JP2014034493A5 - - Google Patents

Description

The hydrogen addition device 4 is connected to the reaction device 3 through a gas extraction port 3d and a hydrogen addition port 3e. That is, the hydrogen adding device 4 is supplied from a hydrogen supply source 4a configured by, for example, a high-pressure hydrogen cylinder, an analyzer 4b for determining the oxygen concentration of argon gas, and a hydrogen supply source 4a according to the oxygen concentration determined by the analyzer 4b. A hydrogen amount adjuster 4c for adjusting the amount of hydrogen produced. The analyzer 4b is connected to the gas extraction port 3d, and obtains the oxygen concentration of the argon gas in the connection region 3C extracted from the gas extraction port 3d. The hydrogen supply source 4a is connected to the hydrogen addition port 3e via the hydrogen amount regulator 4c. The hydrogen amount adjuster 4c adjusts the amount of hydrogen supplied from the hydrogen supply source 4a by, for example, adjusting the opening of a pipe connecting the hydrogen supply source 4a and the hydrogen addition port 3e with a flow control valve or the like. It adjusts according to the oxygen concentration calculated | required by. This adjustment, the amount of hydrogen added from hydrogenated port 3e in argon gas, with less than stoichiometric amount required to react with all of the oxygen remaining in the argon gas by the reaction in the first reaction zone 3A Is done. As a result, a hydrogen addition step of adding less than the stoichiometric amount of hydrogen necessary to react with all of the oxygen remaining in the argon gas by the execution of the first reaction step to the argon gas is executed. The In the present embodiment, the amount of hydrogen added to the argon gas in the hydrogen addition step is 95% or more and 100% of the stoichiometric amount necessary to react with all of the oxygen remaining in the argon gas by performing the first reaction step. Less than. That is, by this hydrogen addition, the hydrogen molar concentration in the argon gas is made 1.9 times or more and less than 2 times the oxygen molar concentration.

FIG. 3 shows a modification of the reaction device 3. The difference from the above embodiment is that the reactor 3 includes a first reaction vessel 3 b ′, a second reaction vessel 3 a ′, and a pipe 3 c ′ connecting the first reaction vessel 3 b ′ and the second reaction vessel 3 a ′. Have The inside of the first reaction vessel 3 b ′ is the first reaction region 3A, the inside of the second reaction vessel 3 a ′ is the second reaction region 3B, the inside of the pipe 3c ′ is the connection region 3C, The catalyst is not filled. The hydrogen addition port 3e is disposed so as to communicate with the connection region 3C. The rest is the same as in the above embodiment.

FIG. 4 shows a purification apparatus α ′ according to a modification of the present invention. In this modification, an activated carbon adsorption tower 22 connected to the heater 2 is provided, and activated carbon that adsorbs part of hydrocarbons and oil contained in argon gas is accommodated in the activated carbon adsorption tower 22 . Argon gas supplied from the supply source 1 is recovered by the gas feeding means 7 and introduced into the heater 2 via the dust removal filter 21 and the activated carbon adsorption tower 22. This modified example contains oxygen, hydrogen, carbon monoxide and nitrogen originally contained as an impurity in the argon gas as well as hydrocarbons and oils added before the first reaction step, and the amount of oxygen contained from the beginning. Is greater than the stoichiometric amount required to react with all of the initially contained hydrogen, carbon monoxide, and added hydrocarbons.