GB2616103A - Nitrogen-doped carbon material and preparation method thereof - Google Patents

Nitrogen-doped carbon material and preparation method thereof Download PDF

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Publication number
GB2616103A
GB2616103A GB2218215.8A GB202218215A GB2616103A GB 2616103 A GB2616103 A GB 2616103A GB 202218215 A GB202218215 A GB 202218215A GB 2616103 A GB2616103 A GB 2616103A
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nitrogen
carbon material
doped carbon
powder
alcohol
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GB202218215D0 (en
Inventor
Yang Chengtao
Xing Mengjiang
Fan Qingyang
Dai Chuanxiang
Xing Mengdao
Liu Yonghong
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Yangtze River Delta Research Institute of UESTC Huzhou
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Yangtze River Delta Research Institute of UESTC Huzhou
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    • CCHEMISTRY; METALLURGY
    • C01INORGANIC CHEMISTRY
    • C01BNON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B21/00Nitrogen; Compounds thereof
    • C01B21/06Binary compounds of nitrogen with metals, with silicon, or with boron, or with carbon, i.e. nitrides; Compounds of nitrogen with more than one metal, silicon or boron
    • C01B21/0605Binary compounds of nitrogen with carbon
    • CCHEMISTRY; METALLURGY
    • C01INORGANIC CHEMISTRY
    • C01BNON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B32/00Carbon; Compounds thereof
    • C01B32/05Preparation or purification of carbon not covered by groups C01B32/15, C01B32/20, C01B32/25, C01B32/30
    • CCHEMISTRY; METALLURGY
    • C01INORGANIC CHEMISTRY
    • C01PINDEXING SCHEME RELATING TO STRUCTURAL AND PHYSICAL ASPECTS OF SOLID INORGANIC COMPOUNDS
    • C01P2002/00Crystal-structural characteristics
    • C01P2002/70Crystal-structural characteristics defined by measured X-ray, neutron or electron diffraction data
    • C01P2002/72Crystal-structural characteristics defined by measured X-ray, neutron or electron diffraction data by d-values or two theta-values, e.g. as X-ray diagram
    • CCHEMISTRY; METALLURGY
    • C01INORGANIC CHEMISTRY
    • C01PINDEXING SCHEME RELATING TO STRUCTURAL AND PHYSICAL ASPECTS OF SOLID INORGANIC COMPOUNDS
    • C01P2006/00Physical properties of inorganic compounds
    • C01P2006/90Other properties not specified above
    • YGENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02EREDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/13Energy storage using capacitors

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  • Chemical & Material Sciences (AREA)
  • Organic Chemistry (AREA)
  • Inorganic Chemistry (AREA)
  • Carbon And Carbon Compounds (AREA)
  • Catalysts (AREA)

Abstract

A nitrogen doped carbon material has a space group of Fd-3c and lattice parameters a = b = c = 1.10592 nm ± 0.5%. A preparation method of the material may comprise adding cyanuric acid and NH2NH2, hydrazine, into distilled water, alcohol or benzene and mixing evenly in an inert atmosphere. The mixture may then be sealed into a reactor which is treated in an oven at a temperature of 700-800 K for 8-12 hours followed by natural cooling to room temperature and letting to stand for 2-5 hours to obtain a powder. The powder may then be washed successively and repeatedly with alcohol, dilute hydrochloric acid and distilled water, followed by filtering. The washing and filtering process may be repeated at least three times before drying at 350-450 K for 3-4 hours. The material may be used in energy storage materials, catalysts for organic reactions, photocatalysts, or sensors.

