Regular Mesoporous Superparticles with a Tailored Opening Window and Tunable Surface Crisscrossed Grooves

Regular hollow mesoporous superparticles with an opening window and controllable surface grooves can significantly improve the high-loading performance of aqueous zinc ion hybrid capacitors, but their synthesis remains a great challenge. Herein, an electrostatic force-assisted monomicelle confined assembly strategy is demonstrated for synthesizing such regular mesoporous hollow superparticles. The mesoporous superparticles feature a hollow (∼250 nm) in the center and a tailored transverse window (35–50 nm) to enable the superparticles to be totally connected from the inner to external surface, and a monolayer of spherical mesopores (∼15 nm) is arrayed in an orderly fashion on the hollow shell to form the unique crisscrossed grooves. Notably, an accurate manipulation in the width (29.5–62.4 nm), depth (2.1–40.7 nm), and number in the horizontal and vertical (11 × 11–5 × 5) grooves can be realized. Finally, the mesoporous superparticles as the high-loading electrodes in aqueous zinc ion hybrid capacitors exhibit a weak polarization, a high specific capacity (205 mAh g,–1 at 0.1 A g–1), and an excellent rate performance (105 mAh g–1 at 10 A g–1). The adjustability of surface grooves enables the orthogonal control of the charge transfer rate and ion diffusion rate. The mesoporous superstructures demonstrate the potential for energy storage applications in different environments.