Integrated process and catalyst for producing hydrogen iodide from hydrogen and iodine

Abstract

To provide a process for producing hydrogen iodide.SOLUTION: The process includes providing a vapor-phase reactant stream comprising hydrogen and iodine and reacting the reactant stream in the presence of a catalyst to produce a product stream comprising hydrogen iodide. The catalyst includes at least one selected from the group of nickel, cobalt, iron, nickel oxide, cobalt oxide, and iron oxide. The catalyst is supported on a support.SELECTED DRAWING: Figure 1

Description

[Technical Field]

[0001] This disclosure relates to a process for producing hydrogen iodide. Specifically, this disclosure relates to: A process for producing anhydrous hydrogen iodide from hydrogen and iodine in the presence of a catalyst. . [Background technology]

[0002] Hydrogen iodide is used as a reducing agent, as well as hydroiodic acid, organic and inorganic iodides. It is an important industrial chemical used in the preparation of iodoalkanes. However, Furthermore, due to its instability and reactivity, hydrogen iodide is extremely difficult to handle. For example, hydrogen iodide decomposes in the presence of heat or light to form hydrogen and iodine. In the presence of moisture, hydrogen iodide forms hydroiodic acid, which can corrode most metals. Due to the instability and reactivity of hydrogen iodide, storage and transportation become difficult. Therefore, Anhydrous hydrogen iodide is often prepared topically for immediate use.

[0003] Various methods for producing hydrogen iodide have been reported. For example, NNGre enwood et al., The Chemistry of the Elements, 2n d edition,Oxford:Butterworth-Heineman,p8 Referring to 09-815, 1997, here hydrogen iodide is an element according to the following equation 1. It is prepared by the reaction of iodine and hydrazine. Equation 1: 2I2+N2H4→4HI+N2

[0004] In another example, Textbook of Practical Organic Chemistry, 3 rdIn this edition, AIVogel is as follows: According to Equation 2, hydrogen iodide can be prepared by reacting a stream of hydrogen sulfide with iodine. It is teaching that you can do it. Equation 2: H2S+I2→2HI+S [Overview of the project] [Problems that the invention aims to solve]

[0005] Each of the above examples uses an expensive starting material such as hydrogen sulfide or hydrazine. However, this limits its use to the economical preparation of large quantities of hydrogen iodide. Furthermore, The use of hydrazine for the preparation of hydrogen gas results in the formation of nitrogen gas as a byproduct. Separating nitrogen gas from hydrogen iodide to purify hydrogen iodide is difficult and expensive. Therefore, it increases manufacturing costs. Similarly, the use of hydrogen sulfide leads to the formation of sulfur. This makes it difficult to separate from unreacted iodine, increasing manufacturing costs. Sulfur can weaken any catalyst used, further increasing manufacturing costs.

[0006] In some other embodiments, hydrogen iodide is converted to elemental iodine according to Equation 3 below. It is prepared from elemental and hydrogen gas. Equation 3: H2+I2→2HI Such examples do not produce nitrogen or sulfur, thus allowing for the production of high-purity hydrogen iodide. It can be easily produced. For example, Japanese Patent Publication No. 4713895B2 describes a catalyst produced by a precious metal-based catalyst. This describes the preparation of hydrogen iodide in a gas phase using hydrogen gas and iodine vapor. Specifically, The disclosed reactions involve magnesium oxide, titanium oxide, silica oxide, alumina, and magnesium oxide. Platinum, rhodium, palladium, and a metal oxide selected from luconia are supported on a metal oxide. It can be catalyzed by ruthenium. However, the use of noble metal catalysts for the preparation of hydrogen iodide will generally further increase the production cost due to the high cost of noble metals. Therefore, an alternative metal catalyst that does not contain noble metals is needed to catalyze the reaction between hydrogen and iodine to produce hydrogen iodide.

[0007] The present disclosure includes the use of a catalyst comprising at least one selected from the group consisting of nickel, cobalt, iron, nickel oxide, cobalt oxide, and iron oxide supported on a carrier, for an integrated process for the production of hydrogen iodide (HI) from hydrogen (H2 ) and elemental iodine (I2).

[0008] In one embodiment, the present invention provides a process for producing hydrogen iodide. The process includes providing a gas-phase reactant stream containing hydrogen and iodine, and reacting the reactant stream in the presence of a catalyst to produce a product stream containing hydrogen iodide. The catalyst comprises at least one selected from the group consisting of nickel, cobalt, iron, nickel oxide, cobalt oxide, and iron oxide. The catalyst is supported on a carrier.

[0009] In another embodiment, the present invention provides a process for producing hydrogen iodide. The process includes reacting hydrogen and iodine in the gas phase in the presence of a catalyst to produce a product stream containing hydrogen iodide and unreacted iodine, cooling the product stream to form solid iodine to remove at least a portion of the unreacted iodine from the product stream, producing liquid iodine from the solid iodine, and recycling the liquefied iodine to the reaction step. Solid iodine is formed in the first or second iodine removal tank. Liquid iodine is, When the product flow is cooled by passing it through the second iodine removal tank, the first iodine removal tank is heated. By liquefying solid iodine, or by passing the product stream through a first iodine removal tank and cooling it... In this case, the second iodine removal tank is heated to liquefy the solid iodine, thereby removing the solid iodine. It is produced from elements. The catalysts are nickel, cobalt, iron, nickel oxide, cobalt oxide, and It contains at least one selected from the group of iron oxides. The catalyst is supported on a carrier. [Brief explanation of the drawing]

[0010] [Figure 1] Figure 1 is a process flow diagram showing the integrated process for producing anhydrous hydrogen iodide.

[0011] [Figure 2] Figure 2 is a process flow diagram showing another integrated process for producing anhydrous hydrogen iodide. [Modes for carrying out the invention]

[0012] This disclosure relates to nickel catalysts, cobalt catalysts, iron catalysts, and nickel oxide supported on a carrier. Hydrogen (H2) and elemental This provides an integrated process for the production of anhydrous hydrogen iodide (HI) from iodine (I2). The use of such catalysts has been found to provide efficient production of hydrogen iodide on a commercial scale. The efficiency of hydrogen iodide production can be further improved by regenerating the reactants. The regeneration of iodine is expensive, with a bulk price of approximately $20 to $100 per kilogram. It is especially important because it is a raw material. However, iodine regeneration is difficult because iodine is 113. Since it is solid below 7°C, this presents a challenge. This disclosure also addresses the efficient and continuous recycling of iodine. This provides an integrated process for producing hydrogen iodide, including raw materials.

[0013] As disclosed herein, anhydrous hydrogen iodide is composed of hydrogen (H2) and iodine (I2) It is produced from a reaction stream containing hydrogen, iodine, and regenerated hydrogen iodide. It may essentially be composed of hydrogen, iodine, and hydrogen iodide. stomach.

[0014] The term "anhydrous iodide" essentially means hydrogen iodide that contains virtually no water. The amount of water in anhydrous hydrogen iodide is approximately 500 ppm by weight, approximately 300 ppm by weight, and approximately 20 0 wt ppm, about 100 wt ppm, about 50 wt ppm, about 30 wt ppm, about 20 wt ppm, approximately 10 ppm by weight, approximately 5 ppm by weight, approximately 3 ppm by weight, approximately 2 ppm by weight, or This is an amount less than approximately 1 ppm by weight, or defined as being between any two of the aforementioned values. The amount is less than any given value. Preferably, the amount of anhydrous hydrogen iodide is less than about 100 ppm by weight. Contains an amount of water. More preferably, anhydrous hydrogen iodide in an amount of less than about 10 ppm by weight of water. It contains. Most preferably, the anhydrous hydrogen iodide contains less than about 1 ppm by weight of water.

[0015] The presence of moisture can be corrosive and harmful to downstream equipment and process lines, such as iodine. To facilitate the formation of hydroacids, it is desirable to have as little water as possible in the reactant stream. This is preferable. In addition, recovering hydrogen iodide from hydroiodic acid increases manufacturing costs. Add.

[0016] Hydrogen contains virtually no water, less than approximately 500 ppm by weight, less than approximately 300 ppm by weight. Less than approximately 200 ppm by weight, less than approximately 100 ppm by weight, less than approximately 50 ppm by weight, approximately 30 ppm by weight Less than ppm, less than approximately 20 ppm by weight, less than 10 ppm by weight, or less than approximately 5 ppm by weight. In an amount of water, or in an amount less than any value defined between any two of the aforementioned values, Preferably, the hydrogen contains any water in an amount of less than about 50 ppm by weight. More preferably The hydrogen is present in any water in an amount of less than about 10 ppm by weight. Most preferably, the hydrogen is present in about 5 Contains any amount of water in amounts less than ppm by weight.

[0017] Hydrogen contains virtually no oxygen. That is, any oxygen in hydrogen is approximately 500g by weight. Less than ppm, less than approximately 300 ppm by weight, less than approximately 200 ppm by weight, less than approximately 100 ppm by weight Full, less than approximately 50 ppm by weight, less than approximately 30 ppm by weight, less than approximately 20 ppm by weight, approximately 10 ppm by weight Less than ppm, less than approximately 5 ppm by weight, less than approximately 3 ppm by weight, less than approximately 2 ppm by weight, or An amount less than approximately 1 ppm by weight, or an amount defined between any two of the aforementioned values. The amount is less than the specified value. Preferably, the amount of oxygen in hydrogen is less than about 100 ppm by weight. More preferably, the amount of oxygen in the hydrogen is less than about 10 ppm by weight. Most preferably, The amount of oxygen in hydrogen is less than approximately 1 ppm by weight. Oxygen can react with hydrogen to form water. Therefore, it is preferable that oxygen is not present in the hydrogen as much as possible.

[0018] Iodine contains virtually no water, at less than approximately 500 ppm by weight, and less than approximately 300 ppm by weight. , less than approximately 200 ppm by weight, less than approximately 100 ppm by weight, less than approximately 50 ppm by weight, approximately 30 ppm by weight Less than ppm by volume, less than approximately 20 ppm by weight, or less than approximately 10 ppm by weight, or the aforementioned values It contains water in an amount less than any value defined between any two of these values. Preferably, iodine is and any amount of water less than approximately 100 ppm by weight. More preferably, iodine is present in approximately 30 ppm by weight. Contains any amount of water in less than ppm. Most preferably, iodine is less than about 10 ppm by weight. Contains any amount of water.

[0019] Elemental iodine in solid form is, for example, SQM, Santiago, Chile, or Kanto Natural Gas Development Co.,Ltd,Ch It is commercially available from IBA, Japan. Compressed hydrogen gas is, for example, Airgas From Radnor, PA, or Air Products and Chemical It is commercially available from s, Inc. (Allentown, PA).

[0020] In the reactant stream, the molar ratio of hydrogen to iodine is, for example, approximately 1:1, approximately 1.5:1, approximately A ratio of 2:1, approximately 2.5:1, approximately 2.7:1, or even as low as approximately 3:1, or approximately 4 :1, approximately 5:1, approximately 6:1, approximately 7:1, approximately 8:1, approximately 9:1, or approximately 10:1 Height is also acceptable, or approximately 1:1 to 10:1, 2:1 to 8:1, 3:1 to 6 :1, approximately 2:1 to approximately 5:1, approximately 2:1 to approximately 3:1, approximately 2.5:1 to approximately 3:1, or approximately Any value defined between any two of the aforementioned values, such as 2.7:1 to approximately 3.0:1 It may be within a certain range. Preferably, the molar ratio of hydrogen to iodine is about 2:1 to about 5:1. Yes. More preferably, the molar ratio of hydrogen to iodine is about 2:1 to about 3:1. More precisely, the molar ratio of hydrogen to iodine is approximately 2.5:1 to approximately 3:1.

