WO2012120291A4 - Electrolytic exfoliation of graphite - Google Patents

Electrolytic exfoliation of graphite Download PDF

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Publication number
WO2012120291A4
WO2012120291A4 PCT/GB2012/050487 GB2012050487W WO2012120291A4 WO 2012120291 A4 WO2012120291 A4 WO 2012120291A4 GB 2012050487 W GB2012050487 W GB 2012050487W WO 2012120291 A4 WO2012120291 A4 WO 2012120291A4
Authority
WO
WIPO (PCT)
Prior art keywords
graphite
amended
electrode
novel
species
Prior art date
Application number
PCT/GB2012/050487
Other languages
French (fr)
Other versions
WO2012120291A1 (en
Inventor
Christopher Stirling
Original Assignee
Morganite Electrical Carbon Limited
Priority date (The priority date is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the date listed.)
Filing date
Publication date
Application filed by Morganite Electrical Carbon Limited filed Critical Morganite Electrical Carbon Limited
Priority to GB1317934.6A priority Critical patent/GB2503838B/en
Publication of WO2012120291A1 publication Critical patent/WO2012120291A1/en
Publication of WO2012120291A4 publication Critical patent/WO2012120291A4/en

Links

Classifications

    • C—CHEMISTRY; METALLURGY
    • C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
    • C25B—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES FOR THE PRODUCTION OF COMPOUNDS OR NON-METALS; APPARATUS THEREFOR
    • C25B1/00—Electrolytic production of inorganic compounds or non-metals
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B32/00—Carbon; Compounds thereof
    • C01B32/15—Nano-sized carbon materials
    • C01B32/182—Graphene
    • C01B32/184—Preparation
    • C01B32/19—Preparation by exfoliation
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B32/00—Carbon; Compounds thereof
    • C01B32/20—Graphite
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B32/00—Carbon; Compounds thereof
    • C01B32/20—Graphite
    • C01B32/21—After-treatment
    • C01B32/22—Intercalation
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B32/00—Carbon; Compounds thereof
    • C01B32/20—Graphite
    • C01B32/21—After-treatment
    • C01B32/22—Intercalation
    • C01B32/225—Expansion; Exfoliation

Landscapes

  • Chemical & Material Sciences (AREA)
  • Organic Chemistry (AREA)
  • Inorganic Chemistry (AREA)
  • Life Sciences & Earth Sciences (AREA)
  • Geology (AREA)
  • General Life Sciences & Earth Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Materials Engineering (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Metallurgy (AREA)
  • Electrochemistry (AREA)
  • Nanotechnology (AREA)
  • Carbon And Carbon Compounds (AREA)

Abstract

An electrolytic technique for exfoliation of graphite is presented. The electrolytic technique utilises a previously disclosed electrode material to yield unexpected results. Intercalated graphite particles comprising a gradation of expansion may be produced according to the technique.

Claims

14
AMENDED CLAIMS
received by the International Bureau on 29 October 2012
Claims
1 : A method of producing intercalating, expanded, and/or exfoliated graphite or
graphene species comprising the step of electrolysis utilising electrode materials comprising graphite, characterised in that the electrode material comprises aligned graphite flakes bonded by a binding material and that the graphite layers of the graphite flakes are oriented within 20° to the plane of a surface of the electrode.
2: A method as claimed in Claim 1, in which the graphite layers are oriented
substantially parallel to the plane of a surface of the electrode.
3: A method as claimed in Claim 1 or Claim 2, in which the surface of the electrode which the graphite layers are oriented in respect of is the surface with the largest surface area.
4: A method as claimed in any preceding Claim, in which said surface of the electrode has a diameter of at least 10mm.
5 : A method as claimed in any preceding Claim, in which the binding material is a mesophase pitch.
6: A method as claimed in any preceding Claim, in which the binding material is a phenolic resin.
7: A method as claimed in any preceding Claim, in which the binding material is
carbonised or graphitised.
8: A method as claimed in any preceding claim, in which the flakes have a flake size of no less than 200 μιη.
9: A method as claimed in any preceding Claim, in which the electrolysis takes place in an electrolyte comprising an ionic liquid. 15 : A method as claimed in Claim 9, in which the ionic liquid is an aqueous solution of poly(sodium 4-styrene-sulfonate). : A method as claimed in any one of Claims 1 to 8, in which the electrolysis takes place in an electrolyte comprising an acid solution. : A method as claimed in Claim 11, in which the acid solution is an aqueous sulphuric acid solution. : A method as claimed in any preceding Claim, comprising the additional step of
subjecting the graphite or graphene species produced subsequent to the conclusion of electrolysis to further treatment. : A method as claimed in Claim 13, wherein the further treatment comprises
ultrasonicating the graphite or graphene species. : A method as claimed in Claim 13, wherein the further treatment comprises expansion of the graphite species. : A graphite or graphene species produced according to the method of any preceding claim. : A graphite species as claimed in Claim 16 comprising intercalated graphite particles, characterised in that there exists a gradation of expansion within the intercalated graphite particles. : A graphite species as claimed in Claim 17, further characterised in that the graphite particles possess a fan-like shape.

16

Statement under Article 19(1) PCT

Re Item V: Novelty

In the new claim set Claim 1 is amended so as to incorporate the subject matter of as-filed Claim 5. Consequently the amended Claim 1 is novel.

