▎ 摘　　要

NOVELTY - Graphene microparticles comprises three-dimensional open pore channels connected to each other due to the empty space between the crumpled multiple graphene unit sheets. The microparticles are spherical, which are assembled by randomly accumulating multiple graphene unit sheets into crumpled state. The average diameter of the spherical structure is 5-15 mu m. USE - The microparticles are useful in electrode active material for electrochemical device (secondary battery, fuel cell and capacitor) and lithium secondary battery (all claimed). ADVANTAGE - The method is simple and economical; produces graphene microparticles in large amount; and can easily adjust the size and composition of the microparticles by controlling the temperature of the reactor, droplet size and composition of the spray solution. The microparticle has high high-capacity. DETAILED DESCRIPTION - INDEPENDENT CLAIMS are also included for: (1) lithium secondary battery comprising an anode, a cathode containing graphene microparticles, a separation film and an electrolyte; and (2) manufacturing graphene microparticles, comprising (a) preparing spray solution by dispersing graphene or graphene oxide in a first solvent, and (b) introducing the obtained spray solution into a spraying device, forming graphene microparticles self-assembling through dropping droplet within a constant temperature reactor containing a second solvent which is immiscible with the first solvent and has higher boiling point than the first solvent by substituting the generated droplet, and recovering.