Spatial distribution of organic functional groups supported on mesoporous silica nanoparticles (2): a study by 1H triple-quantum fast-MAS solid-state NMR

Kobayashi, Takeshi; Singappuli-Arachchige, Dilini; Slowing, Igor I.; Pruski, Marek

doi:10.1039/C8CP04425B

Spatial distribution of organic functional groups supported on mesoporous silica nanoparticles (2): a study by ¹H triple-quantum fast-MAS solid-state NMR

Journal Article · Fri Aug 10 00:00:00 EDT 2018 · Physical Chemistry Chemical Physics. PCCP

DOI:https://doi.org/10.1039/C8CP04425B· OSTI ID:1467595

^[1]; Singappuli-Arachchige, Dilini ^[2]; ^[2]; ^[2]

Ames Lab. and Iowa State Univ., Ames, IA (United States)
Ames Lab. and Iowa State Univ., Ames, IA (United States). Dept. of Chemistry

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.

View Accepted Manuscript (DOE)

Research Organization:: Ames Laboratory (AMES), Ames, IA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: AC02-07CH11358

OSTI ID:: 1467595

Alternate ID(s):: OSTI ID: 1464972

Report Number(s):: IS-J--9736

Journal Information:: Physical Chemistry Chemical Physics. PCCP, Journal Name: Physical Chemistry Chemical Physics. PCCP Journal Issue: 34 Vol. 20; ISSN 1463-9076; ISSN PPCPFQ

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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