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Title: Role of Alumina Basicity in CO 2 Uptake in 3‐Aminopropylsilyl‐Grafted Alumina Adsorbents

Abstract

Abstract Oxide‐supported amine materials are widely known to be effective CO 2 sorbents under simulated flue‐gas and direct‐air‐capture conditions. Most work has focused on amine species loaded onto porous silica supports, though potential stability advantages may be offered through the use of porous alumina supports. Unlike silica materials, which are comparably inert, porous alumina materials can be tuned to have substantial acidity and/or basicity. Owing to their amphoteric nature, alumina supports play a more active role in CO 2 sorption than silica supports, potentially directly participating in the adsorption process. In this work, primary amines associated with 3‐aminopropyltriethoxysilane are grafted onto two different mesoporous alumina materials having different levels of basicity. Adsorbent materials with different amine loadings are prepared, and the CO 2 ‐adsorption behavior of similar amines on the two alumina supports is demonstrated to be different. At low amine loadings, the inherent properties of the support surface play a significant role, whereas at high amine loadings, when the alumina surface is effectively blocked, the sorbents prepared on the two supports behave similarly. At high amine loadings, amine–CO 2 –amine interactions are shown to dominate, leading to adsorbed species that appear similar to the species formed over silica‐supported aminemore » materials. The sorbent properties are comprehensively characterized using N 2 physisorption analysis, in situ FTIR spectroscopy, and adsorption microcalorimetry.« less

Authors:
 [1];  [2];  [1]; ORCiD logo [1]
  1. School of Chemical and Biomolecular Engineering Georgia Institute of Technology 311 Ferst Drive, NW Atlanta GA 30332 USA
  2. School of Chemical and Biomolecular Engineering Georgia Institute of Technology 311 Ferst Drive, NW Atlanta GA 30332 USA, Department of Chemical and Biomolecular Engineering (BK-21 plus) Korea Advanced Institute of Science and Technology Daejeon 305-701 Republic of Korea
Publication Date:
Sponsoring Org.:
USDOE
OSTI Identifier:
1400836
Resource Type:
Publisher's Accepted Manuscript
Journal Name:
ChemSusChem
Additional Journal Information:
Journal Name: ChemSusChem Journal Volume: 10 Journal Issue: 10; Journal ID: ISSN 1864-5631
Publisher:
Wiley Blackwell (John Wiley & Sons)
Country of Publication:
Germany
Language:
English

Citation Formats

Potter, Matthew E., Cho, Kyeong Min, Lee, Jason J., and Jones, Christopher W. Role of Alumina Basicity in CO 2 Uptake in 3‐Aminopropylsilyl‐Grafted Alumina Adsorbents. Germany: N. p., 2017. Web. doi:10.1002/cssc.201700115.
Potter, Matthew E., Cho, Kyeong Min, Lee, Jason J., & Jones, Christopher W. Role of Alumina Basicity in CO 2 Uptake in 3‐Aminopropylsilyl‐Grafted Alumina Adsorbents. Germany. https://doi.org/10.1002/cssc.201700115
Potter, Matthew E., Cho, Kyeong Min, Lee, Jason J., and Jones, Christopher W. Wed . "Role of Alumina Basicity in CO 2 Uptake in 3‐Aminopropylsilyl‐Grafted Alumina Adsorbents". Germany. https://doi.org/10.1002/cssc.201700115.
@article{osti_1400836,
title = {Role of Alumina Basicity in CO 2 Uptake in 3‐Aminopropylsilyl‐Grafted Alumina Adsorbents},
author = {Potter, Matthew E. and Cho, Kyeong Min and Lee, Jason J. and Jones, Christopher W.},
abstractNote = {Abstract Oxide‐supported amine materials are widely known to be effective CO 2 sorbents under simulated flue‐gas and direct‐air‐capture conditions. Most work has focused on amine species loaded onto porous silica supports, though potential stability advantages may be offered through the use of porous alumina supports. Unlike silica materials, which are comparably inert, porous alumina materials can be tuned to have substantial acidity and/or basicity. Owing to their amphoteric nature, alumina supports play a more active role in CO 2 sorption than silica supports, potentially directly participating in the adsorption process. In this work, primary amines associated with 3‐aminopropyltriethoxysilane are grafted onto two different mesoporous alumina materials having different levels of basicity. Adsorbent materials with different amine loadings are prepared, and the CO 2 ‐adsorption behavior of similar amines on the two alumina supports is demonstrated to be different. At low amine loadings, the inherent properties of the support surface play a significant role, whereas at high amine loadings, when the alumina surface is effectively blocked, the sorbents prepared on the two supports behave similarly. At high amine loadings, amine–CO 2 –amine interactions are shown to dominate, leading to adsorbed species that appear similar to the species formed over silica‐supported amine materials. The sorbent properties are comprehensively characterized using N 2 physisorption analysis, in situ FTIR spectroscopy, and adsorption microcalorimetry.},
doi = {10.1002/cssc.201700115},
journal = {ChemSusChem},
number = 10,
volume = 10,
place = {Germany},
year = {Wed Apr 26 00:00:00 EDT 2017},
month = {Wed Apr 26 00:00:00 EDT 2017}
}

