JPH0611642B2 - Layered metal chalcogenide host material - Google Patents
Layered metal chalcogenide host materialInfo
- Publication number
- JPH0611642B2 JPH0611642B2 JP1061856A JP6185689A JPH0611642B2 JP H0611642 B2 JPH0611642 B2 JP H0611642B2 JP 1061856 A JP1061856 A JP 1061856A JP 6185689 A JP6185689 A JP 6185689A JP H0611642 B2 JPH0611642 B2 JP H0611642B2
- Authority
- JP
- Japan
- Prior art keywords
- element selected
- host material
- host
- metal chalcogenide
- layered
- Prior art date
- Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
- Expired - Lifetime
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Classifications
-
- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B19/00—Selenium; Tellurium; Compounds thereof
- C01B19/002—Compounds containing, besides selenium or tellurium, more than one other element, with -O- and -OH not being considered as anions
-
- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B17/00—Sulfur; Compounds thereof
- C01B17/20—Methods for preparing sulfides or polysulfides, in general
-
- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01P—INDEXING SCHEME RELATING TO STRUCTURAL AND PHYSICAL ASPECTS OF SOLID INORGANIC COMPOUNDS
- C01P2002/00—Crystal-structural characteristics
- C01P2002/20—Two-dimensional structures
- C01P2002/22—Two-dimensional structures layered hydroxide-type, e.g. of the hydrotalcite-type
Landscapes
- Chemical & Material Sciences (AREA)
- Organic Chemistry (AREA)
- Inorganic Chemistry (AREA)
- Inorganic Compounds Of Heavy Metals (AREA)
- Glass Compositions (AREA)
- Compositions Of Oxide Ceramics (AREA)
Description
【発明の詳細な説明】 〔技術分野〕 本発明は分子レベルの層構造を有し、層間に分子やイオ
ンを取り込む金属カルコゲナイド・ホスト材料に関する
ものである。Description: TECHNICAL FIELD The present invention relates to a metal chalcogenide host material having a layer structure at a molecular level and incorporating molecules and ions between layers.
層状、鎖状あるいはトンネル構造を持ちそれらの分子レ
ベルの空隙にゲスト（分子やイオン）を取り込むことが
できる物質ホストはゲストの取り込み（インターカレー
ション）や取り出し（デインターカレーション）に伴う
変化を利用して、表示材料、電池の正負極活物質、イオ
ン伝導材料等としての幅広い用途を持っている。層状構
造を持つ金属カルコゲナイドとしてはＭＸ２（Ｍ＝金
属、Ｘ＝カルコゲン）という組成で表わされるダイカル
コゲナイドが有名であり、前述した用途が期待されてい
る。A substance host that has a layered structure, a chain structure, or a tunnel structure and is capable of incorporating a guest (molecule or ion) into the voids at the molecular level is subject to changes due to the incorporation (intercalation) or removal (deintercalation) of the guest. It has a wide range of uses as a display material, a positive and negative electrode active material for batteries, and an ion conductive material. As a metal chalcogenide having a layered structure, a dichalcogenide represented by a composition of MX 2 (M = metal, X = chalcogen) is famous, and the above-mentioned applications are expected.
一方金属二種以上を含む多元系の層状金属カルコゲナイ
ド・ホスト材料は、構造や物性がダイカルコゲナイドよ
りも多様で表示材料、電池の正負極活物質、イオン伝導
材料あるいはその母構造形成材料として優れた機能を発
揮する可能性がある。On the other hand, multi-layered layered metal chalcogenide / host materials containing two or more metals are more excellent in structure and physical properties than dichalcogenide and are excellent as display materials, positive / negative active materials for batteries, ion conductive materials, or materials for forming their mother structure. May function.
そこで本発明は金属を２種以上含む新規な層状金属カル
コゲナイド・ホスト材料を提供することをその課題とす
る。Therefore, it is an object of the present invention to provide a novel layered metal chalcogenide host material containing two or more metals.
本発明者は、前記課題を解決すべく種々研究を重ねた結
果、本発明を完成するに至った。The present inventors have completed the present invention as a result of various studies to solve the above problems.
