Anion-exchange membranes (AEMs) with high conductivity are crucial for realizing next-generation energy storage and conversion systems in an alkaline environment, promising a huge advantage in cost reduction without using precious platinum group metal catalysts. Layered double hydroxide (LDH) nanosheets, exhibiting a remarkably high hydroxide ion (OH-) conductivity approaching 10-1 S cm-1 along the in-plane direction, may be regarded as an ideal candidate material for the fabrication of inorganic solid AEMs. However, two-dimensional anisotropy results in a substantially low conductivity of 10-6 S cm-1 along the cross-plane direction, which poses a hurdle to achieve fast ion conduction across the membrane comprising restacked nanosheets. In the present work, a composite membrane was prepared based on mixing/assembling micron-sized LDH nanosheets with nanosized LDH platelets (nanoparticles) via a facile vacuum filtration process. The hybridization with nanoparticles could alter the orientation of LDH nanosheets and reduce the restacking order, forming diversified fast ion-conducting pathways and networks in the composite membrane. As a result, the transmembrane conductivity significantly improved up to 1000-fold higher than that composed of restacked nanosheets only, achieving a high conductivity of 10-2 to 10-1 S cm-1 in both in-plane and cross-plane directions.
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