As promising battery-type electrode materials, layered single metal hydroxides (LSHs) including a-Ni(OH) 2 and a-Co(OH) 2 based hybrid supercapacitors exhibit larger operating voltages compared with those that are based on activated carbons and double-layer capacitance mechanisms. This study proposes a novel and facile room-temperature method to fabricate a-Ni(OH) 2 and a-Co(OH) 2 superstructures by using the double hydrolysis of Ni 2+ or Co 2+ and NCO À without the presence of any structure directing agent.Two dimensional sheet-like building blocks of the alpha-type metal hydroxide are assembled into various elegant morphologies including a 3D interconnected hierarchical assembly (3D-ICHA), sheet-onsheet, sheet-on-rod and other nanostructures, which depends on the cation-anion mixing mode.Significantly, the 3D-ICHA a-Ni(OH) 2 possesses an ultrahigh specific surface area (320.2 m 2 g À1 ) androbust porous structure. An outstanding initial specific capacity (653.1 C g À1 at 1 A g À1 and 406 C g À1 at 20 A g À1 ) and an excellent cycling retention (86.2% in 20 000 cycles) were obtained for the 3D-ICHA aNi(OH) 2 , which stands out from most of the state-of-the-art a-Ni(OH) 2 powder-based materials. A highloading asymmetric capacitor with excessive activated carbon ($10 mg 3D-ICHA a-Ni(OH) 2 vs. $60 mg activated carbon) is demonstrated and it works very steadily even after 20 000 charge/discharge cycles.
IntroductionElectrochemical capacitors, also called supercapacitors, have attracted many scientic and practical investigations. They can complement or replace batteries in electrical energy storage and harvesting applications due to their high power density, fast charging/discharging rates, and long durability. 1-7 However, supercapacitors that are based on activated carbons and double-layer capacitance mechanisms (i.e., electrical doublelayer capacitors, EDLCs) have limited energy density with aqueous electrolytes because of lower operating voltages (rarely exceeding 1 V). 8 One promising strategy to circumvent such limitations is to design an asymmetric (or hybrid) system that combines an activated carbon negative electrode with a batterytype faradaic electrode (as the positive electrode), which can make use of the different potential windows of the two electrodes to increase the maximum operating voltage while offering the advantages of both supercapacitors (power density) and advanced batteries (energy density). 8,9 To enhance the supercapacitor performance, especially specic energy density while retaining intrinsic high specic power density, many researchers have focused on constructing nanoscale electrode materials because of the short transport paths for ions and electrons in faradaic redox reactions. 10 Among various battery-type faradaic electrode materials reported to date, two-dimensional materials have attracted an enormous amount of attention. 11 Layered single metal hydroxides (LSHs) including the a-hydroxide of nickel and cobalt with hydrotalcite structures have been reported to be promising battery...