[0021] The reactant stream reacts in the presence of the catalyst contained in the reactor, and according to equation 3 above, It produces a product stream containing hydrogen iodide water. The reactor consists of fixed-bed tubes containing a catalyst. It may also be a heated tube reactor such as a tubular reactor. The tubes may be stainless steel, nickel, and / or Nickel alloys, for example, nickel-chromium alloys, nickel-molybdenum alloys, nickel -Chromium-molybdenum alloy, nickel-iron-chromium alloy, or nickel-copper alloy, etc. It may also be made of metal. By heating the tube reactor, the catalyst is also heated. The reactor is, for example, a multi-tube type reactor in which the catalyst is packed into the tubes and the heat transfer medium is in contact with the outside of the tubes. Any type of packed reactor may be used, such as a reactor (e.g., a shell-tube reactor). The reactor may be operated isothermally or adiabatically.

[0022] As mentioned above, the catalyst consists of nickel, cobalt, iron, nickel oxide, and cobalt oxide on a support. The catalyst is nickel, cobalt, iron, and / or iron oxide. Therefore, the catalyst is nickel, cobalt, iron, acid The catalyst comprises at least one selected from the group consisting of nickel oxide, cobalt oxide, and iron oxide. It is supported on a carrier. The carrier is activated carbon, silica gel, zeolite, silicon carbide, metal acid A selection can be made from the group of oxides and combinations thereof. As a non-exclusive example of metal oxides... These include alumina, magnesium oxide, titanium oxide, zinc oxide, zirconia, chromia, and These are some possible combinations.

[0023] The catalyst may contain nickel on a silica gel support. The catalyst may contain nickel on a zeolite support. The catalyst may contain Kel. The catalyst may contain nickel on an activated carbon support. The catalyst may contain silicon carbide support. It may contain nickel on top. The catalyst can essentially consist of nickel on a silica gel support. The catalyst can essentially consist of nickel on a zeolite support. The catalyst can consist of nickel on an activated carbon support. The catalyst can essentially be made from nickel. The catalyst can essentially be made from nickel on a silicon carbide support. The catalyst may consist of nickel on a silica gel support. The catalyst may consist of nickel on a zeolite support. The catalyst may consist of nickel on an activated carbon support. The catalyst may consist of silica carbide. It can consist of nickel on an elementary support.

[0024] The catalyst may contain nickel on a metal oxide support. It can essentially consist of Kel. The catalyst can consist of nickel on a metal oxide support. The catalyst is The catalyst may contain nickel on an alumina support. The catalyst may contain nickel on a titanium oxide support. The catalyst may contain nickel on a zinc oxide support. It may contain nickel. The catalyst may contain nickel on a zirconia support. The catalyst is chromium The support may contain nickel. The catalyst can essentially consist of nickel on an alumina support. The catalyst can essentially consist of nickel on a magnesium oxide support. The catalyst can essentially be made from nickel on a zinc oxide support. It can be qualitative. The catalyst can essentially be nickel on a zirconia support. The catalyst is The catalyst can essentially consist of nickel on a chromia support. The catalyst may consist of nickel on a magnesium oxide support. The catalyst may consist of nickel on a tungsten support. The catalyst may consist of nickel on a zirconia support. The catalyst may consist of nickel on a chromia support. It can consist of.

[0025] The catalyst may contain nickel oxide on a silica gel support. The catalyst may also contain nickel oxide on a zeolite support. It may contain nickel oxide. The catalyst may contain nickel oxide on an activated carbon support. The catalyst is carbon The catalyst may contain nickel oxide on a silicon dioxide support. The catalyst can essentially consist of nickel oxide on a zeolite support. The catalyst can essentially consist of nickel oxide on an activated carbon support. The catalyst can also consist of a silicon carbide support. It can essentially be made from nickel oxide. The catalyst is made from nickel oxide on a silica gel support. The catalyst may consist of nickel oxide on a zeolite support. The catalyst may consist of nickel oxide on an activated carbon support. The catalyst may consist of nickel oxide. The catalyst may consist of nickel oxide on a silicon carbide support.

[0026] The catalyst may contain nickel oxide on a metal oxide support. It can essentially consist of nickel oxide. The catalyst consists of nickel oxide on a metal oxide support. The catalyst may contain nickel oxide on an alumina support. The catalyst may contain magnesium oxide on an alumina support. The catalyst may contain nickel oxide on the body. The catalyst may contain nickel oxide on a titanium oxide support. The catalyst may contain nickel oxide on a zinc oxide support. The catalyst may contain nickel oxide on a zirconia support. The catalyst may contain nickel oxide on a chromia support. The catalyst may contain aluminum It can essentially consist of nickel oxide on a magnesium oxide support. The catalyst is made of nickel oxide on a magnesium oxide support. It can essentially be made from nickel. The catalyst is essentially made from nickel oxide on a titanium oxide support. It is possible. The catalyst can essentially be nickel oxide on a zinc oxide support. The catalyst is zir The catalyst can essentially consist of nickel oxide on a conia support. It can essentially consist of Kell. The catalyst can consist of nickel oxide on an alumina support. Catalyst The catalyst may consist of nickel oxide on a magnesium oxide support. It can consist of nickel oxide. The catalyst can consist of nickel oxide on a zinc oxide support. Catalyst The catalyst may consist of nickel oxide on a zirconia support. It can consist of kel.

[0027] The catalyst may contain nickel and nickel oxide on a silica gel support. The catalyst is a zeola The catalyst may contain nickel and nickel oxide on an activated carbon support. It may contain nickel and nickel oxide. The catalyst contains nickel and nickel oxide on a silicon carbide support. It is possible. The catalyst can essentially consist of nickel and nickel oxide on a silica gel support. The catalyst can essentially consist of nickel and nickel oxide on a zeolite support. The catalyst can essentially consist of nickel and nickel oxide on an activated carbon support. The catalyst can essentially consist of nickel and nickel oxide on a silica gel support. It may consist of nickel and nickel oxide. The catalyst consists of nickel and nickel oxide on a zeolite support. It can consist of nickel. The catalyst can consist of nickel and nickel oxide on an activated carbon support. The catalyst may consist of nickel and nickel oxide on a silicon carbide support.

[0028] The catalyst may contain nickel and nickel oxide on a metal oxide support. The catalyst can essentially consist of nickel and nickel oxide on a metal oxide support. The above may consist of nickel and nickel oxide. The catalyst is made of nickel and acid on an alumina support. It may contain nickel oxide. The catalyst contains nickel and nickel oxide on a magnesium oxide support. It may contain. The catalyst may contain nickel and nickel oxide on a titanium oxide support. The catalyst is The catalyst may contain nickel and nickel oxide on a zinc oxide support. It may contain nickel and nickel oxide. The catalyst is made of nickel and nickel oxide on a chromia support. It may contain nickel. The catalyst can essentially consist of nickel and nickel oxide on an alumina support. The catalyst can essentially consist of nickel and nickel oxide on a magnesium oxide support. The catalyst can essentially consist of nickel and nickel oxide on a titanium oxide support. The catalyst can essentially consist of nickel and nickel oxide on a zinc oxide support. The catalyst may essentially consist of nickel and nickel oxide on a support. It can essentially consist of nickel and nickel oxide. The catalyst is nickel on an alumina support. It can consist of nickel and nickel oxide. The catalyst is nickel and nickel oxide on a magnesium oxide support. It can consist of a kerl. The catalyst can consist of nickel and nickel oxide on a titanium oxide support. The catalyst may consist of nickel and nickel oxide on a zinc oxide support. The catalyst may consist of nickel and nickel oxide on a support. It may also consist of nickel oxide.

[0029] The catalyst may contain cobalt on a silica gel support. The catalyst may contain cobalt on a zeolite support. The catalyst may contain cobalt. The catalyst may contain cobalt on an activated carbon support. The catalyst may contain silicon carbide support It may contain cobalt. The catalyst can essentially consist of cobalt on a silica gel support. The catalyst can essentially consist of cobalt on a zeolite support. The catalyst can also consist of cobalt on an activated carbon support. The catalyst can essentially be made from cobalt on a silicon carbide support. The catalyst may consist of cobalt on a silica gel support. The catalyst may consist of cobalt on a zeolite support. It can consist of balt. The catalyst can consist of cobalt on an activated carbon support. The catalyst is silica carbide. It can consist of cobalt on an elementary support.

[0030] The catalyst may contain cobalt on a metal oxide support. The catalyst can essentially consist of cobalt. The catalyst can consist of cobalt on a metal oxide support. The catalyst is The catalyst may contain cobalt on an alumina support. The catalyst may contain cobalt on a titanium oxide support. The catalyst may contain cobalt on a zinc oxide support. The catalyst may contain cobalt. The catalyst may contain cobalt on a zirconia support. The catalyst may contain chromium The alumina support may contain cobalt. The catalyst can essentially consist of cobalt on an alumina support. The catalyst can essentially consist of cobalt on a magnesium oxide support. The catalyst can essentially be made from cobalt on a tan support. It can be qualitative. The catalyst can essentially be made from cobalt on a zirconia support. The catalyst is It can essentially consist of cobalt on a chromia support. The catalyst is cobalt on an alumina support or The catalyst may consist of cobalt on a magnesium oxide support. The catalyst may consist of cobalt on a tungsten support. The catalyst may consist of cobalt on a zirconia support. The catalyst may consist of cobalt on a chromia support. It can consist of.

[0031] The catalyst may contain cobalt oxide on a silica gel support. The catalyst may also contain cobalt oxide on a zeolite support. It may contain cobalt oxide. The catalyst may contain cobalt oxide on an activated carbon support. The catalyst is carbon The silicon dioxide support may contain cobalt oxide. The catalyst may contain cobalt oxide on a silica gel support. The catalyst can essentially consist of cobalt oxide on a zeolite support. The catalyst can essentially consist of cobalt oxide on an activated carbon support. The catalyst can also consist of cobalt oxide on a silicon carbide support. It can essentially be made from cobalt oxide. The catalyst is made from cobalt oxide on a silica gel support. The catalyst may consist of cobalt oxide on a zeolite support. It can consist of cobalt oxide. The catalyst can consist of cobalt oxide on a silicon carbide support.

[0032] The catalyst may contain cobalt oxide on a metal oxide support. It can essentially consist of cobalt oxide. The catalyst consists of cobalt oxide on a metal oxide support. The catalyst may contain cobalt oxide on an alumina support. The catalyst may contain magnesium oxide on an alumina support. The catalyst may contain cobalt oxide on the body. The catalyst may contain cobalt oxide on the titanium oxide support. The catalyst may contain cobalt oxide on a zinc oxide support. The catalyst may contain cobalt oxide on a zirconia support. May contain balt. The catalyst may contain cobalt oxide on a chromia support. The catalyst may contain aluminum The catalyst can essentially consist of cobalt oxide on a magnesium oxide support. It can essentially be made from cobalt. The catalyst is essentially made from cobalt oxide on a titanium oxide support. It is possible. The catalyst can essentially consist of cobalt oxide on a zinc oxide support. The catalyst is zir The catalyst can essentially consist of cobalt oxide on a conia support. It can essentially consist of oxalt. The catalyst can consist of cobalt oxide on an alumina support. Catalyst The catalyst may consist of cobalt oxide on a magnesium oxide support. It can consist of cobalt oxide. The catalyst can consist of cobalt oxide on a zinc oxide support. Catalyst The catalyst may consist of cobalt oxide on a zirconia support. It can consist of 'rut'.

[0033] The catalyst may contain cobalt and cobalt oxide on a silica gel support. The catalyst may contain cobalt and cobalt oxide on a thread support. It may contain cobalt and cobalt oxide. The catalyst contains cobalt and cobalt oxide on a silicon carbide support. It is possible. The catalyst can essentially consist of cobalt and cobalt oxide on a silica gel support. The catalyst can essentially consist of cobalt and cobalt oxide on a zeolite support. The catalyst can essentially consist of cobalt and cobalt oxide on an activated carbon support. It can essentially consist of cobalt and cobalt oxide on a silica gel support. It may consist of cobalt and cobalt oxide. The catalyst consists of cobalt and cobalt oxide on a zeolite support. It can consist of balt. The catalyst can consist of cobalt and cobalt oxide on an activated carbon support. The catalyst may consist of cobalt and cobalt oxide on a silicon carbide support.

