JP2017164732A - METHOD FOR PRODUCING TANTALUM NITRIDE (Ta3 N5) - Google Patents
METHOD FOR PRODUCING TANTALUM NITRIDE (Ta3 N5) Download PDFInfo
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- JP2017164732A JP2017164732A JP2016156366A JP2016156366A JP2017164732A JP 2017164732 A JP2017164732 A JP 2017164732A JP 2016156366 A JP2016156366 A JP 2016156366A JP 2016156366 A JP2016156366 A JP 2016156366A JP 2017164732 A JP2017164732 A JP 2017164732A
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- MZLGASXMSKOWSE-UHFFFAOYSA-N tantalum nitride Chemical compound [Ta]#N MZLGASXMSKOWSE-UHFFFAOYSA-N 0.000 title claims abstract description 13
- 238000004519 manufacturing process Methods 0.000 title claims abstract description 11
- QGZKDVFQNNGYKY-UHFFFAOYSA-N Ammonia Chemical compound N QGZKDVFQNNGYKY-UHFFFAOYSA-N 0.000 claims abstract description 40
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 claims abstract description 31
- 239000001301 oxygen Substances 0.000 claims abstract description 31
- 229910052760 oxygen Inorganic materials 0.000 claims abstract description 31
- 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 claims abstract description 6
- 238000010438 heat treatment Methods 0.000 claims description 13
- 150000004767 nitrides Chemical class 0.000 claims description 6
- 238000005121 nitriding Methods 0.000 abstract description 11
- 238000000034 method Methods 0.000 abstract description 6
- 229910001936 tantalum oxide Inorganic materials 0.000 abstract description 2
- 238000009776 industrial production Methods 0.000 abstract 1
- JMOHEPRYPIIZQU-UHFFFAOYSA-N oxygen(2-);tantalum(2+) Chemical compound [O-2].[Ta+2] JMOHEPRYPIIZQU-UHFFFAOYSA-N 0.000 abstract 1
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 26
- 238000004458 analytical method Methods 0.000 description 20
- 238000000634 powder X-ray diffraction Methods 0.000 description 20
- 238000006243 chemical reaction Methods 0.000 description 14
- 229910052757 nitrogen Inorganic materials 0.000 description 13
- 230000000052 comparative effect Effects 0.000 description 12
- 239000002131 composite material Substances 0.000 description 12
- DOTMOQHOJINYBL-UHFFFAOYSA-N molecular nitrogen;molecular oxygen Chemical compound N#N.O=O DOTMOQHOJINYBL-UHFFFAOYSA-N 0.000 description 10
- 229910021529 ammonia Inorganic materials 0.000 description 7
- 239000011941 photocatalyst Substances 0.000 description 6
- 238000010521 absorption reaction Methods 0.000 description 4
- 238000000862 absorption spectrum Methods 0.000 description 4
- 230000004907 flux Effects 0.000 description 4
- 229910003071 TaON Inorganic materials 0.000 description 3
- 239000007864 aqueous solution Substances 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
- 150000001875 compounds Chemical class 0.000 description 2
- 239000001257 hydrogen Substances 0.000 description 2
- 229910052739 hydrogen Inorganic materials 0.000 description 2
- 229910052751 metal Inorganic materials 0.000 description 2
- 239000002184 metal Substances 0.000 description 2
- 239000002994 raw material Substances 0.000 description 2
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 2
- 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
- 230000003197 catalytic effect Effects 0.000 description 1
- 238000001816 cooling Methods 0.000 description 1
- 238000001035 drying Methods 0.000 description 1
- 238000005516 engineering process Methods 0.000 description 1
- 230000000802 nitrating effect Effects 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
- 239000007858 starting material 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
- 238000000870 ultraviolet spectroscopy Methods 0.000 description 1
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Abstract
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（特許文献１）。
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, in recent years, from the viewpoint of reducing carbon dioxide emissions and renewable energy, attention has been focused on technology for producing hydrogen and oxygen by using solar energy to decompose water using a photocatalyst. Ta 3 N 5 Can be used as a photocatalyst (Patent Document 1).
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が得られる旨記載されている。
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。
In Non-Patent Document 1, tantalum chloride (TaCl 5 ) is treated with liquid ammonia, and the resulting Ta (NH 2 ) 2 Cl 3 is decomposed at 650 to 750 ° C. in an ammonia stream to obtain Ta 3 N 5. Has been obtained. Patent Document 1 describes that Ta 3 N 5 can be obtained by nitriding tantalum oxide (Ta 2 O 5 ) in an ammonia stream at 850 ° C. for 25 hours.
