Kilogram‐Scale Synthesis of Few‐Layer Graphene‐Skinned Copper Powders via Pulsed‐Pressure Chemical Vapor Deposition

ABSTRACT Copper powders are essential components in electronics and manufacturing but suffer from rapid surface oxidation. Graphene encapsulation offers an effective protective strategy; however, conventional chemical vapor deposition (CVD) methods face challenges such as particle sintering, poor coverage due to inefficient precursor transport, and self‐limited monolayer growth. Here, we report a scalable pulsed‐pressure CVD strategy for kilogram‐scale preparation of few‐layer graphene‐skinned copper powders. This method employs graphite powder as a physical spacer to prevent sintering, while a unique cyclic pressure modulation actively enhances precursor penetration throughout the powder bed. The resulting powders feature a conformal few‐layer graphene skin (3–5 layers) with 98.2% surface coverage and high crystallinity. They exhibit exceptional oxidation resistance, showing an approximately 20‑fold lower oxygen uptake than bare copper after 30 min at 190°C in air. The graphene‐copper composites consolidated from these powders show an ∼8% higher thermal conductivity and an ∼3% higher electrical conductivity than pure copper. This work provides a viable pathway for large‐scale production of high‐performance graphene‐metal composites, opening new opportunities for advanced conductive and thermal management applications.