TWI683790B - Manufacturing method of iodine heptafluoride - Google Patents

Manufacturing method of iodine heptafluoride Download PDF

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TWI683790B
TWI683790B TW105118823A TW105118823A TWI683790B TW I683790 B TWI683790 B TW I683790B TW 105118823 A TW105118823 A TW 105118823A TW 105118823 A TW105118823 A TW 105118823A TW I683790 B TWI683790 B TW I683790B
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iodine
pentafluoride
heptafluoride
gas
liquid phase
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TW201708098A (en
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長友真聖
池田晋也
柴山茂朗
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日商中央硝子股份有限公司
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Abstract

本發明揭示有一種五氟化碘之製造方法，其包括：對於具有包含碘之液相之五氟化碘之反應槽中供給七氟化碘氣體，使碘與七氟化碘反應，從而製造五氟化碘之步驟。利用該方法，可安全且穩定地實現五氟化碘之高速度之生成。 The invention discloses a method for manufacturing iodine pentafluoride, which comprises: supplying iodine heptafluoride gas to a reaction tank having iodine pentafluoride containing a liquid phase containing iodine, and reacting iodine with iodine heptafluoride to produce Steps of iodine pentafluoride. With this method, high-speed generation of iodine pentafluoride can be achieved safely and stably.

Description

七氟化碘之製造方法 Manufacturing method of iodine heptafluoride

本發明係關於一種使碘與七氟化碘反應而製造五氟化碘之方法、及由五氟化碘製造七氟化碘之方法。 The invention relates to a method for producing iodine pentafluoride by reacting iodine with iodine heptafluoride, and a method for producing iodine heptafluoride from iodine pentafluoride.

作為製造有效用作氟化劑或含氟化合物之中間物製造之原料之五氟化碘之方法，已知有使碘與氟反應之方法。 As a method for producing iodine pentafluoride which is effectively used as a raw material for intermediate production of a fluorinating agent or a fluorine-containing compound, a method of reacting iodine with fluorine is known.

例如，專利文獻1中揭示有「由熔融碘之直接氟化製造五氟化碘之方法」。 For example, Patent Document 1 discloses "a method for producing iodine pentafluoride by direct fluorination of molten iodine".

專利文獻2中揭示有「(1)一種五氟化碘之製造方法，其特徵在於：(a)向液狀之碘中通入氟氣使之反應，生成包含五氟化碘及碘之蒸氣混合物；(b)於已生成之液狀之五氟化碘之存在下，使該蒸氣混合物與新的氟氣反應，進而生成五氟化碘」。 Patent Document 2 discloses "(1) A method for producing iodine pentafluoride, which is characterized in that: (a) Fluorine gas is introduced into liquid iodine to react to generate a vapor containing iodine pentafluoride and iodine. Mixture; (b) in the presence of the liquid iodine pentafluoride that has been generated, reacting the vapor mixture with new fluorine gas to produce iodine pentafluoride."

使氟與碘反應而生成五氟化碘之反應其生成熱超過800kJ/mol，並伴隨著大規模放熱。因此，無論固體(非專利文獻1)、液體(專利文獻1)、氣體(專利文獻2)，若使純碘與氟反應，則均有局部進行反應並放熱，難以控制反應之擔憂。 The reaction of fluorine and iodine to generate iodine pentafluoride has a heat of formation exceeding 800 kJ/mol, accompanied by large-scale exotherm. Therefore, regardless of solid (Non-Patent Document 1), liquid (Patent Document 1), and gas (Patent Document 2), if pure iodine is reacted with fluorine, there is a concern that the reaction proceeds locally and exotherms, making it difficult to control the reaction.

鑒於以上情況，為了「平穩地實施氟與碘之反應，最終提供一種更安全、且生產性更優異之五氟化碘之製造方法」，專利文獻3中揭示有「一種五氟化碘之製造方法，其特徵在於：其係使氟與碘反應而製造五氟化碘之方法，且向與包含碘之五氟化碘之液相鄰接之氣相中供給氟」。 In view of the above, in order to "stablely implement the reaction of fluorine and iodine, and ultimately provide a safer and more productive method for producing iodine pentafluoride", Patent Document 3 discloses "a method for producing iodine pentafluoride" The method is characterized in that it reacts fluorine with iodine to produce iodine pentafluoride, and supplies fluorine to the gas phase adjacent to the liquid containing iodine pentafluoride."

專利文獻3所記載之五氟化碘之製造方法係藉由使分散或溶解於液相之五氟化碘中之碘與包含氟氣之氣相接觸，使碘與氟氣反應而製造五氟化碘之方法。 The method for producing iodine pentafluoride described in Patent Document 3 is to produce pentafluoro by contacting iodine dispersed or dissolved in iodine pentafluoride in a liquid phase with a gas phase containing fluorine gas, and reacting iodine with fluorine gas The method of iodine.

[先前技術文獻] [Prior Technical Literature] [專利文獻] [Patent Literature]

[專利文獻1]日本專利特開昭54-65196號公報 [Patent Document 1] Japanese Patent Laid-Open No. 54-65196

[專利文獻2]日本專利特開昭58-145602號公報 [Patent Document 2] Japanese Patent Laid-Open No. 58-145602

[專利文獻3]國際公開WO2008/047871號之說明書 [Patent Document 3] Specification of International Publication No. WO2008/047871

[非專利文獻] [Non-patent literature]

[非專利文獻1]WalterC.Schumb、外1名、「Ind.Eng.Chem.」、1950、42(7)、pp1383~1386 [Non-Patent Document 1] Walter C. Schumb, one outsider, "Ind. Eng. Chem.", 1950, 42(7), pp1383~1386

然而，於專利文獻3所記載之藉由使分散或溶解於液相之五氟化碘中之碘與包含氟氣之氣相接觸，使碘與氟氣反應而製造五氟化碘之五氟化碘之製造方法中，若使氣相中之氟、與自液相汽化之碘或液相中之碘接觸，則有氣相之氟氣難以溶解於液相之五氟化碘中，導致氟氣與碘之反應難以進行之擔憂。 However, in Patent Document 3, by contacting iodine dispersed or dissolved in iodine pentafluoride in the liquid phase with a gas phase containing fluorine gas, and reacting iodine with fluorine gas, pentafluoride of iodine pentafluoride is produced. In the manufacturing method of iodine, if the fluorine in the gas phase is contacted with the iodine vaporized from the liquid phase or the iodine in the liquid phase, the fluorine gas in the gas phase is difficult to dissolve in the iodine pentafluoride in the liquid phase, resulting in There is a concern that the reaction between fluorine gas and iodine is difficult to proceed.

即，本發明之目的在於提供一種五氟化碘之製造方法，其係使五氟化碘藉由溫和之反應，於不發生局部反應及急遽放熱之情況下，五氟化碘之生成速度較高之製造方法，換言之，每單位時間之五氟化碘之生成量較多之製造方法。 That is, the object of the present invention is to provide a method for producing iodine pentafluoride, which allows iodine pentafluoride to undergo a mild reaction without the occurrence of local reactions and rapid exotherm. A high manufacturing method, in other words, a manufacturing method that produces more iodine pentafluoride per unit time.

進而，本發明之目的在於提供一種由所獲得之五氟化碘簡便地製造七氟化碘之七氟化碘之製造方法。 Furthermore, an object of the present invention is to provide a method for easily producing iodine heptafluoride from the obtained iodine pentafluoride.

本發明者等經過銳意研究，結果發現，藉由使七氟化碘氣體溶解或分散於具有包含碘之液相之五氟化碘之反應槽中之反應系中，使碘與七氟化碘接觸並反應，從而能夠以較高之生成速度製造五氟化 碘，以至完成本發明之五氟化碘之製造方法。 The inventors have made intensive studies and found that by dissolving or dispersing the iodine heptafluoride gas in the reaction system of the reaction tank with iodine pentafluoride containing a liquid phase containing iodine, iodine and iodine heptafluoride Contact and react so that pentafluoride can be produced at a higher production rate Iodine, and even the method for producing iodine pentafluoride of the present invention.

