WO2019151636A1 - Method for preparing high-purity mxene - Google Patents

Method for preparing high-purity mxene Download PDF

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WO2019151636A1
WO2019151636A1 PCT/KR2018/015469 KR2018015469W WO2019151636A1 WO 2019151636 A1 WO2019151636 A1 WO 2019151636A1 KR 2018015469 W KR2018015469 W KR 2018015469W WO 2019151636 A1 WO2019151636 A1 WO 2019151636A1
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maxine
carbonate
high purity
reacting
mxene
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PCT/KR2018/015469
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French (fr)
Korean (ko)
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서유경
김연승
이동욱
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주식회사 엘지화학
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    • 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
    • C01B32/90—Carbides
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01P—INDEXING SCHEME RELATING TO STRUCTURAL AND PHYSICAL ASPECTS OF SOLID INORGANIC COMPOUNDS
    • C01P2002/00—Crystal-structural characteristics
    • C01P2002/70—Crystal-structural characteristics defined by measured X-ray, neutron or electron diffraction data
    • C01P2002/78—Crystal-structural characteristics defined by measured X-ray, neutron or electron diffraction data by stacking-plane distances or stacking sequences
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01P—INDEXING SCHEME RELATING TO STRUCTURAL AND PHYSICAL ASPECTS OF SOLID INORGANIC COMPOUNDS
    • C01P2006/00—Physical properties of inorganic compounds
    • C01P2006/80—Compositional purity

Definitions

  • the present invention relates to a manufacturing method, and more particularly, to a method for manufacturing a high purity maxine ( 611 ⁇ 2) having high purity and excellent electrical properties more efficiently.
  • phase « ⁇ 336 a silver transition metal, a group 13 or 14 element
  • X is carbon and / or nitrogen
  • the X phase has electrical conductivity, oxidation resistance, It is also known to have excellent physical properties such as machinability.
  • the present invention relates to a method for producing high purity Maxene (MXene) with higher purity and excellent electrical properties more efficiently.
  • MXene a high purity maxine
  • a method for preparing high purity Maxine (MXene) may be provided.
  • the present inventors conducted a study on a method to more easily provide high purity Maxine (MXene), and by reacting Maxine obtained by reacting the MX phase with a strong acid with carbonate or hydrogen carbonate, The high efficiency of the Maxine (MXene) with high purity can be provided in a short time, and the experiment confirmed that the Maxine (MXene) can achieve excellent electrical conductivity and electromagnetic shielding effect with high purity, and completed the invention. .
  • reaction mechanism is to react with the Max phase and the remaining strong acid and carbonate or hydrogen carbonate reacts to generate carbon dioxide and carbon dioxide bubbles in the dispersion.
  • These bubbles in particular, the bubbles generated by the Maxine interlayer, is a process in which the Maxine interlayer peeling proceeds and desorption of the acid and salt inserted into the layer occurs to increase the purification efficiency.
  • the high purity Maxine ( ⁇ 611 ⁇ 2 ) by-product means less than 30% by weight, or less than 20% by weight, or less than 10% by weight, or less than 5% by weight.
  • carbonate or hydrogen carbonate examples include sodium carbonate, sodium bicarbonate, potassium carbonate, potassium hydrogen carbonate, lithium carbonate, sodium carbonate, rubidium carbonate, cesium carbonate, cesium carbonate, ammonium carbonate, ammonium bicarbonate, or these Two or more kinds of mixtures.
  • the phase may be defined as a silver transition metal, the show is a group 13 or 14 element, X is carbon and / or nitrogen. Specific examples of the phase include three o'clock (: 2, or 3 2, four, Ti 3 GeC2, 3 3 ⁇ 4 ( : 2, 13 ⁇ 4 hours (: 2 , 413 ⁇ 4 , ⁇ 41 (: 3 , ⁇ 3 (: 3,
  • the carbonate or hydrogen carbonate may be used at 0.1 1110 1% to 25 1 ⁇ 1%, or 1 1% to 15% () 1% of the strong acid.
  • the amount of the carbonate or the hydrogen carbonate is too low compared to the amount of the strong acid, since the generation of carbon dioxide that can remove or help by-products present in the maxine is insignificant, the removal efficiency of the acid and the salt may be technically disadvantageous. On the contrary, if the amount of the strong acid is too high, additional purification time of the salt may occur, which may be technically corrected.
