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

Author

Listed:
  • Thomas M. McDonald

    (University of California, Berkeley, California 94720, USA)

  • Jarad A. Mason

    (University of California, Berkeley, California 94720, USA)

  • Xueqian Kong

    (University of California, Berkeley, California 94720, USA
    Zhejiang University)

  • Eric D. Bloch

    (University of California, Berkeley, California 94720, USA)

  • David Gygi

    (University of California, Berkeley, California 94720, USA)

  • Alessandro Dani

    (NIS and INSTM Centre of Reference, University of Turin, Via Quarello 15, I-10135 Torino, Italy)

  • Valentina Crocellà

    (NIS and INSTM Centre of Reference, University of Turin, Via Quarello 15, I-10135 Torino, Italy)

  • Filippo Giordanino

    (NIS and INSTM Centre of Reference, University of Turin, Via Quarello 15, I-10135 Torino, Italy)

  • Samuel O. Odoh

    (Chemical Theory Center and Supercomputing Institute, University of Minnesota, Minneapolis, Minnesota 55455, USA)

  • Walter S. Drisdell

    (Lawrence Berkeley National Laboratory, Berkeley, California 94720, USA)

  • Bess Vlaisavljevich

    (University of California, Berkeley, California 94720, USA)

  • Allison L. Dzubak

    (Chemical Theory Center and Supercomputing Institute, University of Minnesota, Minneapolis, Minnesota 55455, USA)

  • Roberta Poloni

    (Université Grenoble Alpes, Science et Ingénierie des Matériaux et Procédés (SIMAP), F-38000 Grenoble, France
    Centre National de la Recherche Scientifique, SIMAP, F-38000, Grenoble, France)

  • Sondre K. Schnell

    (University of California, Berkeley, California 94720, USA
    Norwegian University of Science and Technology, Høgskoleringen 5, 7491 Trondheim, Norway)

  • Nora Planas

    (Chemical Theory Center and Supercomputing Institute, University of Minnesota, Minneapolis, Minnesota 55455, USA)

  • Kyuho Lee

    (University of California, Berkeley, California 94720, USA
    Molecular Foundry, Lawrence Berkeley National Laboratory, One Cyclotron Road, Berkeley, California 94720, USA)

  • Tod Pascal

    (Molecular Foundry, Lawrence Berkeley National Laboratory, One Cyclotron Road, Berkeley, California 94720, USA)

  • Liwen F. Wan

    (Molecular Foundry, Lawrence Berkeley National Laboratory, One Cyclotron Road, Berkeley, California 94720, USA)

  • David Prendergast

    (Molecular Foundry, Lawrence Berkeley National Laboratory, One Cyclotron Road, Berkeley, California 94720, USA)

  • Jeffrey B. Neaton

    (Molecular Foundry, Lawrence Berkeley National Laboratory, One Cyclotron Road, Berkeley, California 94720, USA
    University of California, Berkeley, California 94720, USA
    Kavli Energy Nanosciences Institute, University of California, Berkeley, California 94720, USA)

  • Berend Smit

    (University of California, Berkeley, California 94720, USA
    Lawrence Berkeley National Laboratory, Berkeley, California 94720, USA
    Institut des Sciences et Ingénierie Chimiques, Valais, École Polytechnique Fédérale de Lausanne (EPFL), Rue de l’Industrie 17, CH-1950 Sion, Switzerland)

  • Jeffrey B. Kortright

    (Lawrence Berkeley National Laboratory, Berkeley, California 94720, USA)

  • Laura Gagliardi

    (Chemical Theory Center and Supercomputing Institute, University of Minnesota, Minneapolis, Minnesota 55455, USA)

  • Silvia Bordiga

    (NIS and INSTM Centre of Reference, University of Turin, Via Quarello 15, I-10135 Torino, Italy)

  • Jeffrey A. Reimer

    (University of California, Berkeley, California 94720, USA
    Lawrence Berkeley National Laboratory, Berkeley, California 94720, USA)

  • Jeffrey R. Long

    (University of California, Berkeley, California 94720, USA
    Lawrence Berkeley National Laboratory, Berkeley, California 94720, USA)

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 with state-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.

Suggested Citation

  • Thomas M. McDonald & Jarad A. Mason & Xueqian Kong & Eric D. Bloch & David Gygi & Alessandro Dani & Valentina Crocellà & Filippo Giordanino & Samuel O. Odoh & Walter S. Drisdell & Bess Vlaisavljevich , 2015. "Cooperative insertion of CO2 in diamine-appended metal-organic frameworks," Nature, Nature, vol. 519(7543), pages 303-308, March.
    • Handle: RePEc:nat:nature:v:519:y:2015:i:7543:d:10.1038_nature14327
    DOI: 10.1038/nature14327
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    Cited by:

    1. Narukulla, Ramesh & Chaturvedi, Krishna Raghav & Ojha, Umaprasana & Sharma, Tushar, 2022. "Carbon dioxide capturing evaluation of polyacryloyl hydrazide solutions via rheological analysis for carbon utilization applications," Energy, Elsevier, vol. 241(C).
    2. Zhu, Xuancan & Ge, Tianshu & Yang, Fan & Wang, Ruzhu, 2021. "Design of steam-assisted temperature vacuum-swing adsorption processes for efficient CO2 capture from ambient air," Renewable and Sustainable Energy Reviews, Elsevier, vol. 137(C).
    3. Yao Fu & Yifeng Yao & Alexander C. Forse & Jianhua Li & Kenji Mochizuki & Jeffrey R. Long & Jeffrey A. Reimer & Gaël Paëpe & Xueqian Kong, 2023. "Solvent-derived defects suppress adsorption in MOF-74," Nature Communications, Nature, vol. 14(1), pages 1-9, December.
    4. Chen, S. & Shi, W.K. & Yong, J.Y. & Zhuang, Y. & Lin, Q.Y. & Gao, N. & Zhang, X.J. & Jiang, L., 2023. "Numerical study on a structured packed adsorption bed for indoor direct air capture," Energy, Elsevier, vol. 282(C).
    5. Irani, Maryam & Jacobson, Andrew T. & Gasem, Khaled A.M. & Fan, Maohong, 2018. "Facilely synthesized porous polymer as support of poly(ethyleneimine) for effective CO2 capture," Energy, Elsevier, vol. 157(C), pages 1-9.

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