Journal Article:
Free Publicly Available Full Text
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https://doi.org/10.1002/cssc.201700115

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Cited by: 38 works
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Works referenced in this record:

Study of Carbon Dioxide Adsorption on Mesoporous Aminopropylsilane-Functionalized Silica and Titania Combining Microcalorimetry and in Situ Infrared Spectroscopy
journal, December 2009

  • Knöfel, Christina; Martin, Céline; Hornebecq, Virginie
  • The Journal of Physical Chemistry C, Vol. 113, Issue 52
  • DOI: 10.1021/jp907054h

An Amine-Functionalized MIL-53 Metal−Organic Framework with Large Separation Power for CO 2 and CH 4
journal, May 2009

  • Couck, Sarah; Denayer, Joeri F. M.; Baron, Gino V.
  • Journal of the American Chemical Society, Vol. 131, Issue 18
  • DOI: 10.1021/ja900555r

Post-Combustion CO2 Capture Using Solid Sorbents: A Review
journal, September 2011

  • Samanta, Arunkumar; Zhao, An; Shimizu, George K. H.
  • Industrial & Engineering Chemistry Research, Vol. 51, Issue 4, p. 1438-1463
  • DOI: 10.1021/ie200686q

Boron and nitrogen-rich carbons from ionic liquid precursors with tailorable surface properties
journal, January 2011

  • Fulvio, Pasquale F.; Lee, Je Seung; Mayes, Richard T.
  • Physical Chemistry Chemical Physics, Vol. 13, Issue 30
  • DOI: 10.1039/c1cp20631a

In-Situ Infrared Study of CO 2 Adsorption on SBA-15 Grafted with γ-(Aminopropyl)triethoxysilane
journal, March 2003

  • Chang, Alex C. C.; Chuang, Steven S. C.; Gray, McMahan
  • Energy & Fuels, Vol. 17, Issue 2
  • DOI: 10.1021/ef020176h

Role of Amine Functionality for CO 2 Chemisorption on Silica
journal, November 2015

  • Hahn, Maximilian W.; Jelic, Jelena; Berger, Edith
  • The Journal of Physical Chemistry B, Vol. 120, Issue 8
  • DOI: 10.1021/acs.jpcb.5b10012

Functionalised micro-/mesoporous silica for the adsorption of carbon dioxide
journal, February 2007


Adsorption of H2, O2, CO, and CO2 on a .gamma.-Alumina: Volumetric and Calorimetric Studies
journal, March 1994

  • Cabrejas Manchado, M.; Guil, J. M.; Perez Masia, A.
  • Langmuir, Vol. 10, Issue 3
  • DOI: 10.1021/la00015a016

Aminosilanes Grafted to Basic Alumina as CO 2 Adsorbents-Role of Grafting Conditions on CO 2 Adsorption Properties
journal, September 2014


Novel Polyethylenimine-Modified Mesoporous Molecular Sieve of MCM-41 Type as High-Capacity Adsorbent for CO2 Capture
journal, November 2002

  • Xu, Xiaochun; Song, Chunshan; Andresen, John M.
  • Energy & Fuels, Vol. 16, Issue 6, p. 1463-1469
  • DOI: 10.1021/ef020058u

Aluminum Local Environment and Defects in the Crystalline Structure of Sol−Gel Alumina Catalyst
journal, January 1999

  • Wang, J. A.; Bokhimi, X.; Morales, A.
  • The Journal of Physical Chemistry B, Vol. 103, Issue 2
  • DOI: 10.1021/jp983130r

Acidic properties of alumina-supported metal oxide catalysts: an infrared spectroscopy study
journal, June 1992

  • Turek, Andrzej M.; Wachs, Israel E.; DeCanio, Elaine
  • The Journal of Physical Chemistry, Vol. 96, Issue 12
  • DOI: 10.1021/j100191a050

