CA3031731C - An improved method for the synthesis of graphene oxide - Google Patents
An improved method for the synthesis of graphene oxide Download PDFInfo
- Publication number
- CA3031731C CA3031731C CA3031731A CA3031731A CA3031731C CA 3031731 C CA3031731 C CA 3031731C CA 3031731 A CA3031731 A CA 3031731A CA 3031731 A CA3031731 A CA 3031731A CA 3031731 C CA3031731 C CA 3031731C
- Authority
- CA
- Canada
- Prior art keywords
- graphene oxide
- graphite
- oxide slurry
- mixture
- graphite source
- Prior art date
- Legal status (The legal status 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 status listed.)
- Expired - Fee Related
Links
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 title claims abstract description 158
- 229910021389 graphene Inorganic materials 0.000 title claims abstract description 107
- 238000000034 method Methods 0.000 title claims abstract description 72
- 230000015572 biosynthetic process Effects 0.000 title description 11
- 238000003786 synthesis reaction Methods 0.000 title description 8
- 229910002804 graphite Inorganic materials 0.000 claims abstract description 45
- 239000010439 graphite Substances 0.000 claims abstract description 45
- QAOWNCQODCNURD-UHFFFAOYSA-N Sulfuric acid Chemical compound OS(O)(=O)=O QAOWNCQODCNURD-UHFFFAOYSA-N 0.000 claims abstract description 17
- 235000011149 sulphuric acid Nutrition 0.000 claims abstract description 16
- 239000002002 slurry Substances 0.000 claims description 28
- 239000000203 mixture Substances 0.000 claims description 17
- 239000011541 reaction mixture Substances 0.000 claims description 16
- 238000006243 chemical reaction Methods 0.000 claims description 14
- 239000006228 supernatant Substances 0.000 claims description 14
- 238000001228 spectrum Methods 0.000 claims description 11
- RTZKZFJDLAIYFH-UHFFFAOYSA-N Diethyl ether Chemical compound CCOCC RTZKZFJDLAIYFH-UHFFFAOYSA-N 0.000 claims description 8
- 238000002441 X-ray diffraction Methods 0.000 claims description 7
- -1 nitrogen-containing compound Chemical class 0.000 claims description 7
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 claims description 6
- 230000002194 synthesizing effect Effects 0.000 claims description 6
- 238000005406 washing Methods 0.000 claims description 5
- 239000007864 aqueous solution Substances 0.000 claims description 4
- 238000004299 exfoliation Methods 0.000 claims description 4
- 239000000758 substrate Substances 0.000 claims description 4
- 239000003795 chemical substances by application Substances 0.000 claims 3
- 238000000527 sonication Methods 0.000 claims 1
- 239000012286 potassium permanganate Substances 0.000 abstract description 11
- 239000000126 substance Substances 0.000 abstract description 9
- 239000003153 chemical reaction reagent Substances 0.000 abstract description 4
- 238000004458 analytical method Methods 0.000 abstract 2
- 230000003647 oxidation Effects 0.000 description 13
- 238000007254 oxidation reaction Methods 0.000 description 13
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Chemical compound O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 12
- 229910001868 water Inorganic materials 0.000 description 12
- 230000007547 defect Effects 0.000 description 11
- NBIIXXVUZAFLBC-UHFFFAOYSA-N Phosphoric acid Chemical compound OP(O)(O)=O NBIIXXVUZAFLBC-UHFFFAOYSA-N 0.000 description 8
- 235000011007 phosphoric acid Nutrition 0.000 description 8
- 238000011020 pilot scale process Methods 0.000 description 7
- 238000006722 reduction reaction Methods 0.000 description 6
- VWDWKYIASSYTQR-UHFFFAOYSA-N sodium nitrate Chemical compound [Na+].[O-][N+]([O-])=O VWDWKYIASSYTQR-UHFFFAOYSA-N 0.000 description 6
- 238000005481 NMR spectroscopy Methods 0.000 description 5
- 238000000089 atomic force micrograph Methods 0.000 description 5
- 229910052799 carbon Inorganic materials 0.000 description 5
- 239000010410 layer Substances 0.000 description 5
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 description 5