由碘(I2)及七氟化碘(IF7)獲得五氟化碘(IF5)時之反應式如下所述。 The reaction formula for obtaining iodine pentafluoride (IF 5 ) from iodine (I 2 ) and iodine heptafluoride (IF 7 ) is as follows.

5IF7+I2→7IF5 5IF 7 +I 2 →7IF 5

本發明者等人著眼於雖然氟氣難以溶解於液相之五氟化碘，但七氟化碘氣體容易溶解於液相之五氟化碘。由於氟氣難溶於液相之五氟化碘，故而液相之五氟化碘中之氟氣與碘之反應為氣液反應或氣固反應，無法期待提高五氟化碘之生成速度。然而，七氟化碘氣體易溶於液相之五氟化碘，液相之五氟化碘中之七氟化碘與碘之反應不僅為氣液反應、氣固反應，而且以七氟化碘與碘之液固反應或液液反應進行，實現五氟化碘之生成速度較高。 The present inventors focused on the fact that although fluorine gas is difficult to dissolve in liquid phase iodine pentafluoride, iodine heptafluoride gas is easily dissolved in liquid phase iodine pentafluoride. Since fluorine gas is insoluble in iodine pentafluoride in the liquid phase, the reaction of fluorine gas and iodine in liquid iodine pentafluoride is a gas-liquid reaction or a gas-solid reaction, and it cannot be expected to increase the generation rate of iodine pentafluoride. However, iodine heptafluoride gas is easily soluble in liquid iodine pentafluoride. The reaction of iodine heptafluoride in liquid iodine pentafluoride with iodine is not only gas-liquid reaction, gas-solid reaction, but also heptafluoride The liquid-solid reaction or liquid-liquid reaction of iodine and iodine proceeds to achieve a higher generation rate of iodine pentafluoride.

如本說明書之實施例1及比較例2所示，以本發明之「向具有包含碘之液相之五氟化碘之反應槽中供給七氟化碘氣體，使碘與七氟化碘反應之五氟化碘之製造方法」而快速進行從而獲得五氟化碘(實施例1)，相對於此，以先前之方法即「向與包含碘之五氟化碘之液相鄰接之氣相供給氟，使碘與氟反應之五氟化碘之製造方法」難以進行(比較例2)。 As shown in Example 1 and Comparative Example 2 of this specification, the iodine heptafluoride gas is supplied to the reaction tank having iodine pentafluoride containing a liquid phase containing iodine according to the present invention to react iodine with iodine heptafluoride The production method of iodine pentafluoride” was carried out quickly to obtain iodine pentafluoride (Example 1). In contrast, the previous method was “to the gas phase adjacent to the liquid containing iodine pentafluoride It is difficult to produce iodine pentafluoride by supplying fluorine to react iodine with fluorine (Comparative Example 2).

又，本發明者等人發現一種由所獲得之五氟化碘簡便地製造七氟化碘之七氟化碘之製造方法。 In addition, the inventors of the present invention have found a method for easily producing iodine heptafluoride from the obtained iodine pentafluoride.

即，本發明包括以下之發明1~9。 That is, the present invention includes the following inventions 1 to 9.

〔發明1〕 〔Invention 1〕

一種五氟化碘之製造方法，其包括：對於具有包含碘之液相之五氟化碘之反應槽中供給七氟化碘，使碘與七氟化碘反應，從而製造五氟化碘之步驟。 A method for manufacturing iodine pentafluoride, which comprises: supplying iodine heptafluoride to a reaction tank with a liquid phase containing iodine containing iodine pentafluoride, and reacting iodine with iodine heptafluoride to produce iodine pentafluoride step.

〔發明2〕 〔Invention 2〕

如發明1之五氟化碘之製造方法，其中於碘與七氟化碘之反應 中，一面於反應槽內進行攪拌一面供給七氟化碘。 The method of manufacturing iodine pentafluoride according to invention 1, wherein the reaction between iodine and iodine heptafluoride In the process, iodine heptafluoride was supplied while stirring in the reaction tank.

〔發明3〕 〔Invention 3〕

如發明1或發明2之五氟化碘之製造方法，其中上述包含碘之液相之五氟化碘係包含溶解之碘之溶液狀態、或液相中分散及沈澱有固體碘之狀態。 The method for producing iodine pentafluoride according to invention 1 or invention 2, wherein the iodine pentafluoride in the liquid phase containing iodine is in a solution state containing dissolved iodine, or a state in which solid iodine is dispersed and deposited in the liquid phase.

〔發明4〕 〔Invention 4〕

如發明1至3之五氟化碘之製造方法，其中於上述包含碘之液相之五氟化碘中，以相對於碘與五氟化碘之總量之含有率表示，包含碘0.01重量%以上且70重量%以下。 The method for producing iodine pentafluoride according to inventions 1 to 3, wherein the iodine pentafluoride in the above-mentioned liquid phase containing iodine is expressed in terms of the content ratio with respect to the total amount of iodine and iodine pentafluoride, including 0.01 weight of iodine % To 70% by weight.

〔發明5〕 〔Invention 5〕

如發明1至4之五氟化碘之製造方法，其中於上述包含碘之液相之五氟化碘中，以相對於碘與五氟化碘及七氟化碘之總量之含有率表示，包含七氟化碘0.001重量%以上且91重量%以下。 The manufacturing method of iodine pentafluoride according to inventions 1 to 4, wherein the iodine pentafluoride in the above-mentioned liquid phase containing iodine is expressed as a content rate relative to the total amount of iodine, iodine pentafluoride and iodine heptafluoride , Containing iodine heptafluoride 0.001% by weight or more and 91% by weight or less.

〔發明6〕 〔Invention 6〕

一種七氟化碘之製造方法，其包括：利用發明1至5之五氟化碘之製造方法，使碘與七氟化碘反應而獲得五氟化碘之步驟、及使氟氣與所獲得之五氟化碘反應而獲得七氟化碘之步驟。 A method for manufacturing iodine heptafluoride, comprising: using the method for manufacturing iodine pentafluoride of inventions 1 to 5, reacting iodine with iodine heptafluoride to obtain iodine pentafluoride, and allowing fluorine gas to obtain The step of reacting iodine pentafluoride to obtain iodine heptafluoride.

〔發明7〕 〔Invention 7〕

如發明6之七氟化碘之製造方法，其中於獲得上述七氟化碘之步驟中，對於內部具有含有金屬氟化物之填充物之反應器中供給五氟化碘氣體及氟氣，並使其等反應。 The manufacturing method of iodine heptafluoride according to invention 6, wherein in the step of obtaining the above iodine heptafluoride, iodine pentafluoride gas and fluorine gas are supplied to a reactor having a filler containing metal fluoride inside, and Its other reactions.

〔發明8〕 〔Invention 8〕

如發明7之七氟化碘之製造方法，其中上述金屬氟化物包含選自由NiF2、FeF3、及CoF2所組成之群中之至少1種化合物。 The method for producing iodine heptafluoride according to invention 7, wherein the metal fluoride contains at least one compound selected from the group consisting of NiF 2 , FeF 3 , and CoF 2 .

〔發明9〕 〔Invention 9〕

如發明7或發明8之七氟化碘之製造方法，其中上述五氟化碘氣體與上述氟氣反應時之上述金屬氟化物之溫度為150℃以上且350℃以下。 The method for producing iodine heptafluoride according to invention 7 or invention 8, wherein the temperature of the metal fluoride when the iodine pentafluoride gas reacts with the fluorine gas is 150°C or more and 350°C or less.

