TY - JOUR
T1 - Face-directed assembly of tailored isoreticular MOFs using centring structure-directing agents
AU - Barsukova, Marina
AU - Sapianik, Aleksandr
AU - Guillerm, Vincent
AU - Shkurenko, Aleksander
AU - Shaikh, Aslam C.
AU - Parvatkar, Prakash
AU - Bhatt, Prashant M.
AU - Bonneau, Mickaele
AU - Alhaji, Abdulhadi
AU - Shekhah, Osama
AU - Balestra, Salvador R.G.
AU - Semino, Rocio
AU - Maurin, Guillaume
AU - Eddaoudi, Mohamed
N1 - Funding Information:
Research reported in this publication was supported by the King Abdullah University of Science and Technology (KAUST). S.R.G.B. was supported with Grant POSTDOC_21_00069 funded by Consejería de Transformación Económica, Industria, Conocimiento y Universidades and Agencia Andaluza del Conocimiento, Junta de Andalucía. We are thankful to C3UPO for the HPC facilities provided.
Publisher Copyright:
© 2023, The Author(s).
PY - 2023
Y1 - 2023
N2 - Building blocks with low connectivity and no embedded directionality are prone to polymorphism, as demonstrated by the diversity of 4-connected zeolitic nets (>250). As a result, their deployment for design in reticular and isoreticular chemistries remains a challenge. However, the ability to control geometrical peculiarities offers potential to deviate from the assembly of default structures. Here we report the face-directed assembly of >20 isoreticular zeolite-like metal–organic frameworks (ZMOFs) by using polytopic expanding and tightening centring structure-directing agents (cSDAs). The cSDAs are selected with the appropriate geometrical coding information to alter and control the orientation of adjacent supermolecular building blocks. The ZMOFs have an underlying sodalite (sod) topology that is remarkably suited for the rational assembly of multinary materials. In addition to a variety of metal cations (In, Fe, Co and Ni), a diverse range of cSDAs (di-, tri-, tetra-, hexa-, pyridyl or imidazole) are used and combined. Our approach enables isoreticular possibilities at both extremities of the porous materials spectrum: In-sod-ZMOF-102 exhibits small pore aperture suitable for efficient separation, while Fe-sod-ZMOF-320 with 48-Å-wide mesopores exhibits high hydrogen uptake, methane storage working capacity and a high gravimetric working capacity for oxygen. [Figure not available: see fulltext.]
AB - Building blocks with low connectivity and no embedded directionality are prone to polymorphism, as demonstrated by the diversity of 4-connected zeolitic nets (>250). As a result, their deployment for design in reticular and isoreticular chemistries remains a challenge. However, the ability to control geometrical peculiarities offers potential to deviate from the assembly of default structures. Here we report the face-directed assembly of >20 isoreticular zeolite-like metal–organic frameworks (ZMOFs) by using polytopic expanding and tightening centring structure-directing agents (cSDAs). The cSDAs are selected with the appropriate geometrical coding information to alter and control the orientation of adjacent supermolecular building blocks. The ZMOFs have an underlying sodalite (sod) topology that is remarkably suited for the rational assembly of multinary materials. In addition to a variety of metal cations (In, Fe, Co and Ni), a diverse range of cSDAs (di-, tri-, tetra-, hexa-, pyridyl or imidazole) are used and combined. Our approach enables isoreticular possibilities at both extremities of the porous materials spectrum: In-sod-ZMOF-102 exhibits small pore aperture suitable for efficient separation, while Fe-sod-ZMOF-320 with 48-Å-wide mesopores exhibits high hydrogen uptake, methane storage working capacity and a high gravimetric working capacity for oxygen. [Figure not available: see fulltext.]
UR - http://www.scopus.com/inward/record.url?scp=85173118127&partnerID=8YFLogxK
U2 - 10.1038/s44160-023-00401-8
DO - 10.1038/s44160-023-00401-8
M3 - Article
AN - SCOPUS:85173118127
SN - 2731-0582
VL - 3
SP - 33
EP - 46
JO - Nature Synthesis
JF - Nature Synthesis
IS - 1
ER -