  • the maxine obtained by reacting the Max phase (3 ⁇ 41 / shank with a strong acid may contain various salt compounds which appear in the reaction with the above-mentioned strong acid, and the Maxine ( ⁇ is hydrochloric acid ( ⁇ 1) and lithium chloride (Ni)). , it can contain by-products, including ammonium fluoride Lyrium (Nishi ⁇ 1 6) or ammonium fluoride (3 ⁇ 4 hour).
  • the high purity maxine obtained through the manufacturing method of high purity maxine (1X 6116 ) of the above embodiment is hydrochloric acid ( ⁇ 1), lithium chloride (Ni): 1, lithium aluminum fluoride (Ni ⁇ 13 ⁇ 4), or aluminum fluoride (Si3 ⁇ 4). It can contain up to 5 wt% of by-products,
  • the purification efficiency may be further improved due to the carbon dioxide bubbles generated in the step of reacting the prepared Maxine) with carbonate or hydrogen carbonate.
  • the high purity maxine ( 0! 1 ⁇ 2 ) manufacturing method of the above embodiment may include a step of purifying with water after the step of reacting the prepared maxine ( ⁇ ) with carbonate or hydrogen carbonate.
  • the amount of water used may be greatly reduced due to the step of reacting the prepared maxine (e) with carbonate or hydrogen carbonate, and in the step of purifying the prepared maxine ( ⁇ ) with water, the preparation May be removed using less than 2000 parts by weight or 100 to 1000 parts by weight of water.
  • the high purity Maxine (Chelene) can have an electrical conductivity of 5.0 X 10 5 / mi or more.
  • the manufactured high purity Maxine » 611 ⁇ 2 can be used as an internal / external electrode of a cathode conductive material for a secondary battery or a secondary battery.
  • the high-purity maxine provided as described above can realize electromagnetic shielding effect by using excellent electrical conductivity, and thus internal and external electrodes, etc. It can be easily applied as a material to various industrial fields.
  • FIG. 1 shows Maxine (Original seedling images prepared in each of Example 1 and Comparative Example 1).
  • the lg MAX phase (Ti 3 AlC 2) was added to 20 mL of 6 M HC1 solution in which lg fluoride was dissolved and stirred at 50 ° C. for 24 hours.
  • the lg MAX phase (Ti 3 AlC 2) was added to 20 mL of 6 M HC1 solution in which lgium fluoride was dissolved and stirred at 50 ° C. for 24 hours. Then, the mixture was filtered using water until the pH of the filtrate was neutral, and dried for 12 hours in a vacuum oven to obtain MXne powder.
  • the electrical conductivity of the maxine (11X 6116 ) of the said Example and the comparative example was measured through 4 ⁇ 01 ⁇ .
  • Example 1 Example 1 and Comparative purification rate, the electric conductivity of Maxine ( ⁇ 611 ⁇ 2) been prepared by Example 1, and a) ®! 2- ⁇ 3 value comparison Example 1 was confirmed to be the greater as higher the electrical conductivity having a short time Maxine obtained though not completed the tablets within, than the distance between layers is also identified in the XI ⁇ 2- 3 value as shown in Table 1 above.
  • the purification rate difference 5 minutes VI 10 minutes
  • Example 1 clearly distinguished the particles between layers as compared with the maxine obtained in Comparative Example 1.

Abstract

The present invention relates to a method for preparing high-purity MXene comprising the steps of: forming MXene by means of reacting a MAX phase with strong acid; and reacting the formed MXene with carbonates or hydrogen carbonates.

Description

2019/151636 1»（：1^1{2018/015469  2019/151636 1 »（： 1 ^ 1 {2018/015469
【발명의 명칭】 [Name of invention]
고순도의 맥신 ( 61½)제조방법 High purity Maxine ( 61½) manufacturing method
【기술분야】  Technical Field
관련출원 (들)과의 상호인용  Citation with Related Application (s)
본출원은 2018년 2월 2일자한국특허출원제 10-2018-0013604호에 기초한우선권의 이익을주장하며， 해당한국특허 출원의 문헌에 개시된모든 내용은본명세서의 일부로서 포함된다.  This application claims the benefit of priority based on Korean Patent Application No. 10-2018-0013604 dated February 2, 2018, and all contents disclosed in the documents of the Korean patent application are included as part of this specification.
본 발명은 고순도의 맥신
Figure imgf000003_0001
제조 방법 에 관한 것으로， 보다 상세하게는 보다 효율적으로 높은 순도 및 우수한 전기적 특성을 갖는 고순도의 맥신 ( 61½)을제조할수있는방법에 관한것이다. High Purity Maxine
Figure imgf000003_0001
The present invention relates to a manufacturing method, and more particularly, to a method for manufacturing a high purity maxine ( 61½) having high purity and excellent electrical properties more efficiently.