In Patent Document 2, a Ta substrate is used and hydrophilicized by irradiation with vacuum ultraviolet light, and then a flux aqueous solution (NaCl and Na 2 CO 3 in a molar ratio of 4: 1) is applied and dried at 100 ° C., After drying, the Ta substrate was heated in an ammonia stream at 850 ° C. for 1 hour. Then, it cooled in the nitrogen stream from 300 degreeC to room temperature in the ammonia stream. After cooling, Ta 3 N 5 is obtained by removing the remaining flux in warm water.
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１記載の方法を追試したところ、酸素量が多く、純度が低いことが判明した。 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 2, the Ta substrate is oxidized to Ta 2 O 5 by applying a flux aqueous solution by making it hydrophilic and applying a flux aqueous solution because the number of steps is long and not industrial. Further, when the method described in Patent Document 1 was further tested, it was found that the amount of oxygen was large and the purity was low.
従って、本発明の課題は、酸素含有量が少なく、かつ単相のＴａ3Ｎ5の工業的な製造方法を提供することにある。 Accordingly, an object of the present invention is to provide an industrial process for producing single-phase Ta 3 N 5 with 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、タンタル酸化物（Ｔａ2Ｏ5）を出発原料として用い、８００〜９５０℃という特定の温度で一定の流量のアンモニアガスを反応させることにより、酸素量が少なく、かつ単相のＴａ3Ｎ5が選択的に得られることを見出した。また、得られた酸素含有量の少ないＴａ3Ｎ5が、従来のＴａ3Ｎ5とは異なり、６２０〜７５０ｎｍという可視光を吸収するものであることも見出した。 Therefore, as a result of studies to solve the above problems, the present inventor uses tantalum oxide (Ta 2 O 5 ) as a starting material, and reacts ammonia gas at a constant flow rate at a specific temperature of 800 to 950 ° C. Thus, it was found that a small amount of oxygen and single phase Ta 3 N 5 can be selectively obtained. It was also found that the obtained Ta 3 N 5 with a low oxygen content absorbs visible light of 620 to 750 nm, unlike the conventional Ta 3 N 5 .
すなわち、本発明は、次の〔１〕〜〔６〕を提供するものである。 That is, the present invention provides the following [1] to [6].
〔１〕タンタル酸化物（Ｔａ2Ｏ5）を８００〜９５０℃で、アンモニアガス雰囲気下で、アンモニアガス流量が、Ｔａ2Ｏ5 １ｇあたり０．０５〜０．８Ｌ／ｍｉｎで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〕加熱温度（℃）と加熱時間（ｈｒ）の積が１００００〜２５０００になる時間、アンモニアガス雰囲気下で窒化する〔１〕記載の製造方法。
〔３〕窒化タンタル（Ｔａ3Ｎ5）の酸素含有量が１ｍａｓｓ％以下である〔１〕又は〔２〕記載の製造方法。
〔４〕６２０〜７５０ｎｍの波長の可視光を吸収する窒化タンタル（Ｔａ3Ｎ5）。
〔５〕酸素含有量が１ｍａｓｓ％以下である〔４〕記載の窒化タンタル（Ｔａ3Ｎ5）。
〔６〕純度が９０％以上である〔４〕又は〔５〕記載の窒化タンタル（Ｔａ3Ｎ5）。
[1] Nitrating tantalum oxide (Ta 2 O 5 ) at 800 to 950 ° C. in an ammonia gas atmosphere at an ammonia gas flow rate of 0.05 to 0.8 L / min per 1 g of Ta 2 O 5. A method for producing tantalum nitride (Ta 3 N 5 ), which is characterized.
[2] The production method according to [1], wherein nitriding is performed in an ammonia gas atmosphere for a time in which the product of the heating temperature (° C.) and the heating time (hr) is 10,000 to 25,000.
[3] The method according to [1] or [2], wherein the oxygen content of tantalum nitride (Ta 3 N 5 ) is 1 mass% or less.
[4] Tantalum nitride (Ta 3 N 5 ) that absorbs visible light having a wavelength of 620 to 750 nm.