- 230000008569 process Effects 0.000 description 5
- 230000009467 reduction Effects 0.000 description 5
- 210000003462 vein Anatomy 0.000 description 5
- 238000005033 Fourier transform infrared spectroscopy Methods 0.000 description 4
- 238000001069 Raman spectroscopy Methods 0.000 description 4
- 238000012512 characterization method Methods 0.000 description 4
- 125000000524 functional group Chemical group 0.000 description 4
- 239000011229 interlayer Substances 0.000 description 4
- 238000003756 stirring Methods 0.000 description 4
- 238000002411 thermogravimetry Methods 0.000 description 4
- 231100000331 toxic Toxicity 0.000 description 4
- 230000002588 toxic effect Effects 0.000 description 4
- 230000009286 beneficial effect Effects 0.000 description 3
- 238000005229 chemical vapour deposition Methods 0.000 description 3
- 239000008367 deionised water Substances 0.000 description 3
- 229910021641 deionized water Inorganic materials 0.000 description 3
- 238000004519 manufacturing process Methods 0.000 description 3
- 239000012528 membrane Substances 0.000 description 3
- 239000010445 mica Substances 0.000 description 3
- 229910052618 mica group Inorganic materials 0.000 description 3
- 238000004098 selected area electron diffraction Methods 0.000 description 3
- 235000010344 sodium nitrate Nutrition 0.000 description 3
- 241000134253 Lanka Species 0.000 description 2
- GRYLNZFGIOXLOG-UHFFFAOYSA-N Nitric acid Chemical compound O[N+]([O-])=O GRYLNZFGIOXLOG-UHFFFAOYSA-N 0.000 description 2
- 238000001237 Raman spectrum Methods 0.000 description 2
- 238000003917 TEM image Methods 0.000 description 2
- 238000004630 atomic force microscopy Methods 0.000 description 2
- 238000001460 carbon-13 nuclear magnetic resonance spectrum Methods 0.000 description 2
- 150000002009 diols Chemical group 0.000 description 2
- 239000000463 material Substances 0.000 description 2
- 238000005259 measurement Methods 0.000 description 2
- QLTDWCHQCKHGGO-UHFFFAOYSA-N methane;sulfuric acid Chemical compound C.C.C.C.C.C.C.C.C.C.C.C.C.C.C.C.C.C.C.C.C.C.C.C.C.C.C.C.C.C.C.C.C.C.C.C.C.C.C.C.C.C.C.C.C.C.C.C.OS(O)(=O)=O.OS(O)(=O)=O.OS(O)(=O)=O.OS(O)(=O)=O.OS(O)(=O)=O.OS(O)(=O)=O.OS(O)(=O)=O QLTDWCHQCKHGGO-UHFFFAOYSA-N 0.000 description 2
- 239000007800 oxidant agent Substances 0.000 description 2
- VKJKEPKFPUWCAS-UHFFFAOYSA-M potassium chlorate Chemical compound [K+].[O-]Cl(=O)=O VKJKEPKFPUWCAS-UHFFFAOYSA-M 0.000 description 2
- 239000002356 single layer Substances 0.000 description 2
- 239000007787 solid Substances 0.000 description 2
- 239000011343 solid material Substances 0.000 description 2
- 230000007704 transition Effects 0.000 description 2
- 238000004627 transmission electron microscopy Methods 0.000 description 2
- 238000001106 transmission high energy electron diffraction data Methods 0.000 description 2
- 230000004580 weight loss Effects 0.000 description 2
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 description 1
- 238000001157 Fourier transform infrared spectrum Methods 0.000 description 1
- 238000005004 MAS NMR spectroscopy Methods 0.000 description 1
- XOJVVFBFDXDTEG-UHFFFAOYSA-N Norphytane Natural products CC(C)CCCC(C)CCCC(C)CCCC(C)C XOJVVFBFDXDTEG-UHFFFAOYSA-N 0.000 description 1
- 241000282320 Panthera leo Species 0.000 description 1
- 229910000831 Steel Inorganic materials 0.000 description 1
- 238000005411 Van der Waals force Methods 0.000 description 1
- 238000002835 absorbance Methods 0.000 description 1
- 238000010521 absorption reaction Methods 0.000 description 1
- 230000002378 acidificating effect Effects 0.000 description 1
- 230000004913 activation Effects 0.000 description 1
- 150000001298 alcohols Chemical class 0.000 description 1
- 230000004075 alteration Effects 0.000 description 1
- 229940045720 antineoplastic alkylating drug epoxides Drugs 0.000 description 1
- 238000013459 approach Methods 0.000 description 1
- 239000003125 aqueous solvent Substances 0.000 description 1
