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Title: Water Enables Efficient CO 2 Capture from Natural Gas Flue Emissions in an Oxidation-Resistant Diamine-Appended Metal–Organic Framework

Abstract

Supported by increasingly available reserves, natural gas is achieving greater adoption as a cleaner-burning alternative to coal in the power sector. As a result, carbon capture and sequestration from natural gas-fired power plants is an attractive strategy to mitigate global anthropogenic CO 2 emissions. However, the separation of CO 2 from other components in the flue streams of gas-fired power plants is particularly challenging due to the low CO 2 partial pressure (~40 mbar), which necessitates that candidate separation materials bind CO 2 strongly at low partial pressures (≤4 mbar) to capture ≥90% of the emitted CO 2. High partial pressures of O 2 (120 mbar) and water (80 mbar) in these flue streams have also presented significant barriers to the deployment of new technologies for CO 2 capture from gas-fired power plants. In this paper, we demonstrate that functionalization of the metal–organic framework Mg 2(dobpdc) (dobpdc 4– = 4,4'-dioxidobiphenyl-3,3'-dicarboxylate) with the cyclic diamine 2-(aminomethyl)piperidine (2-ampd) produces an adsorbent that is capable of ≥90% CO 2 capture from a humid natural gas flue emission stream, as confirmed by breakthrough measurements. This material captures CO 2 by a cooperative mechanism that enables access to a large CO 2 cycling capacity withmore » a small temperature swing (2.4 mmol CO 2/g with Δ T = 100 °C). Significantly, multicomponent adsorption experiments, infrared spectroscopy, magic angle spinning solid-state NMR spectroscopy, and van der Waals-corrected density functional theory studies suggest that water enhances CO 2 capture in 2-ampd–Mg 2(dobpdc) through hydrogen-bonding interactions with the carbamate groups of the ammonium carbamate chains formed upon CO 2 adsorption, thereby increasing the thermodynamic driving force for CO 2 binding. In light of the exceptional thermal and oxidative stability of 2-ampd–Mg 2(dobpdc), its high CO 2 adsorption capacity, and its high CO 2 capture rate from a simulated natural gas flue emission stream, this material is one of the most promising adsorbents to date for this important separation.« less

Authors:
 [1]; ORCiD logo [1]; ORCiD logo [2];  [3];  [4];  [5]; ORCiD logo [6]; ORCiD logo [7]; ORCiD logo [8]
  1. Univ. of California, Berkeley, CA (United States). Dept. of Chemistry; Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Materials Sciences Division
  2. Univ. of California, Berkeley, CA (United States). Dept. of Chemistry, Berkeley Energy and Climate Institute, and Dept. of Chemical and Biomolecular Engineering
  3. Univ. of California, Berkeley, CA (United States). Dept. of Physics
  4. Univ. of California, Berkeley, CA (United States). Dept. of Chemical and Biomolecular Engineering
  5. Univ. of California, Berkeley, CA (United States). Dept. of Physics; Kavli Energy NanoScience Institute, Berkeley, CA (United States)
  6. Univ. of California, Berkeley, CA (United States). Dept. of Chemical and Biomolecular Engineering; Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Materials Sciences Division
  7. ExxonMobile Research and Engineering Company, Annandale, NJ (United States). Corporate Strategic Research
  8. Univ. of California, Berkeley, CA (United States). Dept. of Chemistry and Dept. of Chemical and Biomolecular Engineering; Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Materials Sciences Division
Publication Date:
Research Org.:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); ExxonMobil Research and Engineering Company; National Institutes of Health (NIH)
OSTI Identifier:
1634051
Grant/Contract Number:  
AC02-05CH11231; AC02-112106CH11357; F32GM120799
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Journal of the American Chemical Society
Additional Journal Information:
Journal Volume: 141; Journal Issue: 33; Journal ID: ISSN 0002-7863
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
isotherms; environmental pollution; adsorption; humidity; materials