Infrared Study of CO 2 Sorption over “Molecular Basket” Sorbent Consisting of Polyethylenimine-Modified Mesoporous Molecular Sieve
journal, April 2009

  • Wang, Xiaoxing; Schwartz, Viviane; Clark, Jason C.
  • The Journal of Physical Chemistry C, Vol. 113, Issue 17
  • DOI: 10.1021/jp809946y

CO2 capture by solid adsorbents and their applications: current status and new trends
journal, January 2011

  • Wang, Qiang; Luo, Jizhong; Zhong, Ziyi
  • Energy Environ. Sci., Vol. 4, Issue 1
  • DOI: 10.1039/C0EE00064G

Oxidative Degradation of Aminosilica Adsorbents Relevant to Postcombustion CO 2 Capture
journal, May 2011

  • Bollini, Praveen; Choi, Sunho; Drese, Jeffrey H.
  • Energy & Fuels, Vol. 25, Issue 5
  • DOI: 10.1021/ef200140z

Effect of Amine Surface Coverage on the Co-Adsorption of CO 2 and Water: Spectral Deconvolution of Adsorbed Species
journal, November 2014

  • Didas, Stephanie A.; Sakwa-Novak, Miles A.; Foo, Guo Shiou
  • The Journal of Physical Chemistry Letters, Vol. 5, Issue 23
  • DOI: 10.1021/jz502032c

Polyethylenimine-Impregnated Mesoporous Silica: Effect of Amine Loading and Surface Alkyl Chains on CO 2 Adsorption
journal, October 2011

  • Heydari-Gorji, Aliakbar; Belmabkhout, Youssef; Sayari, Abdelhamid
  • Langmuir, Vol. 27, Issue 20
  • DOI: 10.1021/la202972t

Thermal, Oxidative and CO 2 Induced Degradation of Primary Amines Used for CO 2 Capture: Effect of Alkyl Linker on Stability
journal, May 2014

  • Didas, Stephanie A.; Zhu, Rongshun; Brunelli, Nicholas A.
  • The Journal of Physical Chemistry C, Vol. 118, Issue 23
  • DOI: 10.1021/jp5025137

Adsorption of Carbon Dioxide on 3-Aminopropyl-Triethoxysilane Modified Graphite Oxide
journal, May 2013

  • Hong, Seok-Min; Kim, Sung Hyun; Lee, Ki Bong
  • Energy & Fuels, Vol. 27, Issue 6
  • DOI: 10.1021/ef400467w

Oxidative Stability of Amino Polymer–Alumina Hybrid Adsorbents for Carbon Dioxide Capture
journal, March 2013

  • Bali, Sumit; Chen, Thomas T.; Chaikittisilp, Watcharop
  • Energy & Fuels, Vol. 27, Issue 3
  • DOI: 10.1021/ef4001067

Adsorption characteristics of carbon dioxide on organically functionalized SBA-15
journal, September 2005

  • Hiyoshi, Norihito; Yogo, Katsunori; Yashima, Tatsuaki
  • Microporous and Mesoporous Materials, Vol. 84, Issue 1-3, p. 357-365
  • DOI: 10.1016/j.micromeso.2005.06.010

Temperature-Induced Uptake of CO 2 and Formation of Carbamates in Mesocaged Silica Modified with n -Propylamines
journal, June 2010

  • Bacsik, Zoltán; Atluri, Rambabu; Garcia-Bennett, Alfonso E.
  • Langmuir, Vol. 26, Issue 12
  • DOI: 10.1021/la1001495

Amine-Grafted MCM-48 and Silica Xerogel as Superior Sorbents for Acidic Gas Removal from Natural Gas
journal, June 2003

  • Huang, Helen Y.; Yang, Ralph T.; Chinn, Daniel
  • Industrial & Engineering Chemistry Research, Vol. 42, Issue 12
  • DOI: 10.1021/ie020440u

Interrogating the Carbon and Oxygen K-Edge NEXAFS of a CO 2 -Dosed Hyperbranched Aminosilica
journal, December 2014

  • Espinal, Laura; Green, Martin L.; Fischer, Daniel A.
  • The Journal of Physical Chemistry Letters, Vol. 6, Issue 1
  • DOI: 10.1021/jz502483v

Applications of Pore-Expanded Mesoporous Silicas. 3. Triamine Silane Grafting for Enhanced CO 2 Adsorption
journal, April 2006

  • Harlick, Peter J. E.; Sayari, Abdelhamid
  • Industrial & Engineering Chemistry Research, Vol. 45, Issue 9
  • DOI: 10.1021/ie051286p