- 125000003118 aryl group Chemical group 0.000 description 1
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical group [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 1
- 238000005102 attenuated total reflection Methods 0.000 description 1
- 239000006227 byproduct Substances 0.000 description 1
- 125000004432 carbon atom Chemical group C* 0.000 description 1
- 125000002915 carbonyl group Chemical group [*:2]C([*:1])=O 0.000 description 1
- 150000007942 carboxylates Chemical class 0.000 description 1
- 239000003638 chemical reducing agent Substances 0.000 description 1
- 238000000576 coating method Methods 0.000 description 1
- 229910052802 copper Inorganic materials 0.000 description 1
- 239000010949 copper Substances 0.000 description 1
- 229960004132 diethyl ether Drugs 0.000 description 1
- 125000005594 diketone group Chemical group 0.000 description 1
- 239000007772 electrode material Substances 0.000 description 1
- 238000002003 electron diffraction Methods 0.000 description 1
- 238000004146 energy storage Methods 0.000 description 1
- 150000002118 epoxides Chemical class 0.000 description 1
- 239000003517 fume Substances 0.000 description 1
- 239000007789 gas Substances 0.000 description 1
- 239000007770 graphite material Substances 0.000 description 1
- 125000002887 hydroxy group Chemical group [H]O* 0.000 description 1
- 239000012535 impurity Substances 0.000 description 1
- 238000002329 infrared spectrum Methods 0.000 description 1
- 238000009830 intercalation Methods 0.000 description 1
- 230000002687 intercalation Effects 0.000 description 1
- 150000002500 ions Chemical class 0.000 description 1
- 150000002576 ketones Chemical class 0.000 description 1
- 238000012986 modification Methods 0.000 description 1
- 230000004048 modification Effects 0.000 description 1
- 239000002114 nanocomposite Substances 0.000 description 1
- 229910021382 natural graphite Inorganic materials 0.000 description 1
- 238000000655 nuclear magnetic resonance spectrum Methods 0.000 description 1
- 239000003973 paint Substances 0.000 description 1
- 230000000704 physical effect Effects 0.000 description 1
- 239000003495 polar organic solvent Substances 0.000 description 1
- 238000010791 quenching Methods 0.000 description 1
- 230000000171 quenching effect Effects 0.000 description 1
- 230000035484 reaction time Effects 0.000 description 1
- 238000012827 research and development Methods 0.000 description 1
- 230000029058 respiratory gaseous exchange Effects 0.000 description 1
- 239000000243 solution Substances 0.000 description 1
- 230000003595 spectral effect Effects 0.000 description 1
- 238000004611 spectroscopical analysis Methods 0.000 description 1
- 239000010959 steel Substances 0.000 description 1
- 239000002341 toxic gas Substances 0.000 description 1
- 238000002525 ultrasonication Methods 0.000 description 1
- 238000002371 ultraviolet--visible spectrum Methods 0.000 description 1
- 230000035899 viability Effects 0.000 description 1
Classifications
-
- 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
- C01B32/198—Graphene oxide
-
- 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
- C01B32/23—Oxidation
-
- 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)
- General Life Sciences & Earth Sciences (AREA)
- Geology (AREA)
- Engineering & Computer Science (AREA)
- Materials Engineering (AREA)
- Nanotechnology (AREA)
- Carbon And Carbon Compounds (AREA)
Applications Claiming Priority (3)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| US15/221,386 | 2016-07-27 | ||
| US15/221,386 US10336619B2 (en) | 2016-07-27 | 2016-07-27 | Method for the synthesis of graphene oxide |
| PCT/IB2017/054540 WO2018020439A1 (en) | 2016-07-27 | 2017-07-26 | An improved method for the synthesis of graphene oxide |
Publications (2)
| Publication Number | Publication Date |
|---|---|
| CA3031731A1 CA3031731A1 (en) | 2018-02-01 |
| CA3031731C true CA3031731C (en) | 2021-06-08 |