Description

NITROGEN-DOPED CARBON MATERIAL AND PREPARATION METHOD
THEREOF
TECHNICAL FIELD
[0001] The present disclosure relates to the technical field of materials, in particular to a nitrogen-doped carbon material and preparation method thereof.
BACKGROUND
[0002] Carbon plays a very important role in electrode materials due to excellent physical and chemical properties thereof Electrode materials are an important part of supercapacitors. The research and development of carbon materials is a vital part of the research and development of supercapacitors. As one of the hot research objects in the field of basic materials, carbon materials still have a long way to go in terms of design and discovery of breakthroughs. Herein, doping is one of the main ways to improve the properties of carbon materials. Since nitrogen doping can significantly improve the electrochemical performance of materials, the synthesis and preparation of nitrogen-doped porous carbon materials have attracted more and more attention of researchers.
[0003] Diamond is currently the hardest material known in the world, and more and more researchers began to become interested in this material when it was discovered that carbonitrides exhibited excellent mechanical properties comparable to those of diamond. In 1989, American scientists Liu and Cohen (reference: "Prediction of New Low Compressibility Solids", Science, 1989, 245, 841) used the 13-Si3N4 crystal structure as a model under the local density approximations, in which Si was replaced with C, and they theoretically proposed a 13-C3N4 crystal for the first time, which has a hardness comparable to that of diamond. Recently. Huang et al. (reference: "Tuning Nitrogen Species and Content in Carbon Materials through Constructing Variable Structures for Supercapacitors", Journal of Inorganic Materials, 2021, 36, 7) modulated the type and content of nitrogen doped into the carbon material by the interaction between Si-O-Si network and alumina, so that the nitrogen content was as high as 5.29% at 1,000°C. However, the raw materials and methods used in nitrogen-doped carbon materials still require further research [0004] Chinese Patent Publication No. CN109647474A discloses a nitrogen-doped carbon material, a preparation method and use thereof With glucose as a raw material and melamine as a nitrogen source, the glucose is calcined to a certain temperature in an inert atmosphere to prepare a carbon substrate, and the calcined carbon substrate and the melamine are mixed in an aqueous solution in a certain proportion, heated. stirred, dried, and calcined at low temperature again in an inert atmosphere to obtain the nitrogen-doped carbon material. The preparation method is simple, the energy consumption is low, and the cost is low. The nitrogen-doped carbon material shows high reactivity and can selectively degrade a plurality of organic pollutants, thereby solving the technical problems of complex preparation methods of nitrogen-doped carbon materials in the prior art, high costs, and limited degradation ability of organic pollutants in the environment.
[0005] However, the cost of melamine in the above solution is relatively high, waste liquid is easily produced in the process, and the market has demands for large-scale production, further reduction of production costs and environmental protection.
SUMMARY
[0006] In order to overcome the deficiencies in the prior art, an objective of the present disclosure is to provide a nitrogen-doped carbon material featuring a simple preparation method and easy mass production and a preparation method thereof.
[0007] Technical solutions: A nitrogen-doped carbon material is provided, including: [0008] a space group of the nitrogen-doped carbon material is Fd-3c, and lattice parameters are a = b = c = 1.10592 nm ± 0.5%.
[0009] 2. A preparation method of the nitrogen-doped carbon material according to claim I is provided, including the following steps: [0010] step 1, adding cyarunic chloride and NH2NR2 into distilled water, alcohol or benzene, and mixing these reagents evenly in an inert gas atmosphere to obtain a mixture A; [0011] step 2, putting the mixture A obtained in step 1 into a reactor, scaling the reactor, treating the reactor in an oven at a constant temperature of 700-800 K for 8-12 h, naturally cooling the reactor to room temperature, and letting stand for 2-5 h to obtain a powder B; and [0012] step 3, washing the powder B obtained in step 2 successively and repeatedly with alcohol, dilute hydrochloric acid and distilled water, filtering, repeating the washing and the filtering at least three times successively, and drying the powder B under vacuum at 350-450 K for 3-4 h to obtain the nitrogen-doped carbon material according to claim 1.
[0013] Further, in step 1, the cyanuric chloride, the NH2NE1/ and the solvent may be in a mass ratio of 2:1:(10-80).
[0014] Further, in step 1, the alcohol in the mixture A may have a mass concentration of 50-95%, and the cyanuric chloride and the NH2NH2 may be in a mass ratio of 2:1.
[0015] Further, in step 3, the alcohol may have a mass concentration of 45-80%, and the alcohol and the powder B may be in a volume ratio of (2-8):30.
[0016] Further, in step 3, the dilute hydrochloric acid may have a mass concentration of 5-20%, and the dilute hydrochloric acid and the powder B may be in a volume ratio of (2-8):20.
[0017] Further, in step 3, the distilled water and the powder B may be in a volume ratio of (28):5O.
[0018] Further, use of the nitrogen-doped carbon material in energy storage materials, catalysts for organic reactions, photocatalysts, and/or sensors is provided.
[0019] The present disclosure has the following beneficial effects: In the present disclosure, cyanuric chloride and NH2N1-11 as carbon and nitrogen sources are added to distilled water, alcohol and benzene, and a novel nitrogen-doped carbon material is prepared through hydrothermal treatment and solvotherrnal treatment. The method provided by the present disclosure has a low production rate of waste liquid, impurities in the process are elements like hydrogen, chlorine, oxygen, etc., which are easily removed, and the raw materials are abundant and inexpensive. Process impurities can arise from surface oxidation and adsorption during processing, or from unavoidable moisture contamination from prolonged exposure to air. Powder B is repeatedly washed to remove by-products and reaction residues therein.
BRIEF DESCRIPTION OF THE DRAWINGS
