Three‐Dimensional Binder‐Free Nanoarchitectures for Advanced Pseudocapacitors

Abstract The ever‐increasing energy demands for electrification of transportation and powering of portable electronics are driving the pursuit of energy‐storage technologies beyond the current horizon. Pseudocapacitors have emerged as one of the favored contenders to fill in this technology gap, owing to their potential to deliver both high power and energy densities. The high specific capacitance of pseudocapacitive materials is rooted in the various available oxidation states for fast surface or near‐surface redox charge transfer. However, the practical implementation of pseudocapacitors is plagued by the insulating nature of most pseudocapacitive materials. The wealth of the research dedicated to addressing these critical issues has grown exponentially in the past decade. Here, we briefly survey the current progress in the development of pseudocapacitive electrodes with a focus on the discussion of the recent most exciting advances in the design of three‐dimensional binder‐free nanoarchitectures, including porous metal/graphene‐based electrodes, as well as metal‐atom/ion‐doping‐enhanced systems, for advanced supercapacitors with comparable energy density to batteries, and high power density.