Metal–organic
framework (MOF)/polymer composite proton exchange membranes (PEMs)
are being intensively investigated due to their potentials for the
systematic design of proton-conducting properties. However, the development
of MOF/polymer composite PEMs possessing high selectivity remains
exceedingly desirable and challenging for practical application. Herein,
two-dimensional (2D) zeolitic imidazolate framework (ZIF-8)/carbon
nanotube (CNT) hybrid cross-linked networks (ZCN) were synthesized
via the rational design of the physical form of ZIF-8, and then a
series of composite PEMs were prepared by hybridizing ZCN with sulfonated
poly(ether ether ketone) (SPEEK) matrix. The effect of the incorporation
of zero-dimensional (0D) raw ZIF-8 nanoparticles and 2D ZCN on the
proton conduction and methanol permeability of the composite membranes
was systemically studied. Benefiting from the morphological and compositional
advantages of ZCN, the SPEEK/ZCN composite membranes displayed a significant
enhancement in proton conductivity under various conditions. In particular,
the proton conductivity of SPEEK/ZCN-2.5 membrane was up to 50.24
mS cm<sup>–1</sup> at 120 °C-30% RH, which was 11.2 times
that of the recast SPEEK membrane (4.50 mS cm<sup>–1</sup>)
and 2.1 times that of SPEEK/ZIF membrane (24.1 mS cm<sup>–1</sup>) under the same condition. Meanwhile, the methanol permeability
of the SPEEK/ZCN composite membranes was greatly reduced. Therefore,
novel MOF/polymer composite PEMs with high selectivity were obtained.
Our investigation results reveal that the proton conductivity and
methanol permeability of the MOF/polymer composite membranes can be
effectively tailored via creating more elaborate superstructures of
MOFs rather than altering the chemical component. This effective strategy
may provide a useful guideline to integrate with other interesting
MOFs to design MOF/polymer composite membranes
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