<scp>Single?Molecule</scp> Confinement Induced Intrinsic <scp>Multi?Electron Redox?Activity</scp> to Enhance Supercapacitor Performance

Aggregation of polyoxometalates (POM) is largely responsible for the reduced performance POM-based energy-storage systems. To address this challenge, here, precise confinement single Keggin-type POM molecule in a porous carbon (PC) unimodal super-micropore (micro-PC) realized. Such single-molecule enables sufficient activity center exposure and maximum electron-transfer from micro-PC to POM, which well stabilizes electron-accepting molecules thoroughly activates its inherent multi-electron redox-activity. In particular, redox-activities properties confined are revealed be pore size-dependent by experiment spectroscopy as theoretical calculation. Meanwhile, molecularly dispersed steadily “cage” exhibit unprecedented large-negative-potential stability multiple-peak redox-activity at an ultra-low loading ~11.4 wt%. As result, fabricated solid-state supercapacitor achieves remarkable areal capacitance, ultrahigh energy power density 443 mF cm?2, 0.12 mWh cm?2 21.1 mW respectively. This work establishes novel strategy molecule, providing versatile approach inducing intrinsic POMs advanced