Epitaxial Welding of Carbon Nanotube Networks for Aqueous Battery Current Collectors

Carbon nanomaterials are desirable candidates for lightweight, highly conductive, and corrosion-resistant current collectors. However, a key obstacle is their weak interconnection between adjacent nanostructures, which renders orders of magnitude lower electrical conductivity and mechanical strength in the bulk assemblies. Here we report an “epitaxial welding” strategy to engineer carbon nanotubes (CNTs) into highly crystalline and interconnected structures. Solution-based polyacrylonitrile was conformally coated on CNTs as “nanoglue” to physically join CNTs into a network, followed by a rapid high-temperature annealing (>2800 K, overall ∼30 min) to graphitize the polymer coating into crystalline layers that also bridge the adjacent CNTs to form an interconnected structure. The contact-welded CNTs (W-CNTs) exhibit both a high conductivity (∼1500 S/cm) and a high tensile strength (∼120 MPa), which are 5 and 20 times higher than the unwelded CNTs, respectively. In addition, the W-CNTs display chemical and electrochemical stabilities in strong acidic/alkaline electrolytes (>6 mol/L) when potentiostatically stressing at both cathodic and anodic potentials. With these exceptional properties, the W-CNT films are optimal as high-performance current collectors and were demonstrated in the state-of-the-art aqueous battery using a “water-in-salt” electrolyte.