[0020] FIG. I illustrates a crystal structure of a nitrogen-doped carbon material provided by the present disclosure; [0021] FIG. 2 is an X-ray diffraction pattern of a nitrogen-doped carbon material in Example 1 of the present disclosure; [0022] FIG. 3 is an X-ray diffraction pattern of a nitrogen-doped carbon material in Example 2 of the present disclosure; [0023] FIG. 4 is an X-ray diffraction pattern of a nitrogen-doped carbon material in Example 3 of the present disclosure.
DETAILED DESCRIPTION OF THE EMBODIMENTS
[0024] In order to make the objectives, technical solutions and advantages of the present disclosure clearer, the present disclosure will be further described in detail below with reference to the accompanying drawings and examples. It should be understood that the specific examples described herein are only intended to explain the present disclosure, but not to limit the present disclosure. Based on the examples of the present disclosure, all other examples obtained by those of ordinary skill in the art without creative efforts shall fall within the protection scope of the present disclosure.
[0025] The present disclosure provides a nitrogen-doped carbon material, specifically, referring to the following examples: [0026] Example 1: The nitrogen-doped carbon material in this example, the space group of the nitrogen-doped carbon material was Fd-3c, and the lattice parameters were a = b = c = 1.10592 nm. The crystal structure is shown in FIG. 1, and the nitrogen-doped carbon material has good stability.
[0027] A preparation method of the nitrogen-doped carbon material was provided and the specific steps were as follows: [0028] step 1, cyanuric chloride and NI-2NI-12 were added into distilled water, and mixed evenly in an inert gas atmosphere to obtain a mixture A, where the cyanuric chloride, the NH2N1-1/, and the distilled water were in a mass ratio of 2:1:80; [0029] step 2, the mixture A obtained in step 1 was put into a reactor, and the reactor was sealed, treated in an oven preset at a constant temperature of 800 K for 12 h, naturally cooled to room temperature, and let stand for 2-5 h to obtain a powder B, where the powder B was a C-N-H-0 compound; and [0030] step 3, the resulting powder B was washed successively and repeatedly with alcohol, dilute hydrochloric acid and distilled water and filtered, the washing and the filtering were repeated at least three times successively, and the powder B was dried under vacuum at 450 K for 3-4 h to obtain the a new nitrogen-doped carbon material with an Fd-3c space group, where the mass concentration of the alcohol was 45%, and the alcohol and the powder B were in a volume ratio of 30:(2-8); the mass concentration of the dilute hydrochloric acid was 5%, and the dilute hydrochloric acid and the powder B were in a volume ratio of 20:(2-8); the distilled water and the powder B were in a volume ratio of 50:(2-8).
[0031] The X-ray diffraction pattern of the nitrogen-doped carbon material with an Fd-3c space group in this example is shown in P10.2. The lattice parameters were a = b = c = 1.10592 nm. [0032] The density of the nitrogen-doped carbon material with an Fd-3c space group in this example was 4.1675 g/cm3.
[0033] Example 2: A preparation method of the nitrogen-doped carbon material was provided, and the specific steps were as follows: [0034] step 1, cyanuric chloride and NII2N142 were added into alcohol, and mixed evenly in an inert gas atmosphere to obtain a mixture A, where the cyanuric chloride, the NF2NH2, and the alcohol were in a mass ratio of 2:1:50; [0035] step 2, the mixture A obtained in step 1 was put into a reactor, and the reactor was sealed, treated in an oven preset at a constant temperature of 750 K for 10 h, naturally cooled to room temperature. and let stand for 3-5 h to obtain a powder B; and [0036] step 3, the resulting powder B was washed successively and repeatedly with alcohol, dilute hydrochloric acid and distilled water and filtered, the washing and the filtering were repeated at least three times successively, and the powder B was dried under vacuum at 400 K for 3-4 h to obtain the a new nitrogen-doped carbon material with an Fd-3c space group, where the mass concentration of the alcohol was 75%, and the alcohol and the powder B were in a volume ratio of 30:(2-8); the mass concentration of the dilute hydrochloric acid was 15%, and the dilute hydrochloric acid and the powder B were in a volume ratio of 20:(2-8); the distilled water and the powder B were in a volume ratio of 50:(2-8).
[0037] The X-ray diffraction pattern of the nitrogen-doped carbon material with an Fd-3c space group in this example is shown in FIG. 3. The lattice parameters were a = h = c = 1.11043 nm. [0038] The density of the nitrogen-doped carbon material with an Fd-3c space group in this example was 4.1170 g/cm3.
[0039] Example 3: A preparation method of the nitrogen-doped carbon material was provided, and the specific steps were as follows: [0040] step 1, cyanuric chloride and N11-12NI-I2 were added into a benzene solution, and mixed evenly in an inert gas atmosphere to obtain a mixture A, where the cyanuric chloride, the NH21\1111, and the benzene were in a mass ratio of 2:1:10; [0041] step 2, the mixture A obtained in step I was put into a reactor, and the reactor was sealed, treated in an oven preset at a constant temperature of 700 K for 8 h, naturally cooled to room temperature, and let stand for 2-5 h to obtain a powder B; and [0042] step 3, the resulting powder B was washed successively and repeatedly with alcohol, dilute hydrochloric acid and distilled water and filtered, the washing and the filtering were repeated at least three times successively, and the powder B was dried under vacuum at 350 K for 3-4 h to obtain the a new nitrogen-doped carbon material with an Fd-3c space group, where the mass concentration of the alcohol was 95%, and the alcohol and the powder B were in a volume ratio of 30:(2-8); the mass concentration of the dilute hydrochloric acid was 20%, and the dilute hydrochloric acid and the powder B were in a volume ratio of 20:(2-8); the distilled water and the powder B were in a volume ratio of 50:(2-8).
[0043] The X-ray diffraction pattern of the nitrogen-doped carbon material with an Fd-3c space group in this example is shown in FIG. 4. The lattice parameters were a = h = c = 1.10049 nm. [0044] The density of the nitrogen-doped carbon material with an Fd-3c space group in this example was 4.2127 g/cm3.
[0045] The above descriptions are merely preferred implementations of the present disclosure. It should be noted that a person of ordinary skill in the art may further make several improvements and modifications without departing from the principle of the present disclosure, but such improvements and modifications shall also be deemed as falling within the protection scope of the present disclosure.

