Surface and Interface Engineering of Nanoarrays toward Advanced Electrodes and Electrochemical Energy Storage Devices

Abstract The overall performance of electrochemical energy storage devices (EESDs) is intrinsically correlated with surfaces and interfaces. As a promising electrode architecture, 3D nanoarrays (3D‐NAs) possess relatively ordered, continuous, and fully exposed active surfaces of individual nanostructures, facilitating mass and electron transport within the electrode and charge transfer across interfaces and providing an ideal platform for engineering. Herein, a critical overview of the surface and interface engineering of 3D‐NAs, from electrode and interface designs to device integration, is presented. The general merits of 3D‐NAs and surface/interface engineering principles of 3D‐NA hybrid electrodes are highlighted. The focus is on the use of 3D‐NAs as a superior platform to regulate the interface nature and unveiling new mechanism/materials without the interference of binders. The engineering and utilization of the surface of 3D‐NAs to develop flexible/solid‐state EESDs with 3D integrated electrode/electrolyte interfaces, or 3D triphase interfaces involving other active species, which are characteristic of (quasi‐)solid‐state electrolyte infiltration into the entire device, are also considered. Finally, the challenges and future directions of surface/interface engineering of 3D‐NAs are outlined. In particular, potential strategies to obtain electrode charge balance, optimize the multiphase solid‐state interface, and attain 3D solid electrolyte infiltration are proposed.