JP6660776B2 - Method for producing tantalum nitride (Ta3N5) - Google Patents
Method for producing tantalum nitride (Ta3N5) Download PDFInfo
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- JP6660776B2 JP6660776B2 JP2016050360A JP2016050360A JP6660776B2 JP 6660776 B2 JP6660776 B2 JP 6660776B2 JP 2016050360 A JP2016050360 A JP 2016050360A JP 2016050360 A JP2016050360 A JP 2016050360A JP 6660776 B2 JP6660776 B2 JP 6660776B2
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- 238000004519 manufacturing process Methods 0.000 title claims description 9
- MZLGASXMSKOWSE-UHFFFAOYSA-N tantalum nitride Chemical compound [Ta]#N MZLGASXMSKOWSE-UHFFFAOYSA-N 0.000 title claims description 5
- 229910052751 metal Inorganic materials 0.000 claims description 24
- 239000002184 metal Substances 0.000 claims description 24
- 238000005121 nitriding Methods 0.000 claims description 19
- QGZKDVFQNNGYKY-UHFFFAOYSA-N Ammonia Chemical compound N QGZKDVFQNNGYKY-UHFFFAOYSA-N 0.000 claims description 18
- GUVRBAGPIYLISA-UHFFFAOYSA-N tantalum atom Chemical compound [Ta] GUVRBAGPIYLISA-UHFFFAOYSA-N 0.000 claims description 17
- 229910052715 tantalum Inorganic materials 0.000 claims description 12
- 239000002245 particle Substances 0.000 claims description 10
- 238000000034 method Methods 0.000 claims description 7
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 30
- 238000000634 powder X-ray diffraction Methods 0.000 description 22
- 238000004458 analytical method Methods 0.000 description 20
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 20
- 239000001301 oxygen Substances 0.000 description 20
- 229910052760 oxygen Inorganic materials 0.000 description 20
- 229910052757 nitrogen Inorganic materials 0.000 description 14
- 239000002131 composite material Substances 0.000 description 7
- ZMANZCXQSJIPKH-UHFFFAOYSA-N Triethylamine Chemical compound CCN(CC)CC ZMANZCXQSJIPKH-UHFFFAOYSA-N 0.000 description 6
- 230000000052 comparative effect Effects 0.000 description 6
- 239000002994 raw material Substances 0.000 description 6
- 238000010298 pulverizing process Methods 0.000 description 5
- 238000002441 X-ray diffraction Methods 0.000 description 4
- 150000004767 nitrides Chemical class 0.000 description 4
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 description 3
- 230000004907 flux Effects 0.000 description 3
- VLKZOEOYAKHREP-UHFFFAOYSA-N n-Hexane Chemical compound CCCCCC VLKZOEOYAKHREP-UHFFFAOYSA-N 0.000 description 3
- 239000000758 substrate Substances 0.000 description 3
- CURLTUGMZLYLDI-UHFFFAOYSA-N Carbon dioxide Chemical compound O=C=O CURLTUGMZLYLDI-UHFFFAOYSA-N 0.000 description 2
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 description 2
- FAPWRFPIFSIZLT-UHFFFAOYSA-M Sodium chloride Chemical compound [Na+].[Cl-] FAPWRFPIFSIZLT-UHFFFAOYSA-M 0.000 description 2
- MCMNRKCIXSYSNV-UHFFFAOYSA-N Zirconium dioxide Chemical compound O=[Zr]=O MCMNRKCIXSYSNV-UHFFFAOYSA-N 0.000 description 2
- 229910021529 ammonia Inorganic materials 0.000 description 2
