The use of organic–inorganic hybrid nanoparticles will enable a control of the characteristics of both the nanoparticles and constructed fine structures. In this study, we report the synthesis of acrylate-intercalated layered manganese, cobalt, and nickel hydroxide nanoparticles and their assembly into ordered mesoporous structures. Polymerization of the intercalated acrylates takes place by means of a radical initiator. The formed organic network improved the thermal stability of the layered hydroxides, which results in thermally robust mesoporous structures. Additionally, it is found that the polymerization can be initiated and progressed at 200 °C without any initiators for the layered nickel hydroxide system. This allows for the scalable solid-state thermal polymerization of intercalated acrylates and the formation of thermally robust hierarchically ordered meso/macroporous powders as well as mesoporous films. The electrochemical characterization reveals that the thermally robust mesoporous films having regulated mesopores allow for the effective diffusion of molecules/solvent compared with the films having collapsed mesoporous structures.

The present work is partially supported by JSPS KAKENHI Grant Number JP20K15368, JSPS Core-to-Core Program, MEXT Leading Initiative for Excellent Young Researchers, the Foundation for the Promotion of Ion Engineering, International Network on Polyoxometalate Science at Hiroshima University, and the Izumi Science and Technology Foundation (2019-J-112).