TY - JOUR
T1 - Enriching the Reticular Chemistry Repertoire with Minimal Edge-Transitive Related Nets: Access to Highly Coordinated Metal-Organic Frameworks Based on Double Six-Membered Rings as Net-Coded Building Units.
AU - Chen, Zhijie
AU - Thiam, Zeynabou
AU - Shkurenko, Aleksander
AU - Weselinski, Lukasz Jan
AU - Adil, Karim
AU - Jiang, Hao
AU - Alezi, Dalal
AU - Assen, Ayalew Hussen Assen
AU - O'Keeffe, Michael
AU - Eddaoudi, Mohamed
N1 - KAUST Repository Item: Exported on 2020-10-01
Acknowledgements: Research reported in this publication was supported by King Abdullah University of Science and Technology (KAUST).
PY - 2019/12/3
Y1 - 2019/12/3
N2 - Minimal edge-transitive nets are regarded as suitable blueprints for the successful practice of reticular chemistry, and par excellence ideal for the deliberate design and rational construction of highly coordinated metal-organic frameworks (MOFs). We report the systematic generation of the highly connected minimal edge-transitive related nets (transitivity [32]) from parent edge-transitive nets (transitivity [21] or [11]), and their use as a guide for the deliberate design and directional assembly of highly coordinated MOFs from their associated net-coded building units (net-cBUs), 12-connected (12-c) double six-membered ring (d6R) building units. Notably, the generated related nets enclose the distinctive highly coordinated d6R (12-c) due to the subsequent coordination number increase in one node of the resultant new related net; that is, the (3,4,12)-c kce net is the (4,6)-c soc-related net, and the (3,6,12)-c kex and urx nets are the (6,6)-c nia-related nets. Intuitively, the combination of 12-connected hexagonal prismatic rare-earth (RE) nonanuclear [RE9(μ3-O)2(μ3-OH)12(O2C-)12] carboxylate-based clusters with purposely chosen organic or organic-inorganic hybrid building units led to the formation of the targeted highly coordinated MOFs based on selected minimal edge-transitive related nets. Interestingly, the kex-MOFs can alternatively be regarded as a zeolite-like MOF (ZMOF) based on the zeolite underlying topology afx, by considering the dodecacarboxylate ligand as a d6R building unit, delineating a new avenue toward the construction of ZMOFs through the composite building units as net-cBUs. This represents a significant step toward the effective discovery and design of novel minimal edge-transitive and highly coordinated materials using the d6Rs as net-cBUs.
AB - Minimal edge-transitive nets are regarded as suitable blueprints for the successful practice of reticular chemistry, and par excellence ideal for the deliberate design and rational construction of highly coordinated metal-organic frameworks (MOFs). We report the systematic generation of the highly connected minimal edge-transitive related nets (transitivity [32]) from parent edge-transitive nets (transitivity [21] or [11]), and their use as a guide for the deliberate design and directional assembly of highly coordinated MOFs from their associated net-coded building units (net-cBUs), 12-connected (12-c) double six-membered ring (d6R) building units. Notably, the generated related nets enclose the distinctive highly coordinated d6R (12-c) due to the subsequent coordination number increase in one node of the resultant new related net; that is, the (3,4,12)-c kce net is the (4,6)-c soc-related net, and the (3,6,12)-c kex and urx nets are the (6,6)-c nia-related nets. Intuitively, the combination of 12-connected hexagonal prismatic rare-earth (RE) nonanuclear [RE9(μ3-O)2(μ3-OH)12(O2C-)12] carboxylate-based clusters with purposely chosen organic or organic-inorganic hybrid building units led to the formation of the targeted highly coordinated MOFs based on selected minimal edge-transitive related nets. Interestingly, the kex-MOFs can alternatively be regarded as a zeolite-like MOF (ZMOF) based on the zeolite underlying topology afx, by considering the dodecacarboxylate ligand as a d6R building unit, delineating a new avenue toward the construction of ZMOFs through the composite building units as net-cBUs. This represents a significant step toward the effective discovery and design of novel minimal edge-transitive and highly coordinated materials using the d6Rs as net-cBUs.
UR - http://hdl.handle.net/10754/660908
UR - https://pubs.acs.org/doi/abs/10.1021/jacs.9b11260
UR - http://www.scopus.com/inward/record.url?scp=85076999673&partnerID=8YFLogxK
U2 - 10.1021/jacs.9b11260
DO - 10.1021/jacs.9b11260
M3 - Article
C2 - 31794212
SN - 0002-7863
VL - 141
SP - 20480
EP - 20489
JO - Journal of the American Chemical Society
JF - Journal of the American Chemical Society
IS - 51
ER -