- 239000007864 aqueous solution Substances 0.000 description 2
- 229910001873 dinitrogen Inorganic materials 0.000 description 2
- 238000000227 grinding Methods 0.000 description 2
- 239000001257 hydrogen Substances 0.000 description 2
- 229910052739 hydrogen Inorganic materials 0.000 description 2
- BPUBBGLMJRNUCC-UHFFFAOYSA-N oxygen(2-);tantalum(5+) Chemical compound [O-2].[O-2].[O-2].[O-2].[O-2].[Ta+5].[Ta+5] BPUBBGLMJRNUCC-UHFFFAOYSA-N 0.000 description 2
- 239000011941 photocatalyst Substances 0.000 description 2
- 239000007858 starting material Substances 0.000 description 2
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 2
- QGZKDVFQNNGYKY-UHFFFAOYSA-O Ammonium Chemical compound [NH4+] QGZKDVFQNNGYKY-UHFFFAOYSA-O 0.000 description 1
- 229910001111 Fine metal Inorganic materials 0.000 description 1
- XUIMIQQOPSSXEZ-UHFFFAOYSA-N Silicon Chemical compound [Si] XUIMIQQOPSSXEZ-UHFFFAOYSA-N 0.000 description 1
- 229910002092 carbon dioxide Inorganic materials 0.000 description 1
- 239000001569 carbon dioxide Substances 0.000 description 1
- 238000001816 cooling Methods 0.000 description 1
- 238000009826 distribution Methods 0.000 description 1
- 238000001035 drying Methods 0.000 description 1
- 238000005516 engineering process Methods 0.000 description 1
- 239000010419 fine particle Substances 0.000 description 1
- 239000007789 gas Substances 0.000 description 1
- 238000005259 measurement Methods 0.000 description 1
- 239000000203 mixture Substances 0.000 description 1
- 230000001699 photocatalysis Effects 0.000 description 1
- 239000000843 powder Substances 0.000 description 1
- 230000035484 reaction time Effects 0.000 description 1
- 230000002940 repellent Effects 0.000 description 1
- 239000005871 repellent Substances 0.000 description 1
- 229910052710 silicon Inorganic materials 0.000 description 1
- 239000010703 silicon Substances 0.000 description 1
- 239000011780 sodium chloride Substances 0.000 description 1
- 239000002887 superconductor Substances 0.000 description 1
- OEIMLTQPLAGXMX-UHFFFAOYSA-I tantalum(v) chloride Chemical compound Cl[Ta](Cl)(Cl)(Cl)Cl OEIMLTQPLAGXMX-UHFFFAOYSA-I 0.000 description 1
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Description
本発明は、Ｔａ3Ｎ5の製造方法に関する。 The present invention relates to a method for producing Ta 3 N 5 .
Ｔａ3Ｎ5は、誘電体や超電導体などとして使用される金属窒化物である。さらに、近年では炭酸ガス排出削減、再生可能エネルギーの観点から、太陽光エネルギーを利用して、光触媒により水を分解して、水素や酸素を製造する技術に注目が集まっており、Ｔａ3Ｎ5は光触媒として利用可能である。
一方で、光触媒に含まれる酸素は忌避成分となり、水素の発生を阻害する。そこで、酸素を含まない高純度のＴａ3Ｎ5が求められている。
Ta 3 N 5 is a metal nitride used as a dielectric or a superconductor. Furthermore, carbon dioxide emissions in recent years, from the viewpoint of renewable energy by utilizing solar energy, and by the photocatalytic decomposing water, and attention is paid to a technology for producing hydrogen and oxygen, Ta 3 N 5 Can be used as a photocatalyst.
On the other hand, oxygen contained in the photocatalyst becomes a repellent component and inhibits generation of hydrogen. Therefore, high-purity Ta 3 N 5 containing no oxygen is required.