[0034] The catalyst may contain cobalt and cobalt oxide on a metal oxide support. The catalyst can essentially consist of cobalt and cobalt oxide on an oxide support. The catalyst may consist of cobalt and cobalt oxide. The catalyst consists of cobalt and acid on an alumina support. It may contain cobalt oxide. The catalyst consists of cobalt and cobalt oxide on a magnesium oxide support. It may contain. The catalyst may contain cobalt and cobalt oxide on a titanium oxide support. The catalyst is The catalyst may contain cobalt and cobalt oxide on a zinc oxide support. It may contain balt and cobalt oxide. The catalyst consists of cobalt and cobalt oxide on a chromia support. It may contain. The catalyst may essentially consist of cobalt and cobalt oxide on an alumina support. The catalyst can essentially consist of cobalt and cobalt oxide on a magnesium oxide support. The catalyst can essentially consist of cobalt and cobalt oxide on a titanium oxide support. The catalyst can essentially consist of cobalt and cobalt oxide on a zinc oxide support. The catalyst may essentially consist of cobalt and cobalt oxide on a support. The catalyst can essentially consist of cobalt and cobalt oxide. It can consist of cobalt and cobalt oxide. The catalyst consists of cobalt and cobalt oxide on a magnesium oxide support. The catalyst may consist of cobalt and cobalt oxide on a titanium oxide support. The catalyst may consist of cobalt and cobalt oxide on a zinc oxide support. The catalyst may consist of cobalt and cobalt oxide on a support. It may also consist of cobalt oxide.

[0035] The catalyst may contain iron on a silica gel support. The catalyst may contain iron on a zeolite support. The catalyst may contain iron on an activated carbon support. The catalyst may contain iron on a silicon carbide support. The catalyst can essentially consist of iron on a silica gel support. The catalyst can also consist of iron on a zeolite support. The catalyst can essentially consist of iron on an activated carbon support. The catalyst can essentially consist of iron on an iron-containing support. The catalyst can consist of iron on a silica gel support. The medium may consist of iron on a zeolite support. The catalyst may consist of iron on an activated carbon support. The medium may consist of iron on a silicon carbide support.

[0036] The catalyst may contain iron on a metal oxide support. The catalyst is essentially derived from the iron on the metal oxide support. It can be a target. The catalyst may consist of iron on a metal oxide support. The catalyst may consist of iron on an alumina support. It may contain iron. The catalyst may contain iron on a magnesium oxide support. The catalyst may contain titanium oxide support. The catalyst may contain iron on the body. The catalyst may contain iron on a zinc oxide support. The catalyst may contain iron on a zirconia support. The catalyst may contain iron on top. The catalyst may contain iron on a chromia support. The catalyst may contain iron on an alumina support. It can essentially consist of iron. The catalyst can essentially consist of iron on a magnesium oxide support. The catalyst can essentially consist of iron on a titanium oxide support. The catalyst can also consist of iron on a zinc oxide support. Essentially, it can be. The catalyst can essentially be made from iron on a zirconia support. The catalyst is chrome The catalyst can essentially consist of iron on a mia support. The catalyst can consist of iron on an alumina support. The catalyst may consist of iron on a magnesium oxide support. The catalyst may consist of iron on a zinc oxide support. The catalyst may consist of iron on a zirconia support. It is possible. The catalyst may consist of iron on a chromia support.

[0037] The catalyst may contain iron oxide on a silica gel support. The catalyst may contain iron oxide on a zeolite support. The catalyst may contain iron oxide on an activated carbon support. The catalyst may contain acid on a silicon carbide support. It may contain iron oxide. The catalyst may essentially consist of iron oxide on a silica gel support. The catalyst is ze The catalyst can essentially consist of iron oxide on an olite support. It can be a target. The catalyst can essentially consist of iron oxide on a silicon carbide support. The catalyst is sil The catalyst may consist of iron oxide on a Kagel support. The catalyst may consist of iron oxide on a zeolite support. The catalyst may consist of iron oxide on an activated carbon support. The catalyst may consist of iron oxide on a silicon carbide support. It is possible.

[0038] The catalyst may contain iron oxide on a metal oxide support. It can essentially consist of iron oxide on a metal oxide support. The catalyst can consist of aluminum The magnesium oxide support may contain iron oxide. The catalyst may contain iron oxide on a magnesium oxide support. The catalyst may contain iron oxide on a titanium oxide support. The catalyst may contain iron oxide on a zinc oxide support. The catalyst may contain iron oxide on a zirconia support. The catalyst may contain iron oxide on a chromia support. It may include. The catalyst may essentially consist of iron oxide on an alumina support. The catalyst may be magnesium oxide. The catalyst can essentially consist of iron oxide on a nesium support. The catalyst can be made from iron oxide on a titanium oxide support. Essentially, it can be. The catalyst can essentially be iron oxide on a zinc oxide support. The catalyst is di The catalyst can essentially consist of iron oxide on a chromia support. It can be qualitative. The catalyst can consist of iron oxide on an alumina support. The catalyst can be magnesium oxide. The catalyst may consist of iron oxide on a titanium oxide support. The medium may consist of iron oxide on a zinc oxide support. The catalyst may consist of iron oxide on a zirconia support. The catalyst may consist of iron oxide on a chromia support.

[0039] The catalyst may contain iron and iron oxide on a silica gel support. The catalyst may also contain iron and iron oxide on a zeolite support. It may contain iron and iron oxide. The catalyst may contain iron and iron oxide on an activated carbon support. The catalyst is carbon The catalyst may contain iron and iron oxide on a silicon dioxide support. The catalyst can essentially consist of iron and iron oxide on a zeolite support. The catalyst can essentially consist of iron and iron oxide on an activated carbon support. The catalyst can also consist of iron and iron oxide on a silicon carbide support. It can essentially consist of iron and iron oxide. The catalyst is made of iron and iron oxide on a silica gel support. The catalyst may consist of iron and iron oxide on a zeolite support. The catalyst may consist of iron and iron oxide on a silicon carbide support.

[0040] The catalyst may contain iron and iron oxide on a metal oxide support. It can essentially consist of iron and iron oxide. The catalyst consists of iron and iron oxide on a metal oxide support. The catalyst may contain iron and iron oxide on an alumina support. The catalyst may contain iron and iron oxide on the titanium oxide support. The catalyst may contain iron and iron oxide on a zinc oxide support. The catalyst may contain iron and It may contain iron oxide. The catalyst may contain iron and iron oxide on a chromia support. The catalyst may contain aluminum The catalyst can essentially consist of iron and iron oxide on a magnesium oxide support. The catalyst can essentially consist of iron and iron oxide on a titanium oxide support. It is possible. The catalyst can essentially consist of iron and iron oxide on a zinc oxide support. The catalyst is zir The catalyst can essentially consist of iron and iron oxide on a conia support. It can essentially consist of iron oxides. The catalyst can consist of iron and iron oxides on an alumina support. The catalyst may consist of iron and iron oxide on a magnesium oxide support. It may consist of iron and iron oxide. The catalyst may consist of iron and iron oxide on a zinc oxide support. Catalyst The catalyst may consist of iron and iron oxide on a zirconia support. It can be composed of iron oxides.

[0041] The catalyst may contain nickel and cobalt on a silica gel support. The catalyst is a zeolite. The catalyst may contain nickel and cobalt on the support. The catalyst may contain nickel and cobalt on a silicon carbide support. The catalyst can essentially consist of nickel and cobalt on a silica gel support. The catalyst can essentially consist of nickel and cobalt on a carbonized surface. It can essentially consist of cobalt. The catalyst is nickel and cobalt on a silicon carbide support. Essentially, it can be. The catalyst can consist of nickel and cobalt on a silica gel support. The catalyst may consist of nickel and cobalt on a zeolite support. The catalyst may also consist of nickel and cobalt on an activated carbon support. The catalyst may consist of nickel and cobalt on a silicon carbide support. It can consist of "t".

[0042] The catalyst may contain nickel and cobalt on a metal oxide support. The catalyst can essentially consist of nickel and cobalt on a support. It may consist of nickel and cobalt. The catalyst contains nickel and cobalt on an alumina support. The catalyst may contain nickel and cobalt on a magnesium oxide support. The catalyst may contain nickel and cobalt on a titanium oxide support. The catalyst may also contain cobalt. The catalyst may contain nickel and cobalt on a zirconia support. The catalyst may contain nickel and cobalt on a chromia support. The catalyst may also contain nickel and cobalt on an alumina support. The catalyst can essentially consist of nickel and cobalt. It can essentially consist of nickel and cobalt. The catalyst is nickel and cobalt on a titanium oxide support. The catalyst can essentially be derived from nickel and cobalt on a zinc oxide support. This is possible. The catalyst can essentially consist of nickel and cobalt on a zirconia support. The catalyst can essentially consist of nickel and cobalt on a chromia support. The catalyst can also be aluminum The catalyst may consist of nickel and cobalt on a magnesium oxide support. It may consist of nickel and cobalt. The catalyst is made from nickel and cobalt on a titanium oxide support. It is possible. The catalyst may consist of nickel and cobalt on a zinc oxide support. The catalyst is zir The catalyst may consist of nickel and cobalt on a conia support. The catalyst is nickel on a chromia support. It may also consist of cobalt.

[0043] The catalyst may contain nickel oxide and cobalt oxide on a silica gel support. The catalyst may contain nickel oxide and cobalt oxide on an olite support. It may contain nickel oxide and cobalt oxide. The catalyst is made of nickel oxide and cobalt oxide on a silicon carbide support. It may contain cobalt oxide. The catalyst is nickel oxide and cobalt oxide on a silica gel support. Essentially, the catalyst can be derived from nickel oxide and cobalt oxide on a zeolite support. It can be qualitative. The catalyst is essentially made from nickel oxide and cobalt oxide on an activated carbon support. The catalyst can essentially consist of nickel oxide and cobalt oxide on a silicon carbide support. The catalyst may consist of nickel oxide and cobalt oxide on a silica gel support. The catalyst may consist of nickel oxide and cobalt oxide on a zeolite support. The catalyst may consist of nickel oxide and cobalt oxide. It may consist of ammonium compounds and cobalt oxide.

[0044] The catalyst may contain nickel oxide and cobalt oxide on a metal oxide support. The catalyst can essentially consist of nickel oxide and cobalt oxide on a metal oxide support. The catalyst may consist of nickel oxide and cobalt oxide on an oxide support. The catalyst may contain nickel oxide and cobalt oxide. The catalyst may contain nickel oxide and cobalt oxide on a titanium oxide support. It may contain ruth. The catalyst may contain nickel oxide and cobalt oxide on a zinc oxide support. The catalyst may contain nickel oxide and cobalt oxide on a zirconia support. The catalyst is chromium The catalyst may contain nickel oxide and cobalt oxide on an alumina support. It can essentially consist of oxal and cobalt oxide. The catalyst is an oxidation on a magnesium oxide support. It can essentially consist of nickel and cobalt oxide. The catalyst is nickel oxide on a titanium oxide support. It can essentially consist of nickel oxide and cobalt oxide. The catalyst is nickel oxide on a zinc oxide support and It can essentially consist of nickel oxide and acid on a zirconia support. It can essentially consist of cobalt oxide. The catalyst is nickel oxide and cobalt oxide on a chromia support. It can essentially be made from a rut. The catalyst is nickel oxide and cobalt oxide on an alumina support. It can be. The catalyst consists of nickel oxide and cobalt oxide on a magnesium oxide support. The catalyst may consist of nickel oxide and cobalt oxide on a titanium oxide support. The catalyst may consist of nickel oxide and cobalt oxide on a zinc oxide support. The catalyst may consist of nickel oxide and cobalt oxide on a chromia support. It may consist of kel and cobalt oxide.

