CO2 Uptake and Stability Enhancement in Vinyltrimethoxysilane-Treated SBA-15 Solid Amine-Based Sorbents

Anthony Vallace; Zachary S. Campbell; Hyun June Moon; William J. Koros; Christopher W. Jones; Ryan P. Lively

doi:10.1002/smll.202401422

CO₂ Uptake and Stability Enhancement in Vinyltrimethoxysilane-Treated SBA-15 Solid Amine-Based Sorbents

Anthony Vallace
, Zachary S. Campbell
, Hyun June Moon
, William J. Koros
, Christopher W. Jones
, Ryan P. Lively

Chemical Spectroscopy

Research output: Contribution to journal › Article › peer-review

7 Scopus citations

Abstract

Silica-supported amine absorbents, including materials produced by tethering aminosilanes or infusion of poly(ethyleneimine), represent a promising class of materials for CO₂ capture applications, including direct air and point source capture. Various silica surface treatments and functionalization strategies are explored to enhance stability and CO₂ uptake in amine-based solid sorbent systems. Here, the synthesis and characterization of novel vinyltrimethoxysilane-treated Santa Barbara Amorphous-15 (SBA-15) supports and the corresponding enhancement in CO₂ uptake compared to various SBA-15-based control supports are presented. The relationship between CO₂ diffusion and amine efficiency in these systems is explored using a previously reported kinetic model. The synthesized materials are characterized with CO₂ and H₂O isotherms, diffuse reflectance infrared Fourier transform spectroscopy, ¹H T₁–T₂ relaxation correlation NMR, and rapid thermal cycling experiments. The novel support materials are shown to enable high amine efficiencies, approaching a fourfold improvement over standard SBA-15-supported amines, while simultaneously exhibiting excellent stability when cycled rapidly under humid conditions. As the poly(ethyleneimine) loadings are held constant across the various samples, enhancements in CO₂ uptake are attributed to differences in the way the poly(ethyleneimine) interacts with the support surface.

Original language	English
Article number	2401422
Journal	Small
Volume	20
Issue number	46
DOIs	https://doi.org/10.1002/smll.202401422
State	Published - Nov 14 2024

Funding

A.V. and Z.S.C. contributed equally to this work. The information, data, or work presented herein was funded in part by the Advanced Research Projects Agency-Energy (Grant No. ARPA-E), the US Department of Energy, under Award Number DE-AR0001309. The views and opinions of authors expressed herein did not necessarily state or reflect those of the United States Government or any agency thereof. This work was performed in part at the Materials Characterization Facility (MCF) at the Georgia Tech. The MCF is jointly supported by the GT Institute for Materials (IMat) and the Institute for Electronics and Nanotechnology (IEN), which is a member of the National Nanotechnology Coordinated Infrastructure supported by the National Science Foundation (Grant No. ECCS-2025462). A.V. and Z.S.C. contributed equally to this work. The information, data, or work presented herein was funded in part by the Advanced Research Projects Agency‐Energy (Grant No. ARPA‐E), the US Department of Energy, under Award Number DE‐AR0001309. The views and opinions of authors expressed herein did not necessarily state or reflect those of the United States Government or any agency thereof. This work was performed in part at the Materials Characterization Facility (MCF) at the Georgia Tech. The MCF is jointly supported by the GT Institute for Materials (IMat) and the Institute for Electronics and Nanotechnology (IEN), which is a member of the National Nanotechnology Coordinated Infrastructure supported by the National Science Foundation (Grant No. ECCS‐2025462).