根據本發明之五氟化碘之製造方法，能夠提高五氟化碘之生成速度，進而可由利用該製造方法製造之五氟化碘簡便地製造七氟化碘。 According to the method for producing iodine pentafluoride of the present invention, the generation rate of iodine pentafluoride can be increased, and iodine heptafluoride can be easily produced from the iodine pentafluoride produced by this production method.

10‧‧‧反應裝置 10‧‧‧Reaction device

11‧‧‧反應槽(利用冷卻器冷卻) 11‧‧‧Reaction tank (cooled by cooler)

12‧‧‧固體碘 12‧‧‧Solid iodine

13‧‧‧五氟化碘(溶解有碘) 13‧‧‧Iodine pentafluoride (dissolved iodine)

14‧‧‧氣相 14‧‧‧gas phase

15‧‧‧液相(五氟化碘) 15‧‧‧liquid phase (iodine pentafluoride)

16‧‧‧七氟化碘之供給源 16‧‧‧Supply source of iodine heptafluoride

17‧‧‧碘供給源 17‧‧‧Iodine supply source

18‧‧‧惰性氣體之供給源 18‧‧‧Supply source of inert gas

19‧‧‧泵 19‧‧‧Pump

20‧‧‧攪拌器 20‧‧‧Agitator

圖1係表示實施形態之反應裝置之說明圖。 Fig. 1 is an explanatory diagram showing a reaction apparatus of an embodiment.

1.五氟化碘之製造方法 1. Manufacturing method of iodine pentafluoride

本發明係五氟化碘之製造方法，其包括向具有包含碘之液相之五氟化碘之反應槽中供給七氟化碘氣體，使碘與七氟化碘反應，從而製造五氟化碘之步驟。 The present invention is a method for producing iodine pentafluoride, which includes supplying iodine heptafluoride gas to a reaction tank having iodine pentafluoride containing a liquid phase containing iodine to react iodine with iodine heptafluoride to produce pentafluoride Steps to iodine.

使用圖1對本發明之五氟化碘之製造方法之實施形態之一例進行說明。本發明並不限定於以下所示之實施形態。 An example of the embodiment of the method for producing iodine pentafluoride of the present invention will be described using FIG. 1. The present invention is not limited to the embodiments shown below.

再者，於本發明中，所謂液相係指物質為液體狀態之相，所謂氣相係指物質為氣體狀態之相。 Furthermore, in the present invention, the liquid phase refers to a phase in which a substance is in a liquid state, and the gas phase refers to a phase in which a substance is in a gas state.

〔反應裝置〕 〔Reaction device〕

將本發明之五氟化碘之製造方法之實施形態之反應裝置10示於圖1。反應裝置10係於反應槽11內具有沈澱、分散或溶解有碘12之液相(液狀)之五氟化碘13。向反應槽11內之液相15中供給七氟化碘，於液相15中使七氟化碘與碘12反應，從而可生成五氟化碘。 The reaction device 10 of the embodiment of the method for producing iodine pentafluoride of the present invention is shown in FIG. 1. The reaction device 10 has an iodine pentafluoride 13 in a liquid phase (liquid state) in which iodine 12 is precipitated, dispersed or dissolved in the reaction tank 11. Iodine heptafluoride is supplied to the liquid phase 15 in the reaction tank 11, and the iodine heptafluoride and iodine 12 are reacted in the liquid phase 15, thereby generating iodine pentafluoride.

此時，七氟化碘既可供給至液相15中，亦可供給至氣相14中。於將七氟化碘供給至液相15中之情形時，七氟化碘按照某種比率於氣相14中移動，於將七氟化碘供給至氣相14中之情形時，七氟化碘按照 某種比率於液相15中移動。以將七氟化碘吹入至包含碘12之五氟化碘之液相15中，可使七氟化碘迅速溶解於液相15中，可高效地進行七氟化碘與碘12之反應，從而提高五氟化碘之生成速度。 At this time, iodine heptafluoride may be supplied to the liquid phase 15 or the gas phase 14. When iodine heptafluoride is supplied to the liquid phase 15, iodine heptafluoride moves in the gas phase 14 at a certain ratio. When iodine heptafluoride is supplied to the gas phase 14, heptafluoride Iodine according to A certain ratio moves in the liquid phase 15. By blowing iodine heptafluoride into the liquid phase 15 containing iodine 12 and iodine pentafluoride, the iodine heptafluoride can be quickly dissolved in the liquid phase 15, and the reaction between iodine heptafluoride and iodine 12 can be efficiently carried out , Thereby increasing the rate of iodine pentafluoride formation.

七氟化碘較佳為自附設於反應槽11之七氟化碘供給源16供給至液相15中。由於五氟化碘之蒸氣壓低，故而為了容易控制反應槽11之壓力以及確保泵19之驅動壓力，亦可將惰性氣體作為緩衝氣體(緩衝物)自附設於反應槽11之惰性氣體供給源18供給至反應槽11中，較佳為供給至氣相14中。作為惰性氣體，可舉出的是不與碘、七氟化碘、五氟化碘反應之氣體，例如氮氣、氬氣、氦氣。較佳為容易獲得之氮氣。 The iodine heptafluoride is preferably supplied to the liquid phase 15 from the iodine heptafluoride supply source 16 attached to the reaction tank 11. Since the vapor pressure of iodine pentafluoride is low, in order to easily control the pressure of the reaction tank 11 and ensure the driving pressure of the pump 19, the inert gas can also be used as a buffer gas (buffer) from the inert gas supply source 18 attached to the reaction tank 11 It is preferably supplied to the reaction tank 11 and preferably to the gas phase 14. Examples of the inert gas include gases that do not react with iodine, iodine heptafluoride, or iodine pentafluoride, such as nitrogen, argon, and helium. Nitrogen, which is easily available, is preferred.

於碘12與七氟化碘之反應中，反應槽11內之液相15由泵19或攪拌器20攪拌。 In the reaction between iodine 12 and iodine heptafluoride, the liquid phase 15 in the reaction tank 11 is stirred by the pump 19 or the stirrer 20.

〔碘與七氟化碘之反應〕 [Reaction of iodine with iodine heptafluoride]

碘與七氟化碘之反應係發生於氣相14中、液相15中、或氣相14與液相15之界面。即，於液相15中，存在於五氟化碘13中之碘12成為與蒸氣壓相當之氣體，於氣相14中移動，而與存在於氣相14中之七氟化碘反應。又，存在於氣相14中之七氟化碘自氣相14移動至液相15，而與存在於液相15中之碘12反應。又，存在於氣相14中之七氟化碘與液相15中存在於五氟化碘13中之碘12於氣相14與液相15之界面處進行反應。又，於液相15中，七氟化碘與存在於五氟化碘13中之碘12反應。 The reaction of iodine and iodine heptafluoride occurs in the gas phase 14, the liquid phase 15, or the interface between the gas phase 14 and the liquid phase 15. That is, in the liquid phase 15, the iodine 12 present in the iodine pentafluoride 13 becomes a gas corresponding to the vapor pressure, moves in the gas phase 14, and reacts with the iodine heptafluoride present in the gas phase 14. In addition, the iodine heptafluoride present in the gas phase 14 moves from the gas phase 14 to the liquid phase 15 and reacts with the iodine 12 present in the liquid phase 15. In addition, iodine heptafluoride present in the gas phase 14 and iodine 12 present in the iodine pentafluoride 13 in the liquid phase 15 react at the interface between the gas phase 14 and the liquid phase 15. Also, in the liquid phase 15, iodine heptafluoride reacts with iodine 12 present in iodine pentafluoride 13.

