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Robust and Flexible Micropatterned Electrodes and Micro‐Supercapacitors in Graphene–Silk Biopapers

Robust and flexible micro‐supercapacitors based upon a graphene oxide–silk layered bionanocomposite is reported. Generation of micropatterned electrodes with sub‐micrometer spatial resolution is accomplished using a novel resist‐stenciling technique, enabling the transfer of complex microcircuit designs to a graphene oxide–silk layered substrate as chemically reduced features microfeatures across wafer‐length scales. Resist‐stenciling can produce micropatterned reduction features with over ten times the feature density compared to techniques such as laser‐scribing or screen printing. As a proof‐of‐concept, resist‐stenciling is used to fabricate the first 2D micro‐supercapacitors integrated into a layered graphene bionanocomposite. These demonstrate a specific capacitance of ≈128 F g−1, good capacitance retention under charge cycling (87.5% after 2000 cycles), and repeated mechanical bending without failure. Resist‐stenciling leverages tools currently in use by the microelectronics industry to enable the scalable, high‐resolution conversion of layered nanocomposites into microelectronic circuit, storage, and sensing elements.