[5] The tantalum nitride (Ta 3 N 5 ) according to [4], wherein the oxygen content is 1 mass% or less.
[6] The tantalum nitride (Ta 3 N 5 ) according to [4] or [5], wherein the purity is 90% or more.
本発明方法によれば、酸素量が少なく高純度のＴａ3Ｎ5が工業的に有利に製造できる。また、本発明の６２０〜７５０ｎｍの波長の可視光を吸収するＴａ3Ｎ5は、酸素含有量が少なく高純度であり、可視光で触媒作用を有する光触媒として有用である。 According to the method of the present invention, Ta 3 N 5 having a small amount of oxygen and high purity can be produced industrially advantageously. In addition, Ta 3 N 5 that absorbs visible light having a wavelength of 620 to 750 nm according to the present invention has a low oxygen content and high purity, and is useful as a photocatalyst having catalytic action with visible light.
本発明のＴａ3Ｎ5の製造方法は、Ｔａ2Ｏ5を８００〜９５０℃で、アンモニアガス雰囲気下で、アンモニアガス流量が、Ｔａ2Ｏ5 １ｇあたり０．０５〜０．８Ｌ／ｍｉｎで窒化することを特徴とする。 In the method for producing Ta 3 N 5 of the present invention, Ta 2 O 5 is 800 to 950 ° C. in an ammonia gas atmosphere, and the ammonia gas flow rate is 0.05 to 0.8 L / min per 1 g of Ta 2 O 5. It is characterized by nitriding.
本発明に用いる原料は、Ｔａ2Ｏ5である。このようなタンタル酸化物を原料として用いるにもかかわらず、本発明においては、アンモニアガスとの反応温度及びアンモニアガスの流量を調整することにより、高純度で酸素含有量の少ないＴａ3Ｎ5が得られる。 The raw material used in the present invention is Ta 2 O 5 . Despite the use of such a tantalum oxide as a raw material, in the present invention, Ta 3 N 5 having high purity and low oxygen content can be obtained by adjusting the reaction temperature with ammonia gas and the flow rate of ammonia gas. can get.
窒化する際のアンモニアガス量は、Ｔａ2Ｏ5 １ｇあたり０．０５Ｌ／ｍｉｎ以上０．８Ｌ／ｍｉｎ以下が好ましい。さらに好ましくは、０．１Ｌ／ｍｉｎ以上０．５Ｌ／ｍｉｎ以下である。０．０５Ｌ／ｍｉｎ未満だと窒化時間が長く、工業的ではない。０．８Ｌ／ｍｉｎ超だと、得られるＴａ3Ｎ5の酸素含有量が高くなる場合がある。また、窒化に使用されないアンモニアガス量が多くなり、製造コストが高くなる。 The amount of ammonia gas during nitriding is preferably 0.05 L / min or more and 0.8 L / min or less per gram of Ta 2 O 5 . More preferably, it is 0.1 L / min or more and 0.5 L / min or less. If it is less than 0.05 L / min, the nitriding time is long and not industrial. If it exceeds 0.8 L / min, the oxygen content of the obtained Ta 3 N 5 may be high. In addition, the amount of ammonia gas that is not used for nitriding increases, and the manufacturing cost increases.
窒化する温度（加熱温度）は、８００℃以上９５０℃以下である。８００℃未満の場合、窒化が十分に進行しない。９５０℃超の場合、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。より好ましい窒化温度は、８００℃以上９００℃以下である。 The nitriding temperature (heating temperature) is 800 ° C. or higher and 950 ° C. or lower. When the temperature is less than 800 ° C., nitriding does not proceed sufficiently. When the temperature is higher than 950 ° C., nitrogen is released from Ta 3 N 5 and becomes metal Ta, so that high-purity Ta 3 N 5 cannot be obtained. A more preferable nitriding temperature is 800 ° C. or higher and 900 ° C. or lower.
