Christian Diercks studied chemistry at the University of Heidelberg and carried out undergraduate research in the group of Prof. Jean-Pierre Sauvage at the University of Strasbourg (France), as well as at Northwestern University (USA) under the guidance of Sir James Fraser Stoddart. He obtained his Ph.D. from UC Berkeley under the mentorship of Prof. Omar M. Yaghi in 2018 for his work on covalent organic frameworks. Currently,hei sapostdoctoral researcher in the group of Prof. Peter G. Schultz at the Scripps Research Institute, working on adding new chemistries to the processes of the central dogma of molecular biology.
One
prominent aspect of metal organic frameworks (MOFs) is the
ability to tune the size, shape, and chemical characteristics of their
pores. MOF-5, with its open cubic connectivity of Zn4O
clusters joined by two-dimensional, terephthalate linkers, is the
archetypal example: both functionalized and elongated linkers produce
isoreticular frameworks that define pores with new shapes and chemical
environments. The recent scalable synthesis of cubane-1,4-dicarboxylic
acid (1,4-H2cdc) allows the first opportunity to explore
its application in leading reticular architectures. Herein we describe
the use of 1,4-H2cdc to construct [Zn4O(1,4-cdc)3], referred to as CUB-5. Isoreticular with MOF-5, CUB-5 adopts
a cubic architecture but features aliphatic, rather than aromatic,
pore surfaces. Methine units point directly into the pores, delivering
new and unconventional adsorption locations. Our results show that
CUB-5 is capable of selectively adsorbing high amounts of benzene
at low partial pressures, promising for future investigations into
the industrial separation of benzene from gasoline using aliphatic
MOF materials. These results present an effective design strategy
for the generation of new MOF materials with aliphatic pore environments
and properties previously unattainable in conventional frameworks.
The resurgence of interest in the hydrogen economy could hinge on the distribution of hydrogen in a safe and efficient manner. Whilst great progress has been made with cryogenic hydrogen storage or liquefied ammonia, liquid organic hydrogen carriers (LOHCs) remain attractive due to their lack of need for cryogenic temperatures or high pressures, most commonly a cycle between methylcyclohexane and toluene. Oxidation of methylcyclohexane to release hydrogen will be more efficient if the equilibrium limitations can be removed by separating the mixture. This report describes a family of six ternary and quaternary multicomponent metal–organic frameworks (MOFs) that contain the three‐dimensional cubane‐1,4‐dicarboxylate (cdc) ligand. Of these MOFs, the most promising is a quaternary MOF (CUB‐30), comprising cdc, 4,4′‐biphenyldicarboxylate (bpdc) and tritopic truxene linkers. Contrary to conventional wisdom that adsorptive interactions with larger, hydrocarbon guests are dominated by π–π interactions, here we report that contoured aliphatic pore environments can exhibit high selectivity and capacity for LOHC separations at low pressures. This is the first time, to the best of our knowledge, where selective adsorption for cyclohexane over benzene is witnessed, underlining the unique adsorptive behavior afforded by the unconventional cubane moiety.
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