非特許文献１では、塩化タンタル（ＴａＣｌ5）を液体アンモニアで処理し、得られたＴａ（ＮＨ2）2Ｃｌ3を、アンモニア気流中で６５０〜７５０℃で分解することでＴａ3Ｎ5が得られている。特許文献１では、酸化タンタル（Ｔａ2Ｏ5）をアンモニア気流中、８５０℃で２５時間窒化することでＴａ3Ｎ5が得られている。
また特許文献２では、Ｔａ基板を用い、真空紫外光を照射して親水化した後、フラックス水溶液（ＮａＣｌとＮａ2ＣＯ3がモル比で４：１）を塗布し、１００℃で乾燥させ、乾燥後、Ｔａ基板をアンモニア気流中８５０℃、１時間加熱した。その後、アンモニア気流中で３００℃まで、３００℃から室温まで窒素気流中で冷却した。冷却後、残存するフラックスを温水中で除去することでＴａ3Ｎ5を得ている。さらに、特許文献３では、タンタル金属を窒素ガスによって窒化タンタルを製造する方法が開示されている。一次窒化として、窒化炉にタンタル金属を仕込み、炉内温度を６００〜８００℃になるように窒素流量を制御しながら窒化を行っている。得られた窒化物の窒素含有量は６．１％であった。得られた窒化物は１５００℃で二次窒化し、窒素含有量は７．１％となっている。
In Non-Patent Document 1, Ta 3 N 5 is obtained by treating tantalum chloride (TaCl 5 ) with liquid ammonia and decomposing the obtained Ta (NH 2 ) 2 Cl 3 at 650 to 750 ° C. in an ammonia gas flow. Have been obtained. In Patent Document 1, Ta 3 N 5 is obtained by nitriding tantalum oxide (Ta 2 O 5 ) at 850 ° C. for 25 hours in an ammonia gas flow.
Further, in Patent Document 2, a Ta substrate is used to irradiate it with vacuum ultraviolet light to make it hydrophilic, and then a flux aqueous solution (NaCl and Na 2 CO 3 at a molar ratio of 4: 1) is applied and dried at 100 ° C. After drying, the Ta substrate was heated at 850 ° C. for 1 hour in an ammonia stream. Thereafter, the mixture was cooled to 300 ° C. in an ammonia gas flow and from 300 ° C. to room temperature in a nitrogen gas flow. After cooling, the remaining flux is removed in warm water to obtain Ta 3 N 5 . Further, Patent Document 3 discloses a method for producing tantalum nitride from tantalum metal using nitrogen gas. As primary nitriding, tantalum metal is charged into a nitriding furnace, and nitriding is performed while controlling the flow rate of nitrogen so that the temperature in the furnace becomes 600 to 800 ° C. The nitrogen content of the obtained nitride was 6.1%. The obtained nitride was subjected to secondary nitriding at 1500 ° C., and the nitrogen content was 7.1%.
しかしながら、非特許文献１記載の方法では、７５０℃で６日間もの長時間を要する。特許文献１記載の方法では、酸化物を原料とするため、Ｔａ3Ｎ5中に酸素が残ってしまう。特許文献２記載の方法では、工程数が長く工業的ではなく、親水化しフラックス水溶液を塗布させることで、Ｔａ基板を酸化させＴａ2Ｏ5としている。また、特許文献３で得られる窒化物はＴａＮであり、Ｔａ3Ｎ5ではない。 However, the method described in Non-Patent Document 1 requires as long as 6 days at 750 ° C. In the method described in Patent Document 1, oxygen is used as a raw material, so that oxygen remains in Ta 3 N 5 . In the method described in Patent Document 2, the number of steps is long and not industrial, and the Ta substrate is oxidized to Ta 2 O 5 by applying a flux aqueous solution after hydrophilization. The nitride obtained in Patent Document 3 is TaN, not Ta 3 N 5 .
従って、本発明の課題は、酸素含有量の少ないＴａ3Ｎ5の工業的な製造方法を提供することにある。 Therefore, an object of the present invention is to provide an industrial method for producing Ta 3 N 5 having a low oxygen content.
そこで本発明者は、前記課題を解決すべく検討した結果、酸素量の少ない金属タンタルを原料とし、特定の温度範囲で、アンモニアガスで窒化すれば、酸素量の少ない高純度のＴａ3Ｎ5が得られることを見出し、本発明を完成した。 The present inventor has studied to solve the above problem, and as a result, using a metal tantalum having a low oxygen content as a raw material and nitriding with ammonia gas in a specific temperature range, a high-purity Ta 3 N 5 having a low oxygen content is obtained. Were obtained, and the present invention was completed.