また、加熱時間は、加熱温度との関係で決定され、加熱温度（℃）と加熱時間（ｈｒ）の積が、１００００〜２５０００になる時間が好ましい。この加熱時間が１００００未満の場合には、窒化が十分に進行しないおそれがある。一方、２５０００を超えると、Ｔａ3Ｎ5より窒素量の少ないタンタル窒化物が生成してしまうおそれがある。より好ましい前記積は１２０００〜２００００であり、さらに好ましくは１６０００〜２００００である。
具体的な加熱時間は１３時間以上３０時間以下が好ましく、１５時間以上３０時間以下がより好ましい。なお、ここで加熱時間は、８００〜９５０℃の範囲に加熱されている時間である。
Further, the heating time is determined in relation to the heating temperature, and the time when the product of the heating temperature (° C.) and the heating time (hr) is 10000 to 25000 is preferable. If the heating time is less than 10,000, nitriding may not proceed sufficiently. On the other hand, if it exceeds 25000, tantalum nitride having a smaller amount of nitrogen than Ta 3 N 5 may be produced. More preferably, the product is 12000 to 20000, and more preferably 16000 to 20000.
The specific heating time is preferably 13 hours or longer and 30 hours or shorter, and more preferably 15 hours or longer and 30 hours or shorter. Here, the heating time is a time during which heating is performed in a range of 800 to 950 ° C.
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。 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, or a rotary kiln may be used.
上記の反応により、反応容器中には高純度の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％以上が好ましく、９５％以上であるのがより好ましい。また、得られるＴａ3Ｎ5中の酸素含有量は１ｍａｓｓ％以下が好ましく、０．８５ｍａｓｓ％以下であるのがより好ましい。 By the above reaction, only high-purity Ta 3 N 5 remains in the reaction vessel, so that it can be easily recovered. The purity of Ta 3 N 5 obtained is preferably 90% or more, and more preferably 95% or more. Further, the oxygen content in the obtained Ta 3 N 5 is preferably 1 mass% or less, and more preferably 0.85 mass% or less.
得られたＴａ3Ｎ5の吸収スペクトルを測定したところ、６２０〜７５０ｎｍの波長の可視光を吸収することが判明した。光触媒として有用であることが報告されている特許文献１記載のＴａ3Ｎ5の吸収波長は紫外部から６２０ｎｍまでである。従って、本発明の６２０〜７５０ｎｍの波長の可視光を吸収するＴａ3Ｎ5は、新規なＴａ3Ｎ5であり、可視光を利用できる光触媒として有用である。
また、本発明のＴａ3Ｎ5としては、最大吸収波長が５５０〜７００ｎｍにあるのが好ましく、６００〜７００ｎｍにあるのがより好ましく、６２０〜７００ｎｍにあるのがさらに好ましく、６２０〜６８０ｎｍにあるのが特に好ましい。
When the absorption spectrum of the obtained Ta 3 N 5 was measured, it was found that visible light having a wavelength of 620 to 750 nm was absorbed. The absorption wavelength of Ta 3 N 5 described in Patent Document 1 reported to be useful as a photocatalyst is from the ultraviolet region to 620 nm. Therefore, Ta 3 N 5 that absorbs visible light having a wavelength of 620 to 750 nm according to the present invention is a novel Ta 3 N 5 and is useful as a photocatalyst that can use visible light.
Further, the Ta 3 N 5 of the present invention preferably has a maximum absorption wavelength of 550 to 700 nm, more preferably 600 to 700 nm, further preferably 620 to 700 nm, and more preferably 620 to 680 nm. Is particularly preferred.
本発明のＴａ3Ｎ5の吸収波長は、酸素含有量の低下及び純度の高度化とともに長波長側にシフトする傾向にあり、酸素含有量及び純度が高いことが好ましい。従って、Ｔａ3Ｎ5の純度は９０％以上が好ましく、９５％以上であるのがより好ましい。また、Ｔａ3Ｎ5中の酸素含有量は１ｍａｓｓ％以下が好ましく、０．８５ｍａｓｓ％以下であるのがより好ましい。 The absorption wavelength of Ta 3 N 5 of the present invention tends to shift to a longer wavelength side with a decrease in oxygen content and an increase in purity, and preferably has a high oxygen content and purity. Therefore, the purity of Ta 3 N 5 is preferably 90% or more, and more preferably 95% or more. Further, the oxygen content in Ta 3 N 5 is preferably 1 mass% or less, and more preferably 0.85 mass% or less.
次に実施例を挙げて、本発明を詳細に説明する。 EXAMPLES Next, an Example is given and this invention is demonstrated in detail.
