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Title: Effects of Residual Solvent Molecules Facilitating the Infiltration Synthesis of ZnO in a Nonreactive Polymer

Infiltration synthesis, the atomic-layer-deposition-based organic–inorganic material hybridization technique that enables unique hybrid composites with improved material properties and inorganic nanostructures replicated from polymer templates, is shown to be driven by the binding reaction between reactive chemical groups of polymers and perfusing vapor-phase material precursors. Here in this paper, we discover that residual solvent molecules from polymer processing can react with infiltrating material precursors to enable the infiltration synthesis of metal oxides in a nonreactive polymer. The systematic study, which combines in situ quartz crystal microgravimetry, polarization-modulated infrared reflection–absorption spectroscopy, X-ray photoelectron spectroscopy, and transmission electron microscopy, shows that the ZnO infiltration synthesis in nominally nonreactive SU-8 polymer is mediated by residual processing solvent cyclopentanone, a cyclic ketone whose Lewis-basic terminal carbonyl group can react with the infiltrating Lewis-acidic Zn precursor diethylzinc (DEZ). In addition, we find favorable roles of residual epoxy rings in the SU-8 film in further assisting the infiltration synthesis of ZnO. Lastly, the discovered rationale not only improves the understanding of infiltration synthesis mechanism, but also potentially expands its application to more diverse polymer systems for the generation of unique functional organic–inorganic hybrids and inorganic nanostructures.
Authors:
 [1] ;  [1] ;  [1] ;  [1] ;  [2] ;  [1] ; ORCiD logo [1]
  1. Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN)
  2. Stony Brook Univ., NY (United States). Dept. of Chemistry
Publication Date:
Report Number(s):
BNL-114135-2017-JA
Journal ID: ISSN 0897-4756
Grant/Contract Number:
SC0012704
Type:
Accepted Manuscript
Journal Name:
Chemistry of Materials
Additional Journal Information:
Journal Volume: 29; Journal Issue: 10; Journal ID: ISSN 0897-4756
Publisher:
American Chemical Society (ACS)
Research Org:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 77 NANOSCIENCE AND NANOTECHNOLOGY
OSTI Identifier:
1376164

Ye, Xinyi, Kestell, John, Kisslinger, Kim, Liu, Mingzhao, Grubbs, Robert B., Boscoboinik, J. Anibal, and Nam, Chang-Yong. Effects of Residual Solvent Molecules Facilitating the Infiltration Synthesis of ZnO in a Nonreactive Polymer. United States: N. p., Web. doi:10.1021/acs.chemmater.7b01222.
Ye, Xinyi, Kestell, John, Kisslinger, Kim, Liu, Mingzhao, Grubbs, Robert B., Boscoboinik, J. Anibal, & Nam, Chang-Yong. Effects of Residual Solvent Molecules Facilitating the Infiltration Synthesis of ZnO in a Nonreactive Polymer. United States. doi:10.1021/acs.chemmater.7b01222.
Ye, Xinyi, Kestell, John, Kisslinger, Kim, Liu, Mingzhao, Grubbs, Robert B., Boscoboinik, J. Anibal, and Nam, Chang-Yong. 2017. "Effects of Residual Solvent Molecules Facilitating the Infiltration Synthesis of ZnO in a Nonreactive Polymer". United States. doi:10.1021/acs.chemmater.7b01222. https://www.osti.gov/servlets/purl/1376164.
@article{osti_1376164,
title = {Effects of Residual Solvent Molecules Facilitating the Infiltration Synthesis of ZnO in a Nonreactive Polymer},
author = {Ye, Xinyi and Kestell, John and Kisslinger, Kim and Liu, Mingzhao and Grubbs, Robert B. and Boscoboinik, J. Anibal and Nam, Chang-Yong},
abstractNote = {Infiltration synthesis, the atomic-layer-deposition-based organic–inorganic material hybridization technique that enables unique hybrid composites with improved material properties and inorganic nanostructures replicated from polymer templates, is shown to be driven by the binding reaction between reactive chemical groups of polymers and perfusing vapor-phase material precursors. Here in this paper, we discover that residual solvent molecules from polymer processing can react with infiltrating material precursors to enable the infiltration synthesis of metal oxides in a nonreactive polymer. The systematic study, which combines in situ quartz crystal microgravimetry, polarization-modulated infrared reflection–absorption spectroscopy, X-ray photoelectron spectroscopy, and transmission electron microscopy, shows that the ZnO infiltration synthesis in nominally nonreactive SU-8 polymer is mediated by residual processing solvent cyclopentanone, a cyclic ketone whose Lewis-basic terminal carbonyl group can react with the infiltrating Lewis-acidic Zn precursor diethylzinc (DEZ). In addition, we find favorable roles of residual epoxy rings in the SU-8 film in further assisting the infiltration synthesis of ZnO. Lastly, the discovered rationale not only improves the understanding of infiltration synthesis mechanism, but also potentially expands its application to more diverse polymer systems for the generation of unique functional organic–inorganic hybrids and inorganic nanostructures.},
doi = {10.1021/acs.chemmater.7b01222},
journal = {Chemistry of Materials},
number = 10,
volume = 29,
place = {United States},
year = {2017},
month = {5}
}