[0045] The catalyst may contain nickel and iron on a silica gel support. The catalyst may also contain nickel and iron on a zeolite support. It may contain nickel and iron. The catalyst may contain nickel and iron on an activated carbon support. The catalyst may contain nickel and iron on a silicon carbide support. The catalyst can essentially consist of nickel and iron on a zeolite support. It can be. The catalyst can essentially consist of nickel and iron on an activated carbon support. The catalyst is carbon The catalyst can essentially consist of nickel and iron on a silicon dioxide support. It may consist of nickel and iron. The catalyst may consist of nickel and iron on a zeolite support. The catalyst may consist of nickel and iron on an activated carbon support. The catalyst may consist of nickel on a silicon carbide support. It can consist of kel and iron.

[0046] The catalyst may contain nickel and iron on a metal oxide support. The catalyst may essentially consist of nickel and iron on a metal oxide support. The catalyst may contain nickel and iron on an alumina support. The catalyst may contain magnesium oxide. The catalyst may contain nickel and iron on a titanium oxide support. The catalyst may contain nickel and iron on a zinc oxide support. The catalyst may contain zirconia. The support may contain nickel and iron. The catalyst may contain nickel and iron on a chromia support. The catalyst can essentially consist of nickel and iron on an alumina support. The catalyst is magnesium oxide. The catalyst can essentially consist of nickel and iron on a nesium support. It can essentially consist of nickel and iron. The catalyst essentially consists of nickel and iron on a zinc oxide support. It can be a target. The catalyst can essentially consist of nickel and iron on a zirconia support. Catalyst The catalyst can essentially consist of nickel and iron on a chromia support. It may consist of nickel and iron. The catalyst consists of nickel and iron on a magnesium oxide support. The catalyst may consist of nickel and iron on a titanium oxide support. It may consist of nickel and iron on a body. The catalyst consists of nickel and iron on a zirconia support. The catalyst may consist of nickel and iron on a chromia support.

[0047] The catalyst may contain nickel oxide and iron oxide on a silica gel support. The catalyst may contain nickel oxide and iron oxide on an activated carbon support. It may contain iron oxide. The catalyst may contain nickel oxide and iron oxide on a silicon carbide support. The catalyst can essentially consist of nickel oxide and iron oxide on a silica gel support. The catalyst may essentially consist of nickel oxide and iron oxide on an olite support. The catalyst can essentially consist of nickel oxide and iron oxide. It can essentially consist of nickel oxide and iron oxide. The catalyst is nickel oxide and acid on a silica gel support. It may consist of iron oxides. The catalyst may consist of nickel oxide and iron oxide on a zeolite support. The catalyst may consist of nickel oxide and iron oxide on an activated carbon support. The catalyst may consist of a silicon carbide support. It may consist of the nickel oxide and iron oxide shown above.

[0048] The catalyst may contain nickel oxide and iron oxide on a metal oxide support. The catalyst may essentially consist of nickel oxide and iron oxide on a metal oxide support. It may consist of nickel oxide and iron oxide. The catalyst consists of nickel oxide and iron oxide on an alumina support. It may contain iron. The catalyst may contain nickel oxide and iron oxide on a magnesium oxide support. The catalyst may contain nickel oxide and iron oxide on a titanium oxide support. The catalyst may contain zinc oxide support. The catalyst may contain nickel oxide and iron oxide on a zirconia support. It may contain iron oxide. The catalyst may contain nickel oxide and iron oxide on a chromia support. It can essentially consist of nickel oxide and iron oxide on an alumina support. The catalyst is magnesium oxide. The catalyst can essentially consist of nickel oxide and iron oxide on a nesium support. The catalyst can essentially consist of nickel oxide and iron oxide on a zinc oxide support. It can essentially consist of nickel and iron oxide. The catalyst is nickel oxide and on a zirconia support. It can essentially consist of iron oxide. The catalyst is essentially made from nickel oxide and iron oxide on a chromia support. It can be qualitative. The catalyst may consist of nickel oxide and iron oxide on an alumina support. The catalyst may consist of nickel oxide and iron oxide on a magnesium oxide support. The catalyst may consist of nickel oxide and iron oxide on a zinc oxide support. It may consist of nickel oxide and iron oxide. The catalyst consists of nickel oxide and iron oxide on a zirconia support. The catalyst may consist of nickel oxide and iron oxide on a chromia support.

[0049] The catalyst may contain cobalt and iron on a silica gel support. The catalyst may also be on a zeolite support. It may contain cobalt and iron. The catalyst may contain cobalt and iron on an activated carbon support. The catalyst may contain cobalt and iron on a silicon carbide support. The catalyst can essentially consist of cobalt and iron on a zeolite support. It can be. The catalyst can essentially consist of cobalt and iron on an activated carbon support. The catalyst is carbon The catalyst can essentially consist of cobalt and iron on a silicon dioxide support. It may consist of cobalt and iron. The catalyst may consist of cobalt and iron on a zeolite support. The catalyst may consist of cobalt and iron on an activated carbon support. The catalyst may consist of cobalt on a silicon carbide support. It can consist of ruth and iron.

[0050] The catalyst may contain cobalt and iron on a metal oxide support. The catalyst can essentially consist of cobalt and iron. The catalyst may contain cobalt and iron on an alumina support. The catalyst may contain cobalt and iron on a titanium oxide support. The catalyst may contain cobalt and iron on a zinc oxide support. The support may contain cobalt and iron. The catalyst may contain cobalt and iron on a chromia support. The catalyst can essentially consist of cobalt and iron on an alumina support. The catalyst is magnesium oxide. The catalyst can essentially consist of cobalt and iron on a nesium support. It can essentially consist of cobalt and iron. The catalyst essentially consists of cobalt and iron on a zinc oxide support. It can be a target. The catalyst can essentially consist of cobalt and iron on a zirconia support. Catalyst The catalyst can essentially consist of cobalt and iron on a chromia support. It may consist of cobalt and iron. The catalyst consists of cobalt and iron on a magnesium oxide support. The catalyst may consist of cobalt and iron on a titanium oxide support. It may consist of cobalt and iron on a body. The catalyst consists of cobalt and iron on a zirconia support. The catalyst may consist of cobalt and iron on a chromia support.

[0051] The catalyst may contain cobalt oxide and iron oxide on a silica gel support. The catalyst may contain cobalt oxide and iron oxide on an activated carbon support. It may contain iron oxide. The catalyst may contain cobalt oxide and iron oxide on a silicon carbide support. The catalyst can essentially consist of cobalt oxide and iron oxide on a silica gel support. The catalyst may essentially consist of cobalt oxide and iron oxide on an olite support. The catalyst can essentially consist of cobalt oxide and iron oxide. It can essentially consist of cobalt and iron oxide. The catalyst is cobalt oxide and acid on a silica gel support. It may consist of iron oxides. The catalyst may consist of cobalt oxide and iron oxide on a zeolite support. The catalyst may consist of cobalt oxide and iron oxide on an activated carbon support. The catalyst may consist of a silicon carbide support. It may consist of the above cobalt oxide and iron oxide.

[0052] The catalyst may contain cobalt oxide and iron oxide on a metal oxide support. The catalyst may essentially consist of cobalt oxide and iron oxide on a metal oxide support. It may consist of cobalt oxide and iron oxide. The catalyst consists of cobalt oxide and iron oxide on an alumina support. It may contain iron. The catalyst may contain cobalt oxide and iron oxide on a magnesium oxide support. The catalyst may contain cobalt oxide and iron oxide on a titanium oxide support. The catalyst may contain zinc oxide support. The catalyst may contain cobalt oxide and iron oxide on a zirconia support. It may contain iron oxide. The catalyst may contain cobalt oxide and iron oxide on a chromia support. Catalyst It can essentially consist of cobalt oxide and iron oxide on an alumina support. The catalyst is magnesium oxide. The catalyst can essentially consist of cobalt oxide and iron oxide on a nesium support. The catalyst can essentially consist of cobalt oxide and iron oxide on a zinc oxide support. It can essentially consist of cobalt and iron oxide. The catalyst is cobalt oxide and on a zirconia support. It can essentially consist of iron oxide. The catalyst is essentially made from cobalt oxide and iron oxide on a chromia support. It can be qualitative. The catalyst may consist of cobalt oxide and iron oxide on an alumina support. Catalyst The catalyst may consist of cobalt oxide and iron oxide on a magnesium oxide support. The catalyst may consist of cobalt oxide and iron oxide on a zinc oxide support. It may consist of cobalt oxide and iron oxide. The catalyst consists of cobalt oxide and iron oxide on a zirconia support. The catalyst may consist of cobalt oxide and iron oxide on a chromia support.

[0053] The catalyst may be in the form of beads, pellets, extruded materials, powders, spheres, or meshes. Preferably, the catalyst contains nickel on an alumina support. More preferably, the catalyst is pe In lett form, nickel is contained on an alumina support. Most preferably, the catalyst is about 1 mm The material is in the form of pellets with a diameter ranging from approximately 7 mm, containing nickel on an alumina support.

[0054] Catalysts are commercially available. Various formulations of nickel metal supported on alumina (by weight) -cent) is, for example, Honeywell UOP (Des Plaines, IL, It can be obtained from the USA or Johnson Matthey (London, UK).

[0055] The weight percentage of the catalyst, as the ratio of the total weight of the catalyst and the support, is, for example, approximately 0.1% by weight (weight%), approximately 1% by weight, approximately 3% by weight, approximately 5% by weight, approximately 10% by weight It may be as little as about 15% by weight, or about 20% by weight, or about 35% by weight, about 4 It can be 0% by weight, approximately 45% by weight, or even as much as approximately 50% by weight, or approximately 0%. 1% to approximately 50% by weight, approximately 3% to approximately 45% by weight, approximately 10% to approximately 40% by weight, approximately Among the aforementioned values, such as 15% to approximately 35% by weight, or approximately 3% to approximately 25% by weight. It may be within any range defined between any two of the following. Preferably, the weight of the catalyst The concentration is approximately 5% by weight to approximately 45% by weight. More preferably, the weight percentage of the catalyst. The weight percentage of the catalyst is approximately 10% to 40% by weight. Most preferably, the weight percentage of the catalyst is approximately It ranges from 15% to approximately 35% by weight.

[0056] For example, the catalyst can be spread over approximately 1 square meter (m²) per gram. 2 / g), approx. 5m 2 / g, approx. 1 0m 2 / g, approx. 25m 2 / g, approx. 40m 2 / g, approx. 60m 2 / g, or approximately 80m 2 / It may have a surface area as small as g or about 100 m 2 / g, about 120 m 2 / g, about 1 50 m 2 / g, about 200 m 2 / g, about 250 m 2 / g, about 300 m 2 / g, or it may have a surface area as large as about 1 ,000 m 2 / g, or about 1 m 2 / g to about 10 0 m 2 / g, about 5 m 2 / g to about 300 m 2 / g, about 10 m 2 / g to about 250 m 2 / g, about 25 m 2 / g to about 200 m 2 / g, about 40 m 2 / g to about 150 m 2 / g, about 60 m 2 / g to about 120 m[[ID=**47**]] 2 / g, or about 80 m 2 / g to about 120 m 2 It may have a surface area within any range defined between any two of the foregoing values, such as about 1 m / g, about 5 m / g, about 10 m / g, about 25 m / g, about 40 m / g, about 60 m / g, about 80 m / g, about 120 m / g, about 150 m / g, about 200 m / g, about 250 m / g, about 300 m / g, about 1,000 m / g. The surface area of the catalyst is determined by the BET method according to ISO 9277:2010. <000069​​​​​​​​​​​​ Any two of the aforementioned values, such as 0 seconds to approximately 20 seconds, or approximately 100 seconds to approximately 120 seconds. The catalyst may be in contact with the contact time for any range defined between the two. Preferably, the reaction The material flow is in contact with the catalyst for a contact time of approximately 2 seconds to approximately 200 seconds. More preferably, The material flow is in contact with the catalyst for a contact time of approximately 40 to 100 seconds. Most preferably, The reactant stream is in contact with the catalyst for a contact time of approximately 60 to 80 seconds.