Claims (8)

  1. CLAIMS1. A nitrogen-doped carbon material, wherein a space group of the nitrogen-doped carbon material is Fd-3c, and lattice parameters are a = b = c = 1.10592 nm ± 0.5%.
  2. 2. A preparation method of a nitrogen-doped carbon material according to claim 1, comprising the following steps: step 1, adding cyanuric chloride and NH2NH2 into distilled water, alcohol or benzene, and mixing these reagents evenly in an inert gas atmosphere to obtain a mixture A; step 2, putting the mixture A obtained in step 1 into a reactor, sealing the reactor, treating the reactor in an oven at a constant temperature of 700-800 K for 8-12 h, naturally cooling the reactor to room temperature, and letting stand for 2-5 h to obtain a powder B; and step 3, washing the powder B obtained in step 2 successively and repeatedly with alcohol, dilute hydrochloric acid and distilled water, filtering, repeating the washing and the filtering at least three times successively, and drying the powder B under vacuum at 350-450 K for 3-4 h to obtain the nitrogen-doped carbon material according to claim 1.
  3. 3. The nitrogen-doped carbon material according to claim I. wherein in step I, the cyanuric chloride, the NH-NW and the solvent are in a mass ratio of 2:1:(10-80).
  4. 4. The nitrogen-doped carbon material according to claim 3, wherein in step 1, the alcohol in the mixture A has a mass concentration of 50-95%, and the cyanuric chloride and the NELNI+ are in a mass ratio of 2:1.
  5. 5. The nitrogen-doped carbon material according to claim 4, wherein in step 3, the alcohol has a mass concentration of 45-80%, and the alcohol and the powder B are in a volume ratio of (2-8):30.
  6. 6. The nitrogen-doped carbon material according to claim 1, wherein in step 3, the dilute hydrochloric acid has a mass concentration of 5-20%, and the dilute hydrochloric acid and the powder B are in a volume ratio of (2-8):20.
  7. 7. The nitrogen-doped carbon material according to claim 6, wherein in step 3, the distilled water and the powder B are in a volume ratio of (2-8):50.
  8. 8. Use of the nitrogen-doped carbon material according to claim 1 in energy storage materials, catalysts for organic reactions, photocatalysts, and/or sensors.
GB2218215.8A 2021-12-06 2022-12-05 Nitrogen-doped carbon material and preparation method thereof Pending GB2616103A (en)

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CN115739047B (en) * 2022-11-18 2024-05-03 电子科技大学长三角研究院(湖州) Preparation method and application of nitrogen-enriched adsorbent for removing perfluoro and polyfluoroalkyl substances (PFAS) from water

Citations (1)

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Publication number Priority date Publication date Assignee Title
EP0871587A1 (en) * 1996-01-04 1998-10-21 Carnegie Institution Of Washington Low compressibility carbon nitrides

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JP5294234B2 (en) * 2007-05-10 2013-09-18 独立行政法人物質・材料研究機構 Nitrogen-doped mesoporous carbon (N-KIT-6) and method for producing the same
CN106920973A (en) * 2017-03-02 2017-07-04 华东师范大学 A kind of synthetic method of nitrogen-doped carbon non noble metal oxygen reduction electrocatalysis material
CN109659148B (en) * 2018-12-26 2020-10-09 江南大学 Nitrogen-doped carbon material and preparation method thereof

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* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
EP0871587A1 (en) * 1996-01-04 1998-10-21 Carnegie Institution Of Washington Low compressibility carbon nitrides

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