Spatial distribution of organic functional groups supported on mesoporous silica nanoparticles (2): a study by 1H triple-quantum fast-MAS solid-state NMR
Abstract
The distribution of organic functional groups attached to the surface of mesoporous silica nanoparticles (MSNs) via co-condensation was scrutinized using 1D and 2D 1H solid-state NMR, including the triple-quantum/single-quantum (TQ/SQ) homonuclear correlation technique. The excellent sensitivity of 1H NMR and high resolution provided by fast magic angle spinning (MAS) allowed us to study surfaces with very low concentrations of aminopropyl functional groups. The sequential process, in which the injection of tetraethyl orthosilicate (TEOS) into the aqueous mother liquor was followed by dropwise addition of the organosilane precursor, resulted in deployment of organic groups on the surface, which were highly clustered even in a sample with a very low loading of ~0.1 mmol g-1. The underlying mechanism responsible for clustering could involve fast aggregation of the aminopropyltrimethoxysilane (APTMS) precursor within the liquid phase, and/or co-condensation of the silica-bound molecules. Understanding the deposition process and the resulting topology of surface functionalities with atomic-scale resolution, can help to develop novel approaches to the synthesis of complex inorganic–organic hybrid materials.
- Authors:
-
- Ames Lab. and Iowa State Univ., Ames, IA (United States)
- Ames Lab. and Iowa State Univ., Ames, IA (United States). Dept. of Chemistry
- Publication Date:
- Research Org.:
- Ames Laboratory (AMES), Ames, IA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1467595
- Alternate Identifier(s):
- OSTI ID: 1464972
- Report Number(s):
- IS-J-9736
Journal ID: ISSN 1463-9076; PPCPFQ
- Grant/Contract Number:
- AC02-07CH11358
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Physical Chemistry Chemical Physics. PCCP
- Additional Journal Information:
- Journal Volume: 20; Journal Issue: 34; Journal ID: ISSN 1463-9076
- Publisher:
- Royal Society of Chemistry
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 36 MATERIALS SCIENCE
Citation Formats
Kobayashi, Takeshi, Singappuli-Arachchige, Dilini, Slowing, Igor I., and Pruski, Marek. Spatial distribution of organic functional groups supported on mesoporous silica nanoparticles (2): a study by 1H triple-quantum fast-MAS solid-state NMR. United States: N. p., 2018.
Web. doi:10.1039/C8CP04425B.
Kobayashi, Takeshi, Singappuli-Arachchige, Dilini, Slowing, Igor I., & Pruski, Marek. Spatial distribution of organic functional groups supported on mesoporous silica nanoparticles (2): a study by 1H triple-quantum fast-MAS solid-state NMR. United States. https://doi.org/10.1039/C8CP04425B
Kobayashi, Takeshi, Singappuli-Arachchige, Dilini, Slowing, Igor I., and Pruski, Marek. Fri .
"Spatial distribution of organic functional groups supported on mesoporous silica nanoparticles (2): a study by 1H triple-quantum fast-MAS solid-state NMR". United States. https://doi.org/10.1039/C8CP04425B. https://www.osti.gov/servlets/purl/1467595.
@article{osti_1467595,
title = {Spatial distribution of organic functional groups supported on mesoporous silica nanoparticles (2): a study by 1H triple-quantum fast-MAS solid-state NMR},
author = {Kobayashi, Takeshi and Singappuli-Arachchige, Dilini and Slowing, Igor I. and Pruski, Marek},
abstractNote = {The distribution of organic functional groups attached to the surface of mesoporous silica nanoparticles (MSNs) via co-condensation was scrutinized using 1D and 2D 1H solid-state NMR, including the triple-quantum/single-quantum (TQ/SQ) homonuclear correlation technique. The excellent sensitivity of 1H NMR and high resolution provided by fast magic angle spinning (MAS) allowed us to study surfaces with very low concentrations of aminopropyl functional groups. The sequential process, in which the injection of tetraethyl orthosilicate (TEOS) into the aqueous mother liquor was followed by dropwise addition of the organosilane precursor, resulted in deployment of organic groups on the surface, which were highly clustered even in a sample with a very low loading of ~0.1 mmol g-1. The underlying mechanism responsible for clustering could involve fast aggregation of the aminopropyltrimethoxysilane (APTMS) precursor within the liquid phase, and/or co-condensation of the silica-bound molecules. Understanding the deposition process and the resulting topology of surface functionalities with atomic-scale resolution, can help to develop novel approaches to the synthesis of complex inorganic–organic hybrid materials.},
doi = {10.1039/C8CP04425B},
journal = {Physical Chemistry Chemical Physics. PCCP},
number = 34,
volume = 20,
place = {United States},
year = {Fri Aug 10 00:00:00 EDT 2018},
month = {Fri Aug 10 00:00:00 EDT 2018}
}
Web of Science
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Works referencing / citing this record:
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