【발명의 배경이 되는기술】  【Technology behind the invention】
그래핀과유사한구조를갖는 2차원물질의 하나로 상 «油336 , 은 전이금속， 요는 13 또는 14족 원소, X는 탄소 및/또는 질소)이 알려져 있으며， 이러한 X 상은 전기전도성， 내산화성， 기계가공성 등의 물성이 우수한것으로도알려져 있다.  One of the two-dimensional materials similar to graphene is known as phase «상 336, a silver transition metal, a group 13 or 14 element, X is carbon and / or nitrogen, and the X phase has electrical conductivity, oxidation resistance, It is also known to have excellent physical properties such as machinability.
최근 상인 3차원의 티타늄-알루미늄 카바이드에서 불산 등의 강산을사용하여 상기 쇼에 해당하는 알루미늄층을선택적으로 제거함으로써， 완전히 다른특성을갖는 2차원의 구조로 변형시켜 "맥신 (歌 "이라불리는 2차원 물질이 소개된 바 있다.
Figure imgf000003_0002
그래핀과 같은 유사한 전기전도성과 강도를 가지는데, 이러한 특성으로 인하여 다양한 분야에서 적용하려는시도가있다. In recent years, the commercially available three-dimensional titanium-aluminum carbide was used to selectively remove the aluminum layer corresponding to the show by using a strong acid such as hydrofluoric acid, thereby transforming it into a two-dimensional structure having completely different characteristics. Dimensional matter has been introduced.
Figure imgf000003_0002
It has similar electrical conductivity and strength like graphene, but due to these characteristics, there are attempts to apply in various fields.
상술한 바와 같이， 고순도 맥신을 제조하기 위해
Figure imgf000003_0003
등의 강산을 사용하게 되는데, 이러한 강산을 사용하여 맥신 (1X6116)을 제조하면 부산물로
Figure imgf000003_0005
생성된다. 이러한부산물이
Figure imgf000003_0004
존재하게되면저항으로작용하여 전기 전도도가크게 저하되거나전자파차폐 물성 등이 저하될수있다. As described above, to manufacture high purity maxine
Figure imgf000003_0003
Strong acids, such as Maxine (1X 6116) is used as a by-product
Figure imgf000003_0005
Is generated. These by-products
Figure imgf000003_0004
When present, it acts as a resistance, greatly reducing the electrical conductivity or electromagnetic wave shielding properties.
이전에는 상술한 부산물을 제거하기 위해서 단순히 물을 사용한 원심분리를통하여 정제를하고 있는더ᅵ， 정제 효율이 많이 저하되어 양산성이 떨어질 뿐만 아니라 과량의 물을 사용해야 하고， 긴 정제 시간이 요구되는 한계가있었다. 【발명의 내용】 Previously, the above-mentioned by-products were purified simply by centrifugation with water, and the purification efficiency was much lowered, not only the productivity was lowered, but also excessive water was used, and a long purification time was required. There was. [Content of invention]
【해결하고자하는과제】  [Task to be solved]
본발명은， 보다효율적으로높은순도 및 우수한 전기적 특성을갖는 고순도의 맥신 (MXene)을제조할수있는방법에 관한것이다.  The present invention relates to a method for producing high purity Maxene (MXene) with higher purity and excellent electrical properties more efficiently.
【과제의 해결수단】  [Measures of problem]
본명세서에서는, 맥스상(MX phase)을강산과반응시켜 맥신 (MXene)을 형성하는단계; 및상기 형성된맥신을탄산염 또는탄산수소염과반응시키는 단계를포함하는， 고순도의 맥신 (MXene)제조방법이 제공된다.  In the present specification, the step of reacting the Max phase (MX phase) with a strong acid to form a Maxine (MXene); And reacting the formed maxine with a carbonate or a hydrogen carbonate salt. A high purity maxine (MXene) manufacturing method is provided.
이하 발명의 구체적인 구현예에 고순도의 맥신 (MXene) 제조 방법에 대해서 보다구체적으로설명하기로한다. 상술한 바와 같이， 발명의 일 구현예에 따르면, 맥스상(MAX phase)을 강산과반응시켜 맥신 (MXene)을형성하는단계; 및상기 형성된 맥신을탄산염 또는탄산수소염과반응시키는단계를포함하는， 고순도의 맥신 (MXene) 제조 방법이 제공될수있다.  Hereinafter, the method of manufacturing high purity Maxine (MXene) will be described in more detail with reference to specific embodiments of the present invention. As described above, according to one embodiment of the invention, the step of reacting the MAX phase (MAX phase) with a strong acid to form a maxine (MXene); And reacting the formed maxine with a carbonate or hydrogen carbonate salt. A method for preparing high purity Maxine (MXene) may be provided.
