All-in-one configured supercapacitor holds great promise
in addressing
cyclic deformation-induced relative displacement and delamination
among electrode/electrolyte/electrode faced by the conventional laminated
supercapacitor, but its interfacial interactions among heterogeneous
electrode/electrolyte/electrode only depend on weak secondary or physical
bonds, leading to insufficient mechanical durability. Herein, a concept
of covalent bonding homo-all-in-one configuration is proposed to construct
strong covalent bonding interfaces among electrode/electrolyte/electrode
comprising homomatrix polymer PVA through simultaneous chemical cross-linking
of the homomatrixes and interfaces, thereby achieving mechanically
durable homo-all-in-one supercapacitors (cPMP/cPVA/cPMP HSCs). Based
on the adjustment in cross-linking time, seamlessly integrated interfaces
form in the cPMP/cPVA/cPMP HSCs, which achieve high mechanical properties,
remarkable interfacial bonding strength, and low interfacial charge
transfer resistance. In sharp contrast to conventional laminated supercapacitors,
the cPMP/cPVA/cPMP HSCs deliver superior areal capacitance of 268.8
mF cm–2 at 5 mV s–1 and unexpected
cyclic stability with capacitance retention of 104% after 20 000
charge–discharge cycles. It is highlighted that the cPMP/cPVA/cPMP
HSCs reach an unprecedented level of mechanical durability with capacitance
retention of 103% and 101% exceeding 50 000 bending and twisting
cycles, respectively. Furthermore, the cPMP/cPVA/cPMP HSCs are demonstrated
to light up a red LED bulb under flat, bending, twisting, and even
folding conditions. Those findings are intended to lead to an advanced
design trend for the development of covalent bonding homo-all-in-one
configured supercapacitors toward flexible and wearable electronic
applications.