即ち、本発明によれば、下記一般式（Ｉ）〜（IV）で表
わされる組成を有する層状金属カルコゲナイトからな
り、その層状の空隙に対し、分子及びイオンから選ばれ
たゲストの取り込み及び取り出しを行う、ホストとして
用いることを特徴とする新規な層状金属カルコゲナイド
・ホスト材料が提供される。これらのものは基本的に同
一の結晶構造を有するものである。That is, according to the present invention, it is composed of a layered metal chalcogenite having a composition represented by the following general formulas (I) to (IV), and a guest selected from molecules and ions can be taken in and taken out from the layered voids. Provided is a novel layered metal chalcogenide host material characterized by being used as a host. These have basically the same crystal structure.
一般式（Ｉ） ＡｘＢｙＣｚ （式中、ＡはＢｉ、Ｓｂ及びＡｓの中から選ばれる少な
くとも１種の元素、ＢはＴｉ、Ｖ、Ｎｂ及びＴａの中か
ら選ばれる少なくとも１種の元素及びＣはＳ、Ｓｅ及び
Ｔｅの中から選ばれる少なくとも１種の元素を示し、ｘ
は０．８≦ｘ≦１．２の数、ｙは１．６≦ｙ≦２．４の
数及びｚは４．０≦ｚ≦６．０の数を示す） 一般式（II） ＡｘＢｙＣｚ （式中、ＡはＰｂ、Ｓｎ及びＧｅの中から選ばれる少な
くとも１種の元素、ＢはＴｉ、Ｖ、Ｎｂ及びＴａの中か
ら選ばれる少なくとも１種の元素及びＣはＳ、Ｓｅ及び
Ｔｅの中から選ばれる少なくとも１種の元素を示し、ｘ
は０．８≦ｘ≦１．２の数、ｙは１．６≦ｙ≦２．４の
数及びｚは４．０≦ｚ≦６．０の数を示す） 一般式（III） ＡｘＢｙＣｚ （式中、Ａは希土類元素の中から選ばれる少なくとも１
種の元素、ＢはＴｉ、Ｚｒ、Ｈｆ、Ｖ、Ｎｂ、Ｔａ、Ｃ
ｒ、Ｍｏ及びＷの中から選ばれる少なくとも１種の元素
及びＣはＳ、Ｓｅ及びＴｅの中から選ばれる少なくとも
１種の元素を示し、ｘは０．８≦ｘ≦１．２の数、ｙは
１．６≦ｙ≦２．４の数及びｚは４．０≦ｚ≦６．０の
数を示す） 一般式（IV） ＡｘＢｙＣｚ （式中、ＡはＢｉ、Ｓｂ、Ａｓ、Ｐｂ、Ｓｎ、Ｇｅ、及
び希土類元素の中から選ばれる少なくとも１種の元素、
ＢはＴｉ、Ｚｒ、Ｈｆ、Ｖ、Ｎｂ、Ｔａ、Ｃｒ、Ｍｏ及
びＷの中から選ばれる少なくとも１種の元素、ＣはＳ、
Ｓｅ及びＴｅの中から選ばれる少なくとも１種の元素を
示し、ｘは０．８≦ｘ≦１．２の数、ｙは１．６≦ｙ≦
２．４の数及びｚは４．０≦ｚ≦６．０の数を示す） 本発明の層状金属カルコゲナイド・ホスト材料は、前記
組成に対応する成分の元素粉末あるいは金属カルコゲナ
イド粉末を、その組成割合に秤取して、石英等の耐熱耐
酸化性容器中に真空封入し、４００〜１２００℃で加熱
処理した後室温まで冷却することによって製造すること
ができる。General formula (I) AxByCz (In the formula, A is at least one element selected from Bi, Sb, and As, B is at least one element selected from Ti, V, Nb, and Ta, and C is Represents at least one element selected from S, Se and Te, x
Is a number of 0.8 ≦ x ≦ 1.2, y is a number of 1.6 ≦ y ≦ 2.4, and z is a number of 4.0 ≦ z ≦ 6.0.) General formula (II) AxByCz ( In the formula, A is at least one element selected from Pb, Sn, and Ge, B is at least one element selected from Ti, V, Nb, and Ta, and C is S, Se, and Te. X represents at least one element selected from
Is a number of 0.8 ≦ x ≦ 1.2, y is a number of 1.6 ≦ y ≦ 2.4, and z is a number of 4.0 ≦ z ≦ 6.0.) General formula (III) AxByCz ( In the formula, A is at least 1 selected from rare earth elements
Seed element, B is Ti, Zr, Hf, V, Nb, Ta, C
At least one element selected from r, Mo and W and C represents at least one element selected from S, Se and Te, and x is a number of 0.8 ≦ x ≦ 1.2, y represents a number of 1.6 ≦ y ≦ 2.4 and z represents a number of 4.0 ≦ z ≦ 6.0) General formula (IV) AxByCz (where A is Bi, Sb, As, Pb, At least one element selected from Sn, Ge, and rare earth elements,
