairchild Foundation, Inc., Toyota Research Institute, Inc., and the Air Force Office of Scientific Research award FA9550-17-1-0348. L.J. was supported by the National Science Foundation through the National Science Foundation Graduate Research Fellowship Program under Grant No. DGE-1842165. Any opinions, findings, and conclusions or recommendations expressed in this material are those of the authors and do not necessarily reflect the views of the National Science Foundation. This work utilized the EPIC, Bio-Cryo, and Keck II facilities of Northwestern University’s NUANCE Center, which has received support from the Soft and Hybrid Nanotechnology Experimental (SHyNE) resource (NSF ECCS-1542205), the MRSEC program (NSF DMR-1121262) at the Materials Research Center, The International Institute for Nanotechnology (IIN), the Keck Foundation, and the State of Illinois through the IIN. This work also utilized the Northwestern University Quantitative Bioelement Imaging Center (QBIC) and Reactor Engineering and Catalyst Testing (REACT) core facilities. The authors would like to acknowledge Drs. Kun He, Neil Schweitzer, and Selim Alayoglu for experimental advice and helpful discussion.
Publisher Copyright:
© 2022 American Chemical Society.
PY - 2022/6/14
Y1 - 2022/6/14
N2 - Inspired by the scanning probe block copolymer lithography process, hollow silica shells were loaded with polymer─metal ink mixtures and investigated as solution-based nanoreactors for the synthesis of gold nanoparticles. The incorporation of poly(ethylene oxide) (PEO) into these hollow silica nanoreactors (approximately 40 nm in size) and the use of a two-step reductive annealing process (first at 200 °C and then at 600 °C) results in a high yield (76%) of larger (∼6 nm) single nanoparticles; when the polymer is not used, smaller (∼3 nm) particles dominate, and the yield of single particles is only 6%. It was determined that particle coarsening mostly occurs in the temperature range where the polymer is present and not degraded (i.e., <400 °C for PEO), as indicted by correlative in situ scanning/transmission electron microscopy in a reductive gas-phase environment. Thus, polymer incorporation in this nanoreactor system, which is amenable to scale up, drives the complete conversion of nanoreactor contents without excessive metal loss, highlighting the impact of nanoreactor composition and structural design on particle synthesis.
AB - Inspired by the scanning probe block copolymer lithography process, hollow silica shells were loaded with polymer─metal ink mixtures and investigated as solution-based nanoreactors for the synthesis of gold nanoparticles. The incorporation of poly(ethylene oxide) (PEO) into these hollow silica nanoreactors (approximately 40 nm in size) and the use of a two-step reductive annealing process (first at 200 °C and then at 600 °C) results in a high yield (76%) of larger (∼6 nm) single nanoparticles; when the polymer is not used, smaller (∼3 nm) particles dominate, and the yield of single particles is only 6%. It was determined that particle coarsening mostly occurs in the temperature range where the polymer is present and not degraded (i.e., <400 °C for PEO), as indicted by correlative in situ scanning/transmission electron microscopy in a reductive gas-phase environment. Thus, polymer incorporation in this nanoreactor system, which is amenable to scale up, drives the complete conversion of nanoreactor contents without excessive metal loss, highlighting the impact of nanoreactor composition and structural design on particle synthesis.
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U2 - 10.1021/acs.chemmater.2c00510
DO - 10.1021/acs.chemmater.2c00510
M3 - Article
AN - SCOPUS:85131750994
SN - 0897-4756
VL - 34
SP - 5094
EP - 5102
JO - Chemistry of Materials
JF - Chemistry of Materials
IS - 11
ER -