すなわち、本発明は、次の〔１〕〜〔３〕を提供するものである。 That is, the present invention provides the following [1] to [3].
〔１〕金属タンタルを８００〜９５０℃で、アンモニアガス下窒化することを特徴とする窒化タンタル（Ｔａ3Ｎ5）の製造方法。
〔２〕アンモニアガス流量が金属タンタル１ｇに対して０．０３Ｌ／ｍｉｎ以上０．５Ｌ／ｍｉｎ以下で窒化する〔１〕記載の製造方法。
〔３〕用いる金属タンタルが、最大粒子径が５０μｍ以下になるように粉砕されたものである〔１〕又は〔２〕記載の製造方法。
[1] A method for producing tantalum nitride (Ta 3 N 5 ), comprising nitriding metal tantalum at 800 to 950 ° C. under ammonia gas.
[2] The production method according to [1], wherein the nitriding is performed at an ammonia gas flow rate of 0.03 L / min or more and 0.5 L / min or less per 1 g of metal tantalum.
[3] The production method according to [1] or [2], wherein the metal tantalum used is pulverized so that the maximum particle size is 50 μm or less.
本発明方法によれば、高純度で酸素量の少ないＴａ3Ｎ5が工業的に有利に製造できる。 According to the method of the present invention, Ta 3 N 5 having high purity and a small amount of oxygen can be industrially advantageously produced.
本発明のＴａ3Ｎ5の製造方法は、金属タンタルを８００〜９５０℃で、アンモニアガス下窒化することを特徴とする。 The method for producing Ta 3 N 5 according to the present invention is characterized in that metal tantalum is nitrided at 800 to 950 ° C. under ammonia gas.
本発明に用いる原料は、金属タンタルである。金属タンタルは、細かい粒子を用いるのが窒化温度を低くできる点から好ましく、金属タンタルの最大粒子径は５０μｍ以下が好ましく、３０μｍ以下がより好ましく、２０μｍ以下がさらに好ましく、１０μｍ以下がさらに好ましい。また、平均粒子径（Ｄ50）が２０μｍ以下のものを用いるのが好ましく、１５μｍ以下がより好ましく、１０μｍ以下がさらに好ましく、５μｍ以下がさらに好ましい。 The raw material used in the present invention is metal tantalum. It is preferable to use fine particles of metal tantalum from the viewpoint that the nitriding temperature can be lowered, and the maximum particle diameter of metal tantalum is preferably 50 μm or less, more preferably 30 μm or less, further preferably 20 μm or less, and still more preferably 10 μm or less. Further, it is preferable to use those having an average particle diameter (D 50 ) of 20 μm or less, more preferably 15 μm or less, further preferably 10 μm or less, and still more preferably 5 μm or less.
このような微細化金属タンタルは、市販の金属タンタルを粉砕することにより得られる。粉砕装置としては遊星ボールミル、振動ミル、アトライターミル等を用いることが可能である。粉砕方法は、乾式または湿式のどちらでも良い。湿式の場合の粉砕助剤としては、エタノール、トリエチルアミン、ヘキサン等が利用できる。
粉砕時間は、１０分以上２時間以下が好ましく、さらに好ましくは２０分以上１時間以下である。
Such fine metal tantalum is obtained by pulverizing commercially available metal tantalum. As a pulverizing device, a planetary ball mill, a vibration mill, an attritor mill, or the like can be used. The pulverization method may be either dry or wet. Ethanol, triethylamine, hexane and the like can be used as a grinding aid in the case of a wet method.
The grinding time is preferably from 10 minutes to 2 hours, more preferably from 20 minutes to 1 hour.