反應槽11亦可藉由未圖示之水冷裝置進行冷卻。於碘與七氟化碘之反應中，較佳為藉由將反應槽11中之液相15之溫度保持於10℃以上且95℃以下，而維持液相之狀態。於將液相15維持於未達10℃之情形時，有五氟化碘13凝固之擔憂，冷卻所需之能量消耗亦變大。另一方面，於將液相15維持於高於95℃之溫度之情形時，反應過程中不僅反應槽11內之壓力變高，而且有產生於液相15中溶解於五氟化碘13之七 氟化碘之量減少，導致五氟化碘之生成速度下降等問題之虞。液相15之維持溫度較佳為15℃以上且75℃以下，更佳為20℃以上且50℃以下。 The reaction tank 11 may be cooled by a water cooling device (not shown). In the reaction of iodine and iodine heptafluoride, it is preferable to maintain the state of the liquid phase by maintaining the temperature of the liquid phase 15 in the reaction tank 11 at 10°C or higher and 95°C or lower. When the liquid phase 15 is maintained at less than 10°C, there is a concern that the iodine pentafluoride 13 solidifies, and the energy consumption required for cooling also increases. On the other hand, when the liquid phase 15 is maintained at a temperature higher than 95°C, not only does the pressure in the reaction tank 11 become higher during the reaction, but it also occurs in the liquid phase 15 dissolved in iodine pentafluoride 13 Seven The decrease in the amount of iodine fluoride may cause problems such as a decrease in the production rate of iodine pentafluoride. The maintenance temperature of the liquid phase 15 is preferably 15°C or higher and 75°C or lower, more preferably 20°C or higher and 50°C or lower.

反應過程中之反應槽11內之氣相14之壓力較佳為以絕對壓計為40kPa以上且133kPa以下，更佳為67kPa以上且101kPa以下。若反應槽11內之壓力為未達40kPa，則溶解於五氟化碘13之七氟化碘之量減少，五氟化碘之生成速度下降。若反應槽11內之壓力高於133kPa，則必須將反應槽11設為耐壓之結構。壓力可根據七氟化碘氣體16之供給速度、反應槽11之冷卻、惰性氣體之添加等進行調整。七氟化碘之供給速度雖取決於反應裝置之大小及反應之規模，但於反應中，反應槽11內之氣相14之壓力較佳為落於上述範圍內。 The pressure of the gas phase 14 in the reaction tank 11 during the reaction is preferably 40 kPa or more and 133 kPa or less in absolute pressure, more preferably 67 kPa or more and 101 kPa or less. If the pressure in the reaction tank 11 is less than 40 kPa, the amount of iodine heptafluoride dissolved in iodine pentafluoride 13 decreases, and the production rate of iodine pentafluoride decreases. If the pressure in the reaction tank 11 is higher than 133 kPa, the reaction tank 11 must have a pressure-resistant structure. The pressure can be adjusted according to the supply rate of iodine heptafluoride gas 16, cooling of the reaction tank 11, addition of inert gas, and the like. Although the supply rate of iodine heptafluoride depends on the size of the reaction device and the scale of the reaction, during the reaction, the pressure of the gas phase 14 in the reaction tank 11 preferably falls within the above range.

〔反應時之碘及七氟化碘之含有率〕 [Content of iodine and iodine heptafluoride during the reaction]

碘12既可於反應開始前裝入反應槽11內，亦可於反應開始時及反應過程中間接地或連續地自碘供給源17供給至反應槽11中。於本發明之五氟化碘之製造方法中，反應槽11中之碘12之含有率係以將反應槽11中之碘與五氟化碘之總量設為100重量%之含有率表示，較佳為0.01重量%以上且70重量%以下。 Iodine 12 may be charged into the reaction tank 11 before the start of the reaction, or may be grounded or continuously supplied from the iodine supply source 17 into the reaction tank 11 at the start of the reaction and in the middle of the reaction process. In the method for producing iodine pentafluoride of the present invention, the content rate of iodine 12 in the reaction tank 11 is expressed as a content rate in which the total amount of iodine in the reaction tank 11 and iodine pentafluoride is 100% by weight, It is preferably 0.01% by weight or more and 70% by weight or less.

若碘之含有率少於0.01重量%，則生成之五氟化碘之量較少。若碘之含有率多於70重量%，則有未能去除反應熱而引起局部反應或反應失控之虞。再者，為了提高五氟化碘之生產量，碘12之濃度較佳為較高，更佳為1重量%以上且60重量%以下。 If the content of iodine is less than 0.01% by weight, the amount of iodine pentafluoride produced is small. If the content of iodine is more than 70% by weight, there is a possibility that the reaction heat may not be removed, causing a local reaction or a reaction out of control. Furthermore, in order to increase the production volume of iodine pentafluoride, the concentration of iodine 12 is preferably higher, more preferably 1% by weight to 60% by weight.

再者，雖亦取決於溫度壓力等條件，但於液相15中，碘12無法於液狀之五氟化碘13中溶解約1質量%以上。無法溶解於五氟化碘13中之碘12會以固體之狀態分散及沈澱於液相15中。 Furthermore, although it also depends on conditions such as temperature and pressure, in the liquid phase 15, iodine 12 cannot be dissolved in the liquid iodine pentafluoride 13 by about 1% by mass or more. Iodine 12, which cannot be dissolved in iodine pentafluoride 13, will be dispersed in a solid state and deposited in the liquid phase 15.

於反應過程中，較佳為將七氟化碘自七氟化碘供給源16供給至反應槽11之液相15中。藉由將七氟化碘氣體供給至氣相14中，亦進行 碘12與七氟化碘之反應，從而亦可製造五氟化碘。然而，為了提高碘12與七氟化碘之反應效率，以較高之生成速度製造五氟化碘，較佳為將七氟化碘供給至液相15中。 During the reaction, it is preferable to supply iodine heptafluoride from the iodine heptafluoride supply source 16 to the liquid phase 15 of the reaction tank 11. By supplying iodine heptafluoride gas into the gas phase 14, it is also carried out The reaction of iodine 12 with iodine heptafluoride can also produce iodine pentafluoride. However, in order to improve the reaction efficiency of iodine 12 and iodine heptafluoride, iodine pentafluoride is produced at a relatively high production rate, and it is preferable to supply iodine heptafluoride to the liquid phase 15.

於反應過程中，反應槽11中之液相15中之七氟化碘之含有率係以將反應槽11中之五氟化碘13與七氟化碘之總量設為100重量%之含有率表示，較佳為0.001重量%以上且91重量%以下。若液相15中之七氟化碘之含有率少於0.001重量%，則生成之五氟化碘之量變少。若七氟化碘之濃度多於91重量%，則有反應槽11之溫度及壓力上升，發生局部反應或反應失控之虞。更佳為七氟化碘之含有率為0.01重量%以上且64重量%以下。 During the reaction, the content of iodine heptafluoride in the liquid phase 15 in the reaction tank 11 is such that the total amount of iodine pentafluoride 13 and iodine heptafluoride in the reaction tank 11 is set to 100% by weight The ratio indicates that it is preferably 0.001% by weight or more and 91% by weight or less. If the content of iodine heptafluoride in the liquid phase 15 is less than 0.001% by weight, the amount of iodine pentafluoride produced becomes smaller. If the concentration of iodine heptafluoride is more than 91% by weight, the temperature and pressure of the reaction tank 11 may rise, and there is a risk of local reaction or runaway reaction. More preferably, the content of iodine heptafluoride is 0.01% by weight or more and 64% by weight or less.

供給至液相15中之七氟化碘之純度較佳為純度98重量%以上，更佳為純度99重量%以上。於七氟化碘之純度較低之情形時，有作為生成物之五氟化碘之純度下降之虞。 The purity of the iodine heptafluoride supplied to the liquid phase 15 is preferably 98% by weight or more, and more preferably 99% by weight or more. When the purity of iodine heptafluoride is low, the purity of iodine pentafluoride as a product may decrease.

