Characterization of a Mixture of CO2 Adsorption Products in Hyperbranched Aminosilica Adsorbents by (13)C Solid-State NMR

Hyperbranched amine polymers (HAS) grown from the mesoporous silica SBA-15 (hereafter "SBA-15-HAS") exhibit large capacities for CO2 adsorption. We have used static in situ and magic-angle spinning (MAS) ex situ (13)C nuclear magnetic resonance (NMR) to examine the adsorption of CO2 by SBA...

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Veröffentlicht in:Environmental science & technology 2015-11, Vol.49 (22), p.13684-13691
Hauptverfasser: Moore, Jeremy K, Sakwa-Novak, Miles A, Chaikittisilp, Watcharop, Mehta, Anil K, Conradi, Mark S, Jones, Christopher W, Hayes, Sophia E
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container_end_page 13691
container_issue 22
container_start_page 13684
container_title Environmental science & technology
container_volume 49
creator Moore, Jeremy K
Sakwa-Novak, Miles A
Chaikittisilp, Watcharop
Mehta, Anil K
Conradi, Mark S
Jones, Christopher W
Hayes, Sophia E
description Hyperbranched amine polymers (HAS) grown from the mesoporous silica SBA-15 (hereafter "SBA-15-HAS") exhibit large capacities for CO2 adsorption. We have used static in situ and magic-angle spinning (MAS) ex situ (13)C nuclear magnetic resonance (NMR) to examine the adsorption of CO2 by SBA-15-HAS. (13)C NMR distinguishes the signal of gas-phase (13)CO2 from that of the chemisorbed species. HAS polymers possess primary, secondary, and tertiary amines, leading to multiple chemisorption reaction outcomes, including carbamate (RnNCOO(-)), carbamic acid (RnNCOOH), and bicarbonate (HCO3(-)) moieties. Carbamates and bicarbonate fall within a small (13)C chemical shift range (162-166 ppm), and a mixture was observed including carbamic acid and carbamate, the former disappearing upon evacuation of the sample. By examining the (13)C-(14)N dipolar coupling through low-field (B0 = 3 T) (13)C{(1)H} cross-polarization MAS NMR, carbamate is confirmed through splitting of the (13)C resonance. A third species that is either bicarbonate or a second carbamate is evident from bimodal T2 decay times of the ∼163 ppm peak, indicating the presence of two species comprising that single resonance. The mixture of products suggests that (1) the presence of amines and water leads to bicarbonate being present and/or (2) the multiple types of amine sites in HAS permit formation of chemically distinct carbamates.
doi_str_mv 10.1021/acs.est.5b02930
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source MEDLINE; American Chemical Society Journals
subjects Adsorption
Amines - chemistry
Carbamates - chemistry
Carbon Dioxide - chemistry
Carbon Isotopes
Magnetic Resonance Spectroscopy - methods
Polymers - chemistry
Silicon Dioxide
Water - chemistry
title Characterization of a Mixture of CO2 Adsorption Products in Hyperbranched Aminosilica Adsorbents by (13)C Solid-State NMR
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