맥스상(MAX phase)을 강산으로 처리하여 제조되는 맥신 (MXene)을 단순히 물을 사용하여 정제하는 이전에 방법에 따르면， 맥신의 층 내에 존재하는불소계 염 등은물과 같은 친수성 용매에 대해 용해도가 매우 낮고 층간에 삽입되어 있기 때문에 물 정제에 의한 제거가 상당히 어려운 한계가 있었다.  According to the previous method of simply purifying MXene, prepared by treating the MAX phase with a strong acid, using water, the solubility in hydrophilic solvents such as fluorine-based salts, such as water, in the Maxine layer Due to the very low intercalation, removal by water purification was quite difficult.
이에 본 발명자는 높은 순도를 갖는 맥신 (MXene)을 보다 용이하게 제공할수 있는방법에 대하여 연구를진행하여， 맥스상(MX phase)을강산과 반응시켜 얻어진맥신을탄산염 또는탄산수소염과반응시킴으로서 , 보다높은 효율로짧은시간내에 높은 순도를 갖는 맥신 (MXene)을 제공할수 있으며， 이러한 맥신 (MXene)이 고순도와 함께 우수한 전기 전도성 및 전자파 차폐 효과를구현할수있다는점을실험을통하여 확인하고발명을완성하였다. 보다 구체적으로, 맥스상(MAX phase)을 강산과 반응시켜 얻어진 맥신 분산액에 탄산염 또는 탄산수소염을 첨가하게 되면 이산화탄소가 발생할 수 있는데， 이러한 이산화탄소의 발생으로생성되는소정의 힘 또는압력에 의해 맥신 내부의 층들간의 거리가 확장되어 부산물인 불소계 염과 산 등이 보다 2019/151636 1»（：1^1{2018/015469 Accordingly, the present inventors conducted a study on a method to more easily provide high purity Maxine (MXene), and by reacting Maxine obtained by reacting the MX phase with a strong acid with carbonate or hydrogen carbonate, The high efficiency of the Maxine (MXene) with high purity can be provided in a short time, and the experiment confirmed that the Maxine (MXene) can achieve excellent electrical conductivity and electromagnetic shielding effect with high purity, and completed the invention. . More specifically, when carbonate or hydrogen carbonate is added to the maxine dispersion obtained by reacting the MAX phase with a strong acid, carbon dioxide may be generated, and due to a predetermined force or pressure generated by the generation of carbon dioxide, The distance between the layers has been extended to see the byproducts of fluorine salts and acids 2019/151636 1 »（： 1 ^ 1 {2018/015469
쉽게 정제 또는 제거 될 수 있다. 보다 구체적인 반응 메커니즘은 맥스상과 반응하고 남은 강산과 탄산염 또는 탄산수소염이 반응하여 이산화탄소를 발생시키고분산액 내에서 이산화탄소기포를발생시키게 된다. 이러한기포， 특히 맥신 층간발생되는 기포에 의해 맥신 층간박리가진행되고층내부에 삽입되어 있는 산과 염의 탈리현상이 발생하여 정제 효율이 높아지게 되는 과정이다. It can be easily purified or removed. More specific reaction mechanism is to react with the Max phase and the remaining strong acid and carbonate or hydrogen carbonate reacts to generate carbon dioxide and carbon dioxide bubbles in the dispersion. These bubbles, in particular, the bubbles generated by the Maxine interlayer, is a process in which the Maxine interlayer peeling proceeds and desorption of the acid and salt inserted into the layer occurs to increase the purification efficiency.
상기 고순도 맥신 （歌61½） 부산물의 함량이 30중량% 미만, 또는 20중량%이하， 또는 10중량%이하， 또는 5중량%이하인맥신을의미한다. The high purity Maxine (歌61½ ) by-product means less than 30% by weight, or less than 20% by weight, or less than 10% by weight, or less than 5% by weight.
상기 탄산염 또는 탄산수소염의 구체적인 예로는， 탄산 나트륨, 탄산수소나트륨, 탄산칼륨， 탄산수소칼륨， 탄산리튬, 탄산수소리륨， 탄산 루비듐， 탄산 세슘， 탄산수소 세슘, 탄산 암모늄， 탄산수소 암모늄， 또는 이들의 2종이상의혼합물을들수있다.  Specific examples of the carbonate or hydrogen carbonate include sodium carbonate, sodium bicarbonate, potassium carbonate, potassium hydrogen carbonate, lithium carbonate, sodium carbonate, rubidium carbonate, cesium carbonate, cesium carbonate, ammonium carbonate, ammonium bicarbonate, or these Two or more kinds of mixtures.