実施例１
グローブボックス内にて炉心管（内径５０ｍｍ、長さ６００ｍｍ）に酸化物（Ｔａ2Ｏ5）５ｇ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（Ｔａ2Ｏ5 １ｇあたり０．２Ｌ／ｍｉｎ）雰囲気下で、反応温度８５０℃、２０時間で窒化した。
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、酸素含有量は０．７６ｍａｓｓ％と低く、窒素含有量は１１．４１ｍａｓｓ％であり、理論量（１１．４３ｍａｓｓ％）から算出した純度は９９．８％であった。
Example 1
In a glove box, 5 g of oxide (Ta 2 O 5 ) was placed in a core tube (
The resulting composite single phase and by performing powder XRD analysis of a Ta 3 N 5 (Fig. 1). When the obtained Ta 3 N 5 was quantified with a nitrogen-oxygen simultaneous analyzer, the oxygen content was as low as 0.76 mass% and the nitrogen content was 11.41 mass%, which was calculated from the theoretical amount (11.43 mass%). The purity obtained was 99.8%.
実施例２
アンモニアガス量をＴａ2Ｏ5仕込み量１ｇに対し、０．５Ｌ／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２）。得られたＴａ3Ｎ5を窒素酸素同時分析計で定量したところ、酸素含有量は０．５９ｍａｓｓ％と低く、窒素含有量は１０．６５ｍａｓｓ％であり、理論量（１１．４３ｍａｓｓ％）から算出した純度は９３．２％であった。
Example 2
The same operation as in Example 1 was performed except that the ammonia gas amount was 0.5 L / min with respect to 1 g of the charged amount of Ta 2 O 5 .
The resulting composite single phase and by performing powder XRD analysis of a Ta 3 N 5 (Fig. 2). When the obtained Ta 3 N 5 was quantified with a nitrogen-oxygen simultaneous analyzer, the oxygen content was as low as 0.59 mass%, the nitrogen content was 10.65 mass%, and was calculated from the theoretical amount (11.43 mass%). The purity was 93.2%.
実施例３
仕込み量を１０ｇとした以外は、実施例１と同様の操作（アンモニアガスをＴａ2Ｏ5 １ｇあたり０．１Ｌ／ｍｉｎ）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、酸素含有量は０．６６ｍａｓｓ％と低く、窒素含有量は１１．４０ｍａｓｓ％であり、理論量（１１．４３ｍａｓｓ％）から算出した純度は９９．７％であった。
Example 3
The same operation as in Example 1 (ammonia gas was 0.1 L / min per 1 g of Ta 2 O 5 ) except that the amount charged was 10 g.
The resulting composite single phase and by performing powder XRD analysis of a Ta 3 N 5 (Figure 3). When the obtained Ta 3 N 5 was quantified with a nitrogen-oxygen simultaneous analyzer, the oxygen content was as low as 0.66 mass% and the nitrogen content was 11.40 mass%, which was calculated from the theoretical amount (11.43 mass%). The purity was 99.7%.
実施例４
反応温度を９００℃とした以外は、実施例１と同様の操作（アンモニアガスをＴａ2Ｏ5 １ｇあたり０．２Ｌ／ｍｉｎ）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、酸素含有量は０．８４ｍａｓｓ％と低く、窒素含有量は１０．８８ｍａｓｓ％であり、理論量（１１．４３ｍａｓｓ％）から算出した純度は９５．２％であった。
Example 4
The same operation as in Example 1 was performed except that the reaction temperature was 900 ° C. (ammonia gas was 0.2 L / min per 1 g of Ta 2 O 5 ).
The resulting composite single phase and by performing powder XRD analysis of a Ta 3 N 5 (Fig. 4). When the obtained Ta 3 N 5 was quantified with a nitrogen-oxygen simultaneous analyzer, the oxygen content was as low as 0.84 mass% and the nitrogen content was 10.88 mass%, which was calculated from the theoretical amount (11.43 mass%). The purity obtained was 95.2%.
実施例５
反応温度を８００℃とし、実施例１と同様の操作（アンモニアガスをＴａ2Ｏ5 １ｇあたり０．２Ｌ／ｍｉｎ）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であった（図５）。得られた合成物を窒素酸素同時分析計で定量したところ、酸素含有量は０．９８ｍａｓｓ％と低く、窒素含有量は１０．４１ｍａｓｓ％であり、理論量（１１．４３ｍａｓｓ％）から算出した純度は９１．１％であった。
Example 5
The reaction temperature was set to 800 ° C., and the same operation as in Example 1 (ammonia gas was 0.2 L / min per 1 g of Ta 2 O 5 ) was performed. The resulting compound was Ta 3 N 5 where the powder XRD analysis was performed (Fig. 5). When the obtained composite was quantified with a nitrogen-oxygen simultaneous analyzer, the oxygen content was as low as 0.98 mass%, the nitrogen content was 10.41 mass%, and the purity calculated from the theoretical amount (11.43 mass%) Was 91.1%.