[0058] The reactant flow and catalyst may be preheated to the reaction temperature. The reaction temperature is, for example, about 1 50℃, approximately 200℃, approximately 250℃, approximately 280℃, approximately 290℃, approximately 300℃, approximately 310℃, Alternatively, it can be about 320°C lower, or about 330°C, about 340°C, about 350°C, about 3 60°C, approximately 380°C, approximately 400°C, approximately 450°C, approximately 500°C, approximately 550°C, or approximately 6 The reaction temperature can be as high as 00°C, or approximately 150°C to 600°C, or approximately 200°C. ℃ to approximately 550℃, approximately 250℃ to approximately 500℃, approximately 280℃ to approximately 450℃, approximately 290℃ to approximately 4 00℃, approximately 300℃ to approximately 380℃, approximately 310℃ to approximately 360℃, approximately 320℃ to approximately 350℃, Alternatively, it can be defined as being between any two of the aforementioned values, such as approximately 320°C to approximately 340°C. It may be within any range. Preferably, the reaction temperature is about 200°C to about 500°C. More preferably, the reaction temperature is about 300°C to about 400°C. Most preferably, the reaction The temperature is approximately 300°C to 350°C.

[0059] Hydrogen in the flow of reactants into the reactor is converted to the corresponding metals, nickel oxide, and nickel oxide. A catalyst containing balt and / or iron oxide is reduced. Preferably, such a catalyst reacts The catalyst is reduced by the flow of hydrogen passing through the reactor, and then reduced to the corresponding metal.

[0060] The operating pressure of the reactor is, for example, about 10 kPag (kilopascals, gauge pressure), about 50 kPag, approximately 100kPag, approximately 200kPag, approximately 300kPag, approximately 400kPag Alternatively, it may be lower, around 600kPag, or around 800kPag, or around 1,000k Pag, about 1,500kPag, about 2,000kPag, about 2,500kPag, about 3, 000kPag, or even about 4,000kPag higher, or about 10kPag ag ~ approximately 4,000 kPag, approximately 50 kPag ~ approximately 3,000 kPag, approximately 100 kPa g ~ approx. 2,500kPag, approx. 200kPag ~ approx. 2,000kPag, approx. 300kPa g ~ approximately 1,500 kPag, approximately 400 kPag ~ approximately 1,000 kPag, approximately 600 kPa g to approximately 800 kPag, or approximately 10 kPag to approximately 800 kPag, etc., the aforementioned values It may be any range defined between any two of us. Preferably, the reactor The operating pressure is approximately 10 kPag to approximately 800 kPag. More preferably, the reactor operation The pressure is approximately 10 kPag to approximately 400 kPag. Most preferably, the operating pressure of the reactor. The range is approximately 10kPag to 200kPag.

[0061] Iodine is continuously or intermittently supplied from solid iodine to the reactor, and then to the heated iodine liquefaction apparatus. It is added and supplied to maintain a specific concentration of liquid iodine in the liquefaction device. Liquid iodine Positive pressure is maintained in the liquefaction unit to deliver the liquid iodine to the iodine evaporator. For example, when a pump is used, it is calculated based on the pump stroke volume. Therefore, and / or by passing liquid iodine through a flow meter, the weight of the tank supplying iodine This can be provided by monitoring the decrease. The temperature of iodine in the iodine liquefaction apparatus is the temperature of the iodine The temperature is sufficient to dissolve it, but low enough to avoid the evaporation of iodine. It is maintained in this manner. Liquid iodine evaporates in the evaporator to form iodine vapor. Evaporator The iodine vapor emitted can mix with hydrogen gas from a hydrogen source to form a reactant flow. Alternatively, or in addition to that, hydrogen gas from a hydrogen supply helps in the evaporation of iodine. Therefore, it may be supplied to the iodine evaporator, and thus the evaporation temperature will decrease. In addition, the hydrogen gas may further contain regenerated hydrogen gas and hydrogen iodide. The reactor is preheated to the desired temperature and supplied with one of the catalysts mentioned above. Thermal tracing of the process line between the evaporator and the evaporator indicates whether the iodine remains liquid within these lines. Ensure that it is present up to that point. Process for transporting iodine vapor and hydrogen / iodine vapor mixtures. Thermally trace the line to ensure the gas phase is maintained. Alternatively, iodine can be added in liquid form. Solid iodine may be supplied to a tank that generates iodine vapor by ionization and evaporation.

[0062] Product streams containing hydrogen iodide, unreacted hydrogen, and unreacted iodine are released from the reactor in more than one direction. It is then guided to an iodine removal tank, where the product flow is cooled and unreacted iodine condenses, and the product is formed. This allows at least a portion of the iodine to be removed from the logistics and recycled as a reaction product. Optionally, the product stream may condense unreacted iodine in one or more iodine removal tanks before it condenses. The material is guided to a cooler to remove some of the heat from the material flow. One or more iodine removal tanks. Within the product flow, the boiling point of iodine is lower than that of iodine in order to recover iodine in liquid form. It may be cooled to a temperature above its primary melting point. Alternatively, or in addition, it may be removed from the reactor. The resulting product stream is cooled to a temperature below the melting point of iodine in order to recover iodine in solid form. The product stream may be transported from one or more iodine removal tanks to one or more further iodine removal tanks. The process can then proceed to remove further unreacted iodine for regeneration.

[0063] The product stream, which is substantially free of iodine, is guided from one or more iodine removal tanks to the compressor. This allows the pressure of the product flow to be increased to a separation pressure sufficient for the efficient recovery of unreacted hydrogen. The separation pressure is greater than the reactor's operating pressure. The separation pressure is, for example, approximately 800 kPag. Approximately 850 kPag, approximately 900 kPag, approximately 950 kPag, or approximately 1,000 kPa It can be as low as g, or about 1,100 kPag, about 1,200 kPag, about 1,3 The height is approximately 00kPag, 1,400kPag, or 1,500kPag. To obtain, or approximately 800kPag to approximately 1,500kPag, approximately 850kPag to approximately 1, 400kPag, approximately 900kPag to approximately 1,300kPag, approximately 950kPag to approximately 1, 200kPag, approximately 1,000kPag to approximately 1,100kPag, or approximately 900kPag ag ~ approximately 1,100 kPag, any value defined between any two of the aforementioned values. It may be within the range of approximately 10 kPag to approximately 2,000 kPag. Preferably, the separation pressure is approximately 10 kPag to approximately 2,000 kPag. More preferably, the separation pressure is approximately 300 kPag to approximately 1,500 kPag. Most preferably, the separation pressure is about 600 kPag to about 1,000 kPag.

[0064] The compressed product flow is flash-cooled in one step to recover the liquid and vapor flows. It is subjected to distillation. The vapor stream contains hydrogen and a small amount of hydrogen iodide. The liquid stream contains virtually no hydrogen. It does not contain hydrogen iodide, residual iodine, and other high-boiling-point substances such as any water. The vapor flow can be recycled back into the reactor. The liquid flow contains residual iodine and any residual water in the bottom flow of the tower. From other high-boiling point substances including [unspecified substance], [unspecified substance] is drawn into a distillation column to separate liquid hydrogen iodide in the upper stream. The high-boiling point substances are then directed to the bottom of the distillation column for further processing, including iodine recovery and regeneration. It is derived from the flow. Vapor venting from the overhead of the distillation column is for any non-condensable substance such as hydrogen. It may also be performed as a purge to remove gas.

[0065] Alternatively, the product stream may contain unreacted high-boiling-point substances such as hydrogen iodide and any residual iodine. To separate from low-boiling-point substances such as hydrogen, heavier distillation is performed from one or more iodine removal tanks. It can be guided into a tower. High-boiling-point substances are used to separate hydrogen iodide from residual iodine by heavy vaporization. The bottom flow from the distillation column is guided to the iodine regeneration distillation column. It contains hydrogen and any residual hydrogen iodide. The upper flow from the heavy column is directed to the product distillation column. The column contains residual iodine in the iodine regeneration distillation column. The undercurrent is recycled into an iodine liquefaction unit. Hydrogen iodide is separated from hydrogen, and other non-condensable substances are removed. To separate the gas from the heavy tower and the iodine regeneration tower, hydrogen iodide is used on top of the iodine regeneration tower. The stream is directed to the product distillation column. The upper stream of the product column, containing hydrogen and residual hydrogen iodide, It may be recycled back into the reactor. The bottom flow of the product column contains purified hydrogen iodide.

[0066] In any of the above processes, additional products are produced to increase the purity of hydrogen iodide. A column may be added. The purified hydrogen iodide is then used in subsequent processes, such as any of the above processes. Before use in the process, pass through with an appropriate desiccant to remove any residual moisture. Alternatively, purified hydrogen iodide may be supplied directly to the subsequent process. In addition, purified hydrogen iodide is stored for short-term storage before being used in subsequent processes. It may be collected in a storage tank. The regeneration of iodine and hydrogen is for producing hydrogen iodide. It leads to an efficient process.

[0067] Nickel, cobalt, iron, nickel oxide, and cobalt oxide supported on a carrier according to this disclosure Hydrogen (H2) and elemental iodine (I) are produced using iron oxide and / or iron oxide catalysts. The process for producing hydrogen iodide (HI) from 2) is a batch process, as described below. It may be a single process, or it may be a continuous process.

[0068] Figure 1 is a process flow diagram showing the integrated process for producing anhydrous hydrogen iodide. As shown in Figure 1, the integrated process 10 uses solid iodine 12 and hydrogen gas 14 as materials. This includes flow. Solid iodine 12 can be added to the solid storage tank 16 continuously or intermittently. The flow of solid iodine-18 is carried by a solid transport system (not shown) or by gravity. The iodine is transferred continuously or intermittently from the solid storage tank 16 to the iodine liquefaction device 20, but here Then, solid iodine is heated to a temperature above its melting point but below its boiling point, and then iodine liquefaction apparatus 2 Maintain the level of liquid iodine within 0. Only one liquefaction device 20 is shown, but multiple It is understood that the liquefaction apparatus 20 may be used in parallel. Liquid iodine 22 is iodine The liquid iodine flows from the iodine liquefaction device 20 to the iodine evaporator 24. The flow in step 2 may be pressurized with an inert gas. Examples of inert gases include: For example, nitrogen, argon, or helium, or mixtures thereof may be cited. In addition, the flow of liquid iodine 22 is driven by a pump (not shown). The flow rate of liquid iodine 22 may be controlled by the liquid flow rate control device 26. In the iodine evaporator 24, the iodine is heated above its boiling point, and the flow of iodine vapor 28 is generated. It forms.

[0069] The flow rate of hydrogen 14 may be controlled by the gas flow rate control device 30. Iodine vapor 2 The flow of 8 and the flow of hydrogen 14 are supplied to the superheater 36 and heated to the reaction temperature to react the reactants. A flow 38 is formed. The reactant flow 38 is supplied to the reactor 40.

[0070] The reactant stream 38 reacts in the presence of catalyst 42 contained in reactor 40, and the product stream 44 is produced. Catalyst 42 may be any of the catalysts described herein. Flow 44 contains hydrogen iodide, unreacted iodine, unreacted hydrogen, and trace amounts of water and other high-boiling point hydrogen. It may contain pure substances.

