DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Role of Amine Structure on Hydrogen Sulfide Capture from Dilute Gas Streams Using Solid Adsorbents

Abstract

The hydrogen sulfide composition in biogas ranges from 0 to 5% depending on the feed source to the biogas digester. To meet renewable natural gas specifications of 0–4 ppm of H2S content, technologies that remove H2S from raw biogas feeds are needed. This contribution assesses three adsorbents with similar textural and physical properties but with different amines grafted to the surface. Specifically, materials containing primary, secondary, and tertiary amines at the end of a propyl surface linker grafted on a silica support are explored. H2S adsorption isotherms and cyclic studies are presented for these materials, and it is shown that secondary amines have the best amine efficiency while tertiary amines are the most stable for H2S capture, of the materials studied. The results suggest the consideration of secondary and tertiary amines for the design of amine adsorbents suitable for H2S removal in dilute gas streams over multiple cycles.

Authors:
 [1];  [1];  [1]; ORCiD logo [1]; ORCiD logo [1]
  1. Georgia Inst. of Technology, Atlanta, GA (United States). School of Chemical & Biomolecular Engineering
Publication Date:
Research Org.:
Energy Frontier Research Centers (EFRC) (United States). Center for Understanding and Control of Acid Gas-induced Evolution of Materials for Energy (UNCAGE-ME)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1470627
Grant/Contract Number:  
SC0012577
Resource Type:
Accepted Manuscript
Journal Name:
Energy and Fuels
Additional Journal Information:
Journal Volume: 32; Journal Issue: 6; Related Information: UNCAGE-ME partners with Georgia Institute of Technology (lead); Lehigh University; Oak Ridge National Laboratory; University of Alabama; University of Florida; University of Wisconsin; Washington University in St. Louis; Journal ID: ISSN 0887-0624
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
09 BIOMASS FUELS; catalysis (heterogeneous); defects, membrane; carbon capture; materials and chemistry by design; synthesis (novel materials); synthesis (self-assembly); synthesis (scalable processing)

Citation Formats

Okonkwo, Claudia N., Okolie, Chukwuemeka, Sujan, Achintya, Zhu, Guanghui, and Jones, Christopher W. Role of Amine Structure on Hydrogen Sulfide Capture from Dilute Gas Streams Using Solid Adsorbents. United States: N. p., 2018. Web. doi:10.1021/acs.energyfuels.8b00936.
Okonkwo, Claudia N., Okolie, Chukwuemeka, Sujan, Achintya, Zhu, Guanghui, & Jones, Christopher W. Role of Amine Structure on Hydrogen Sulfide Capture from Dilute Gas Streams Using Solid Adsorbents. United States. https://doi.org/10.1021/acs.energyfuels.8b00936
Okonkwo, Claudia N., Okolie, Chukwuemeka, Sujan, Achintya, Zhu, Guanghui, and Jones, Christopher W. Tue . "Role of Amine Structure on Hydrogen Sulfide Capture from Dilute Gas Streams Using Solid Adsorbents". United States. https://doi.org/10.1021/acs.energyfuels.8b00936. https://www.osti.gov/servlets/purl/1470627.
@article{osti_1470627,
title = {Role of Amine Structure on Hydrogen Sulfide Capture from Dilute Gas Streams Using Solid Adsorbents},
author = {Okonkwo, Claudia N. and Okolie, Chukwuemeka and Sujan, Achintya and Zhu, Guanghui and Jones, Christopher W.},
abstractNote = {The hydrogen sulfide composition in biogas ranges from 0 to 5% depending on the feed source to the biogas digester. To meet renewable natural gas specifications of 0–4 ppm of H2S content, technologies that remove H2S from raw biogas feeds are needed. This contribution assesses three adsorbents with similar textural and physical properties but with different amines grafted to the surface. Specifically, materials containing primary, secondary, and tertiary amines at the end of a propyl surface linker grafted on a silica support are explored. H2S adsorption isotherms and cyclic studies are presented for these materials, and it is shown that secondary amines have the best amine efficiency while tertiary amines are the most stable for H2S capture, of the materials studied. The results suggest the consideration of secondary and tertiary amines for the design of amine adsorbents suitable for H2S removal in dilute gas streams over multiple cycles.},
doi = {10.1021/acs.energyfuels.8b00936},
journal = {Energy and Fuels},
number = 6,
volume = 32,
place = {United States},
year = {Tue May 01 00:00:00 EDT 2018},
month = {Tue May 01 00:00:00 EDT 2018}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Citation Metrics:
Cited by: 24 works
Citation information provided by
Web of Science

Save / Share:

Works referenced in this record:

A comparative analysis of biogas upgrading technologies: Photosynthetic vs physical/chemical processes
journal, July 2017


Upgrading biogas produced at dairy farms into renewable natural gas by methanation
journal, January 2018

  • Walker, Sean B.; Sun, Duo; Kidon, Dominika
  • International Journal of Energy Research, Vol. 42, Issue 4
  • DOI: 10.1002/er.3981

Removal of minor concentration of H2S on MDEA-modified SBA-15 for gas purification
journal, January 2012


Amine-Bearing Mesoporous Silica for CO 2 and H 2 S Removal from Natural Gas and Biogas
journal, December 2009

  • Belmabkhout, Youssef; De Weireld, Guy; Sayari, Abdelhamid
  • Langmuir, Vol. 25, Issue 23
  • DOI: 10.1021/la903238y