比較例１
反応温度を７５０℃とした以外は、実施例１と同様の操作（アンモニアガスをＴａ2Ｏ5 １ｇあたり０．２Ｌ／ｍｉｎ）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ＴａＯＮとＴａ2Ｏ5の混合相であった（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、酸素含有量は３．８９ｍａｓｓ％と高く、窒素含有量は８．９９ｍａｓｓ％であった。
Comparative Example 1
The same operation as in Example 1 was performed except that the reaction temperature was 750 ° C. (ammonia gas was 0.2 L / min per 1 g of Ta 2 O 5 ).
The resulting compound was a mixed phase of Ta 3 where a powder XRD analysis was carried out of N 5 and TaON and Ta 2 O 5 (Fig. 6). When the obtained Ta 3 N 5 was quantified with a nitrogen-oxygen simultaneous analyzer, the oxygen content was as high as 3.89 mass% and the nitrogen content was 8.9 mass%.
比較例２
反応温度を８５０℃とし、（アンモニア量は仕込み量１ｇに対し、０．０３Ｌ／ｍｉｎ）とし、それ以外は実施例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ＴａＯＮの混合相であった（図７）。得られた合成物を窒素酸素同時分析計で定量したところ、酸素含有量は４．６３ｍａｓｓ％、窒素含有量は９．３５ｍａｓｓ％であった。
Comparative Example 2
The reaction temperature was 850 ° C. (the amount of ammonia was 0.03 L / min with respect to 1 g of the charged amount), and the other operations were performed in the same manner as in Example 1.
When the powder XRD analysis of the obtained composite was conducted, it was a mixed phase of Ta 3 N 5 and TaON (FIG. 7). When the obtained composite was quantified with a nitrogen-oxygen simultaneous analyzer, the oxygen content was 4.63 mass% and the nitrogen content was 9.35 mass%.
比較例３（特開２００２−２３３７６９号公報の追試）
酸化物（Ｔａ2Ｏ5）１ｇを入れ、仕込み量１ｇに対してアンモニアガスを１．０Ｌ／ｍｉｎ雰囲気下で、反応温度８５０℃、２５時間で窒化した。得られた合成物の粉末ＸＲＤ解析を行ったところＴａ3Ｎ5とＴａＯＮの混合相であった（図８）。得られた合成物を窒素酸素同時分析計で定量したところ、酸素含有量は５．８３ｍａｓｓ％、窒素含有量は１０．０１ｍａｓｓ％であった。
Comparative Example 3 (Additional Examination of JP 2002-233769 A)
1 g of oxide (Ta 2 O 5 ) was added, and ammonia gas was nitrided at a reaction temperature of 850 ° C. for 25 hours in an atmosphere of 1.0 L / min with respect to the charged amount of 1 g. When the powder XRD analysis of the obtained composite was performed, it was a mixed phase of Ta 3 N 5 and TaON (FIG. 8). When the obtained composite was quantified with a nitrogen-oxygen simultaneous analyzer, the oxygen content was 5.83 mass% and the nitrogen content was 10.01 mass%.
比較例４
反応温度を１０００℃とし、アンモニア量をＴａ2Ｏ5仕込み量１ｇに対し、０．１Ｌ／ｍｉｎとする以外は、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、Ｔａ窒化物の混合相であった（図９）。得られた合成物を窒素酸素同時分析計で定量したところ、酸素含有量は３．３３ｍａｓｓ％、窒素含有量は１０．００ｍａｓｓ％であった。
Comparative Example 4
The same operation as in Example 1 was performed except that the reaction temperature was 1000 ° C. and the ammonia amount was 0.1 L / min with respect to 1 g of the charged amount of Ta 2 O 5 .
When the powder XRD analysis of the obtained composite was performed, it was a mixed phase of Ta nitride (FIG. 9). When the obtained synthesized product was quantified with a nitrogen-oxygen simultaneous analyzer, the oxygen content was 3.33 mass% and the nitrogen content was 10.00 mass%.