상기 상은 은 전이금속， 쇼는 13 또는 14족 원소， X는 탄소 및/또는질소로정의될수 있으며， 이러한 상의 구체적인 예로는 3시（：2 , 또는 3 2 , 사 ， Ti3GeC2, 3¾（:2 , 1¾시（:2， 41¾， ¥41（:3， 本3（:3 , The phase may be defined as a silver transition metal, the show is a group 13 or 14 element, X is carbon and / or nitrogen. Specific examples of the phase include three o'clock (： 2, or 3 2, four, Ti 3 GeC2, 3 ¾ ( : 2, 1¾ hours （: 2 , 41¾ ， ¥ 41 （: 3 ， 本3 （: 3,
Figure imgf000005_0001
Figure imgf000005_0001
2況, 故， 뀨比， 1¾시（：， ^ ^, 2¾£, 少比， 2¾ ， 2就등을들 수있다. 2 況, 故, 뀨 比, 1 ¾ hr （：， ^ ^, 2 ¾ £, 少 比 ， 2 ¾ ， 2就.
상기 형성된 맥신을 탄산염 또는 탄산수소염과 반응 시키는 단계에서， 상기 탄산염 또는탄산수소염은상기 강산의 0.1 11101 %내지 25 1¥1 %, 또는 1 1 %내지 15미（）1 %로사용할수있다. In the step of reacting the formed maxine with carbonate or hydrogen carbonate, the carbonate or hydrogen carbonate may be used at 0.1 1110 1% to 25 1 ¥ 1%, or 1 1% to 15% () 1% of the strong acid.
상기 탄산염 또는 탄산수소염의 사용량이 상기 강산의 사용량 대비 너무낮은경우, 맥신 내에 존재하는부산물을제거하거나이를도울수 있는 이산화탄소의 발생이 미미하여 산과 염의 제거효율이 낮아지므로 기술적으로 불리할수 있다. 반대로강산의 사용량대비 너무많은경우， 염의 추가정제 시간이 발생하여 기술적으로 4리할수있다.  When the amount of the carbonate or the hydrogen carbonate is too low compared to the amount of the strong acid, since the generation of carbon dioxide that can remove or help by-products present in the maxine is insignificant, the removal efficiency of the acid and the salt may be technically disadvantageous. On the contrary, if the amount of the strong acid is too high, additional purification time of the salt may occur, which may be technically corrected.
상기 형성된 맥신을 탄산염 또는 탄산수소염과 반응 시키는 단계는 2019/151636 1»（：1^1{2018/015469 Reacting the formed maxine with carbonate or hydrogen carbonate 2019/151636 1 »（： 1 ^ 1 {2018/015469
그리 높지 않은온도범위에서 수행되어도높은정제 효율을구현할수있으며， 예를들어
Figure imgf000006_0001
내지 80 °（：의 온도에서 수행될수있다. Even in the non-high temperature range, high purification efficiency can be achieved.
Figure imgf000006_0001
It can be carried out at a temperature of ~ 80 ° (：).
상기 맥스상（¾1/伏 크 을강산과반응시켜 얻어진 맥신 내에는상술한 강산과의 반응에서 나타나는각종염화합물등이 포함될수있으며， 상기 맥신 （歌 은 염산（狀1）, 염화 리륨（니이）, 불화 알루미늄 리륨（니必1 6） 또는 불화알루미늄（시¾）을포함한부산물을포함할수있다. The maxine obtained by reacting the Max phase (¾1 / shank with a strong acid may contain various salt compounds which appear in the reaction with the above-mentioned strong acid, and the Maxine (歌 is hydrochloric acid (狀 1) and lithium chloride (Ni)). , it can contain by-products, including ammonium fluoride Lyrium (Nishi必1 6) or ammonium fluoride (¾ hour).
