Oxygen vacancy-engineered Fe₂O₃ nanoarrays as free-standing electrodes for flexible asymmetric supercapacitors

The charge storage performance of Fe₂O₃ nanoarrays (NAs) as negative electrodes are limited by their poor conductivity and rate capability. Herein, we have reported the delicate interfacial engineering on carbon cloth (CC) fibers and oxygen vacancy (V_O) generation on Fe₂O₃ nanorod arrays to boost the capacitive performance. Polydopamine-derived nitrogen-doped carbon layers were fabricated on CC fibers to govern the growth of FeOOH NAs. Rich V_Os were generated in Fe₂O₃ NAs to construct a unique heterostructure with a crystalline core and amorphous shell via successive N₂ thermal treatment and chemical reduction. Optimized by 2 h chemical reduction, the V_O-rich Fe₂O₃ NA electrode, featuring a charged voltage of -1.10 V, exhibited a high areal specific capacitance of 2.63 F cm^-2 at 0.5 mA cm^-2 and 0.12 F cm^-2 even at 60 mA cm^-2. Impressively, 86.7% specific capacitance was retained after 10 000 cycles at 10 mA cm^-2. The flexible asymmetric supercapacitor by assembling free-standing CN-Fe₂O₃-2 h (negative electrode) and MnO₂ (positive electrode) showed an energy density of 1.33 mW h cm^-3 at 15.4 mW cm^-3. To the best of our knowledge, these results are the record performance for Fe₂O₃-based electrodes. The two-step interfacial engineering reported in this study may open a new door in the design of high energy-density electrodes for advanced energy storage.