比較例５
反応時間を３５時間とし、アンモニア量をＴａ2Ｏ5仕込み量１ｇに対し、０．１Ｌ／ｍｉｎとする以外は、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、Ｔａ窒化物の混合相であった（図１０）。得られた合成物を窒素酸素同時分析計で定量したところ、酸素含有量は２．６７ｍａｓｓ％、窒素含有量は１０．８０ｍａｓｓ％であった。
Comparative Example 5
The same operation as in Example 1 was performed except that the reaction time was 35 hours and the ammonia amount was 0.1 L / min with respect to 1 g of the charged amount of Ta 2 O 5 .
When the powder XRD analysis of the obtained composite was performed, it was a mixed phase of Ta nitride (FIG. 10). When the obtained composite was quantified with a nitrogen-oxygen simultaneous analyzer, the oxygen content was 2.67 mass% and the nitrogen content was 10.80 mass%.
実施例１〜５より、Ｔａ2Ｏ5を８００〜９５０℃の温度で、アンモニアガスの量がＴａ2Ｏ5 １ｇあたり０．０５〜０．８Ｌ／ｍｉｎでアンモニアガスを反応させた場合、酸素含有量の少ない高純度のＴａ3Ｎ5が得られる。一方、反応温度が低い（７５０℃）比較例１では反応が十分に進行しなかった。また、反応温度が高い（１０００℃）比較例４では、Ｔａ窒化物ではあるがＴａ3Ｎ5以外の窒化物が混入していた。アンモニアガスの量がＴａ2Ｏ5 １ｇあたり０．０５〜０．８Ｌ／ｍｉｎの範囲外の場合は、高純度のＴａ3Ｎ5が得られなかった。 From Examples 1 to 5, when Ta 2 O 5 was reacted with ammonia gas at a temperature of 800 to 950 ° C. and an ammonia gas amount of 0.05 to 0.8 L / min per gram of Ta 2 O 5 , oxygen High purity Ta 3 N 5 with a low content is obtained. On the other hand, in Comparative Example 1 where the reaction temperature was low (750 ° C.), the reaction did not proceed sufficiently. In Comparative Example 4 where the reaction temperature was high (1000 ° C.), nitrides other than Ta 3 N 5 were mixed although they were Ta nitrides. When the amount of ammonia gas was outside the range of 0.05 to 0.8 L / min per gram of Ta 2 O 5 , high-purity Ta 3 N 5 could not be obtained.
実施例６
実施例１〜５で得られたＴａ3Ｎ5の吸収スペクトルを、紫外可視分光光度計を用いて測定した。実施例１のＴａ3Ｎ5の吸収スペクトルを図１１に示す。その結果、実施例１〜５で得られたＴａ3Ｎ5は６２０〜７５０ｎｍの波長の可視光を吸収することが判明した。最大吸収波長と純度との関係を表１に示す。
Example 6
The absorption spectra of Ta 3 N 5 obtained in Examples 1 to 5 were measured using an ultraviolet-visible spectrophotometer. The absorption spectrum of Ta 3 N 5 of Example 1 is shown in FIG. As a result, it was found that Ta 3 N 5 obtained in Examples 1 to 5 absorbs visible light having a wavelength of 620 to 750 nm. Table 1 shows the relationship between the maximum absorption wavelength and purity.
Claims (6)
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| JP2019155270A (en) * | 2018-03-13 | 2019-09-19 | 太平洋セメント株式会社 | photocatalyst |
| CN113634266A (en) * | 2021-07-05 | 2021-11-12 | 宁波工程学院 | ReS2Ta loaded by ultrathin nanosheets3N5Hollow nanosphere composite material and application thereof |
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| JP2019155270A (en) * | 2018-03-13 | 2019-09-19 | 太平洋セメント株式会社 | photocatalyst |
| JP7005394B2 (en) | 2018-03-13 | 2022-01-21 | 太平洋セメント株式会社 | photocatalyst |
| JP7058151B2 (en) | 2018-03-13 | 2022-04-21 | 太平洋セメント株式会社 | Tantalum nitride crystal |
| CN113634266A (en) * | 2021-07-05 | 2021-11-12 | 宁波工程学院 | ReS2Ta loaded by ultrathin nanosheets3N5Hollow nanosphere composite material and application thereof |
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