Since all subsequent method claims are dependent on claim 1, they too are novel.

Since all product claims relate to products obtained via methodologies incorporating the subject matter of Claim 1, the product claims all relate to products obtained by a novel method.

Consequently they too are novel.

As such, all amended claims are novel by virtue of the novelty of amended Claim 1.

Re Item V: Inventive Step

Claim 1 as amended incorporates the features of Claim 5. The Written Opinion asserted that as-filed Claim 5 lacks inventive step over a combination of Dl and D3 or a combination of D2 and D3.

The electrode material of D3 makes no suggestion that the material in question is especially suited to the type of exfoliation process presented in the application. Indeed D3 stresses chemical inertness [paragraph 0260].

Claim 1 as amended thus provides a novel combination which gives rise to an unexpected technical effect, as amply demonstrated in Table 1 in the specification, which depicts the results of experiments in which exfoliation occurs at electrodes comprising aligned graphite flakes and a binder, and experiments in which exfoliation occurs at pure graphite electrodes.

Therefore, amended Claim 1 and all subsequent claims possess inventive step.

PCT/GB2012/050487 2011-03-10 2012-03-05 Electrolytic exfoliation of graphite WO2012120291A1 (en)

Priority Applications (1)

Application Number Priority Date Filing Date Title
GB1317934.6A GB2503838B (en) 2011-03-10 2012-03-05 Electrolytic exfoliation of graphite

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
GB1104078.9A GB2488825A (en) 2011-03-10 2011-03-10 Electrolytic exfoliation of graphite
GB1104078.9 2011-03-10

Publications (2)

Publication Number Publication Date
WO2012120291A1 WO2012120291A1 (en) 2012-09-13
WO2012120291A4 true WO2012120291A4 (en) 2012-12-13

Family

ID=43980774

Family Applications (1)

Application Number Title Priority Date Filing Date
PCT/GB2012/050487 WO2012120291A1 (en) 2011-03-10 2012-03-05 Electrolytic exfoliation of graphite

Country Status (2)

Country Link
GB (2) GB2488825A (en)
WO (1) WO2012120291A1 (en)

Families Citing this family (11)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US9309124B2 (en) 2010-06-25 2016-04-12 National University Of Singapore Methods of forming graphene by graphite exfoliation
GB2523154B (en) * 2014-02-14 2016-04-27 Cambridge Entpr Ltd Method of producing graphene
EP2933356A1 (en) * 2014-04-17 2015-10-21 Basf Se Two-dimensional carbon materials prepared by electrochemical exfoliation
CN105088261B (en) * 2014-05-14 2017-10-20 国能纳米科技有限公司 The preparation method of graphene
CN104264178B (en) * 2014-09-17 2016-11-30 中国科学院青海盐湖研究所 A kind of electrocatalytic oxidation prepares the method for graphene oxide
CN104264179B (en) * 2014-09-17 2016-06-22 中国科学院山西煤炭化学研究所 A kind of method being prepared Graphene by graphite raw ore electrolysis
CN104894594A (en) * 2015-05-26 2015-09-09 广东烛光新能源科技有限公司 Graphene preparation method
CN106542525B (en) * 2016-10-27 2018-09-11 董兰田 Continuous adhesive tape legal system takes stripping degumming and the packing method of graphene
JP7148396B2 (en) * 2017-06-15 2022-10-05 積水化学工業株式会社 Carbon materials, electrode materials for power storage devices, and power storage devices
DE102017223892A1 (en) * 2017-12-29 2019-07-04 Sixonia Tech Gmbh Process for the preparation of a functionalized semiconductor or conductor material and its use
CN111453719B (en) * 2020-04-24 2022-05-24 湖北航天化学技术研究所 High-quality graphene and preparation method thereof

Family Cites Families (8)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US6406612B1 (en) * 1999-05-20 2002-06-18 Graftech Inc. Expandable graphite and method
GB2375501B (en) * 2001-05-03 2003-07-09 Morgan Crucible Co Extrusion of graphitic bodies
JP2004181383A (en) * 2002-12-04 2004-07-02 Nippon Telegr & Teleph Corp <Ntt> Carbon material for storing hydrogen
DE10328342B4 (en) * 2003-06-24 2006-05-04 Graphit Kropfmühl AG Process for producing expanded graphite, expanded graphite and use
US7658901B2 (en) * 2005-10-14 2010-02-09 The Trustees Of Princeton University Thermally exfoliated graphite oxide
GB2432830A (en) * 2005-12-02 2007-06-06 Morganite Elect Carbon Formation of thermally anisotropic carbon material
US8524067B2 (en) 2007-07-27 2013-09-03 Nanotek Instruments, Inc. Electrochemical method of producing nano-scaled graphene platelets
US7999027B2 (en) * 2009-08-20 2011-08-16 Nanotek Instruments, Inc. Pristine nano graphene-modified tires

Also Published As

Publication number Publication date
GB2503838A (en) 2014-01-08
GB2503838B (en) 2017-10-25
WO2012120291A1 (en) 2012-09-13
GB201317934D0 (en) 2013-11-27
GB2488825A (en) 2012-09-12
GB201104078D0 (en) 2011-04-27

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