窒化する温度（窒化温度）は、８００℃以上９５０℃以下が好ましい。８００℃以下の場合、窒化が進行しない。９５０℃以上の場合、Ｔａ3Ｎ5から窒素が放出され金属Ｔａとなるため高純度のＴａ3Ｎ5が得られない。 The nitriding temperature (nitriding temperature) is preferably 800 ° C. or more and 950 ° C. or less. If the temperature is lower than 800 ° C., nitriding does not proceed. When the temperature is 950 ° C. or higher, high-purity Ta 3 N 5 cannot be obtained because nitrogen is released from Ta 3 N 5 to become metal Ta.
窒化する際のアンモニア流量は、単相のＴａ3Ｎ5を得る点、アンモニウムガスの過剰使用を防止する点から、原料の金属タンタル１ｇに対し０．０３Ｌ／ｍｉｎ以上０．５Ｌ／ｍｉｎ以下が好ましい。さらに好ましくは、原料の金属Ｔａ １ｇに対し０．０５Ｌ／ｍｉｎ以上０．３Ｌ／ｍｉｎ以下である。 From the viewpoint of obtaining single-phase Ta 3 N 5 and preventing excessive use of ammonium gas, the ammonia flow rate during nitriding is preferably 0.03 L / min or more and 0.5 L / min or less per 1 g of metal tantalum as a raw material. preferable. More preferably, it is 0.05 L / min or more and 0.3 L / min or less with respect to 1 g of metal Ta as a raw material.
反応装置は、１０００℃程度の熱に耐えられる装置であればよく、例えば、管状炉、電気炉、バッチ式キルン、ロータリーキルンを用いれば良い。反応時間は、１０時間以上４８時間以下が好ましく１５時間以上３０時間以下がさらに好ましい。 The reaction apparatus may be an apparatus that can withstand heat of about 1000 ° C., and for example, a tubular furnace, an electric furnace, a batch kiln, and a rotary kiln may be used. The reaction time is preferably from 10 hours to 48 hours, more preferably from 15 hours to 30 hours.
上記の反応により、反応容器中には高純度Ｔａ3Ｎ5のみが残存するので回収が容易である。得られるＴａ3Ｎ5の純度は９０％以上であり、９５％以上であるのがより好ましい。また、得られるＴａ3Ｎ5中の酸素量は１．０ｍａｓｓ％以下であるのが好ましく、０．７ｍａｓｓ％以下であるのがより好ましい。 Due to the above reaction, only high-purity Ta 3 N 5 remains in the reaction vessel, so that it is easy to recover. The purity of the obtained Ta 3 N 5 is 90% or more, and more preferably 95% or more. Further, the amount of oxygen in the obtained Ta 3 N 5 is preferably 1.0 mass% or less, more preferably 0.7 mass% or less.
次に実施例を挙げて本発明を詳細に説明する。 Next, the present invention will be described in detail with reference to examples.
実施例１
グローブボックス内にて炉心管（内径５０ｍｍ、長さ６００ｍｍ）に金属Ｔａ３ｇを入れ、シリコンキャップで密閉した。グローブボックスから取り出した炉心管を管状炉にセットした。その後、アンモニアガスを１Ｌ／ｍｉｎ雰囲気下で、反応温度９００℃、２０時間で窒化した。原料の金属Ｔａの最大粒子径は４７．８μｍ、Ｄ５０は１４．９μｍであった。
得られた合成物の粉末ＸＲＤ解析を行ったところ単相のＴａ３Ｎ５であった（図１）。得られたＴａ3Ｎ5を窒素酸素同時分析計で定量したところ、Ｎ量は１１．２ｍａｓｓ％であり理論量（１１．４３ｍａｓｓ％）から算出した純度は９８．０％であった。また、Ｏ量は０．５ｍａｓｓ％と低かった。得られた合成物の最大粒子径は２９．９μｍ、Ｄ５０は９．８μｍであった。
Example 1
In a glove box, 3 g of metal Ta was put into a core tube (
Powder XRD analysis of the obtained synthesized product showed single-phase Ta 3 N 5 (FIG. 1). When the obtained Ta 3 N 5 was quantified by a nitrogen and oxygen simultaneous analyzer, the N amount was 11.2 mass%, and the purity calculated from the theoretical amount (11.43 mass%) was 98.0%. Further, the O content was as low as 0.5 mass%. Maximum particle size of the resulting composite is 29.9μm, D 50 was 9.8 .mu.m.