B is at least one element selected from Ti, Zr, Hf, V, Nb, Ta, Cr, Mo and W, C is S,
At least one element selected from Se and Te is shown, x is a number of 0.8 ≦ x ≦ 1.2, and y is 1.6 ≦ y ≦.
The number of 2.4 and z indicate the number of 4.0 ≦ z ≦ 6.0) The layered metal chalcogenide host material of the present invention comprises an elemental powder or a metal chalcogenide powder of a component corresponding to the above composition. It can be manufactured by weighing in proportions, vacuum-sealed in a heat-resistant and oxidation-resistant container such as quartz, heat-treated at 400 to 1200 ° C., and then cooled to room temperature.
このようにして得られたものは、褐色から黒色の粉末
で、粉末Ｘ線回折パターンが殆ど１つの面からの回折線
のみを示す。また条件によっては薄片状結晶が得られ、
それが容易に劈開することとあわせ、何らかの層状構造
を持つと推定される。本発明の金属カルコゲナイドの場
合、成分Ａ、Ｂ、Ｃをそれぞれ一定の範囲で複合化（固
溶化）させることが可能である。本発明のホスト材料は
種々の分子又はイオンをその層状の空隙に対し取り込む
のに使用され、また適宜条件下で取り出しが行われ、各
種の機能材料のホスト材料として用いられる。The product thus obtained is a brown to black powder, and the powder X-ray diffraction pattern shows only the diffraction line from almost one plane. Depending on the conditions, flaky crystals can be obtained,
It is presumed that it has some kind of layered structure along with the fact that it is easily cleaved. In the case of the metal chalcogenide of the present invention, the components A, B and C can be compounded (solubilized) within a certain range. The host material of the present invention is used as a host material for various functional materials by incorporating various molecules or ions into the voids of the layered structure and by performing extraction under appropriate conditions.
本発明の層状金属カルコゲナイド・ホスト材料は、層間
に分子やイオンを取り込むことができ、それを利用して
表示材料、Ｌｉ電池の正負極活物質、イオン伝導材料あ
るいはその母構造形成材料として用いられると期待され
る。The layered metal chalcogenide host material of the present invention can incorporate molecules and ions between layers, and by utilizing it, it is used as a display material, a positive and negative electrode active material of a Li battery, an ion conductive material or a material for forming a mother structure thereof. Is expected.
次に本発明を実施例によりさらに詳細に説明する。 Next, the present invention will be described in more detail with reference to Examples.
実施例１ 前記一般式（Ｉ）の組成に対応する層状金属カルコゲナ
イド・ホスト材料ＢｉＮｂ２Ｓｅ５を次のようにして合
成した。Example 1 A layered metal chalcogenide / host material BiNb 2 Se 5 corresponding to the composition of the general formula (I) was synthesized as follows.
