Ultrathin Paper Microsupercapacitors for Electronic Skin Applications

Ultrathin devices are rapidly developing for skin‐compatible medical applications and wearable electronics. Powering skin‐interfaced electronics requires thin and lightweight energy storage devices, where solution‐processing enables scalable fabrication. To attain such devices, a sequential deposition is employed to achieve all spray‐coated symmetric microsupercapacitors (μSCs) on ultrathin parylene C substrates, where both electrode and gel electrolyte are based on the cheap and abundant biopolymer, cellulose. The optimized spraying procedure allows an overall device thickness of ≈11 µm to be obtained with a 40% active material volume fraction and a resulting volumetric capacitance of 7 F cm−3. Long‐term operation capability (90% of capacitance retention after 104 cycles) and mechanical robustness are achieved (1000 cycles, capacitance retention of 98%) under extreme bending (rolling) conditions. Finite element analysis is utilized to simulate stresses and strains in real‐sized μSCs under different bending conditions. Moreover, an organic electrochromic display is printed and powered with two serially connected μ‐SCs as an example of a wearable, skin‐integrated, fully organic electronic application.