[0071] The product flow 44 may be supplied to the upstream valve 46. The upstream valve 46 controls the product flow 44. The product stream 44 may be guided to the iodine removal process. Before being used, it may pass through a cooler (not shown) to remove some heat. In iodine removal, The first iodine removal apparatus 48a consists of a first iodine removal tank 50a and a second iodine removal tank 50b It may also include the following. The product stream 44 is the boiling point of iodine in the first iodine removal tank 50a. It is cooled to a temperature below 44, causing at least some of the iodine to condense or solidify, resulting in a product flow 44 It may be separated from. The product stream 44 is further treated with iodine in the first iodine removal tank 50a. Cooled to a temperature below its melting point, it separates even more iodine from the product stream 44, and the first iodine In the removal tank 50a, at least a portion of the iodine is deposited as a solid, and the de-iodine product stream 52 It may also generate the deiodine product stream 52, which is then supplied to the second iodine removal tank 50b and cooled. The mixture is then filtered, and at least some of the remaining iodine is separated from the de-iodine product stream 52 for further crude extraction. A hydrogen iodide product flow 54 may be generated.

[0072] The first iodine removal device 48a consists of two iodine removal tanks operating in series, The first iodine removal apparatus 48a consists of two or more iodine removal tanks operating in parallel. , including two or more iodine removal tanks operating in series, or any combination thereof. But please understand that this is good. The first iodine removal device 48a uses a single iodine removal tank It should also be understood that it is acceptable to include a heat exchanger in any of the iodine removal tanks. It is further understood that the form may be a squid or a heat exchanger. The continuous tanks may be multiple It is also understood that they may be combined into a single tank having a cooling stage.

[0073] The iodine collected in the first iodine removal tank 50a forms the first iodine regeneration stream 56a. It is also possible to do so. Similarly, the iodine collected in the second iodine removal tank 50b is used in the second iodine reprocessing tank. A fresh flow 56b may be formed. First iodine regeneration flow 56a and second iodine regeneration flow 56b Each of these can be supplied to the iodine liquefaction device 20 continuously or intermittently, as shown. It may be good and / or may be supplied to the iodine evaporator 24.

[0074] To collect iodine in solid form while providing continuous operation, the upstream valve 46 may be configured to selectively divert the production stream 44 to the second iodine removal device 48b. The second iodine removal device 48b may be substantially similar to the above-described first iodine removal device 48a. Either the first iodine removal tank 50a or the second iodine removal tank 50b of the first iodine removal device 48a accumulates sufficient solid iodine convenient for the removal of solid iodine, and the upstream valve 46 is selected to divert the production stream 44 from the first iodine removal device 48a to the second iodine removal device 48b. Substantially simultaneously, the downstream valve 58 configured to selectively divert the crude hydrogen iodide production stream 54 from either the first iodine removal device 48a or the second iodine removal device 48b is selected to divert the crude hydrogen iodide production stream 54 from the second iodine removal device 48b, whereby the process of removing iodine from the production stream 44 to produce the crude hydrogen iodide production stream 54 may continue without interruption. When the production stream 44 is no longer directed to the first iodine removal device 48a, the first iodine removal tank 50a and the second iodine removal tank 50b of the first iodine removal device 48a may be heated above the melting point of iodine to liquefy the solid iodine, whereby the liquefied iodine may flow through the first iodine regeneration stream 56a and the second iodine regeneration stream 56b of the first iodine removal device 48a to the iodine liquefaction device 20. As the process continues, the first iodine removal tank 5 of the second iodine removal device 48b 0a may be heated above the melting point of iodine to liquefy the solid iodine, whereby the liquefied iodine may flow through the first iodine regeneration stream 56a and the second iodine regeneration stream 56b of the first iodine removal device 48a to the iodine liquefaction device 20. It may flow to the iodine liquefaction device 20.

[0075] As the process continues, the first iodine removal tank 5 of the second iodine removal device 48b Either the 0a or the second iodine removal tank 50b has sufficient for the removal of solid iodine. When solid iodine accumulates, the upstream valve 46 can be selected to direct the product stream 44 back from the second iodine removal device 48b to the first iodine removal device 48a, or the downstream valve 58 can be selected to direct the crude hydrogen iodide product stream 54 from the first iodine removal device 48a. However, this allows the process of removing iodine from the product stream 44 to produce the crude hydrogen iodide product stream 54 to continue without interruption. When the product stream 44 no longer flows into the second iodine removal device 48b, the first iodine removal tank 50a and the second iodine removal tank 50b of the second iodine removal device 48b can be heated above the melting point of iodine to liquefy the solid iodine so that the liquefied iodine can flow through the first iodine regeneration stream 56a and the second iodine regeneration stream 56b of the second iodine removal device 48b to the iodine liquefaction device 20 . By continuously switching between the first iodine removal device 48a and the second iodine removal device 48b, the unreacted iodine in the product stream 44 can be efficiently and continuously removed and regenerated as well. As described above, the liquid iodine can flow through the first iodine regeneration stream 56a and the second iodine regeneration stream 56b of the first iodine removal device 48a and the second iodine removal device 48b to the iodine liquefaction device 20. Alternatively, the liquid iodine can flow through the first iodine regeneration stream 56a and the second iodine regeneration stream 56b of the first iodine removal device 48a and the second iodine removal device 48b to the iodine evaporator 24, bypassing the iodine liquefaction device 20 and the liquid flow control device 26 .

[0076] As described above, the liquid iodine can flow through the first iodine regeneration stream 56a and the second iodine regeneration stream 56b of the first iodine removal device 48a and the second iodine removal device 48b to the iodine liquefaction device 20. Alternatively, the liquid iodine can flow through the first iodine regeneration stream 56a and the second iodine regeneration stream 56b of the first iodine removal device 48a and the second iodine removal device 48b to the iodine liquefaction device 20. Alternatively, the liquid iodine can flow through the first iodine regeneration stream 56a and the second iodine regeneration stream 56b of the first iodine removal device 48a and the second iodine removal device 48b to the iodine evaporator 24, bypassing the iodine liquefaction device 20 and the liquid flow control device 26

[0077] In the integrated process shown in Figure 1, the crude hydrogen iodide product stream 54 is further processed in the heavier distillation column 60. It is provided to the heavy distillation column 60, which extracts hydrogen iodide and residue from low-boiling point substances such as unreacted hydrogen. It may be configured for the separation of high-boiling-point substances such as unreacted iodine. From the heavy distillation column 60 The bottom flow 62 containing hydrogen iodide and residual unreacted iodine is supplied to the iodine regeneration tower 64. This is also good. The iodine regeneration tower 64 is configured for the separation of residual unreacted iodine from hydrogen iodide. It may also be used. The bottom flow 66 of the iodine regeneration tower 64 containing unreacted iodine is used in the iodine liquefaction device 20. It may be returned and regenerated. Alternatively, the bottom flow of the iodine regeneration tower 64 containing unreacted iodine. 66 may be returned to the iodine liquefaction device 24 for regeneration. Iodine regeneration including hydrogen iodide. The upper flow 68 of column 64 may be supplied to the product distillation column 70.

[0078] The upper stream 72 from the heavy distillation column 60, which contains hydrogen and residual hydrogen iodide, is also used for product distillation. It may be supplied to column 70. The product distillation column 70 separates unreacted hydrogen from hydrogen iodide. It may be configured as follows: The upper flow of the product column 70 containing unreacted hydrogen and residual hydrogen iodide 4 may be returned to reactor 40 and regenerated. The purified hydrogen iodide product obtained is produced The material may also be collected from the bottom flow 76 of the tower 70.

[0079] Figure 2 is a process flow diagram showing another integrated process for producing anhydrous hydrogen iodide. The integration process 78 shown in Figure 2 is similar to the integration process 10 described above, with reference to Figure 1. This process continues until the generation of crude hydrogen iodide product flow 54. In the integrated process 78 shown in Figure 2, The crude hydrogen iodide product stream 54 is supplied to the compressor 80, and the crude hydrogen iodide product stream 54 The pressure is increased to facilitate the recovery of hydrogen and hydrogen iodide. The compressor 80 is used to recover crude iodide The pressure of the hydrogen product stream 54 is increased to a separation pressure greater than the operating pressure of the reactor 42. This generates a compressed product stream 82. The compressed product stream 82 contains unreacted hydrogen and other elements. To separate high-boiling-point substances such as hydrogen iodide and trace amounts of residual unreacted iodine from low-boiling-point substances. The first step is to guide the mixture to a partial condenser 84 that undergoes a one-stage flash cooling process. The upper flow 86, containing hydrogen and residual hydrogen iodide, may be returned to the reactor 40 for regeneration. . Bottom flow 88 from partial condenser 84 containing hydrogen iodide, trace amounts of residual unreacted iodine and trace amounts Water may be supplied to the product column 90. The product column 90 is used to process residual unreacted hydrogen iodide. It may be configured for the separation of iodine, water, and other high-boiling point compounds. The bottom flow 92 of the product column 90 containing the element may be returned to the liquefaction unit 20 and regenerated. The bottom flow 92 of the product column 90 containing unreacted iodine is returned to the iodine liquefaction unit 24. It may be recycled. The purified hydrogen iodide product obtained is collected from the upper flow 94 of the product column 90. It may be collected. The purge flow 96 controls the accumulation of low-boiling point impurities in the product column 90. It may be removed from there. A portion of the purge flow 96 may be returned to reactor 40 and regenerated. However, other parts may be discarded.

[0080] Although the present invention has been described in terms of exemplary designs, the present invention is intended to be in accordance with the spirit of this disclosure. Further modifications may be made to the gist and scope of the invention. Furthermore, this application relates to the relevant technical fields. Including such deviations from this disclosure that belong to known or customary practices in It is intended.

[0081] As used herein, the phrase "within any range defined between any two of the foregoing values" means that any range may be selected from any two of the values enumerated before such phrase, whether those values are in the lower portion of the enumeration or the higher portion of the enumeration. For example, a pair of values may be selected from two lower values, two higher values, or a lower value and a higher value. Whether those values are in the lower portion of the enumeration or the higher portion of the enumeration, any range may be selected from any two of the values enumerated before such phrase. For example, a pair of values may be selected from two lower values, two higher values, or a lower value and a higher value.