Dynamics of CO 2 Adsorption on Amine Adsorbents. 2. Insights Into Adsorbent Design
journal, November 2012

  • Bollini, Praveen; Brunelli, Nicholas A.; Didas, Stephanie A.
  • Industrial & Engineering Chemistry Research, Vol. 51, Issue 46
  • DOI: 10.1021/ie3017913

Synthesis–Structure–Property Relationships for Hyperbranched Aminosilica CO 2 Adsorbents
journal, December 2009

  • Drese, Jeffrey H.; Choi, Sunho; Lively, Ryan P.
  • Advanced Functional Materials, Vol. 19, Issue 23
  • DOI: 10.1002/adfm.200901461

Microcalorimetric and Infrared Spectroscopic Studies of .gamma.-Al2O3 Modified by Basic Metal Oxides
journal, August 1994

  • Shen, Jianyi; Cortright, R. D.; Chen, Yi
  • The Journal of Physical Chemistry, Vol. 98, Issue 33
  • DOI: 10.1021/j100084a025

Probing Intramolecular versus Intermolecular CO 2 Adsorption on Amine-Grafted SBA-15
journal, November 2015


Adsorption and Activation of CO2 by Amine-Modified Nanoporous Materials Studied by Solid-State NMR and 13CO2 Adsorption
journal, March 2011

  • Pinto, Moisés L.; Mafra, Luís; Guil, José M.
  • Chemistry of Materials, Vol. 23, Issue 6, p. 1387-1395
  • DOI: 10.1021/cm1029563

Study of the Interaction between Silica Surfaces and the Carbon Dioxide Molecule
journal, September 2010

  • Roque-Malherbe, R.; Polanco-Estrella, R.; Marquez-Linares, F.
  • The Journal of Physical Chemistry C, Vol. 114, Issue 41
  • DOI: 10.1021/jp107754g

Adsorptive removal of carbon dioxide using polyethyleneimine-loaded mesoporous silica materials
journal, August 2008


Role of Amine Structure on Carbon Dioxide Adsorption from Ultradilute Gas Streams such as Ambient Air
journal, July 2012

  • Didas, Stephanie A.; Kulkarni, Ambarish R.; Sholl, David S.
  • ChemSusChem, Vol. 5, Issue 10, p. 2058-2064
  • DOI: 10.1002/cssc.201200196

Mesoporous Alumina-Supported Amines as Potential Steam-Stable Adsorbents for Capturing CO 2 from Simulated Flue Gas and Ambient Air
journal, November 2011

  • Chaikittisilp, Watcharop; Kim, Hyung-Ju; Jones, Christopher W.
  • Energy & Fuels, Vol. 25, Issue 11
  • DOI: 10.1021/ef201224v

FTIR Study of CO2 Adsorption on Amine-Grafted SBA-15: Elucidation of Adsorbed Species
journal, May 2011

  • Danon, Alon; Stair, Peter C.; Weitz, Eric
  • The Journal of Physical Chemistry C, Vol. 115, Issue 23, p. 11540-11549
  • DOI: 10.1021/jp200914v

Adsorbent Materials for Carbon Dioxide Capture from Large Anthropogenic Point Sources
journal, September 2009

  • Choi, Sunho; Drese, Jeffrey H.; Jones, Christopher W.
  • ChemSusChem, Vol. 2, Issue 9, p. 796-854
  • DOI: 10.1002/cssc.200900036

Monitoring Solid Oxide CO 2 Capture Sorbents in Action
journal, October 2014

  • Keturakis, Christopher J.; Ni, Fan; Spicer, Michelle
  • ChemSusChem, Vol. 7, Issue 12
  • DOI: 10.1002/cssc.201402474

Amine-bearing mesoporous silica for CO2 removal from dry and humid air
journal, June 2010

  • Belmabkhout, Youssef; Serna-Guerrero, Rodrigo; Sayari, Abdelhamid
  • Chemical Engineering Science, Vol. 65, Issue 11
  • DOI: 10.1016/j.ces.2010.02.044

Tailoring Pore Properties of MCM-48 Silica for Selective Adsorption of CO 2
journal, April 2005

  • Kim, Sangil; Ida, Junichi; Guliants, Vadim V.
  • The Journal of Physical Chemistry B, Vol. 109, Issue 13
  • DOI: 10.1021/jp045634x

Adsorption of CO 2 on amine-functionalised MCM-41: experimental and theoretical studies
journal, January 2015

  • dos Santos, Thiago Custódio; Bourrelly, Sandrine; Llewellyn, Philip L.
  • Physical Chemistry Chemical Physics, Vol. 17, Issue 16
  • DOI: 10.1039/C5CP00581G

