Reticular Chemistry at Its Best: Directed Assembly of Hexagonal Building Units into the Awaited Metal-Organic Framework with the Intricate Polybenzene Topology, pbz-MOF.
The ability to direct the assembly of hexagonal building units offers great prospective to construct the awaited and looked-for hypothetical polybenzene (pbz) or "cubic graphite" structure, described 70 years ago. Here, we demonstrate the successful use of reticular chemistry as an appropriate strategy for the design and deliberate construction of a zirconium-based metal-organic framework (MOF) with the intricate pbz underlying net topology. The judicious selection of the perquisite hexagonal building units, six connected organic and inorganic building blocks, allowed the formation of the pbz-MOF-1, the first example of a Zr(IV)-based MOF with pbz topology. Prominently, pbz-MOF-1 is highly porous, with associated pore size and pore volume of 13 Å and 0.99 cm3g-1, respectively, and offers high gravimetric and volumetric methane storage capacities (0.23 g g-1and 210.4 cm3(STP) cm-3at 80 bar). Notably, the pbz-MOF-1 pore system permits the attainment of one of the highest CH4adsorbed phase density enhancements at high pressures (0.15 and 0.21 g cm-3at 35 and 65 bar, respectively) as compared to benchmark microporous MOFs.
Functional Materials Design, Discovery & Development (FMD3), Advanced Membranes & Porous Materials Center, Division of Physical Sciences and Engineering, King Abdullah University of Science and Technology (KAUST) , Thuwal 23955-6900, Kingdom of Saudi Arabia.
Dalal
D
Alezi
Department of Chemistry, University of Crete , Voutes 71003 Heraklion, Greece.
Ioannis
I
Spanopoulos
Department of Chemistry, University of Crete , Voutes 71003 Heraklion, Greece.
Constantinos
C
Tsangarakis
Functional Materials Design, Discovery & Development (FMD3), Advanced Membranes & Porous Materials Center, Division of Physical Sciences and Engineering, King Abdullah University of Science and Technology (KAUST) , Thuwal 23955-6900, Kingdom of Saudi Arabia.
Aleksander
A
Shkurenko
Functional Materials Design, Discovery & Development (FMD3), Advanced Membranes & Porous Materials Center, Division of Physical Sciences and Engineering, King Abdullah University of Science and Technology (KAUST) , Thuwal 23955-6900, Kingdom of Saudi Arabia.
Karim
K
Adil
Functional Materials Design, Discovery & Development (FMD3), Advanced Membranes & Porous Materials Center, Division of Physical Sciences and Engineering, King Abdullah University of Science and Technology (KAUST) , Thuwal 23955-6900, Kingdom of Saudi Arabia.
Youssef
Y
Belmabkhout
School of Molecular Sciences, Arizona State University , Tempe, Arizona 85287, United States.
Michael
M
O Keeffe
Functional Materials Design, Discovery & Development (FMD3), Advanced Membranes & Porous Materials Center, Division of Physical Sciences and Engineering, King Abdullah University of Science and Technology (KAUST) , Thuwal 23955-6900, Kingdom of Saudi Arabia.
Mohamed
M
Eddaoudi
Department of Chemistry, University of Crete , Voutes 71003 Heraklion, Greece.
Pantelis N
PN
Trikalitis