Abstract
Vertically standing graphene (VSG) films have demonstrated various appealing functionalities on the basis of excellent electrical/thermal conductivity and electrochemical/catalytic properties, owing to their unique morphology, preferable orientation of the basal planes, and adequate defects as effective catalytic sites. Most fabrication processes for VSG suffer from the disadvantage of high processing temperature, difficulty in structural control, or poor scalability, which limits their many potential applications. Herein, a scalable high‐flux plasma‐enhanced chemical vapor deposition system is designed, with streamlined magnetic field to enable high and uniform ion density over a spatially extended plasma flux, which facilitates large‐area deposition of structurally tuned VSG independent of substrate materials without additional heating, for the first time. The orientation, density, and the degree of order for the as‐fabricated VSG can be tailored through adjusting the plasma environment, which in turn affects crystallization mechanisms. Such low‐temperature synthesized VSG films are demonstrated as high‐performance anode in sodium ion batteries, achieving a high capacity retention of 86% after 2000 cycles at a current density of 1 A g−1. It is expected that the current VSG films would have great potential for electrochemical applications that request catalytic sites together with favorable conductivity for ions and electrons.