Family
ID=61012180
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| CA3031731A Expired - Fee Related CA3031731C (en) | 2016-07-27 | 2017-07-26 | An improved method for the synthesis of graphene oxide |
Country Status (6)
| Country | Link |
|---|---|
| US (1) | US10336619B2 (cg-RX-API-DMAC7.html) |
| JP (1) | JP6917454B2 (cg-RX-API-DMAC7.html) |
| KR (1) | KR102268849B1 (cg-RX-API-DMAC7.html) |
| AU (1) | AU2017304275B2 (cg-RX-API-DMAC7.html) |
| CA (1) | CA3031731C (cg-RX-API-DMAC7.html) |
| WO (1) | WO2018020439A1 (cg-RX-API-DMAC7.html) |
Families Citing this family (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN108545724B (zh) * | 2018-07-23 | 2020-06-09 | 山东玉皇新能源科技有限公司 | 石墨烯及其生产方法、用途与电池 |
| CN113213464B (zh) * | 2021-05-31 | 2022-04-29 | 杭州高烯科技有限公司 | 一种纺丝级单层氧化石墨烯浆料的制备方法 |
| KR102483223B1 (ko) * | 2021-12-23 | 2023-01-02 | 주식회사 랩엠제로 | 화학적 박리법에 기반한 산화 그래핀 제조 방법 |
Family Cites Families (15)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US2798878A (en) | 1954-07-19 | 1957-07-09 | Nat Lead Co | Preparation of graphitic acid |
| CN102803135A (zh) | 2009-05-22 | 2012-11-28 | 威廉马歇莱思大学 | 高度氧化的氧化石墨烯及其制备方法 |
| US20110262341A1 (en) * | 2010-04-25 | 2011-10-27 | Sri Lanka Institute of Nanotechnology (Pvt) Ltd. | Process for preparation of carbon nanotubes from vein graphite |
| GB201016925D0 (en) | 2010-10-07 | 2010-11-24 | Univ Manchester | Graphene oxide |
| KR102120603B1 (ko) * | 2011-09-30 | 2020-06-08 | 가부시키가이샤 한도오따이 에네루기 켄큐쇼 | 그래핀 및 축전 장치, 및 이들의 제작 방법 |
| WO2014003252A1 (en) * | 2012-06-28 | 2014-01-03 | Idt International Co., Ltd. | Method and apparatus for manufacturing graphite oxide |
| JP2014034480A (ja) * | 2012-08-07 | 2014-02-24 | Toshiba Corp | 微細炭素の製造方法、その製造方法により製造された微細炭素及びその微細炭素を母材に添加した複合材料 |
| KR101472915B1 (ko) * | 2012-10-09 | 2014-12-16 | 주식회사 그래핀올 | 산화그래핀 형성 방법 |
| US9755227B2 (en) * | 2012-11-20 | 2017-09-05 | Nanyang Technological University | Method for forming a reduced graphene oxide/metal sulfide composite and its use as an anode for batteries |
| KR101500692B1 (ko) * | 2013-04-11 | 2015-03-09 | 주식회사 아이디티인터내셔널 | 산화흑연의 제조방법 및 제조장치 |
| WO2014168629A1 (en) | 2013-04-12 | 2014-10-16 | General Electric Company | Membranes comprising graphene |
| US9637388B2 (en) * | 2013-05-24 | 2017-05-02 | Council Of Scientific & Industrial Research | Process for preparation of nanoporous graphene and graphene quantum dots |
| DE102014009814A1 (de) * | 2013-07-05 | 2015-04-02 | Daimler Ag | Poröse Einsätze für eine verbesserte Kühlmittelverteilung in Bipolarplatten-Anordnungen für Brennstoffzellen |
| US9452934B2 (en) * | 2013-09-12 | 2016-09-27 | The Hong Kong University Of Science And Technology | Synthesis of ultra-large graphene oxide sheets |
| CN105540869B (zh) | 2015-12-17 | 2018-04-03 | 苏州大学 | 一种负载脱氮副球菌的改性氧化石墨烯复合材料及其制备方法和用途 |
-
2016
- 2016-07-27 US US15/221,386 patent/US10336619B2/en active Active - Reinstated
-
2017
- 2017-07-26 WO PCT/IB2017/054540 patent/WO2018020439A1/en not_active Ceased
- 2017-07-26 KR KR1020197005673A patent/KR102268849B1/ko not_active Expired - Fee Related
- 2017-07-26 CA CA3031731A patent/CA3031731C/en not_active Expired - Fee Related
- 2017-07-26 AU AU2017304275A patent/AU2017304275B2/en not_active Ceased
- 2017-07-26 JP JP2019526384A patent/JP6917454B2/ja not_active Expired - Fee Related
Also Published As
| Publication number | Publication date |
|---|---|
| KR102268849B1 (ko) | 2021-06-28 |
| US20180029887A1 (en) | 2018-02-01 |
| JP2019523210A (ja) | 2019-08-22 |
| KR20190038585A (ko) | 2019-04-08 |
| CA3031731A1 (en) | 2018-02-01 |
| AU2017304275B2 (en) | 2019-11-14 |
| AU2017304275A1 (en) | 2019-03-14 |
| JP6917454B2 (ja) | 2021-08-11 |
| WO2018020439A1 (en) | 2018-02-01 |
| US10336619B2 (en) | 2019-07-02 |
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Legal Events
| Date | Code | Title | Description |
|---|---|---|---|
| EEER | Examination request |
Effective date: 20190123 |
|
| MKLA | Lapsed |
Effective date: 20220726 |