그리고， 상기 구현예의 고순도의 맥신 （1X6116） 제조 방법을 통하여 얻어지는 고순도의 맥신은 염산（狀1）, 염화 리륨（니（：1）， 불화 알루미늄 리튬（니必1¾） 또는 불화 알루미늄（시¾）을 포함한 부산물을 5 중량% 이하로 포함할수있다. In addition, the high purity maxine obtained through the manufacturing method of high purity maxine (1X 6116 ) of the above embodiment is hydrochloric acid (狀 1), lithium chloride (Ni): 1, lithium aluminum fluoride (Ni 必 1¾), or aluminum fluoride (Si¾). It can contain up to 5 wt% of by-products,
상술한 바와 같이， 상기 제조된 맥신 ）을 탄산염 또는 탄산수소염과반응시키는단계에서 발생하는 이산화탄소 기포로 인하여 정제 효율은보다향상될수있다.  As described above, the purification efficiency may be further improved due to the carbon dioxide bubbles generated in the step of reacting the prepared Maxine) with carbonate or hydrogen carbonate.
이에 따라, 상기 구현예의 고순도의 맥신 （ 0!½） 제조 방법은 상기 제조된 맥신 （ ^ 을 탄산염 또는 탄산수소염과 반응 시키는 단계 이후에， 물을사용하여 정제하는단계를포함할수있다. Accordingly, the high purity maxine ( 0! ½ ) manufacturing method of the above embodiment may include a step of purifying with water after the step of reacting the prepared maxine (^) with carbonate or hydrogen carbonate.
상술한 바와 같이， 상기 제조된 맥신 （ 에 을 탄산염 또는 탄산수소염과 반응 시키는 단계로 인하여 상기 사용되는 물의 양은 크게 줄어들 수 있으며, 상기 제조된 맥신 （炯 ）을 물을 사용하여 정제하는 단계에서는상기 제조된맥신 （歌에 100중량부대비 2000중량부이하， 또는 100내지 1000중량부의 물을사용하여 제거하는단계를포함할수있다.  As described above, the amount of water used may be greatly reduced due to the step of reacting the prepared maxine (e) with carbonate or hydrogen carbonate, and in the step of purifying the prepared maxine (炯) with water, the preparation May be removed using less than 2000 parts by weight or 100 to 1000 parts by weight of water.
상기 고순도의 맥신 （獻레 은 5.0 X 105 /미 이상의 전기 전도도를 가질수있다. The high purity Maxine (Chelene) can have an electrical conductivity of 5.0 X 10 5 / mi or more.
상기 제조된 고순도의 맥신 » 61½）은 이차전지용 양극 도전재, 또는 이차전지 등의 내부/외부전극으로사용가능하다. The manufactured high purity Maxine » 61½ ) can be used as an internal / external electrode of a cathode conductive material for a secondary battery or a secondary battery.
【발명의 효과】  【Effects of the Invention】
본 발명에 따르면, 보다 효율적으로 높은 순도 및 우수한 전기적 특성을갖는고순도의 맥신（ 을제조할수있는방법이 제공된다.  According to the present invention, there is provided a method for manufacturing a high purity maxine having high purity and excellent electrical properties more efficiently.
이와 같이 제공되는 고순도의 맥신은 우수한 전기 전도성을 이용하여 전자파 차폐 효과를 구현할 수 있으며， 이에 따라 내부 및 외부 전극 등 다양한산업 분야에 재료로서 용이하게 적용될수있다. The high-purity maxine provided as described above can realize electromagnetic shielding effect by using excellent electrical conductivity, and thus internal and external electrodes, etc. It can be easily applied as a material to various industrial fields.
【도면의 간단한설명】  【Brief Description of Drawings】
도 1은 실시예 1및 비교예 1 각각에서 제조된 맥신 (歌래 의 묘 이미지를나타낸것이다.  FIG. 1 shows Maxine (Original seedling images prepared in each of Example 1 and Comparative Example 1).
【발명을실시하기 위한구체적인내용】  [Specific contents for carrying out the invention]
발명의 구현예를 하기의 실시예에서 보다 상세하게 설명한다. 단, 하기의 실시예는발명의 구현예를예시하는것일뿐， 본발명의 내용이 하기의 실시예에 의하여 한정되는것은아니다. 실시예 1  Embodiments of the invention are described in more detail in the following examples. However, the following examples are merely to illustrate the embodiment of the invention, the content of the present invention is not limited by the following examples. Example 1
lg의 MAX phase (Ti3AlC2)를 lg의 불화리륨이 녹아있는 20 mL의 6 M HC1용액에 넣고 50 °C에서 24시간동안교반하였다. The lg MAX phase (Ti 3 AlC 2) was added to 20 mL of 6 M HC1 solution in which lg fluoride was dissolved and stirred at 50 ° C. for 24 hours.