〔攪拌〕 〔Stirring〕

於使液相15中之碘12與七氟化碘反應而獲得五氟化碘之反應中，為了避免產生反應局部進行之非勻相反應，或產生過度之反應熱，較佳為攪拌液相15。作為反應槽11內之液相15之攪拌方法，可例示藉由泵19使液相15循環之攪拌、或利用具有旋轉翼之攪拌機20進行之攪拌。於藉由泵19攪拌液相15之情形時，為了確保泵19之驅動壓力，較佳為將特定壓力之惰性氣體導入至反應槽11內。例如，惰性氣體係自惰性氣體供給源18供給。作為惰性氣體，可列舉不與碘、七氟化碘、五氟化碘反應之氣體，例如氮氣、氬氣、氦氣。作為惰性氣體之純度，為了不影響作為生成物之五氟化碘之純度，較佳為高純度，較佳為純度99重量%以上。較佳為容易獲得之氮氣。 In the reaction of reacting iodine 12 in liquid phase 15 with iodine heptafluoride to obtain iodine pentafluoride, it is preferred to stir the liquid phase in order to avoid local heterogeneous reaction or excessive heat of reaction. 15. As a method for agitating the liquid phase 15 in the reaction tank 11, agitation in which the liquid phase 15 is circulated by the pump 19 or agitation using a stirrer 20 having a rotary wing can be exemplified. When the liquid phase 15 is stirred by the pump 19, in order to ensure the driving pressure of the pump 19, it is preferable to introduce an inert gas at a specific pressure into the reaction tank 11. For example, the inert gas system is supplied from the inert gas supply source 18. Examples of the inert gas include gases that do not react with iodine, iodine heptafluoride, or iodine pentafluoride, such as nitrogen, argon, and helium. As the purity of the inert gas, in order not to affect the purity of the product iodine pentafluoride, it is preferably high purity, preferably 99% by weight or more. Nitrogen, which is easily available, is preferred.

〔碘與七氟化碘之純度〕 [Purity of iodine and iodine heptafluoride]

本發明之五氟化碘之製造方法所使用之碘及七氟化碘之純度於 實施本發明之方面上並無特別限制。然而，碘及七氟化碘之純度會影響生成之五氟化碘之純度。例如為了獲得99重量%以上之五氟化碘，較佳為使用純度99重量%以上之碘及七氟化碘。 The purity of iodine and iodine heptafluoride used in the method for producing iodine pentafluoride of the present invention is There is no particular limitation on the aspect of implementing the present invention. However, the purity of iodine and iodine heptafluoride will affect the purity of the generated iodine pentafluoride. For example, in order to obtain 99% by weight or more of iodine pentafluoride, it is preferable to use iodine and iodine heptafluoride having a purity of 99% by weight or more.

又，於自七氟化碘供給源16所供給之七氟化碘氣體中含有惰性氣體之情形時，惰性氣體具有如下效果：藉由起泡而對反應槽11中之液相15進行攪拌，從而去除使碘12與七氟化碘反應而獲得五氟化碘時之反應熱。然而，由於反應槽11之壓力因惰性氣體之分壓之增加而經時增加，故而需要設置壓力調整閥來控制壓力。 In addition, when the iodine heptafluoride gas supplied from the iodine heptafluoride supply source 16 contains an inert gas, the inert gas has the effect of stirring the liquid phase 15 in the reaction tank 11 by bubbling, Thus, the heat of reaction when iodine 12 is reacted with iodine heptafluoride to obtain iodine pentafluoride is removed. However, since the pressure of the reaction tank 11 increases with time due to the increase of the partial pressure of the inert gas, it is necessary to install a pressure adjustment valve to control the pressure.

2.七氟化碘之製造方法 2. Manufacturing method of iodine heptafluoride

本發明係七氟化碘之製造方法，其包括：利用上述五氟化碘之製造方法使碘與七氟化碘反應而獲得五氟化碘之步驟、及使所獲得之五氟化碘與氟氣反應而獲得七氟化碘之步驟。 The present invention is a method for producing iodine heptafluoride, which comprises the steps of obtaining iodine pentafluoride by reacting iodine with iodine heptafluoride using the method for producing iodine pentafluoride, and making the obtained iodine pentafluoride and The step of reacting fluorine gas to obtain iodine heptafluoride.

藉由使利用本發明之上述五氟化碘之製造方法所獲得之五氟化碘與氟氣反應，可製造七氟化碘。 By reacting the iodine pentafluoride obtained by the above-mentioned method for producing iodine pentafluoride of the present invention with fluorine gas, iodine heptafluoride can be produced.

作為使五氟化碘與氟氣反應而獲得七氟化碘之方法之例，可列舉以下之方法：將向五氟化碘之液體中吹入氟氣所獲得之五氟化碘氣體與氟氣一同導入至反應器中，使五氟化碘氣體與氟氣反應而獲得七氟化碘。或者，亦可考慮藉由加熱使五氟化碘氣化而製為五氟化碘氣體並供給至反應器之方法，或直接將液相之五氟化碘供給至反應器之方法。 As an example of a method for obtaining iodine heptafluoride by reacting iodine pentafluoride with fluorine gas, the following method may be mentioned: iodine pentafluoride gas and fluorine obtained by blowing fluorine gas into a liquid of iodine pentafluoride The gas is introduced into the reactor together, and iodine pentafluoride gas is reacted with fluorine gas to obtain iodine heptafluoride. Alternatively, a method of vaporizing iodine pentafluoride by heating to produce iodine pentafluoride gas and supplying it to the reactor, or a method of directly supplying iodine pentafluoride in the liquid phase to the reactor may also be considered.

於採用將五氟化碘氣體及氟氣供給至反應器並使其等反應而獲得七氟化碘之方法之情形時，於該步驟中，較佳為向於內部具有含有金屬氟化物之高溫填充物之反應器中，供給五氟化碘氣體及氟氣。藉由使用填充物，可提高以五氟化碘為基準之七氟化碘之產率，例如可將產率提高至70%以上。 In the case where a method of supplying iodine pentafluoride gas and fluorine gas to a reactor and reacting it to obtain iodine heptafluoride is adopted, in this step, it is preferable to have a high temperature containing metal fluoride inside Iodine pentafluoride gas and fluorine gas are supplied to the reactor of the packing. By using fillers, the yield of iodine heptafluoride based on iodine pentafluoride can be increased, for example, the yield can be increased to more than 70%.

本發明之七氟化碘之製造方法所使用之填充物中所含有之金屬 氟化物只要為使金屬氟化者即可，並無特別限制。例如，作為金屬氟化物，可列舉NiF2、FeF3、CoF2、LiF、NaF、KF、CsF、MgF2或CaF2，亦可將該等之2種以上混合。若考慮到廉價且對產率提高之助益較大，則較佳為使用包含作為過渡金屬之氟化物之NiF2、FeF3、及CoF2之任1種以上之填充物。 The metal fluoride contained in the filler used in the method for producing iodine heptafluoride of the present invention is not particularly limited as long as it fluorinates the metal. For example, examples of the metal fluoride include NiF 2 , FeF 3 , CoF 2 , LiF, NaF, KF, CsF, MgF 2 or CaF 2 , or two or more of these may be mixed. In consideration of cheapness and a large contribution to the improvement in yield, it is preferable to use any one or more fillers including NiF 2 , FeF 3 , and CoF 2 as fluorides of transition metals.

關於所使用之填充物之形狀，只要五氟化碘氣體與氟氣高效地接觸且於流通時該等氣體不發生閉塞，則並無特別限制。填充物例如可以藉由利用氟氣、三氟化氯氣體、七氟化碘氣體等使網狀之金屬片氟化而於金屬表面生成金屬氟化物之形式獲得，或將粉體狀之金屬氟化物成型為顆粒形狀而獲得。 The shape of the filler used is not particularly limited as long as the iodine pentafluoride gas and fluorine gas are efficiently contacted and the gas does not block during circulation. The filler can be obtained, for example, by fluorinating a net-shaped metal sheet with fluorine gas, chlorine trifluoride gas, iodine heptafluoride gas, etc. to generate metal fluoride on the metal surface, or by powdering metal fluoride The compound is obtained by molding into a particle shape.