実施例２
反応温度を８５０℃とした以外は、実施例１と同様の操作を行った。
得られた合成物の粉末ＸＲＤ解析を行ったところ単相のＴａ3Ｎ5であった（図２）。得られたＴａ3Ｎ5を窒素酸素同時分析計で定量したところ、Ｎ量は１１．０ｍａｓｓ％であり理論量（１１．４３ｍａｓｓ％）から算出した純度は９６．２％であった。また、Ｏ量は０．６ｍａｓｓ％と低かった。
Example 2
The same operation as in Example 1 was performed except that the reaction temperature was 850 ° C.
XRD analysis of the obtained composite product by powder XRD showed that it was a single-phase Ta 3 N 5 (FIG. 2). When the obtained Ta 3 N 5 was quantified by a nitrogen and oxygen simultaneous analyzer, the N amount was 11.0 mass%, and the purity calculated from the theoretical amount (11.43 mass%) was 96.2%. Also, the O content was as low as 0.6 mass%.
実施例３
窒化時間を３０時間とした以外は、実施例２と同様の操作を行った。
得られた合成物の粉末ＸＲＤ解析を行ったところ単相のＴａ３Ｎ５であった（図３）。
得られたＴａ３Ｎ５を窒素酸素同時分析計で定量したところ、Ｎ量は１１．２ｍａｓｓ％であり理論量（１１．４３ｍａｓｓ％）から算出した純度は９８．０％であった。また、Ｏ量は０．４ｍａｓｓ％と低かった。
Example 3
The same operation as in Example 2 was performed except that the nitriding time was changed to 30 hours.
The obtained composite was subjected to powder XRD analysis, and was found to be single-phase Ta 3 N 5 (FIG. 3).
When the obtained Ta 3 N 5 was quantified with a nitrogen and oxygen simultaneous analyzer, the N amount was 11.2 mass%, and the purity calculated from the theoretical amount (11.43 mass%) was 98.0%. Also, the O content was as low as 0.4 mass%.
実施例４
窒化時間を１０時間とした以外は、実施例２と同様の操作を行った。
得られた合成物の粉末ＸＲＤ解析を行ったところ単相のＴａ３Ｎ５であった（図４）。得られたＴａ３Ｎ５を窒素酸素同時分析計で定量したところ、Ｎ量は１０．９ｍａｓｓ％であり理論量（１１．４３ｍａｓｓ％）から算出した純度は９５．４％であった。また、Ｏ量は０．７ｍａｓｓ％と低かった。
Example 4
The same operation as in Example 2 was performed except that the nitriding time was changed to 10 hours.
Powder XRD analysis of the obtained composite showed single-phase Ta 3 N 5 (FIG. 4). When the obtained Ta 3 N 5 was quantified by a nitrogen and oxygen simultaneous analyzer, the N amount was 10.9 mass%, and the purity calculated from the theoretical amount (11.43 mass%) was 95.4%. Further, the O content was as low as 0.7 mass%.
実施例５
窒化時間を４８時間とした以外は、実施例２と同様の操作を行った。
得られた合成物の粉末ＸＲＤ解析を行ったところ単相のＴａ３Ｎ５であった（図５）。
得られたＴａ３Ｎ５を窒素酸素同時分析計で定量したところ、Ｎ量は１１．１ｍａｓｓ％であり理論量（１１．４３ｍａｓｓ％）から算出した純度は９７．１％であった。またＯ量は０．６ｍａｓｓ％と低かった。
Example 5
The same operation as in Example 2 was performed except that the nitriding time was changed to 48 hours.