상기 교반이후에 상온으로식힌후, 상기 용액에 첨가된 HC1 농도의 약 10 mol %에 해당하는 0.1 N 탄산 나트륨을 첨가하여 10분간 교반하였다. 그리고， 여액의 pH가중성이 될 때까지 물을사용하여 여과하고, Vacuum oven 에서 12시간건조한후맥신 (MXene)분말을얻었다. 비교예 1  After the stirring, the mixture was cooled to room temperature, and 0.1 N sodium carbonate corresponding to about 10 mol% of the concentration of HC1 added to the solution was added thereto, followed by stirring for 10 minutes. Then, the mixture was filtered using water until the pH of the filtrate was weighted, and dried for 12 hours in a vacuum oven to obtain MXene powder. Comparative Example 1
lg의 MAX phase (Ti3AlC2)를 lg의 불화리륨이 녹아있는 20 mL의 6 M HC1 용액에 넣고 50 °C에서 24시간동안 교반하였다. 그리고， 여액의 pH가 중성이 될 때까지 물을사용하여 여과하고， Vacuum oven에서 12시간 건조한 후맥신 (MXene)분말을얻었다. The lg MAX phase (Ti 3 AlC 2) was added to 20 mL of 6 M HC1 solution in which lgium fluoride was dissolved and stirred at 50 ° C. for 24 hours. Then, the mixture was filtered using water until the pH of the filtrate was neutral, and dried for 12 hours in a vacuum oven to obtain MXne powder.
［실험예］ [Experimental example]
1.실험예: 정제속도개선  Experimental Example: Improvement of Purification Speed
1용의 맥신 (歌 분말을 수득하기 위한 여과기를 통한 여과 시간을 비교함으로써 상기 실시예 및 비교예의
Figure imgf000007_0001
정제하는 속도를 확인하였다. Of the above Examples and Comparative Examples by comparing the filtration time through a filter for obtaining Maxine for 1
Figure imgf000007_0001
The rate of purification was confirmed.
2. ¾犯-2 크값 ｝（-대 회절기를통하여 상기 실시예 및 비교예의 맥신 » 61½）의 XI犯 2 -
Figure imgf000008_0001
으로써 층간거리를비교하였다. 2. ¾ 犯 -2 magnitude XI # 2 of Maxine » 61½ of the above Examples and Comparative Examples via -Diffractometer
Figure imgf000008_0001
The distance between the floors was compared.
3. 전기 전도도측정 3. Electrical conductivity measurement
4^01^ （止근를 통하여 상기 실시예 및 비교예의 맥신（11X6116）의 전기전도도를측정하였다. The electrical conductivity of the maxine (11X 6116 ) of the said Example and the comparative example was measured through 4 ^ 01 ^.
4.모폴로지 관찰 4. Observation of morphology
況 ¾!을 통하여 상기 실시예 및 비교예의 맥신（歌61½）의 모폴로지를 관찰하였고， 그결과실시예의 층간이 탄산염 또는탄산수소염에 의해 발생한 이산화탄소기포에 의해더 벌어진것을확인할수있었다. The morphology of the Maxine (歌61½ ) of the above Examples and Comparative Examples was observed through ¾ ¾ !, and as a result, it was confirmed that the interlayers of the examples were further opened by carbon dioxide bubbles generated by carbonate or hydrogen carbonate.
【표 1]실시예 1과 비교예 1에 의해 제조되어진 맥신（獻61½）의 정제 속도, 전기전도도， 그리고）®!） 2-比 3값비교
Figure imgf000008_0002
상기 표 1에 나타난 바와 같이， 실시예 1에서는 보다 짧은 시간 이내에 정제를완료하였음에도 얻어진 맥신이 갖는전기 전도도가높을뿐만아니라， XI犯 2- 3 값에서 확인되는층간거리도보다큰 것으로 확인되었다. 또한 정제 속도 차이 （5분 VI 10분）가 미미해 보이므로, 비교예 1의 정제 속도를 30분정도로하는것을추천함. [Table 1] Example 1 and Comparative purification rate, the electric conductivity of Maxine (獻61½) been prepared by Example 1, and a) ®!) 2-比3 value comparison
Figure imgf000008_0002
Example 1 was confirmed to be the greater as higher the electrical conductivity having a short time Maxine obtained though not completed the tablets within, than the distance between layers is also identified in the XI犯2- 3 value as shown in Table 1 above. In addition, since the purification rate difference (5 minutes VI 10 minutes) seems to be insignificant, it is recommended to set the purification speed of Comparative Example 1 to about 30 minutes.
또한， 도 1에 나타난 바와 같이， 실시예 1에서 얻어진 맥신이 비교예 1에서 얻어진 맥신에 비하여 층과 층 사이의 입자가 명확하게 구분이 되는점이 확인되었다.  In addition, as shown in FIG. 1, it was confirmed that the maxine obtained in Example 1 clearly distinguished the particles between layers as compared with the maxine obtained in Comparative Example 1.