Ｂｉ、Ｎｂ、Ｓｅをモル比で１：２：５に秤取し石英管
中に真空封入した後４００〜１２００℃の温度に加熱
し、次いで室温まで冷却した。石英管を開けて生成物を
粉砕し、粉末Ｘ線回折を測定すると主たる回折パターン
は面間隔１８．５Åを持つ面からの回折線およびその高
次回折線として帰属できた。一方この物質をヒドラジン
水和物に加え、一夜撹拌した後、別し粉末Ｘ線回折を
測定すると主たる回折パターンは、面間隔２２．３Åを
持つ面からの回折線およびその高次回折線として帰属さ
れた。処理前後の面間隔の伸び３．８Åは、ダイカルコ
ゲナイドであるＮｂＳｅ２の層間にヒドラジンが取り込
まれた場合の伸び３．３Åとほぼ一致する。それ故Ｂｉ
Ｎｂ２Ｓｅ５は他の物質を取り込むことのできる層間を
持つ層状金属カルコゲナイド・ホスト材料であることが
明らかとなった。Bi, Nb, and Se were weighed in a molar ratio of 1: 2: 5, vacuum-sealed in a quartz tube, heated to a temperature of 400 to 1200 ° C., and then cooled to room temperature. When the product was crushed by opening the quartz tube and the powder X-ray diffraction was measured, the main diffraction pattern could be assigned as a diffraction line from a plane having a face spacing of 18.5Å and its higher-order diffraction lines. On the other hand, when this substance was added to hydrazine hydrate, stirred overnight, and separated and powder X-ray diffraction was measured, the main diffraction patterns were attributed to the diffraction lines from the plane with a face spacing of 22.3Å and its higher diffraction lines. It was The elongation 3.8 Å of the interplanar spacing before and after the treatment is almost the same as the elongation 3.3 Å when hydrazine is incorporated between the layers of NbSe 2 which is a dichalcogenide. Hence Bi
It has been revealed that Nb 2 Se 5 is a layered metal chalcogenide host material having an interlayer capable of incorporating other substances.
実施例２ 実施例１と同様の方法で一般式（II）の組成を持つＰｂ
Ｔｉ２Ｓ５を合成した。粉末Ｘ線回折により測定した面
間隔はヒドラジン水和物処理前１７．４Åから処理後の
２１．４Åへと４．０Å伸長した。この値はＴｉＳ２の
層間にヒドラジンが取り込まれた場合の伸び３．９Åに
良く一致する。それ故ＰｂＴｉ２Ｓ５は他の物質を取り
込むことのできる層間を持つ層状金属カルコゲナイド・
ホスト材料であることが明らかとなった。Example 2 Pb having the composition of general formula (II) was prepared in the same manner as in Example 1.
Ti 2 S 5 was synthesized. The interplanar spacing measured by powder X-ray diffraction was extended from 17.4 Å before hydrazine hydrate treatment to 21.4 Å after treatment by 4.0 Å. This value is in good agreement with the elongation of 3.9Å when hydrazine is incorporated between the layers of TiS 2 . Therefore, PbTi 2 S 5 is a layered metal chalcogenide with an interlayer that can incorporate other substances.
It became clear that it was a host material.
実施例３ 実施例１と同様の方法で一般式（III）の組成を持つＬ
ａＮｂ２Ｓ５を合成した。粉末Ｘ線回折により測定した
面間隔はヒドラジン水和物処理前１７．３Åから処理後
の２０．５Åへと３．２Å伸長した。この値はＮｂＳ２
の層間にヒドラジンが取り込まれた場合の伸び２．９Å
に良く一致する。それ故ＬａＮｂ２Ｓ５は他の物質を取
り込むことのできる層間を持つ層状金属カルコゲナイド
・ホスト材料であることが明らかとなった。Example 3 In the same manner as in Example 1, L having the composition of general formula (III) was used.
aNb 2 S 5 was synthesized. The interplanar spacing measured by powder X-ray diffraction extended 3.2 Å from 17.3 Å before the hydrazine hydrate treatment to 20.5 Å after the treatment. This value is NbS 2
2.9Å when hydrazine is incorporated between layers
Matches well. Therefore, it was revealed that LaNb 2 S 5 is a layered metal chalcogenide host material having an interlayer capable of incorporating other substances.