Powder XRD analysis of the obtained synthesized product showed single-phase Ta 3 N 5 (FIG. 5).
When the obtained Ta 3 N 5 was quantified with a nitrogen and oxygen simultaneous analyzer, the N amount was 11.1 mass%, and the purity calculated from the theoretical amount (11.43 mass%) was 97.1%. The O content was as low as 0.6 mass%.
実施例６
金属Ｔａ１０ｇにアンモニアガスを０．３Ｌ／ｍｉｎとした以外は、実施例１と同様の操作を行った。
得られた合成物の粉末ＸＲＤ解析を行ったところ単相のＴａ3Ｎ5であった（図６）。得られたＴａ3Ｎ5を窒素酸素同時分析計で定量したところ、Ｎ量は１１．０ｍａｓｓ％であり理論量（１１．４３ｍａｓｓ％）から算出した純度は９６．２％であった。また、Ｏ量は０．６ｍａｓｓ％と低かった。
Example 6
The same operation as in Example 1 was performed, except that 10 g of metal Ta was changed to 0.3 L / min of ammonia gas.
Powder XRD analysis of the obtained synthesized product showed single-phase Ta 3 N 5 (FIG. 6). When the obtained Ta 3 N 5 was quantified by a nitrogen and oxygen simultaneous analyzer, the N amount was 11.0 mass%, and the purity calculated from the theoretical amount (11.43 mass%) was 96.2%. Also, the O content was as low as 0.6 mass%.
実施例７
金属Ｔａ１０ｇにアンモニアガスを３Ｌ／ｍｉｎとした以外は、実施例１と同様の操作を行った。
得られた合成物の粉末ＸＲＤ解析を行ったところ単相のＴａ3Ｎ5であった（図７）。得られたＴａ3Ｎ5を窒素酸素同時分析計で定量したところ、Ｎ量は１１．１ｍａｓｓ％であり理論量（１１．４３ｍａｓｓ％）から算出した純度は９７．１％であった。また、Ｏ量は０．５ｍａｓｓ％と低かった。
Example 7
The same operation as in Example 1 was performed, except that ammonia gas was changed to 3 L / min for 10 g of metal Ta.
The obtained composite was subjected to powder XRD analysis, and was found to be single-phase Ta 3 N 5 (FIG. 7). When the obtained Ta 3 N 5 was quantified by a nitrogen and oxygen simultaneous analyzer, the N amount was 11.1 mass%, and the purity calculated from the theoretical amount (11.43 mass%) was 97.1%. Further, the O content was as low as 0.5 mass%.
実施例８
金属Ｔａ１０ｇにアンモニアガス流量を、５Ｌ／ｍｉｎとした以外は、実施例１と同様の操作を行った。
得られた合成物の粉末ＸＲＤ解析を行ったところ単相のＴａ3Ｎ5であった（図８）。得られたＴａ3Ｎ5を窒素酸素同時分析計で定量したところ、Ｎ量は１１．２ｍａｓｓ％であり理論量（１１．４３ｍａｓｓ％）から算出した純度は９８．０％であった。また、Ｏ量は０．７ｍａｓｓ％と低かった。
Example 8
The same operation as in Example 1 was performed, except that the flow rate of ammonia gas was set to 5 L / min for 10 g of metal Ta.
XRD analysis of the obtained synthesized product showed single-phase Ta 3 N 5 (FIG. 8). When the obtained Ta 3 N 5 was quantified by a nitrogen and oxygen simultaneous analyzer, the N amount was 11.2 mass%, and the purity calculated from the theoretical amount (11.43 mass%) was 98.0%. Further, the O content was as low as 0.7 mass%.
