Tailored Nanoarchitecturing of Microporous ZIF-8 to Hierarchically Porous Double-Shell Carbons and Their Intrinsic...

Mesostructured polydopamine (PDA) coating has been successfully achieved on the surface of zeolitic imidazolate framework-8 (ZIF-8) particles by incorporating Pluronic F127 (with a pore-expanding agent, 1,3,5-trimethylbenzene) as a pore-directing agent during dopamine polymerization. Upon pyrolysis at high temperatures, mesostructured PDA-coated ZIF-8 particles become hierarchically porous double-shell carbons (HPDCs) with a wide pore size distribution ranging from micro- and meso- to macropores. The formation of a hollow inner shell progresses initially with the shrinkage of ZIF-8 at the periphery where the interface interactions with mesostructured PDA exist, and then the subsequent disintegration of the ZIF-8 core at higher temperatures occurs. Our HPDCs prepared in this study feature physical and electrochemical advantages of hierarchically porous carbons such as high electrochemically accessible surface area, short diffusion distance, and high mass-transfer rate, thus demonstrating significantly improved ion diffusion and surface-enhanced high specific capacitance at high charge-discharge rates. HPDC_5.0 therefore exhibits the capacitance retention of up to 76.7% from 1 to 10 A g^-1 and maximum specific capacitance of 344.7 F g^-1 at 1 mV s^-1. It also possesses superior electrochemical stability with about 108% capacitance retention even after 10,000 consecutive cycles of galvanostatic charge-discharge at 10 A g^-1.