実施例４ 実施例１と同様の方法で一般式（IV）の組成を持つＢｉ
0・5Pb0・5Ta2S5を合成した。粉末Ｘ線回折により測定し
た面間隔はヒドラジン水和物処理前１７．８Åから処理
後の２１．４Åへと３．６Å伸長した。この値はＴａＳ
２の層間にヒドラジンが取り込まれた場合の伸び３．０
〜４．０Åと一致する。それ故Ｂｉ0・5Pb0・5Ta2S5は他
の物質を取り込むことのできる層間を持つ層状金属カル
コゲナイド・ホスト材料であることが明らかとなった。Example 4 Bi having the composition of general formula (IV) was prepared in the same manner as in Example 1.
0 - 5 was synthesized Pb 0 · 5 Ta 2 S 5 . The interplanar spacing measured by powder X-ray diffraction extended by 3.6 Å from 17.8 Å before the hydrazine hydrate treatment to 21.4 Å after the treatment. This value is TaS
Elongation 3.0 when hydrazine is incorporated between the two layers
~ Matches 4.0Å. Therefore Bi 0 · 5 Pb 0 · 5 Ta 2 S 5 was found to be a layered metal chalcogenide host material having an interlayer that can incorporate other materials.
Claims (5)
くとも１種の元素、ＢはＴｉ、Ｖ、Ｎｂ及びＴａの中か
ら選ばれる少なくとも１種の元素及びＣはＳ、Ｓｅ及び
Ｔｅの中から選ばれる少なくとも１種の元素を示し、ｘ
は０．８≦ｘ≦１．２の数、ｙは１．６≦ｙ≦２．４の
数及びｚは４．０≦ｚ≦６．０の数を示す） で表わされる組成を有する層状金属カルコゲナイドから
なり、その層状の空隙に対し分子及びイオンから選ばれ
たゲストの取り込み及びその空隙からの取り出しを行
う、ホストとして用いることを特徴とするホスト材料。1. General formula (I) AxByCz (wherein A is at least one element selected from Bi, Sb and As, B is at least one element selected from Ti, V, Nb and Ta). Element and C represent at least one element selected from S, Se and Te, and x
Is a number of 0.8 ≦ x ≦ 1.2, y is a number of 1.6 ≦ y ≦ 2.4, and z is a number of 4.0 ≦ z ≦ 6.0). A host material comprising a metal chalcogenide, which is used as a host for incorporating a guest selected from molecules and ions into the layered void and taking it out from the void.
くとも１種の元素、ＢはＴｉ、Ｖ、Ｎｂ及びＴａの中か
ら選ばれる少なくとも１種の元素及びＣはＳ、Ｓｅ及び
Ｔｅの中から選ばれる少なくとも１種の元素を示し、ｘ
は０．８≦ｘ≦１．２の数、ｙは１．６≦ｙ≦２．４の
数及びｚは４．０≦ｚ≦６．０の数を示す） で表わされる組成を有する層状金属カルコゲナイドから
なり、その層状の空隙に対し分子及びイオンから選ばれ
たゲストの取り込み及びその空隙からの取り出しを行
う、ホストとして用いることを特徴とするホスト材料。2. General formula (II) AxByCz (wherein A is at least one element selected from Pb, Sn and Ge, and B is at least one element selected from Ti, V, Nb and Ta). Element and C represent at least one element selected from S, Se and Te, and x
Is a number of 0.8 ≦ x ≦ 1.2, y is a number of 1.6 ≦ y ≦ 2.4, and z is a number of 4.0 ≦ z ≦ 6.0). A host material comprising a metal chalcogenide, which is used as a host for incorporating a guest selected from molecules and ions into the layered void and taking it out from the void.
種の元素、ＢはＴｉ、Ｚｒ、Ｈｆ、Ｖ、Ｎｂ、Ｔａ、Ｃ
ｒ、Ｍｏ及びＷの中から選ばれる少なくとも１種の元素
及びＣはＳ、Ｓｅ及びＴｅの中から選ばれる少なくとも
１種の元素を示し、ｘは０．８≦ｘ≦１．２の数、ｙは
１．６≦ｙ≦２．４の数及びｚは４．０≦ｚ≦６．０の
数を示す） で表わされる組成を有する層状金属カルコゲナイドから
なり、その層状の空隙に対し分子及びイオンから選ばれ
たゲストの取り込み及びその空隙からの取り出しを行
う、ホストとして用いることを特徴とするホスト材料。3. General formula (III) AxByCz (wherein A is at least 1 selected from rare earth elements).
