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Peer-reviewedCC BY-NC-NDNature Materials

Methane storage using metal–dipyrazolate frameworks

  • Xiang‐Jing Kong1,2
  • Varvara I. Nikolayenko1,3
  • Alan C. Eaby1
  • Lenore Miller4
  • Debobroto Sensharma1
  • Daqiang Yuan5
  • Hongliang Huang6
  • Guang-Rui Si2
  • X Li1
  • Soumya Mukherjee1
  • Leonard J. Barbour3,7
  • Brian Space4
5 more authors
  • Xian‐He Bu8
  • Zuoren Nie9
  • Tao He10,11
  • Jian‐Rong Li12
  • Michael John Zaworotko13
13 affiliations
  1. 1Bernal Institute and Department of Chemical Sciences, University of Limerick, Limerick, Ireland
  2. 2State Key Laboratory of Materials Low-Carbon Recycling, Beijing University of Technology, Beijing, China
  3. 3Department of Chemistry and Polymer Science, Stellenbosch University, Matieland, South Africa
  4. 4Department of Chemistry, North Carolina State University, Raleigh, NC, USA
  5. 5State Key Laboratory of Structure Chemistry, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou, China
  6. 6State Key Laboratory of Separation Membranes and Membrane Processes, School of Chemical Engineering and Technology, Tiangong University, Tianjin, China
  7. 7Department of Chemistry, School of Natural Sciences, University of Lincoln, Lincoln, UK
  8. 8School of Materials Science and Engineering and TKL of Metal and Molecule-Based Material Chemistry, Nankai University, Tianjin, China
  9. 9State Key Laboratory of Materials Low-Carbon Recycling, Beijing University of Technology, Beijing, China. [email protected]
  10. 10Bernal Institute and Department of Chemical Sciences, University of Limerick, Limerick, Ireland. [email protected]
  11. 11State Key Laboratory of Materials Low-Carbon Recycling, Beijing University of Technology, Beijing, China. [email protected]
  12. 12State Key Laboratory of Materials Low-Carbon Recycling, Beijing University of Technology, Beijing, China. [email protected]
  13. 13Bernal Institute and Department of Chemical Sciences, University of Limerick, Limerick, Ireland. [email protected]
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Abstract

Adsorbed natural gas storage using porous materials at ambient temperature and relatively low pressure promises to address safety and cost concerns of conventional natural gas storage technologies (liquefaction and compression), but its utility is hindered by low deliverable capacity. Flexible porous materials such as metal–organic frameworks can exhibit isotherms with the potential to afford enhanced deliverable capacity. However, prototypal flexible adsorbed natural gas sorbents, exemplified by the metal–organic framework cobalt benzenedipyrazolate, Co(bdp), suffer from hydrolytic instability and are unsuitable for pelletization. Here we report a family of metal–bipyrazolate frameworks, including hydrophobic sorbents, Zn(dpt) and Co(dpt) (H2dpt = 2,5-di(1H-pyrazol-4-yl)thiophene), that exhibit methane-induced reversible transformations between narrow-pore and large-pore phases. Zn(dpt) shows exceptionally high methane deliverable capacities for 5–35 and 5–65 bar, that is, 173 cm3 (STP) cm−3 and 225 cm3 (STP) cm−3, respectively, but, unlike Co(bdp), is hydrolytically stable. In situ structural characterization, high-pressure gas sorption and modelling provide an insight into the narrow-pore–large-pore transformations, whereas testing with 250-ml tanks reveals that Zn(dpt) retains high deliverable capacity over multiple cycles. We demonstrate a practical alternative to pelletization through a formulation approach that is probably generally suitable for flexible sorbents. Reversible phase transformations enable flexible metal–bipyrazolate frameworks to offer high deliverable methane capacities, high stability and recyclability, indicating utility in natural gas storage.

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Cite

BibTeXRIS
BibTeX
@article{kong2026methane,
  title = {{Methane storage using metal–dipyrazolate frameworks}},
  author = {Xiang‐Jing Kong and Varvara I. Nikolayenko and Alan C. Eaby and Lenore Miller and Debobroto Sensharma and Daqiang Yuan and Hongliang Huang and Guang-Rui Si and X Li and Soumya Mukherjee and Leonard J. Barbour and Brian Space and Xian‐He Bu and Zuoren Nie and Tao He and Jian‐Rong Li and Michael John Zaworotko},
  journal = {Nature Materials},
  year = {2026},
  month = jun,
  doi = {10.1038/s41563-026-02621-7},
  url = {https://doi.org/10.1038/s41563-026-02621-7},
  note = {CC BY-NC-ND},
}
RIS
TY  - JOUR
TI  - Methane storage using metal–dipyrazolate frameworks
AU  - Xiang‐Jing Kong
AU  - Varvara I. Nikolayenko
AU  - Alan C. Eaby
AU  - Lenore Miller
AU  - Debobroto Sensharma
AU  - Daqiang Yuan
AU  - Hongliang Huang
AU  - Guang-Rui Si
AU  - X Li
AU  - Soumya Mukherjee
AU  - Leonard J. Barbour
AU  - Brian Space
AU  - Xian‐He Bu
AU  - Zuoren Nie
AU  - Tao He
AU  - Jian‐Rong Li
AU  - Michael John Zaworotko
PY  - 2026
DA  - 2026/06/18
JO  - Nature Materials
DO  - 10.1038/s41563-026-02621-7
UR  - https://doi.org/10.1038/s41563-026-02621-7
AB  - Adsorbed natural gas storage using porous materials at ambient temperature and relatively low pressure promises to address safety and cost concerns of conventional natural gas storage technologies (liquefaction and compression), but its utility is hindered by low deliverable capacity. Flexible porous materials such as metal–organic frameworks can exhibit isotherms with the potential to afford enhanced deliverable capacity. However, prototypal flexible adsorbed natural gas sorbents, exemplified by the metal–organic framework cobalt benzenedipyrazolate, Co(bdp), suffer from hydrolytic instability and are unsuitable for pelletization. Here we report a family of metal–bipyrazolate frameworks, including hydrophobic sorbents, Zn(dpt) and Co(dpt) (H2dpt = 2,5-di(1H-pyrazol-4-yl)thiophene), that exhibit methane-induced reversible transformations between narrow-pore and large-pore phases. Zn(dpt) shows exceptionally high methane deliverable capacities for 5–35 and 5–65 bar, that is, 173 cm3 (STP) cm−3 and 225 cm3 (STP) cm−3, respectively, but, unlike Co(bdp), is hydrolytically stable. In situ structural characterization, high-pressure gas sorption and modelling provide an insight into the narrow-pore–large-pore transformations, whereas testing with 250-ml tanks reveals that Zn(dpt) retains high deliverable capacity over multiple cycles. We demonstrate a practical alternative to pelletization through a formulation approach that is probably generally suitable for flexible sorbents. Reversible phase transformations enable flexible metal–bipyrazolate frameworks to offer high deliverable methane capacities, high stability and recyclability, indicating utility in natural gas storage.
SN  - 1476-1122
SN  - 1476-4660
ER  -