於使五氟化碘氣體與氟氣反應而獲得七氟化碘時之填充物之溫度較佳為150℃以上且350℃以下。若填充物之溫度未達150℃，則有由五氟化碘氣體及氟氣製造七氟化碘時之生成速度下降之虞，若超過350℃，則有發生所生成之七氟化碘分解為五氟化碘及氟之逆反應之虞。特佳之填充物之溫度為200℃以上且330℃以下。例如，可藉由於填充有填充物之狀態下，利用電加熱器或蒸氣等對反應器進行加熱，而將填充物設為所需溫度。 The temperature of the filler when reacting iodine pentafluoride gas with fluorine gas to obtain iodine heptafluoride is preferably 150° C. or higher and 350° C. or lower. If the temperature of the filling material does not reach 150°C, the production rate of iodine heptafluoride from iodine pentafluoride gas and fluorine gas may decrease. If it exceeds 350°C, the generated iodine heptafluoride may decompose It is the risk of reverse reaction of iodine pentafluoride and fluorine. The temperature of the particularly good filler is above 200°C and below 330°C. For example, the filler can be set to a desired temperature by heating the reactor with an electric heater, steam, or the like while being filled with the filler.

於上述使五氟化碘氣體與氟氣反應而獲得七氟化碘之反應中，只要為逆反應不會變得顯著之反應溫度，則不僅反應器內之五氟化碘氣體與氟氣之滯留時間增加，並且七氟化碘之產率亦增加。有七氟化碘之生產性因滯留時間之增加而下降之虞，考慮到七氟化碘之所需之產率及生產性，反應器內之五氟化碘氣體與氟氣之滯留時間可進行各種選擇。於考慮到七氟化碘之生產性之情形時，期望反應器中之五氟化碘氣體與氟氣之滯留時間較短。例如，於F2/IF5之莫耳比為1以上之條件下使五氟化碘氣體與氟氣反應而獲得七氟化碘之情形時，若金屬氟化物之溫度為200℃以上且330℃以下，並且至少五氟化碘氣體與氟 氣之滯留時間為4秒以上，即可獲得80%以上之產率。 In the above reaction of reacting iodine pentafluoride gas with fluorine gas to obtain iodine heptafluoride, as long as the reaction temperature does not become significant in the reverse reaction, not only the iodine pentafluoride gas and fluorine gas in the reactor are retained The time increases, and the yield of iodine heptafluoride also increases. There is a risk that the productivity of iodine hexafluoride will decrease due to the increase in residence time. Considering the required yield and productivity of iodine hexafluoride, the residence time of iodine pentafluoride gas and fluorine gas in the reactor can be Make various choices. When considering the productivity of iodine heptafluoride, the residence time of the iodine pentafluoride gas and fluorine gas in the reactor is expected to be shorter. For example, when the molar ratio of F 2 /IF 5 is 1 or more, when iodine pentafluoride gas is reacted with fluorine gas to obtain iodine heptafluoride, if the temperature of the metal fluoride is 200° C. or more and 330 Below ℃, and at least the residence time of iodine pentafluoride gas and fluorine gas is more than 4 seconds, you can get more than 80% yield.

於使用流通式反應器，使五氟化碘氣體與氟氣反應而獲得七氟化碘之情形時之五氟化碘氣體與氟氣之導入時之流量比、或於使用密閉式反應器之情形時之五氟化碘氣體與氟氣之混合比，均較佳為以五氟化碘與氟之莫耳比(F2/IF5)計為1以上。尤其是，若莫耳比為1.3以上，則於五氟化碘氣體與氟氣之滯留時間為4秒以上之情況下可獲得七氟化碘之產率80%以上，但若將莫耳比(F2/IF5)設為35以上，則相對於七氟化碘之產率之提高，因氟氣之使用量增加導致經濟性下降變得顯著，因此欠佳。又，若莫耳比(F2/IF5)未達1，則有因未反應之五氟化碘增加，導致七氟化碘之產率下降之虞。 In the case of using a flow-through reactor to react iodine pentafluoride gas with fluorine gas to obtain iodine heptafluoride, the flow rate ratio at the time of introduction of iodine pentafluoride gas and fluorine gas, or when using a closed reactor In this case, the mixing ratio of iodine pentafluoride gas and fluorine gas is preferably 1 or more in terms of the molar ratio of iodine pentafluoride to fluorine (F 2 /IF 5 ). In particular, if the molar ratio is 1.3 or more, the yield of iodine heptafluoride can be more than 80% when the residence time of iodine pentafluoride gas and fluorine gas is 4 seconds or more, but if the molar ratio is When (F 2 /IF 5 ) is set to 35 or more, the yield of iodine heptafluoride is improved, and the decrease in economic efficiency due to the increase in the use of fluorine gas becomes significant, which is not good. In addition, if the molar ratio (F 2 /IF 5 ) is less than 1, there is a possibility that the yield of iodine heptafluoride may decrease due to an increase in unreacted iodine pentafluoride.

關於由五氟化碘氣體及氟氣獲得七氟化碘之反應時之反應器內之壓力，由於氟、五氟化碘、七氟化碘有毒性，故而為了防止洩漏，較佳為大氣壓以下，若考慮到經濟性，則較佳為40kPa(絕對壓)以上。 The pressure in the reactor during the reaction to obtain iodine heptafluoride from iodine pentafluoride gas and fluorine gas is fluorine, iodine pentafluoride, and iodine heptafluoride are toxic, so in order to prevent leakage, it is preferably below atmospheric pressure In consideration of economy, it is preferably 40 kPa (absolute pressure) or more.

[實施例] [Example]

以下，一併列舉本發明之實施例以及比較例，但本發明並不限制於以下之實施例。 The examples and comparative examples of the present invention are listed below, but the present invention is not limited to the following examples.

實施例1 Example 1

如圖1所示，向將槽內氣體經氮氣置換之容積2.3L之不鏽鋼製反應槽11中，加入質量3036g之液狀之五氟化碘13，接著加入重量3710g之固體碘12。添加時之液狀之五氟化碘13中之碘12之濃度相對於五氟化碘13中與固體碘12合計重量，為約55重量%。作為液相15中之包含固體碘12之五氟化碘13之攪拌方法，將泵19驅動而使液相15循環。自七氟化碘供給源16以0.6L/min之流量將七氟化碘氣體供給至液相15中，使七氟化碘氣體與五氟化碘13內之固體碘12反應，而獲得五氟化碘。反應過程中將反應槽11內之壓力保持為93kPa(絕對壓)。又，一 面冷卻使反應中之反應槽11之內部溫度成為30~60℃，一面反應60分鐘。除實驗開始前裝入部分以外，五氟化碘之新生成量為499g。 As shown in FIG. 1, to a 2.3 L stainless steel reaction tank 11 in which the gas in the tank was replaced with nitrogen, liquid iodine pentafluoride 13 with a mass of 3036 g was added, followed by solid iodine 12 with a weight of 3710 g. The concentration of iodine 12 in the liquid iodine pentafluoride 13 at the time of addition was about 55% by weight relative to the total weight of iodine pentafluoride 13 and solid iodine 12 in total. As a method of stirring the solid iodine 12 and iodine pentafluoride 13 in the liquid phase 15, the pump 19 is driven to circulate the liquid phase 15. The iodine heptafluoride gas is supplied to the liquid phase 15 at a flow rate of 0.6 L/min from the iodine heptafluoride supply source 16 to react the iodine heptafluoride gas with the solid iodine 12 in the iodine pentafluoride 13 to obtain five Iodine fluoride. During the reaction, the pressure in the reaction tank 11 was maintained at 93 kPa (absolute pressure). Again, one The surface cooling makes the internal temperature of the reaction tank 11 during the reaction 30 to 60°C, and the reaction is carried out for 60 minutes. Except for the portion charged before the start of the experiment, the newly generated amount of iodine pentafluoride is 499g.

