Electrochemical method of producing nano graphene platelets
View Patent ↗A method of producing nano-scaled graphene platelets with an average thickness smaller than 30 nm from a layered graphite material. The method comprises (a) forming a carboxylic acid-intercalated graphite compound by an electrochemical reaction; (b) exposing the intercalated graphite compound to a thermal shock to produce exfoliated graphite; and (c) subjecting the exfoliated graphite to a mechanical shearing treatment to produce the nano-scaled graphene platelets. Preferred carboxylic acids are formic acid and acetic acid. The exfoliation step in the instant invention does not involve the evolution of undesirable species, such as NO x and SO x , which are common by-products of exfoliating conventional sulfuric or nitric acid-intercalated graphite compounds. The nano-scaled platelets are candidate reinforcement fillers for polymer nanocomposites. Nano-scaled graphene platelets are much lower-cost alternatives to carbon nano-tubes or carbon nano-fibers.
1. A method of producing nano-scaled graphene platelets with an average thickness smaller than 30 nm from a layered graphite material, said method comprising:
a) forming a carboxylic acid-intercalated graphite compound by an electrochemical reaction which uses a carboxylic acid as both an electrolyte and an intercalate source, said layered graphite material as an anode material, and a metal or graphite as a cathode material, and wherein a current is imposed upon said cathode and said anode at a current density for a duration of time sufficient for effecting said electrochemical reaction, wherein said carboxylic acid is selected from the group consisting of propionic, butyric, pentanoic, hexanoic acids, anhydrides thereof, and combinations thereof;
b) exposing said carboxylic acid-intercalated graphite compound to a thermal shock to form exfoliated graphite; and
c) subjecting said exfoliated graphite to a mechanical shearing treatment to produce said nano-scaled graphene platelets.
2. The method of claim 1 wherein said layered graphite material is selected from natural graphite, synthetic graphite, highly oriented pyrolytic graphite, graphite fiber, graphitic nano-fiber, graphite oxide, graphite fluoride, chemically modified graphite, graphite intercalation compound, exfoliated graphite, or a combination thereof.
3. The method of claim 1 wherein said mechanical shearing treatment comprises using air milling, airjet milling, ball milling, rotating-blade mechanical shearing, ultrasonication, or a combination thereof.
4. The method of claim 1 wherein the imposing current provides a current density in the range of 50 to 600 A/m 2 .
5. The method of claim 1 wherein said step of exposing comprises heating said carboxylic acid-intercalated graphite to a temperature in the range of 300-800° C. for a period of 15 seconds to 2 minutes.
6. The method of claim 1 wherein said mechanical shearing treatment comprises operating an air mill or air jet mill at a desired air velocity sufficient for breaking up flakes of exfoliated graphite.
7. The method of claim 1 , further comprising additional steps of electrochemically intercalating said nano-scaled graphene platelets to obtain a further intercalated compound and exfoliating said further intercalated compound to produce thinner nano-scaled graphene platelets.
8. The method of claim 1 wherein the imposing current provides a current density in the range of 100 to 400 A/m 2 .