US 2019/0067732 Al  16  Feb.28,2019  Example 2: Preparation of Pristine Graphene Sheets  (0% Oxygen)  Example 3: Preparation of Prelithiated and  Pre-Sodiated Graphene Fluoride Sheets as an  Anode Active Material of a Lithium-Ion Battery or  Sodium-Ion Battery  [0159]  Subsequently, a small amount of FHEG (approxi› mately 0.5 mg) was mixed with 20-30 mL of an organic  solvent (methanol and ethanol, separately) and subjected to  an ultrasound treatment (280 W) for 30 min, leading to the  [0153]  RGO was used as a conductive additive in either or  both of the anode and cathode active material in certain  lithium batteries presently invented. Pre-lithiated RGO (e.g.  RGO+lithium particles or RGO pre-deposited with lithium  coating) was also used as an anode active material that was  mixed with a liquid electrolyte to form wet anode active  material mixtures for selected lithium-ion cells. Selected  cathode active materials (TiS$_{2 }$ nano particles and LiCoO$_{2 }$ particles, respectively) and non-lithiated RGO sheets were  dispersed in a liquid electrolyte to prepare wet cathode  active material mixture. The wet anode active mixture and  [0158]  Several processes have been used by us to produce  GF, but only one process is herein described as an example.  In a typical procedure, highly exfoliated graphite (HEG) was  prepared from intercalated compound C$_{2}$F.xClF$_{3}$ .  HEG was  further fluorinated by vapors of chlorine trifluoride to yield  fluorinated highly exfoliated graphite (FHEG). Pre-cooled  Teflon reactor was filled with 20-30 mL of liquid pre-cooled  ClF$_{3}$ ,  the reactor was closed and cooled to liquid nitrogen  temperature. Then, no more than 1 g of HEG was put in a  container with holes for ClF $_{3 }$ gas to access and situated  inside the reactor. In 7-10 days a gray-beige product with  approximate formula C$_{2}$F was formed.  [0152]  Surfactant-stabilized  RGO  (RGO-BS)  was  obtained by diluting the wet-cake in an aqueous solution of  surfactants instead of pure water. A commercially available  mixture of cholate sodium (50 wt. %) and deoxycholate  sodium (50 wt. %) salts provided by Sigma Aldrich was  used. The surfactant weight fraction was 0.5 wt. %. This  fraction was kept constant for all samples. Sonication was  performed using a Branson Sonifier S-250A equipped with  a 13 mm step disruptor horn and a 3 mm tapered micro-tip,  operating at a 20 kHz frequency. For instance, 10 mL of  aqueous solutions containing 0.1 wt.% of GO was sonicated  for 10 min and subsequently centrifuged at 2700 g for 30  min to remove any non-dissolved large particles, aggregates,  and impurities. Chemical reduction of as-obtained GO to  yield RGO was conducted by following the method, which  involved placing 10 mL of a 0.1 wt. % GO aqueous solution  in a boiling flask of 50 mL. Then, 10 µL of a 35 wt. %  aqueous solution ofN$_{2}$H$_{4 }$ (hydrazine) and 70 mL of a 28 wt.  % of an aqueous solution ofNH$_{4}$OH (ammonia) were added  to the mixture, which was stabilized by surfactants. The  solution was heated to 90°  C. and refluxed for 1 h. The pH  value measured after the reaction was approximately 9. The  color of the sample turned dark black during the reduction  reaction.  [0157]  Pristine graphene sheets, as a conductive additive,  along with an anode active material ( or cathode active  material in the cathode) were then incorporated in a battery  using both the presently invented procedure and conven› tional procedure of slurry coating, drying and layer lami› nating. Both lithium-ion batteries and lithium metal batteries  ( containing a wet cathode electrode) were investigated.  Sodium-ion cells were also studied.  [0156]  In a typical procedure, five grams of graphite  flakes, ground to approximately 20 µm  or less in sizes, were  dispersed in 1,000 mL of deionized water ( containing  O  .1 %  by weight of a dispersing agent, Zonylfi FSO from DuPont)  to obtain a suspension. An ultrasonic energy level of 85 W  (Branson S450 Ultrasonicator) was used for exfoliation,  separation, and size reduction of graphene sheets for a  period of 15 minutes to 2 hours. The resulting graphene  sheets are pristine graphene that have never been oxidized  and are oxygen-free and relatively defect-free. Pristine gra› phene is essentially free from any non-carbon elements.  [0155]  Recognizing the possibility of the high defect  population in GO sheets acting to reduce the conductivity of  individual graphene plane, we decided to study if the use of  pristine graphene sheets (non-oxidized and oxygen-free,  non-halogenated and halogen-free, etc.) can lead to a con› ductive additive having a high electrical and thermal con› ductivity. Pre-lithiated pristine graphene and pre-sodiated  pristine graphene were also used as an anode active material  for a lithium-ion battery and a sodium-ion battery, respec› tively. Pristine graphene sheets were produced by using the  direct ultrasonication or liquid-phase production process.  [0151]  For the second oxidation process, the previously  collected wet cake was placed in a boiling flask that contains  69 mL ofa concentrated aqueous solution ofH$_{2}$ SO$_{4 }$ (96%).  The flask was kept in an ice bath as 9 g of KMnO$_{4 }$ was  slowly added. Care was taken to avoid overheating. The  resulting mixture was stirred at 35°  C. for 2 hours (the  sample color turning dark green), followed by the addition  of 140 mL of water. After 15 min, the reaction was halted by  adding 420 mL of water and 15 mL of an aqueous solution  of30 wt% H$_{2}$O$_{2}$ .  The color of the sample at this stage turned  bright yellow. To remove the metallic ions, the mixture was  filtered and rinsed with a 1: 10 HCl aqueous solution. The  collected material was gently centrifuged at 2700 g and  rinsed with deionized water. The final product was a wet  cake that contained 1.4 wt % of GO, as estimated from dry  extracts. Subsequently, liquid dispersions of GO platelets  were obtained by lightly sonicating wet-cake materials,  which were diluted in deionized water.  [0154]  For comparison purposes, slurry coating and dry› ing procedures were conducted to produce conventional  electrodes. Electrodes and a separator disposed between two  dried electrodes were then assembled and encased in an  Al-plastic laminated packaging envelop, followed by liquid  electrolyte injection to form a lithium battery cell.  cathode active mixtures were delivered to surfaces of graph› ite foams for forming an anode layer and a cathode layer,  respectively.  method, which involved two oxidation stages. In a typical  procedure, the first oxidation was achieved in the following  conditions: 1100 mg of graphite was placed in a 1000 mL  boiling flask. Then, 20 g of K$_{2}$S$_{2}$O$_{8}$ ,  20 g of P $_{2}$0 5 ,  and 400  mL of a concentrated aqueous solution of H$_{2}$SO$_{4 }$ (96%)  were added in the flask. The mixture was heated under reflux  for 6 hours and then let without disturbing for 20 hours at  room temperature. Oxidized graphite was filtered and rinsed  with abundant distilled water until neutral pH. A wet cake› like material was recovered at the end of this first oxidation. 