實施例2 Example 2

作為攪拌方法，使具備旋轉翼之攪拌器20以轉數100rpm進行旋轉以攪拌液相15，代替實施例1中所進行之利用泵19使液相15循環，除此之外與實施例1同樣地，使七氟化碘氣體與固體碘12反應。除實驗開始前裝入部分以外，五氟化碘之新生成量為499g。 As a stirring method, the stirrer 20 equipped with a rotating wing was rotated at 100 rpm to stir the liquid phase 15, and the liquid phase 15 was circulated by using the pump 19 instead of the pump in Example 1 except that the liquid phase 15 was circulated. Ground, reacting iodine heptafluoride gas with solid iodine 12. Except for the portion charged before the start of the experiment, the newly generated amount of iodine pentafluoride is 499g.

無論利用泵、攪拌機、任意之攪拌裝置，均可藉由使五氟化碘中之碘與七氟化碘反應，而高效地除熱，安全且穩定地製造五氟化碘。 Irrespective of the use of a pump, agitator, or any agitating device, by reacting iodine in iodine pentafluoride with iodine heptafluoride, heat can be efficiently removed, and iodine pentafluoride can be produced safely and stably.

比較例1 Comparative example 1

向將槽內氣體經氮氣置換之容積2.3L之不鏽鋼製反應槽11中，加入質量3710g之固體碘12，自七氟化碘氣體供給源16以0.6L/min供給七氟化碘氣體，使之與固體碘12直接反應。反應過程中之反應槽內之壓力雖控制於93kPa(絕對壓)，但自七氟化碘氣體之供給開始經過5分鐘後，於反應槽11之七氟化碘氣體之供給口附近發現因反應熱所引起之溫度上升，不得不停止七氟化碘氣體之供給，中斷反應。 To a 2.3 L stainless steel reaction tank 11 in which the gas in the tank was replaced with nitrogen, solid iodine 12 with a mass of 3710 g was added, and iodine heptafluoride gas was supplied from an iodine heptafluoride gas supply source at 0.6 L/min to make It reacts directly with solid iodine 12. The pressure in the reaction tank during the reaction was controlled to 93 kPa (absolute pressure), but after 5 minutes from the supply of iodine heptafluoride gas, a reaction was found near the supply port of iodine heptafluoride gas in the reaction tank 11 The temperature rise caused by heat had to stop the supply of iodine heptafluoride gas and interrupt the reaction.

將各實施例之製造條件及結果示於表1。 Table 1 shows the production conditions and results of each example.

Figure 105118823-A0305-02-0014-1
Figure 105118823-A0305-02-0014-1

於液體之5氟化碘中，於使七氟化碘與碘發生反應之實施例1~2中，於以0.6L/min向液相15中供給七氟化碘氣體之供給速度下，不會伴隨局部放熱而反應「5IF7+I2→7IF5」迅速地進行，每小時獲得499g之五氟化碘。如此，可確認：藉由本發明之五氟化碘之製造方法，每單位時間之產量較多且可高速度地生產五氟化碘。 Among the liquid 5 iodine fluoride, in Examples 1 to 2 in which iodine heptafluoride reacts with iodine, at a supply rate of 0.6 L/min to the liquid phase 15 to supply iodine heptafluoride gas, no The reaction "5IF 7 +I 2 →7IF 5 "is accompanied by local exotherm, and 499 g of iodine pentafluoride is obtained every hour. In this way, it can be confirmed that the production method of iodine pentafluoride of the present invention has a large output per unit time and can produce iodine pentafluoride at a high speed.

然而，於不屬於本發明之範疇之使七氟化碘與固定碘直接反應之比較例1中，反應「5IF7+I2→7IF5」產生局部引起之放熱，不得不中斷反應。 However, in Comparative Example 1, which does not belong to the scope of the present invention, which directly reacts iodine heptafluoride with fixed iodine, the reaction "5IF 7 +I 2 →7IF 5 "generates local exotherm, and the reaction has to be interrupted.

比較例2 Comparative example 2

向將槽內氣體經氮氣置換之容積2.3L之不鏽鋼製反應槽11中，加入質量3036g之液狀之五氟化碘13，加入質量3710g之固體碘12。相對於添加時之五氟化碘13與固體碘12合計重量，固體碘12之濃度約為55重量%。藉由具備旋轉翼之攪拌器，以轉數100rpm攪拌液相15。 To a 2.3 L stainless steel reaction tank 11 in which the gas in the tank was replaced with nitrogen, liquid iodine pentafluoride 13 with a mass of 3036 g was added, and solid iodine 12 with a mass of 3710 g was added. The concentration of solid iodine 12 is about 55% by weight relative to the total weight of iodine pentafluoride 13 and solid iodine 12 at the time of addition. The liquid phase 15 was stirred at 100 rpm with a stirrer equipped with a rotating wing.

於攪拌下，向反應槽11之氣相14中供給經氮氣稀釋至70體積%之氟氣，開始由碘及氟氣獲得五氟化碘之反應。反應過程中之反應槽11內之壓力藉由壓力調整閥保持於93kPa(絕對壓)。又，一面冷卻使反應中之反應槽11之溫度成為30~60℃，一面反應60分鐘。 Under stirring, fluorine gas diluted with nitrogen to 70% by volume was supplied to the gas phase 14 of the reaction vessel 11 to start the reaction to obtain iodine pentafluoride from iodine and fluorine gas. The pressure in the reaction tank 11 during the reaction is maintained at 93 kPa (absolute pressure) by the pressure regulating valve. Furthermore, while cooling, the temperature of the reaction tank 11 during the reaction is 30 to 60°C, and the reaction is performed for 60 minutes.

關於自壓力調整閥排出之氟氣之濃度，利用使用分光光度計UV-Vis(日立高新技術股份有限公司製，型號U2810)之紫外-可視-近紅外分光法所獲得之分光分析，結果以約70體積%進行推移，氟氣幾乎未被消耗，由碘及氟氣獲得五氟化碘之反應未進行。除實驗開始前裝入部分以外，五氟化碘之新生成量僅為0.0025g。 Regarding the concentration of the fluorine gas discharged from the pressure adjustment valve, the spectrophotometric analysis obtained by the ultraviolet-visible-near infrared spectrophotometry using a spectrophotometer UV-Vis (manufactured by Hitachi High-Technologies Co., Ltd. model U2810), the results are approximately As 70% by volume progresses, the fluorine gas is almost not consumed, and the reaction to obtain iodine pentafluoride from iodine and fluorine gas does not proceed. Except for the part loaded before the experiment, the newly generated amount of iodine pentafluoride is only 0.0025g.

實施例3 Example 3

使用實施例1中所獲得之五氟化碘，合成七氟化碘。具體之製造順序如下所述。 Using the iodine pentafluoride obtained in Example 1, iodine heptafluoride was synthesized. The specific manufacturing sequence is as follows.

將作為金屬氟化物之氟化鎳(NiF2)(純度99%，Apollo Scientific Limited製造)藉由加壓成型製為顆粒狀(大小4mm×4mm×2mm)。向用作反應器之具備電加熱器及壓力計之鎳製之光亮退火管(內徑為22.1mm，長度為0.3m)中，填充顆粒狀之氟化鎳48g(0.5莫耳)。利用電加熱器對光亮退火管進行加熱，藉此將作為填充物之上述顆粒之溫度設為270℃。於該溫度下，將氟(F2)與五氟化碘(IF5)之混合氣體(莫耳比(F2/IF5)=30.3(F2濃度96.8體積%、IF5濃度3.20體積%))自光亮退火管之兩端之一端(入口)導入，自另一端(出口)排出。 Nickel fluoride (NiF 2 ) (purity 99%, manufactured by Apollo Scientific Limited), which is a metal fluoride, was formed into particles (4 mm×4 mm×2 mm in size) by press molding. A bright annealed tube made of nickel (inner diameter 22.1 mm, length 0.3 m) equipped with an electric heater and a pressure gauge used as a reactor was filled with 48 g (0.5 mole) of particulate nickel fluoride. The bright annealing tube is heated by an electric heater, thereby setting the temperature of the above-mentioned particles as a filler to 270°C. At this temperature, the mixed gas of fluorine (F 2 ) and iodine pentafluoride (IF 5 ) (mol ratio (F 2 /IF 5 )=30.3 (F 2 concentration 96.8% by volume, IF 5 concentration 3.20% by volume )) is introduced from one end (inlet) of the two ends of the bright annealing tube and discharged from the other end (outlet).