実施例９
グローブボックス内にて金属Ｔａ１０ｇをジルコニア製粉砕容器（５００ｍＬ）に仕込み、粉砕助剤としてトリエチルアミンを数滴入れ、遊星ボールミル装置にて３５０ｒｐｍ、３０分粉砕した。粉砕した金属Ｔａはグローブボックス内で取り出した。粉砕した金属Ｔａの粒度は粒子径分布測定装置で測定したところ、最大粒子径は８．０μｍ、Ｄ５０は２．３μｍであった。
粉砕した金属Ｔａを出発原料として、反応温度８００℃以外は、実施例１と同様の操作を行った。
得られた合成物の粉末ＸＲＤ解析を行ったところ単相のＴａ3Ｎ5であった（図９）。得られたＴａ３Ｎ５を窒素酸素同時分析計で定量したところ、Ｎ量は１１．３ｍａｓｓ％であり理論量（１１．４３ｍａｓｓ％）から算出した純度は９８．９％であった。また、Ｏ量は０．５ｍａｓｓ％と低かった。得られた合成物の最大粒子径は１６．０μｍ、Ｄ５０は４．５μｍであった。
Example 9
In a glove box, 10 g of metal Ta was charged into a pulverizing container (500 mL) made of zirconia, and several drops of triethylamine were added as a pulverizing aid, and pulverized by a planetary ball mill at 350 rpm for 30 minutes. The crushed metal Ta was taken out in the glove box. The particle size of the milled metal Ta is as measured by particle size distribution measurement device, a maximum particle size 8.0 .mu.m, D 50 was 2.3 .mu.m.
The same operation as in Example 1 was performed using pulverized metal Ta as a starting material except for the reaction temperature of 800 ° C.
Powder XRD analysis of the obtained synthesized product showed single-phase Ta 3 N 5 (FIG. 9). When the obtained Ta 3 N 5 was quantified by a nitrogen and oxygen simultaneous analyzer, the N amount was 11.3 mass%, and the purity calculated from the theoretical amount (11.43 mass%) was 98.9%. Further, the O content was as low as 0.5 mass%. Maximum particle size of the resulting composite is 16.0 .mu.m, D 50 was 4.5 [mu] m.
比較例１
反応温度を７００℃とした以外は、実施例１と同様の操作を行った。
得られた合成物の粉末ＸＲＤ解析を行ったところ金属のＴａであった（図１０）。
Comparative Example 1
The same operation as in Example 1 was performed except that the reaction temperature was 700 ° C.
XRD analysis of the obtained composite product by powder XRD showed metallic Ta (FIG. 10).
比較例２
反応温度を１０００℃とした以外は、実施例１と同様の操作を行った。
得られた合成物の粉末ＸＲＤ解析を行ったところＴａ3Ｎ5と金属Ｔａの混合相であった（図１１）。
Comparative Example 2
The same operation as in Example 1 was performed except that the reaction temperature was changed to 1000 ° C.
XRD analysis of the powder of the obtained synthesized product showed a mixed phase of Ta 3 N 5 and metal Ta (FIG. 11).
比較例３
出発原料を酸化タンタル（Ｔａ2Ｏ5）とした以外は、実施例１と同様の操作を行った。
得られた合成物の粉末ＸＲＤ解析を行ったところ単相のＴａ3Ｎ5であった（図１２）。得られたＴａ3Ｎ5を窒素酸素同時分析計で定量したところ、Ｎ量は１１．３ｍａｓｓ％であり理論量（１１．４３ｍａｓｓ％）から算出した純度は９８．９％であった。しかし、Ｏ量は１．１ｍａｓｓ％と高かった。
Comparative Example 3
The same operation as in Example 1 was performed except that the starting material was tantalum oxide (Ta 2 O 5 ).
Powder XRD analysis of the obtained synthesized product showed single-phase Ta 3 N 5 (FIG. 12). When the obtained Ta 3 N 5 was quantified by a nitrogen and oxygen simultaneous analyzer, the N amount was 11.3 mass%, and the purity calculated from the theoretical amount (11.43 mass%) was 98.9%. However, the O content was as high as 1.1 mass%.
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