The rapid development of wearable, highly integrated, and flexible electronics has stimulated great demand for on-chip and miniaturized energy storage devices. By virtue of their high power density and long cycle life, micro-supercapacitors (MSCs), especially those with interdigital structures, have attracted considerable attention. In recent years, tremendous theoretical and experimental explorations have been carried out on the structures and electrode materials of MSCs, aiming to obtain better mechanical and electrochemical properties. The high-performance MSCs can be used in many fields, such as energy storage and medical assistant examination. Here, this review focuses on the recent progress of advanced MSCs in fabrication strategies, structural design, electrode materials design and function, and integrated applications, where typical examples are highlighted and analyzed. Furthermore, the current challenges and future development directions of advanced MSCs are also discussed.

2D nanomaterials are well suited for energy conversion and storage because of their thickness-dependent physical and chemical properties. However, current synthetic methods for translating 2D materials from the laboratory to industry cannot integrate both advantages of liquid-phase method (i.e., solution processibility, homogeneity, and massive production), and gas-phase method (i.e., high quality and large lateral size). Here, inspired by Chinese Sugar Figure Blowing Art, a rapid "gel-blowing" strategy is proposed for the mass production of 2D nonlayered nanosheets by thermally expanding the viscous gel precursors within a short time (≈1 min). A wide variety of 2D nanosheets including oxides, carbon, oxides/carbon and metal/carbon composites are synthesized on a large scale and with no impurities. Importantly, this method unifies the merits of both liquid-phase and gas-phase syntheses, giving rise to 2D products with high uniformity, nanometer thickness, and large lateral sizes (up to hundreds of micrometers) simultaneously. The success of this strategy highly relies on the speed of "blowing" and control of the amount of reactants. The as-synthesized nanosheet electrodes manifest excellent electrochemical performance for alkali-ion batteries and electrocatalysis. This method opens up a new avenue for economical and massive preparation of good-quality nonlayered 2D nanosheets for energy-related applications and beyond.

Silicon−carbon (Si−C) hybrids have been proven to be the most promising anodes for the next-generation lithium-ion batteries (LIBs) due to their superior theoretical capacity (∼4200 mAh g −1 ). However, it is still a critical challenge to apply this material for commercial LIB anodes because of the large volume expansion of Si, unstable solid-state interphase (SEI) layers, and huge internal stresses upon lithiation/delithiation. Here, we propose an engineering concept of multiscale buffering, taking advantage of a nanosized Si−C nanowire architecture through fabricating specific microsized wool-ball frameworks to solve all the above-mentioned problems. These wool-ball-like frameworks, prepared at high yields, nearly matching industrial scales (they can be routinely produced at a rate of ∼300 g/h), are composed of Si/C nanowire building blocks. As anodes, the Si−C wool-ball frameworks show ultrastable Li + storage (2000 mAh g −1 for 1000 cycles), high initial Coulombic efficiency of ∼90%, and volumetric capacity of 1338 mAh cm −3 . In situ TEM proves that the multiscale buffering design enables a small volume variation, only ∼19.5%, reduces the inner stresses, and creates a very thin SEI. The perfect multiscale elastic buffering makes this material more stable compared to common Si nanoparticle-assembled counterpart electrodes.

Metal oxides with surface protonation exhibit versatile physical and chemical properties suitable for use in many fields. Here, we develop an electrochemical route to directly protonize the physically assembled oxide particles, such as TiO 2 , Nb 2 O 5 , and WO 3 , in a Na 2 SO 4 neutral electrolyte, which is a result of electrochemically induced oxygen vacancies reacting with water molecules. With no need of electric connection among particles or between particles and conductive substrate, the electrochemical protonation follows a bottom-up particle-by-particle surface protonation mechanism due to the fact that the protonation inducing high surface conductivity creates an efficient electron transfer pathway among particles. Our results show that electrochemical protonation of particles provides a chance to finely functionalize the surface of a single particle by only adjusting electrode potentials. Such a facile, cost-efficient, and green route is easy to run for a large-scale production and unlocks the potential of semiconductor oxides for various applications.