Examples

[0082] Example 1: Preparation of hydrogen iodide from hydrogen and iodine catalyzed by a nickel catalyst In Example 1, the production of hydrogen iodide (HI) from hydrogen (H2) and elemental iodine (I2) according to Equation 3 above was demonstrated over a range of reaction conditions using an alumina-supported nickel catalyst. Before introducing the mixture of hydrogen gas and iodine vapor into the reactor, the catalyst in the fixed-bed tubular reactor was activated. The catalyst was purged with nitrogen gas and then hydrogen gas was introduced, the reactor was heated to 120 °C and held for 2 hours, then the reactor temperature was raised to 230 °C and held for an additional 1 hour to activate the catalyst. Next, the temperature of the reactor was adjusted to the desired reaction temperature. A predetermined fixed flow rate of hydrogen was bubbled into an iodine evaporator initially filled with a predetermined amount of solid elemental iodine. The temperature of the iodine evaporator was controlled at 150 °C to 170 °C to generate iodine vapor. The temperature of the evaporator and the hydrogen flow rate were adjusted as appropriate to obtain the desired molar ratio of hydrogen to iodine. The mixture of hydrogen and iodine vapor was fed into the reactor and reacted in the presence of the catalyst to form hydrogen iodide. Next, the reactor effluent was passed through a two-stage iodine trap to collect any unreacted iodine in solid form. Next, the crude hydrogen iodide product was contained using an alumina-supported nickel catalyst over a range of reaction conditions. Before introducing the mixture of hydrogen gas and iodine vapor into the reactor, the catalyst in the fixed-bed tubular reactor was activated. The catalyst was purged with nitrogen gas and then hydrogen gas was introduced, the reactor was heated to 120 °C and held for 2 hours, then the reactor temperature was raised to 230 °C and held for an additional 1 hour to activate the catalyst. Next, the temperature of the reactor was adjusted to the desired reaction temperature. A predetermined fixed flow rate of hydrogen was bubbled into an iodine evaporator initially filled with a predetermined amount of solid elemental iodine. The temperature of the iodine evaporator was controlled at 150 °C to 170 °C to generate iodine vapor. The temperature of the evaporator and the hydrogen flow rate were adjusted as appropriate to obtain the desired molar ratio of hydrogen to iodine. The mixture of hydrogen and iodine vapor was fed into the reactor and reacted in the presence of the catalyst to form hydrogen iodide. Next, the reactor effluent was passed through a two-stage iodine trap to collect any unreacted iodine in solid form. Next, the crude hydrogen iodide product was contained into the reactor. Before introducing the mixture of hydrogen gas and iodine vapor into the reactor, the catalyst in the fixed-bed tubular reactor was activated. The catalyst was purged with nitrogen gas and then hydrogen gas was introduced, the reactor was heated to 120 °C and held for 2 hours, then the reactor temperature was raised to 230 °C and held for an additional 1 hour to activate the catalyst. Next, the temperature of the reactor was adjusted to the desired reaction temperature. A predetermined fixed flow rate of hydrogen was bubbled into an iodine evaporator initially filled with a predetermined amount of solid elemental iodine. The temperature of the iodine evaporator was controlled at 150 °C to 170 °C to generate iodine vapor. The temperature of the evaporator and the hydrogen flow rate were adjusted as appropriate to obtain the desired molar ratio of hydrogen to iodine. The mixture of hydrogen and iodine vapor was fed into the reactor and reacted in the presence of the catalyst to form hydrogen iodide. Next, the reactor effluent was passed through a two-stage iodine trap to collect any unreacted iodine in solid form. Next, the crude hydrogen iodide product was contained The catalyst in the fixed-bed tubular reactor was activated by purging the catalyst with nitrogen gas and then introducing hydrogen gas, heating the reactor to 120 °C and holding for 2 hours, then raising the reactor temperature to 230 °C and holding for an additional 1 hour. Next, the temperature of the reactor was adjusted to the desired reaction temperature. A predetermined fixed flow rate of hydrogen was bubbled into an iodine evaporator initially filled with a predetermined amount of solid elemental iodine. The temperature of the iodine evaporator was controlled at 150 °C to 170 °C to generate iodine vapor. The temperature of the evaporator and the hydrogen flow rate were adjusted as appropriate to obtain the desired molar ratio of hydrogen to iodine. The mixture of hydrogen and iodine vapor was fed into the reactor and reacted in the presence of the catalyst to form hydrogen iodide. Next, the reactor effluent was passed through a two-stage iodine trap to collect any unreacted iodine in solid form. Next, the crude hydrogen iodide product was contained <000​​​​​​​​​​​​​​​​The iodine collector's outflow was collected in a dry eye trap. The outflow logistics are bubbling through a scrubber filled with deionized water to remove unreacted hydrogen gas. Residual hydrogen iodide was captured from the stream. After a predetermined period, the system was shut down, and the iodine evaporator was... The average H2 / I2 supply molar ratio was calculated by measuring the weight decrease and the weight increase of the iodine collector. The residual time is calculated based on the combined supply rate of hydrogen and iodine, and the conversion rate is collected. The calculation was based on the amount of hydrogen iodide and iodine supplied to the reactor.

[0083] All reactions were carried out in the range of 0-5 psig. Alumina support (Ni / Al2O3) The above experiments using 21% by weight of nickel catalyst each had an experiment duration of 24 hours. The procedure using a 20 wt% Ni / Al2O3 or 5 wt% Ni / Al2O3 catalyst is performed. Each reaction took 72 hours to complete. Other reaction conditions are shown in Table 1.

[0084] The results of each experiment are shown in Table 1. As shown in Table 1, 21 wt% nickel catalyst was When placed on a Lumina carrier and the contact time exceeds 7 seconds, the average conversion rate is over 90%, and average Productivity is approximately 35 lb / h / ft for reaction temperatures of approximately 320°C to 360°C. 3 was 20% by weight of nickel catalyst on an alumina support under comparable reaction conditions. It was performed slightly better than with a 21 wt% nickel catalyst on a body, but on an alumina support. The 5 wt% nickel catalyst showed much lower activity. [Table 1] Example 2: Preparation of hydrogen iodide from nickel-catalyzed hydrogen and iodine The effectiveness of the H2 / I2 molar ratio in

[0085] In Example 2, the effectiveness of the H2 / I2 molar ratio in HI collection efficiency was demonstrated by using 21% by weight of Ni The reaction was demonstrated using the Al2O3 catalyst across a range of reaction conditions, as described in Example 1. The same experimental setup and procedure were used in Example 2, and each experiment had a 24-hour execution time. The HI collection rate was calculated as the amount of HI collected in the dry eye trap relative to the total HI generated. It was defined as the proportion of I. As shown in Table 2, the H2 / I2 molar ratio is 2.7 (less than 3). In this case, the HI collection rate exceeded 90%, but when the H2 / I2 molar ratio was increased, the HI collection rate The rate decreased dramatically. Although not bound by theory, this is due to the presence of an excess amount of hydrogen. The following suggests that condensation of HI becomes more difficult. [Table 2] manner

[0086] Embodiment 1 is a process for producing hydrogen iodide. This process involves hydrogen and iodide. To provide a gas-phase reactant stream containing ion, and to react the reactant stream in the presence of a catalyst. The process includes generating a product stream containing hydrogen iodide. The catalyst is nickel, cobalt, iron. It includes at least one selected from the group consisting of nickel oxide, cobalt oxide, and iron oxide. The catalyst is supported on a carrier.

[0087] Embodiment 2 is a provisioning process in which water containing less than approximately 500 ppm by weight of hydrogen and approximately 500 ppm by weight This is the process according to embodiment 1, which contains less than ppm of oxygen.

[0088] Embodiment 3 is an embodiment in which the supply process includes water containing less than approximately 500 ppm by weight of iodine, as in Embodiment 1. Or it is either the process of embodiment 2.

[0089] Embodiment 4 is a process in which the molar ratio of hydrogen to iodine in the reaction material stream is approximately 1:1. The process is one of the three embodiments, with a ratio of approximately 10:1.

[0090] Embodiment 5 is a compound of Embodiment 4, wherein the molar ratio of hydrogen to iodine is approximately 2.5:1 to approximately 3:1. It's Seth.

[0091] Embodiment 6 is a carrier made of activated carbon, silica gel, zeolite, silicon carbide, metal oxide, or This is a process selected from the group of these combinations, one of embodiments 1 to 5.

[0092] Embodiment 7 is a metal oxide support, and the metal oxide support is alumina, magnesium oxide Includes sium, titanium dioxide, zinc oxide, zirconia, chromia, and combinations thereof. This is the process of aspect 6.

[0093] Embodiment 8 is the process of Embodiment 7, wherein the catalyst contains nickel and the support is alumina. .

[0094] Embodiment 9 is an embodiment in which the catalyst is present in an amount of approximately 0.1% to approximately 50% by weight of the total weight of the catalyst and the support. The process is one of the embodiments 1 to 8.

[0095] Embodiment 10 is a reaction process in which the contact time between the reaction material flow and the catalyst is approximately 0.1 seconds to approximately 1 The process is one of embodiments 1 to 9, and takes 800 seconds.

[0096] In embodiment 11, before the reaction step, the reaction material stream is brought to a reaction temperature of approximately 150°C to approximately 600°C. The process is any of embodiments 1 to 10, further comprising heating.

[0097] Embodiment 12 further contains unreacted iodine in the product stream, and the process is carried out from the product stream to the unreacted iodine. An additional step involves separating iodine as solid iodine and heating the solid iodine to produce liquid iodine. Embodiment 1 further includes an additional step of making a reaction and an additional step of returning liquid iodine to the reactant stream. It is one of the following 11 processes.

[0098] Embodiment 13 is a process of any of Embodiments 1 to 12, where the process is a continuous process. be.

[0099] Embodiment 14 further contains unreacted hydrogen in the product stream, and the process separates hydrogen from the product stream. An embodiment further comprising the additional step of separating and the additional step of returning the separated hydrogen to the reactant stream. It is one of the processes from 1 to 13.

[0100] Embodiment 15 is a step in which hydrogen is separated from the product stream, and the step is to compress the product stream and The process according to embodiment 14 includes flash cooling of the generated product stream.

[0101] Embodiment 16 is a process for producing hydrogen iodide. This process involves hydrogen and iodide. It provides a gas-phase reaction material stream containing hydrogen and iodine in a molar ratio of approximately 1:1 to 10:1. This involves heating the reaction material stream to a reaction temperature of approximately 150°C to approximately 600°C, and the reactants This includes reacting a slag flow in the presence of a catalyst to produce a product flow containing hydrogen iodide. The catalyst is selected from the group consisting of nickel, cobalt, iron, nickel oxide, cobalt oxide, and iron oxide. It includes at least one selected type. The catalyst is supported on a support. The catalyst is supported on the support. It is approximately 0.1% to 50% by weight of the total weight. The contact time between the reactant flow and the catalyst is The range is approximately 0.1 seconds to approximately 1,800 seconds.

[0102] Embodiment 17 is a process for producing hydrogen iodide. This process involves hydrogen and iodide. This provides a gas-phase reaction material stream containing hydrogen and iodine in a molar ratio of approximately 2:1 to 5:1. Furthermore, the reactant stream is heated to a reaction temperature of approximately 200°C to approximately 500°C, and the reactant This includes reacting a flow in the presence of a catalyst to produce a product flow containing hydrogen iodide. The catalyst comprises at least one selected from the group consisting of nickel, cobalt, and iron. The catalyst is supported on a carrier. The catalyst is present in an amount of approximately 5% to 45% by weight of the total weight of the catalyst and carrier. Yes, it exists. The contact time between the reactant stream and the catalyst is approximately 2 seconds to 100 seconds.

[0103] Embodiment 18 is a process for producing hydrogen iodide. This process involves hydrogen and iodide. This provides a gas-phase reaction material stream containing hydrogen and iodine in a molar ratio of approximately 2:1 to 3:1. Furthermore, the reactant stream is heated to a reaction temperature of approximately 300°C to 400°C, and the reactant This includes reacting a flow in the presence of a catalyst to produce a product flow containing hydrogen iodide. The catalyst contains nickel. The catalyst is supported on a carrier. The total weight of the catalyst and the carrier is... The concentration is approximately 10% to 40% by weight. The contact time between the reactant stream and the catalyst is approximately 2 seconds to 6 seconds. It's 0 seconds.

[0104] Embodiment 19 is a process for producing hydrogen iodide. This process involves hydrogen and iodide. It provides a gas-phase reaction material stream containing hydrogen and iodine in a molar ratio of approximately 2.5:1 to 3:1. This involves heating the reaction material stream to a reaction temperature of approximately 300°C to 350°C, and the reaction The process involves reacting a material flow in the presence of a catalyst to produce a product flow containing hydrogen iodide, and includes the following: The catalyst contains nickel. The catalyst is supported on an alumina support. The catalyst and the support are It is approximately 15% to 35% by weight of the total weight. The contact time between the reactant flow and the catalyst is The duration is approximately 2 to 40 seconds.

[0105] Embodiment 20 is a provisioning process in which water containing less than approximately 500 ppm by weight of hydrogen and approximately 500 ppm by weight Aspect 16-1 contains oxygen in less than ppm and water containing iodine in less than approximately 500 ppm by weight. It is one of the 9 processes.

[0106] Embodiment 21 is a provisioning process in which water containing less than approximately 50 ppm by weight of hydrogen and approximately 100 ppm Any of embodiments 16 to 19, containing less than 1 m of oxygen and water with less than approximately 100 ppm of iodine. That is the process.