“Molecular Basket” Sorbents for Separation of CO 2 and H 2 S from Various Gas Streams
journal, April 2009

  • Ma, Xiaoliang; Wang, Xiaoxing; Song, Chunshan
  • Journal of the American Chemical Society, Vol. 131, Issue 16
  • DOI: 10.1021/ja8074105

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

Simultaneous Adsorption of H 2 S and CO 2 on Triamine-Grafted Pore-Expanded Mesoporous MCM-41 Silica
journal, March 2011

  • Belmabkhout, Youssef; Heymans, Nicolas; De Weireld, Guy
  • Energy & Fuels, Vol. 25, Issue 3
  • DOI: 10.1021/ef1015704

Stability of Supported Amine Adsorbents to SO 2 and NO x in Postcombustion CO 2 Capture. 2. Multicomponent Adsorption
journal, July 2014

  • Rezaei, Fateme; Jones, Christopher W.
  • Industrial & Engineering Chemistry Research, Vol. 53, Issue 30
  • DOI: 10.1021/ie502024z

Amine-oxide hybrid materials for acid gas separations
journal, January 2011

  • Bollini, Praveen; Didas, Stephanie A.; Jones, Christopher W.
  • Journal of Materials Chemistry, Vol. 21, Issue 39
  • DOI: 10.1039/c1jm12522b

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

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

Poly(ethyleneimine)-Loaded Silica Monolith with a Hierarchical Pore Structure for H 2 S Adsorptive Removal
journal, November 2010

  • Chen, Qingjun; Fan, Feichao; Long, Donghui
  • Industrial & Engineering Chemistry Research, Vol. 49, Issue 22
  • DOI: 10.1021/ie101464f

Mesoporous-molecular-sieve-supported Polymer Sorbents for Removing H2S from Hydrogen Gas Streams
journal, April 2008


A nanoporous polymeric sorbent for deep removal of H2S from gas mixtures for hydrogen purification
journal, January 2007

  • Wang, Xiaoxing; Ma, Xiaoliang; Sun, Lu
  • Green Chemistry, Vol. 9, Issue 6
  • DOI: 10.1039/b614621j

Amine modified silica xerogel for H 2 S removal at low temperature
journal, December 2014


Effect of the structure of the support and the aminosilane type on the adsorption of H2S from model gas
journal, January 2014

  • Abdouss, Majid; Hazrati, Nastaran; Miran Beigi, Ali Akbar
  • RSC Advances, Vol. 4, Issue 12
  • DOI: 10.1039/c3ra43181a

Hydrogen Sulfide Capture: From Absorption in Polar Liquids to Oxide, Zeolite, and Metal–Organic Framework Adsorbents and Membranes
journal, May 2017


Selective Removal of H 2 S from Biogas Using Solid Amine-Based “Molecular Basket” Sorbent
journal, August 2017


Post-Grafting Amination of Alkyl Halide-Functionalized Silica for Applications in Catalysis, Adsorption, and 15 N NMR Spectroscopy
journal, February 2015

  • Moschetta, Eric G.; Sakwa-Novak, Miles A.; Greenfield, Jake L.
  • Langmuir, Vol. 31, Issue 7
  • DOI: 10.1021/la5046817

An Infrared Study of the Amine-Catalyzed Reaction of Methoxymethylsilanes with Silica
journal, July 2000

  • White, L. D.; Tripp, C. P.
  • Journal of Colloid and Interface Science, Vol. 227, Issue 1
  • DOI: 10.1006/jcis.2000.6895

Characterization of Micro- and Mesoporosity in SBA-15 Materials from Adsorption Data by the NLDFT Method
journal, July 2001

  • Ravikovitch, Peter I.; Neimark, Alexander V.
  • The Journal of Physical Chemistry B, Vol. 105, Issue 29
  • DOI: 10.1021/jp010621u

Shaping amine-based solid CO2 adsorbents: Effects of pelletization pressure on the physical and chemical properties
journal, March 2015


Morphological Control of Highly Ordered Mesoporous Silica SBA-15
journal, February 2000

  • Zhao, Dongyuan; Sun, Jinyu; Li, Quanzhi
  • Chemistry of Materials, Vol. 12, Issue 2
  • DOI: 10.1021/cm9911363

Correlation of the Base Strengths of Amines 1
journal, October 1957

  • Hall, H. K.
  • Journal of the American Chemical Society, Vol. 79, Issue 20
  • DOI: 10.1021/ja01577a030

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

On thermodynamic separation efficiency: Adsorption processes
journal, April 2016

  • Lively, Ryan P.; Realff, Matthew J.
  • AIChE Journal, Vol. 62, Issue 10
  • DOI: 10.1002/aic.15269

Works referencing / citing this record:

Amine‐functionalized ordered mesoporous silicas as model materials for liquid phase acid capture
journal, January 2020

  • Miller, Peter J.; Shantz, Daniel F.
  • AIChE Journal, Vol. 66, Issue 4
  • DOI: 10.1002/aic.16918

Stability of amine-functionalized CO 2 adsorbents: a multifaceted puzzle
journal, January 2019

  • Jahandar Lashaki, Masoud; Khiavi, Soheil; Sayari, Abdelhamid
  • Chemical Society Reviews, Vol. 48, Issue 12
  • DOI: 10.1039/c8cs00877a