Claims

2019/151636 1»（：1^1{2018/015469  2019/151636 1 »（： 1 ^ 1 {2018/015469
【청구범위】 [Claim]
【청구항 11  [Claim 11
맥스상（!¾ 336）을 강산과 반응시켜 맥신（1\0（6116）을 형성하는 단계; 및 Reacting the max phase (! ¾ 336 ) with a strong acid to form maxine (1 \ 0 ( 6116 )); And
상기 형성된 맥신을 탄산염 또는 탄산수소염과 반응 시키는 단계를 포함하는， 고순도의 맥신 （歌61½）제조방법 . A method for producing high purity maxine (歌61½ ) comprising the step of reacting the formed maxine with carbonate or hydrogen carbonate.
【청구항 2] [Claim 2]
제 1항에 있어서，  The method of claim 1,
상기 탄산염 또는 탄산수소염은 상기 강산의 0.1 11101 % 내지 25 1 %로사용되는, 고순도의 맥신 （¾61½）제조방법 . The carbonate or hydrogen carbonate salt is used in 0.1 1110 1% to 25 1% of the strong acid, high purity Maxine (¾ 61½ ) manufacturing method.
【청구항 3] [Claim 3]
제 1항에 있어서，  The method of claim 1,
상기 탄산염은또는탄산수소염은탄산나트륨， 탄산수소나트륨， 탄산 칼륨， 탄산수소 칼륨， 탄산 리륨, 탄산수소 리튬， 탄산 루비듐, 탄산 세슘， 탄산수소세슘, 탄산암모늄 및 탄산수소 암모늄으로 이루어진 군에서 선택된 1종이상을포함하는， 고순도의 맥신 （歌레 제조방법 .  The silver carbonate or the hydrogen carbonate is one selected from the group consisting of sodium carbonate, sodium bicarbonate, potassium carbonate, potassium bicarbonate, lithium carbonate, lithium bicarbonate, rubidium carbonate, cesium carbonate, cesium bicarbonate, ammonium carbonate and ammonium bicarbonate High purity maxine containing the above (Manure manufacturing method.
【청구항 4] [Claim 4]
제 1항에 있어서，  The method of claim 1,
상기 형성된 맥신을 탄산염 또는 탄산수소염과 반응 시키는 단계는 내지 8얘의 온도에서 수행되는， 고순도의 맥신 （歌61½）제조방법. The step of reacting the formed maxine with carbonate or hydrogen carbonate is carried out at a temperature of 8 to 8, high-purity maxine ( 61½ ) manufacturing method.
【청구항 5] [Claim 5]
제 1항에 있어서，  The method of claim 1,
상기 제조된 맥신 （淑에 중， 염산（狀1）， 염화 리튬（니（：1）， 불화 알루미늄 리튬（니3시¾） 또는 불화 알루미늄（시¾）을 포함한 부산물의 함량이 5중량%이하인， 고순도의 맥신 （ 제조방법 . 2019/151636 1»（：1^1{2018/015469 5% by weight or less of the by-products including the prepared Maxine (Hexane, hydrochloric acid (狀 1), lithium chloride (Ni (1)), lithium aluminum fluoride (Ni 3 ¾) or aluminum fluoride (ci ¾)) , Maxine of high purity). 2019/151636 1 »（： 1 ^ 1 {2018/015469
【청구항 6] [Claim 6]
제 1항에 있어서,  The method of claim 1,
상기 제조된 맥신 » 61½)을 탄산염 또는 탄산수소염과 반응 시키는 단계 이후에， After reacting the prepared Maxine » 61½) with carbonate or hydrogen carbonate,
상기 제조된 맥신 ( 61½) 100중량부 대비 2000 중량부 이하의 물을 사용하여 제거하는단계를더 포함하는， 고순도의 맥신 (¾1)(6116)제조방법 . Further comprising the step of removing using less than 2000 parts by weight of water compared to 100 parts by weight of the prepared maxine ( 61½) , high purity maxine (¾1) ( 6116) manufacturing method.
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CN114361570A (en) * 2022-01-11 2022-04-15 山东大学 Sodium battery and preparation method thereof
CN114361570B (en) * 2022-01-11 2023-09-01 山东大学 Sodium battery and preparation method thereof
CN114423269A (en) * 2022-01-24 2022-04-29 同济大学 Nitrogen-doped MXene @ HCF electromagnetic composite wave-absorbing material and preparation method thereof

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