Mechanisms and Kinetics for Sorption of CO 2 on Bicontinuous Mesoporous Silica Modified with n -Propylamine
journal, September 2011

  • Bacsik, Zoltán; Ahlsten, Nanna; Ziadi, Asraa
  • Langmuir, Vol. 27, Issue 17
  • DOI: 10.1021/la202033p

Amine–Oxide Hybrid Materials for CO 2 Capture from Ambient Air
journal, September 2015

  • Didas, Stephanie A.; Choi, Sunho; Chaikittisilp, Watcharop
  • Accounts of Chemical Research, Vol. 48, Issue 10
  • DOI: 10.1021/acs.accounts.5b00284

Amine-modified MCM-41 mesoporous silica for carbon dioxide capture
journal, August 2011

  • Mello, Marília R.; Phanon, Delphine; Silveira, Gleiciani Q.
  • Microporous and Mesoporous Materials, Vol. 143, Issue 1
  • DOI: 10.1016/j.micromeso.2011.02.022

CO 2 -Induced Degradation of Amine-Containing Adsorbents: Reaction Products and Pathways
journal, August 2012

  • Sayari, Abdelhamid; Heydari-Gorji, Aliakbar; Yang, Yong
  • Journal of the American Chemical Society, Vol. 134, Issue 33
  • DOI: 10.1021/ja304888a

New Insights into the Interactions of CO 2 with Amine-Functionalized Silica
journal, December 2008

  • Serna-Guerrero, Rodrigo; Da’na, Enshirah; Sayari, Abdelhamid
  • Industrial & Engineering Chemistry Research, Vol. 47, Issue 23
  • DOI: 10.1021/ie801186g

Increasing Selective CO 2 Adsorption on Amine-Grafted SBA-15 by Increasing Silanol Density
journal, October 2011

  • Wang, Lifeng; Yang, Ralph T.
  • The Journal of Physical Chemistry C, Vol. 115, Issue 43
  • DOI: 10.1021/jp206976d

Important Roles of Enthalpic and Entropic Contributions to CO 2 Capture from Simulated Flue Gas and Ambient Air Using Mesoporous Silica Grafted Amines
journal, September 2014

  • Alkhabbaz, Mustafa A.; Bollini, Praveen; Foo, Guo Shiou
  • Journal of the American Chemical Society, Vol. 136, Issue 38
  • DOI: 10.1021/ja507655x

CO2 capture using mesoporous alumina prepared by a sol–gel process
journal, January 2011


Elucidation of Surface Species through in Situ FTIR Spectroscopy of Carbon Dioxide Adsorption on Amine-Grafted SBA-15
journal, August 2016


Thermal and Chemical Stability of Regenerable Solid Amine Sorbent for CO 2 Capture
journal, July 2006

  • Khatri, Rajesh A.; Chuang, Steven S. C.; Soong, Yee
  • Energy & Fuels, Vol. 20, Issue 4
  • DOI: 10.1021/ef050402y

Quantification of chemisorption and physisorption of carbon dioxide on porous silica modified by propylamines: Effect of amine density
journal, September 2012


Evaluating Pore Sizes in Mesoporous Materials:  A Simplified Standard Adsorption Method and a Simplified Broekhoff−de Boer Method
journal, August 1999

  • Lukens,, Wayne W.; Schmidt-Winkel, Patrick; Zhao, Dongyuan
  • Langmuir, Vol. 15, Issue 16
  • DOI: 10.1021/la990209u

Enhanced selective CO 2 adsorption on polyamine/MIL-101(Cr) composites
journal, January 2014

  • Lin, Yichao; Lin, Hao; Wang, Haimin
  • J. Mater. Chem. A, Vol. 2, Issue 35
  • DOI: 10.1039/C4TA01174K

An efficient low-temperature route to nitrogen-doping and activation of mesoporous carbons for CO 2 capture
journal, January 2015

  • Huang, Kuan; Chai, Song-Hai; Mayes, Richard T.
  • Chemical Communications, Vol. 51, Issue 97
  • DOI: 10.1039/C5CC05619E

Spectroscopic Investigation of the Mechanisms Responsible for the Superior Stability of Hybrid Class 1/Class 2 CO 2 Sorbents: A New Class 4 Category
journal, May 2016

  • Wilfong, Walter Christopher; Kail, Brian W.; Jones, Christopher W.
  • ACS Applied Materials & Interfaces, Vol. 8, Issue 20
  • DOI: 10.1021/acsami.6b02062