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Most metal-organic frameworks (MOFs) suffer from insufficient stability, which limits the scope of their applications. Thus, the design and synthesis of stable size/morphology-controlled MOF nanocrystals is critical but challenging. In this study, dual-ligand and hard-soft-acid-base strategies were used to fabricate a variety of 3D pillared-layer [Ni(thiophene-2,5-dicarboxylate)(4,4’-bipyridine)]n MOF nanocrystals (1D nanofibers, 2D nanosheets, and 3D aggregates) with controllable morphology by varying the concentration of 4,4’-bipyridine and thus controling the crystal growth direction. Owing to the shorter ion diffusion length, enhanced electron/ion transfer, and strong interactions between thiophene-2,5-dicarboxylate and 4,4’-bipyridine, the 2D nanosheets showed much larger specific capacitance than 1D nanofibers and 3D aggregates. A single device with an output voltage as high as 3.0 V and exceptional cycling performance (95% of retention after 5000 cycles at 3 mA cm–2) was realized by configurating two aqueous asymmetric supercapacitor devices in series. The excellent cycling property and charge–discharge mechanism is consistent with the hard-soft-acid-base theory.

Dual-ligand and hard-soft-acid-base strategies to optimize metal-organic framework nanocrystals for stable electrochemical cycling performance