此時，將光亮退火管內之壓力設為66.7kPa(絕對壓)，以流量1730cm3/min(滯留時間4秒)使混合氣體流通1小時。又，於混合氣體之流通時，將來自反應器出口之氣體導入至冷卻捕獲器。使用液體氬(溫度：-186℃)作為冷卻捕獲器之冷媒，冷卻捕獲七氟化碘及五氟化碘。於混合氣體之流通結束後，進行冷卻捕獲器內之捕獲物之重量測定、及利用傅立葉變換紅外分光光度計(FT-IR)(島津製作所股份有限公司製造，商品名：Prestige21)對獲得之七氟化碘與五氟化碘之組成進行分析。基於重量測定及組成分析結果，算出以五氟化碘IF5之供給量為基準之相對於七氟化碘之理論捕獲量的產率，結果以五氟化碘為基準之七氟化碘之產率為99.8%。 At this time, the pressure in the bright annealing tube was set to 66.7 kPa (absolute pressure), and the mixed gas was circulated for 1 hour at a flow rate of 1730 cm 3 /min (retention time 4 seconds). In addition, when the mixed gas flows, the gas from the outlet of the reactor is introduced to the cooling trap. Using liquid argon (temperature: -186°C) as the cooling medium for cooling the trap, the iodine heptafluoride and iodine pentafluoride are cooled and captured. After the circulation of the mixed gas is completed, the weight of the captured object in the cooling trap is measured, and the obtained seventh is obtained by using Fourier Transform Infrared Spectrophotometer (FT-IR) (Shimadzu Corporation, trade name: Prestige21). The composition of iodine fluoride and iodine pentafluoride was analyzed. Based on the results of gravimetry and composition analysis, the yield relative to the theoretical capture amount of iodine pentafluoride based on the supply of iodine pentafluoride IF 5 was calculated. The yield was 99.8%.

10‧‧‧反應裝置 10‧‧‧Reaction device

11‧‧‧反應槽(利用冷卻器冷卻) 11‧‧‧Reaction tank (cooled by cooler)

12‧‧‧固體碘 12‧‧‧Solid iodine

13‧‧‧五氟化碘(溶解有碘) 13‧‧‧Iodine pentafluoride (dissolved iodine)

14‧‧‧氣相 14‧‧‧gas phase

15‧‧‧液相(五氟化碘) 15‧‧‧liquid phase (iodine pentafluoride)

16‧‧‧七氟化碘之供給源 16‧‧‧Supply source of iodine heptafluoride

17‧‧‧碘供給源 17‧‧‧Iodine supply source

18‧‧‧惰性氣體之供給源 18‧‧‧Supply source of inert gas

19‧‧‧泵 19‧‧‧Pump

20‧‧‧攪拌器 20‧‧‧Agitator

Claims (7)

一種七氟化碘之製造方法，其包括：對於具有包含碘之液相之五氟化碘之反應槽中供給七氟化碘，且於液相之五氟化碘中使碘與七氟化碘反應，從而獲得五氟化碘之步驟；及使氟氣與所獲得之五氟化碘反應而獲得七氟化碘之步驟，獲得上述七氟化碘之步驟係對於內部具有含有選自由NiF2、FeF3、及CoF2所組成之群之至少1種之金屬氟化物之填充物之反應器中供給五氟化碘氣體及氟氣，並於上述金屬氟化物之溫度為150℃以上且350℃以下而進行反應。 A method for manufacturing iodine heptafluoride, comprising: supplying iodine heptafluoride to a reaction tank having a liquid phase containing iodine containing iodine pentafluoride, and iodine and heptafluoride in liquid phase iodine pentafluoride The step of reacting iodine to obtain iodine pentafluoride; and the step of reacting fluorine gas with the obtained iodine pentafluoride to obtain iodine heptafluoride. 2. Iodine pentafluoride gas and fluorine gas are supplied to the reactor of the filler of at least one metal fluoride of the group consisting of FeF 3 and CoF 2 , and the temperature of the metal fluoride is 150°C or more and The reaction proceeds below 350°C. 如請求項1之七氟化碘之製造方法，其中於獲得上述五氟化碘之步驟中，於上述碘與七氟化碘之反應中，一面於反應槽內進行攪拌，一面供給七氟化碘氣體。 The method for producing iodine heptafluoride according to claim 1, wherein in the step of obtaining the iodine pentafluoride, in the reaction of iodine and iodine heptafluoride, heptafluoride is supplied while stirring in the reaction tank Iodine gas. 如請求項1之七氟化碘之製造方法，其中於獲得上述五氟化碘之步驟中，上述包含碘之液相之五氟化碘係包含溶解之碘之溶液狀態，或於液相中分散及沈澱有固體碘之狀態。 The method for producing iodine heptafluoride according to claim 1, wherein in the step of obtaining the iodine pentafluoride, the iodine pentafluoride in the liquid phase containing iodine is in the state of a solution containing dissolved iodine, or in the liquid phase The state of solid iodine dispersed and Shendian. 如請求項2之七氟化碘之製造方法，其中於獲得上述五氟化碘之步驟中，上述包含碘之液相之五氟化碘係包含溶解之碘之溶液狀態，或於液相中分散及沈澱有固體碘之狀態。 The method for producing iodine heptafluoride according to claim 2, wherein in the step of obtaining the iodine pentafluoride, the iodine pentafluoride in the liquid phase containing iodine is in the state of a solution containing dissolved iodine, or in the liquid phase The state of solid iodine dispersed and Shendian. 如請求項1至4中任一項之七氟化碘之製造方法，其中於獲得上述五氟化碘之步驟中，上述包含碘之液相之五氟化碘中，以相對於碘與五氟化碘之總量之含有率表示，包含碘0.01重量%以上且70重量%以下。 The method for producing iodine heptafluoride according to any one of claims 1 to 4, wherein in the step of obtaining the iodine pentafluoride, the iodine pentafluoride in the liquid phase containing iodine is compared with The content rate of the total amount of iodine fluoride is 0.01% or more and 70% or less of iodine. 如請求項1至4中任一項之七氟化碘之製造方法，其中於獲得上述五氟化碘之步驟中，上述包含碘之液相之五氟化碘中，以相 對於五氟化碘與七氟化碘之總量之含有率表示，包含七氟化碘0.001重量%以上且91重量%以下。 The method for producing iodine heptafluoride according to any one of claims 1 to 4, wherein in the step of obtaining the iodine pentafluoride, in the iodine pentafluoride in the liquid phase containing iodine, the phase The content rate of the total amount of iodine pentafluoride and iodine heptafluoride is expressed as including 0.001 wt% or more and 91 wt% or less of iodine heptafluoride. 如請求項5之七氟化碘之製造方法，其中於獲得上述五氟化碘之步驟中，上述包含碘之液相之五氟化碘中，以相對於五氟化碘與七氟化碘之總量之含有率表示，包含七氟化碘0.001重量%以上且91重量%以下。 The method for producing iodine heptafluoride according to claim 5, wherein in the step of obtaining the iodine pentafluoride, the iodine pentafluoride in the liquid phase containing iodine is compared with the iodine pentafluoride and iodine heptafluoride The content rate of the total amount indicates that iodine heptafluoride is included in 0.001% by weight or more and 91% by weight or less.
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