Citation Formats

Siegelman, Rebecca L., Milner, Phillip J., Forse, Alexander C., Lee, Jung-Hoon, Colwell, Kristen A., Neaton, Jeffrey B., Reimer, Jeffrey A., Weston, Simon C., and Long, Jeffrey R. Water Enables Efficient CO2 Capture from Natural Gas Flue Emissions in an Oxidation-Resistant Diamine-Appended Metal–Organic Framework. United States: N. p., 2019. Web. doi:10.1021/jacs.9b05567.
Siegelman, Rebecca L., Milner, Phillip J., Forse, Alexander C., Lee, Jung-Hoon, Colwell, Kristen A., Neaton, Jeffrey B., Reimer, Jeffrey A., Weston, Simon C., & Long, Jeffrey R. Water Enables Efficient CO2 Capture from Natural Gas Flue Emissions in an Oxidation-Resistant Diamine-Appended Metal–Organic Framework. United States. doi:10.1021/jacs.9b05567.
Siegelman, Rebecca L., Milner, Phillip J., Forse, Alexander C., Lee, Jung-Hoon, Colwell, Kristen A., Neaton, Jeffrey B., Reimer, Jeffrey A., Weston, Simon C., and Long, Jeffrey R. Fri . "Water Enables Efficient CO2 Capture from Natural Gas Flue Emissions in an Oxidation-Resistant Diamine-Appended Metal–Organic Framework". United States. doi:10.1021/jacs.9b05567. https://www.osti.gov/servlets/purl/1634051.
@article{osti_1634051,
title = {Water Enables Efficient CO2 Capture from Natural Gas Flue Emissions in an Oxidation-Resistant Diamine-Appended Metal–Organic Framework},
author = {Siegelman, Rebecca L. and Milner, Phillip J. and Forse, Alexander C. and Lee, Jung-Hoon and Colwell, Kristen A. and Neaton, Jeffrey B. and Reimer, Jeffrey A. and Weston, Simon C. and Long, Jeffrey R.},
abstractNote = {Supported by increasingly available reserves, natural gas is achieving greater adoption as a cleaner-burning alternative to coal in the power sector. As a result, carbon capture and sequestration from natural gas-fired power plants is an attractive strategy to mitigate global anthropogenic CO2 emissions. However, the separation of CO2 from other components in the flue streams of gas-fired power plants is particularly challenging due to the low CO2 partial pressure (~40 mbar), which necessitates that candidate separation materials bind CO2 strongly at low partial pressures (≤4 mbar) to capture ≥90% of the emitted CO2. High partial pressures of O2 (120 mbar) and water (80 mbar) in these flue streams have also presented significant barriers to the deployment of new technologies for CO2 capture from gas-fired power plants. In this paper, we demonstrate that functionalization of the metal–organic framework Mg2(dobpdc) (dobpdc4– = 4,4'-dioxidobiphenyl-3,3'-dicarboxylate) with the cyclic diamine 2-(aminomethyl)piperidine (2-ampd) produces an adsorbent that is capable of ≥90% CO2 capture from a humid natural gas flue emission stream, as confirmed by breakthrough measurements. This material captures CO2 by a cooperative mechanism that enables access to a large CO2 cycling capacity with a small temperature swing (2.4 mmol CO2/g with ΔT = 100 °C). Significantly, multicomponent adsorption experiments, infrared spectroscopy, magic angle spinning solid-state NMR spectroscopy, and van der Waals-corrected density functional theory studies suggest that water enhances CO2 capture in 2-ampd–Mg2(dobpdc) through hydrogen-bonding interactions with the carbamate groups of the ammonium carbamate chains formed upon CO2 adsorption, thereby increasing the thermodynamic driving force for CO2 binding. In light of the exceptional thermal and oxidative stability of 2-ampd–Mg2(dobpdc), its high CO2 adsorption capacity, and its high CO2 capture rate from a simulated natural gas flue emission stream, this material is one of the most promising adsorbents to date for this important separation.},
doi = {10.1021/jacs.9b05567},
journal = {Journal of the American Chemical Society},
issn = {0002-7863},
number = 33,
volume = 141,
place = {United States},
year = {2019},
month = {7}
}

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