Seed element, B is Ti, Zr, Hf, V, Nb, Ta, C
At least one element selected from r, Mo and W and C represents at least one element selected from S, Se and Te, and x is a number of 0.8 ≦ x ≦ 1.2, y represents a number of 1.6 ≦ y ≦ 2.4 and z represents a number of 4.0 ≦ z ≦ 6.0), and is composed of a layered metal chalcogenide having a composition represented by A host material, which is used as a host for incorporating a guest selected from ions and extracting the guest from the void.
希土類元素の中から選ばれる少なくとも１種の元素、Ｂ
はＴｉ、Ｚｒ、Ｈｆ、Ｖ、Ｎｂ、Ｔａ、Ｃｒ、Ｍｏ及び
Ｗの中から選ばれる少なくとも１種の元素、ＣはＳ、Ｓ
ｅ及びＴｅの中から選ばれる少なくとも１種の元素を示
し、ｘは０．８≦ｘ≦１．２の数、ｙは１．６≦ｙ≦
２．４の数及びｚは４．０≦ｚ≦６．０の数を示す） で表わされる組成を有する層状金属カルコゲナイドから
なり、その層状の空隙に対し分子及びイオンから選ばれ
たゲストの取り込み及びその空隙からの取り出しを行
う、ホストとして用いることを特徴とするホスト材料。4. General formula (IV) AxByCz (wherein A is at least one element selected from Bi, Sb, As, Pb, Sn, Ge and rare earth elements, B
Is at least one element selected from Ti, Zr, Hf, V, Nb, Ta, Cr, Mo and W, and C is S or S.
and at least one element selected from e and Te, x is a number 0.8 ≦ x ≦ 1.2, and y is 1.6 ≦ y ≦
2.4 represents the number and z represents the number of 4.0 ≦ z ≦ 6.0), and is composed of a layered metal chalcogenide having a composition represented by And a host material which is used as a host for taking out from the voids.
極活物質もしくはイオン伝導材料又はそれらの母構造形
成材料におけるホストであることを特徴とする請求項
１、２、３又は４記載のホスト材料。5. The host material according to claim 1, 2, 3 or 4, wherein the host material is a display material, a positive / negative active material for a battery, an ionic conductive material or a host in a material for forming a mother structure thereof. Host material.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP1061856A JPH0611642B2 (en) | 1989-03-14 | 1989-03-14 | Layered metal chalcogenide host material |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP1061856A JPH0611642B2 (en) | 1989-03-14 | 1989-03-14 | Layered metal chalcogenide host material |
Publications (2)
| Publication Number | Publication Date |
|---|---|
| JPH02239107A JPH02239107A (en) | 1990-09-21 |
| JPH0611642B2 true JPH0611642B2 (en) | 1994-02-16 |
Family
ID=13183163
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| JP1061856A Expired - Lifetime JPH0611642B2 (en) | 1989-03-14 | 1989-03-14 | Layered metal chalcogenide host material |
Country Status (1)
| Country | Link |
|---|---|
| JP (1) | JPH0611642B2 (en) |
Families Citing this family (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JP2002270907A (en) * | 2001-03-06 | 2002-09-20 | Nec Corp | Thermoelectric conversion material and device using the same |
Family Cites Families (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JPH02199006A (en) * | 1989-01-30 | 1990-08-07 | Agency Of Ind Science & Technol | Multielement-based metal chalocogenide having 1/2/5 composition |
-
1989
- 1989-03-14 JP JP1061856A patent/JPH0611642B2/en not_active Expired - Lifetime
Also Published As
| Publication number | Publication date |
|---|---|
| JPH02239107A (en) | 1990-09-21 |
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