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Title

Cooperative insertion of CO2 in diamine-appended metal-organic frameworks

Publication Year

2015

Author(s)
  • McDonald, Thomas M.
  • Mason, Jarad A.
  • Kong, Xueqian
  • Bloch, Eric D.
  • Gygi, David
  • Dani, Alessandro
  • Crocella, Valentina
  • Giordanino, Filippo
  • Odoh, Samuel O.
  • Drisdell, Walter S.
  • Vlaisavljevich, Bess
  • Dzubak, Allison L.
  • Poloni, Roberta
  • Schnell, Sondre K.
  • Planas, Nora
  • Lee, Kyuho
  • Pascal, Tod
  • Wan, Liwen F.
  • Prendergast, David
  • Neaton, Jeffrey B.
  • Smit, Berend
  • Kortright, Jeffrey B.
  • Gagliardi, Laura
  • Bordiga, Silvia
  • Reimer, Jeffrey A.
  • Long, Jeffrey R.
Source
NATURE Volume: 519 Issue: 7543 Pages: 303-+ Published: 2015
ISSN
0028-0836 eISSN: 1476-4687
Abstract

The process of carbon capture and sequestration has been proposed as a method of mitigating the build-up of greenhouse gases in the atmosphere. If implemented, the cost of electricity generated by a fossil fuel-burning power plant would rise substantially, owing to the expense of removing CO2 from the effluent stream. There is therefore an urgent need for more efficient gas separation technologies, such as those potentially offered by advanced solid adsorbents. Here we show that diamine-appended metal-organic frameworks can behave as 'phase-change' adsorbents, with unusual step-shaped CO2 adsorption isotherms that shift markedly with temperature. Results from spectroscopic, diffraction and computational studies show that the origin of the sharp adsorption step is an unprecedented cooperative process in which, above a metal-dependent threshold pressure, CO2 molecules insert into metal-amine bonds, inducing a reorganization of the amines into well-ordered chains of ammonium carbamate. As a consequence, large CO2 separation capacities can be achieved with small temperature swings, and regeneration energies appreciably lower than achievable withstate-of-the-art aqueous amine solutions become feasible. The results provide a mechanistic framework for designing highly efficient adsorbents for removing CO2 from various gas mixtures, and yield insights into the conservation of Mg2+ within the ribulose-1,5-bisphosphate carboxylase/oxygenase family of enzymes.

Author Keyword(s)
    KeyWord(s) Plus
    • CARBON-DIOXIDE CAPTURE
    • TOTAL-ENERGY CALCULATIONS
    • AUGMENTED-WAVE METHOD
    • COORDINATION POLYMER
    • POWDER DIFFRACTION
    • MOLECULAR-DYNAMICS
    • CRYSTAL-STRUCTURE
    • BASIS-SET
    • FLUE-GAS
    • ADSORPTION
    ESI Discipline(s)
    • Multidisciplinary
    Web of Science Category(ies)
    • Multidisciplinary Sciences
    Adress(es)

    [McDonald, Thomas M.; Mason, Jarad A.; Bloch, Eric D.; Gygi, David; Long, Jeffrey R.] Univ Calif Berkeley, Dept Chem, Berkeley, CA 94720 USA; [Kong, Xueqian; Vlaisavljevich, Bess; Schnell, Sondre K.; Lee, Kyuho; Smit, Berend; Reimer, Jeffrey A.] Univ Calif Berkeley, Dept Chem & Biol Engn, Berkeley, CA 94720 USA; [Kong, Xueqian] Zhejiang Univ, Dept Chem, Hangzhou 310027, Zhejiang, Peoples R China; [Dani, Alessandro; Crocella, Valentina; Giordanino, Filippo; Bordiga, Silvia] Univ Turin, NIS & INSTM Ctr Reference, Dept Chem, I-10135 Turin, Italy; [Odoh, Samuel O.; Dzubak, Allison L.; Planas, Nora; Gagliardi, Laura] Univ Minnesota, Dept Chem, Chem Theory Ctr, Minneapolis, MN 55455 USA; [Odoh, Samuel O.; Dzubak, Allison L.; Planas, Nora; Gagliardi, Laura] Univ Minnesota, Supercomp Inst, Minneapolis, MN 55455 USA; [Drisdell, Walter S.; Smit, Berend; Kortright, Jeffrey B.; Reimer, Jeffrey A.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Mat Sci Div, Berkeley, CA 94720 USA; [Poloni, Roberta] Univ Grenoble Alpes, F-38000 Grenoble, France; [Poloni, Roberta] Sci & Ingn Mat & Proc SIMAP, F-38000 Grenoble, France; [Poloni, Roberta] CNRS, SIMAP, F-38000 Grenoble, France; [Schnell, Sondre K.] Norwegian Univ Sci & Technol, Dept Chem, N-7491 Trondheim, Norway; [Pascal, Tod; Wan, Liwen F.; Prendergast, David; Neaton, Jeffrey B.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Mol Foundry, Berkeley, CA 94720 USA; [Neaton, Jeffrey B.] Univ Calif Berkeley, Dept Phys, Berkeley, CA 94720 USA; [Neaton, Jeffrey B.] Univ Calif Berkeley, Kavli Energy Nanosci Inst, Berkeley, CA 94720 USA; [Smit, Berend] EPFL, Inst Sci & Ingn Chim, Valais, CH-1950 Sion, Switzerland

    Reprint Adress

    Long, JR (reprint author), Univ Calif Berkeley, Dept Chem, Berkeley, CA 94720 USA.

    Country(ies)
    • France
    • Italy
    • Norway
    • People's Republic of China
    • Switzerland
    • United States
    CNRS - Adress(es)
    • Sciences et Ingenierie, des MAtériaux et Procédés (SIMAP), UMR5266
    Accession Number
    WOS:000351171900031
    uid:/SLT43SLK
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