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With the ever-growing interests in ubiquitous smart electronics and the Internet of Things, the demand for high-energy-density power sources with aesthetic versatility has increased tremendously. High-energy-density Li-metal batteries have attracted considerable attention for fulfilling the high-energy-density requirement of smart electronics. To obtain form factor-free Li-metal batteries with both design diversity and electrochemical reliability, printed solid-state electrolytes are required as a key component because of their viability for the printing/solidification-based fabrication process and electrode-customized chemical/physical properties. This review present an overview of printed solid-state electrolytes for form factor-free Li-metal batteries with a focus on the materials chemistry and fabrication requirements. In addition, their structural/physical/electrochemical properties were discussed in terms of compatibility with Li-metal batteries.

Solid-state microsupercapacitors with ultrahigh areal-number-density are integrated on a chip via high-fidelity printing., Microsupercapacitors (MSCs) have garnered considerable attention as a promising power source for microelectronics and miniaturized portable/wearable devices. However, their practical application has been hindered by the manufacturing complexity and dimensional limits. Here, we develop a new class of ultrahigh areal number density solid-state MSCs (UHD SS–MSCs) on a chip via electrohydrodynamic (EHD) jet printing. This is, to the best of our knowledge, the first study to exploit EHD jet printing in the MSCs. The activated carbon-based electrode inks are EHD jet-printed, creating interdigitated electrodes with fine feature sizes. Subsequently, a drying-free, ultraviolet-cured solid-state gel electrolyte is introduced to ensure electrochemical isolation between the SS–MSCs, enabling dense SS–MSC integration with on-demand (in-series/in-parallel) cell connection on a chip. The resulting on-chip UHD SS–MSCs exhibit exceptional areal number density [36 unit cells integrated on a chip (area = 8.0 mm × 8.2 mm), 54.9 cells cm−2] and areal operating voltage (65.9 V cm−2).