Redox Tuning in Crystalline and Electronic Structure of Bimetal–Organic Frameworks Derived Cobalt/Nickel Boride/Sulfide for Boosted Faradaic Capacitance

The development of efficient electrode materials is a cutting‐edge approach for high‐performance energy storage devices. Herein, an effective chemical redox approach is reported for tuning the crystalline and electronic structures of bimetallic cobalt/nickel–organic frameworks (Co‐Ni MOFs) to boost faradaic redox reaction for high energy density. The as‐obtained cobalt/nickel boride/sulfide exhibits a high specific capacitance (1281 F g −1 at 1 A g −1 ), remarkable rate performance (802.9 F g −1 at 20 A g −1 ), and outstanding cycling stability (92.1% retention after 10 000 cycles). An energy storage device fabricated with a cobalt/nickel boride/sulfide electrode exhibits a high energy density of 50.0 Wh kg −1 at a power density of 857.7 W kg −1 , and capacity retention of 87.7% (up to 5000 cycles at 12 A g −1 ). Such an effective redox approach realizes the systematic electronic tuning that activates the fast faradaic reactions of the metal species in cobalt/nickel boride/sulfide which may shed substantial light on inspiring MOFs and their derivatives for energy storage devices.