Keywords

adsorption
CO capture
functionalization
porous materials
T–T relaxation correlation NMR

Access to Document

10.1002/smll.202401422

Cite this

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title = "CO2 Uptake and Stability Enhancement in Vinyltrimethoxysilane-Treated SBA-15 Solid Amine-Based Sorbents",

abstract = "Silica-supported amine absorbents, including materials produced by tethering aminosilanes or infusion of poly(ethyleneimine), represent a promising class of materials for CO2 capture applications, including direct air and point source capture. Various silica surface treatments and functionalization strategies are explored to enhance stability and CO2 uptake in amine-based solid sorbent systems. Here, the synthesis and characterization of novel vinyltrimethoxysilane-treated Santa Barbara Amorphous-15 (SBA-15) supports and the corresponding enhancement in CO2 uptake compared to various SBA-15-based control supports are presented. The relationship between CO2 diffusion and amine efficiency in these systems is explored using a previously reported kinetic model. The synthesized materials are characterized with CO2 and H2O isotherms, diffuse reflectance infrared Fourier transform spectroscopy, 1H T1–T2 relaxation correlation NMR, and rapid thermal cycling experiments. The novel support materials are shown to enable high amine efficiencies, approaching a fourfold improvement over standard SBA-15-supported amines, while simultaneously exhibiting excellent stability when cycled rapidly under humid conditions. As the poly(ethyleneimine) loadings are held constant across the various samples, enhancements in CO2 uptake are attributed to differences in the way the poly(ethyleneimine) interacts with the support surface.",

keywords = "adsorption, CO capture, functionalization, porous materials, T–T relaxation correlation NMR",

author = "Anthony Vallace and Campbell, \{Zachary S.\} and Moon, \{Hyun June\} and Koros, \{William J.\} and Jones, \{Christopher W.\} and Lively, \{Ryan P.\}",

note = "Publisher Copyright: {\textcopyright} 2024 The Author(s). Small published by Wiley-VCH GmbH.",

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AU - Vallace, Anthony

AU - Campbell, Zachary S.

AU - Moon, Hyun June

AU - Koros, William J.

AU - Jones, Christopher W.

AU - Lively, Ryan P.

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N2 - Silica-supported amine absorbents, including materials produced by tethering aminosilanes or infusion of poly(ethyleneimine), represent a promising class of materials for CO2 capture applications, including direct air and point source capture. Various silica surface treatments and functionalization strategies are explored to enhance stability and CO2 uptake in amine-based solid sorbent systems. Here, the synthesis and characterization of novel vinyltrimethoxysilane-treated Santa Barbara Amorphous-15 (SBA-15) supports and the corresponding enhancement in CO2 uptake compared to various SBA-15-based control supports are presented. The relationship between CO2 diffusion and amine efficiency in these systems is explored using a previously reported kinetic model. The synthesized materials are characterized with CO2 and H2O isotherms, diffuse reflectance infrared Fourier transform spectroscopy, 1H T1–T2 relaxation correlation NMR, and rapid thermal cycling experiments. The novel support materials are shown to enable high amine efficiencies, approaching a fourfold improvement over standard SBA-15-supported amines, while simultaneously exhibiting excellent stability when cycled rapidly under humid conditions. As the poly(ethyleneimine) loadings are held constant across the various samples, enhancements in CO2 uptake are attributed to differences in the way the poly(ethyleneimine) interacts with the support surface.

AB - Silica-supported amine absorbents, including materials produced by tethering aminosilanes or infusion of poly(ethyleneimine), represent a promising class of materials for CO2 capture applications, including direct air and point source capture. Various silica surface treatments and functionalization strategies are explored to enhance stability and CO2 uptake in amine-based solid sorbent systems. Here, the synthesis and characterization of novel vinyltrimethoxysilane-treated Santa Barbara Amorphous-15 (SBA-15) supports and the corresponding enhancement in CO2 uptake compared to various SBA-15-based control supports are presented. The relationship between CO2 diffusion and amine efficiency in these systems is explored using a previously reported kinetic model. The synthesized materials are characterized with CO2 and H2O isotherms, diffuse reflectance infrared Fourier transform spectroscopy, 1H T1–T2 relaxation correlation NMR, and rapid thermal cycling experiments. The novel support materials are shown to enable high amine efficiencies, approaching a fourfold improvement over standard SBA-15-supported amines, while simultaneously exhibiting excellent stability when cycled rapidly under humid conditions. As the poly(ethyleneimine) loadings are held constant across the various samples, enhancements in CO2 uptake are attributed to differences in the way the poly(ethyleneimine) interacts with the support surface.

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KW - T–T relaxation correlation NMR

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