[0107] Embodiment 22 is a provisioning process in which water containing less than about 10 ppm by weight of hydrogen and about 10 ppm by weight of hydrogen Any of embodiments 16 to 19, containing oxygen below 1 / pm and water with iodine below approximately 30 ppm That is the process.

[0108] Embodiment 23 is a provisioning process in which water containing less than approximately 5 ppm by weight of hydrogen and approximately 1 ppm by weight A water containing less than 10 ppm of oxygen and less than 10 ppm of iodine, any of embodiments 16 to 19 It is a process.

[0109] Embodiment 24 further comprises unreacted iodine and unreacted hydrogen in the product stream, and the process is unreacted An additional step to separate the iodine from the product stream as solid iodine, and heating the solid iodine. An additional step of generating liquid iodine, and an additional step of returning the liquid iodine to the reactant stream, and generation By compressing the logistics and applying flash cooling to the compressed product flow, the product flow can be reduced. An additional step to separate hydrogen, and an additional step to return the separated hydrogen to the reactant stream, further The process is a continuous process, as described in any of embodiments 16 to 23.

[0110] Embodiment 25 further comprises unreacted iodine and unreacted hydrogen in the product stream, and the process is unreacted An additional step to separate the iodine from the product stream as solid iodine, and heating the solid iodine. An additional step of generating liquid iodine, and an additional step of returning the liquid iodine to the reactant stream, and generation By compressing the logistics and applying flash cooling to the compressed product flow, the product flow can be reduced. An additional step to separate hydrogen, and an additional step to return the separated hydrogen to the reactant stream, further This includes any process in any of embodiments 16 to 23, where the process is a batch process.

[0111] Embodiment 26 is a process for producing hydrogen iodide. This process involves the following steps This process involves reacting hydrogen and iodine in the gas phase in the presence of a catalyst to produce hydrogen iodide and unreacted hydrogen. A step to generate a product stream containing iodine, wherein the catalyst is nickel, cobalt, iron, acid The catalyst comprises at least one of nickel oxide, cobalt oxide, and iron oxide, and the catalyst is supported on a support. The process involves cooling the product flow to form solid iodine, thereby reducing the product flow. The first iodine removal step involves removing at least a portion of the unreacted iodine, wherein solid iodine removes the first iodine The process involves forming in either the removal tank or the second iodine removal tank, and the product flow into the second iodine removal tank. When cooling by passing through the iodine removal tank, the first iodine removal tank is heated to liquefy the solid iodine. Or, when the product flow is cooled by passing it through the first iodine removal tank, the second iodine removal tank A process to produce liquid iodine from solid iodine by heating it to liquefy it. The process involves regenerating the liquefied iodine into the reaction process.

[0112] Embodiment 27 further contains unreacted hydrogen in the product stream, and the process separates hydrogen from the product stream. The process further includes an additional step of separation and an additional step of regenerating the separated hydrogen into the reaction process. This is the process of embodiment 26.

[0113] Embodiment 28 is a step in which hydrogen is separated from the product stream, and the step is to compress the product stream and The process according to embodiment 27 includes flash cooling of the generated product stream.

[0114] Embodiment 29 is a process in any of Embodiments 26 to 28, wherein the process is a continuous process. That is the case.

[0115] Embodiment 30 is a process in any of Embodiments 26 to 28 in which the process is a batch process. It is S.

[0116] Embodiment 31 is a carrier made of activated carbon, silica gel, zeolite, silicon carbide, metal oxide, Or a process selected from the group of combinations thereof, one of the processes in embodiments 26 to 30. ru.

[0117] Embodiment 32 is a metal oxide support, and the metal oxide support is alumina, magnesium oxide Contains nesium, titanium dioxide, zinc oxide, zirconia, chromia, or combinations thereof. This is the process of embodiment 31.

[0118] Embodiment 33 is the process of Embodiment 32, wherein the catalyst contains nickel on an alumina support.

[0119] Embodiment 34 describes a method in which hydrogen and iodine are reacted in the gas phase in the presence of a catalyst, for approximately 15 minutes. The process is one of embodiments 26 to 33, with a reaction temperature of 0°C to approximately 600°C.

[0120] Embodiment 35 is a process for producing hydrogen iodide. This process involves the following steps Including the degree: In the presence of a catalyst, with a molar ratio of hydrogen to iodine of approximately 1:1 to approximately 10:1, approximately 15 With a reaction temperature of 0°C to approximately 600°C and a contact time of approximately 0.1 seconds to approximately 1,800 seconds, water in the gas phase reacts with water. A process of reacting a ion with iodine to produce a product stream containing hydrogen iodide and unreacted iodine. The catalyst is nickel, cobalt, iron, nickel oxide, cobalt oxide, and iron oxide. The catalyst is supported on a support and comprises at least one of the following, and the total weight of the catalyst and the support is The process involves a quantity of approximately 0.1% to 50% by weight, followed by cooling the product stream to form solid iodine. This process removes at least a portion of the unreacted iodine from the product stream. Then, solid iodine is formed in one of the first or second iodine removal tanks. In the process, when the product flow is passed through a second iodine removal tank and cooled, the first iodine removal The tank is heated to liquefy the solid iodine, or the product stream is passed through the first iodine removal tank and cooled. In this case, the second iodine removal tank is heated to liquefy the solid iodine, A process for producing liquid iodine from iodine, and a process for regenerating the liquefied iodine into the reaction process.

[0121] Embodiment 36 is a process for producing hydrogen iodide. This process involves the following steps This includes: in the presence of a catalyst, with a hydrogen-to-iodine molar ratio of approximately 2:1 to approximately 5:1, and at approximately 200°C. At a reaction temperature of approximately 500°C and a contact time of approximately 2 to 100 seconds, hydrogen and iodine react in the gas phase. A step of reacting to produce a product stream containing hydrogen iodide and unreacted iodine, The medium contains at least one of nickel, cobalt, and iron, and the catalyst is supported on a carrier. The process involves the catalyst being present in an amount of approximately 5% to 45% by weight of the total weight of the catalyst and support, and the production process. By cooling the flow to form solid iodine, less unreacted iodine is removed from the product flow. In both cases, a portion is removed, and solid iodine is removed from the first iodine removal tank or the second iodine removal tank. The process is carried out in one of the removal tanks, and the product flow is passed through a second iodine removal tank for cooling. In this case, the first iodine removal tank is heated to liquefy the solid iodine, or the product flow is used as follows: When cooling by passing through the iodine removal tank 1, the second iodine removal tank is heated to remove solid iodine. The process involves liquefying solid iodine to produce liquid iodine, and then reacting the liquefied iodine. A process for regeneration.

[0122] Embodiment 37 is a process for producing hydrogen iodide. This process involves the following steps This includes: in the presence of a catalyst, with a hydrogen-to-iodine molar ratio of approximately 2:1 to 3:1, and at approximately 300°C. At a reaction temperature of approximately 400°C and a contact time of approximately 2 to 60 seconds, hydrogen and iodine are reacted in the gas phase. A step of reacting to produce a product stream containing hydrogen iodide and unreacted iodine, wherein a catalyst The catalyst contains nickel, is supported on a support, and weighs approximately 10 times the total weight of the catalyst and support. The process involves a quantity of approximately 40% by weight, followed by cooling the product stream to form solid iodine. This is a step to remove at least some of the unreacted iodine from the product stream, and solid iodine The process involves forming in one of the first or second iodine removal tanks, and When the material is cooled by passing it through the second iodine removal tank, the first iodine removal tank is heated to solidify... When liquefying solid iodine or cooling the product stream by passing it through the first iodine removal tank, By heating the iodine removal tank (2) to liquefy the solid iodine, liquid iodine is obtained from the solid iodine. The process involves generating iodine and regenerating the liquefied iodine into the reaction process.

[0123] Embodiment 38 is a process for producing hydrogen iodide. This process involves the following steps Including the following: In the presence of a catalyst, the molar ratio of hydrogen to iodine is approximately 2.5:1 to approximately 3:1, and approximately 30 Hydrogen and iodine react in the gas phase at a reaction temperature of 0°C to approximately 350°C and a contact time of approximately 2 seconds to approximately 40 seconds. A step of reacting with to produce a product stream containing hydrogen iodide and unreacted iodine, The catalyst contains nickel on an alumina support, the catalyst is supported on the support, and the catalyst and the support The process involves cooling the product flow to produce solid yogurt, which is approximately 15% to 35% by weight of the total weight. A process to remove at least a portion of unreacted iodine from the product stream by forming a particle. And the solid iodine is formed in one of the first iodine removal tank or the second iodine removal tank. When the process is carried out and the product flow is cooled by passing it through a second iodine removal tank, the first iodine The iodine removal tank is heated to liquefy the solid iodine, or the product stream is passed through the first iodine removal tank. When cooling, the second iodine removal tank is heated to liquefy the solid iodine, A process for producing liquid iodine from solid iodine, and a process for regenerating the liquefied iodine into the reaction process.

[0124] Embodiment 39 further contains unreacted hydrogen in the product stream, and the process compresses the product stream to a pressure By flash cooling the condensed product flow, hydrogen is separated from the product flow. The process further includes an additional step of regenerating the separated hydrogen into the reaction step, and The process is a continuous process, as described in any of embodiments 35 to 38.

[0125] Embodiment 40 further contains unreacted hydrogen in the product stream, and the process compresses the product stream to pressure By flash cooling the condensed product flow, hydrogen is separated from the product flow. The process further includes an additional step of regenerating the separated hydrogen into the reaction step, The process is a batch process, or one of the processes shown in embodiments 35 to 39.

[0126] Embodiment 41 is water containing less than approximately 500 ppm by weight of hydrogen and less than approximately 500 ppm by weight of oxygen. A process of any of embodiments 35 to 40, which includes water containing less than approximately 500 ppm of iodine. That is the case.

[0127] Embodiment 42 contains water with hydrogen at less than about 50 ppm by weight and oxygen at less than about 100 ppm. The process is one of embodiments 35 to 41, which includes water containing less than approximately 100 ppm of iodine. .

[0128] Embodiment 43 contains water with less than approximately 10 ppm by weight of hydrogen and less than approximately 10 ppm by weight of oxygen. The process is one of embodiments 35 to 42, and includes water containing less than approximately 30 ppm of iodine. .

[0129] Embodiment 44 is a process according to any of Embodiments 35 to 43, comprising water containing less than approximately 5 ppm by weight of hydrogen and less than approximately 1 ppm by weight of oxygen, and water containing less than approximately 10 ppm of iodine. The present invention includes the following embodiments. [1] A process for producing hydrogen iodide, To provide a gas-phase reaction material stream containing hydrogen and iodine, A process comprising reacting the reaction material stream in the presence of a catalyst to produce a product stream containing hydrogen iodide, wherein the catalyst comprises at least one selected from the group consisting of nickel, cobalt, iron, nickel oxide, cobalt oxide, and iron oxide, and the catalyst is supported on a carrier to produce a product stream containing hydrogen iodide. [2] The process according to [1], wherein the hydrogen in the supplying step comprises water in less than about 500 ppm by weight and oxygen in less than about 500 ppm by weight. [3] The process according to [1], wherein the iodine in the providing step contains water at a concentration of less than approximately 500 ppm by weight. [4] The process according to [1], wherein in the providing step, the molar ratio of hydrogen to iodine in the reaction material stream is about 1:1 to about 10:1. [5] The process according to [1], wherein the carrier is selected from the group consisting of activated carbon, silica gel, zeolite, silicon carbide, metal oxide, or a combination thereof. [6] The process according to [5], wherein the carrier is a metal oxide carrier, and the metal oxide carrier comprises alumina, magnesium oxide, titanium oxide, zinc oxide, zirconia, chromia, and combinations thereof. [7] The process according to [6], wherein the catalyst contains nickel and the support is alumina. [8] The product stream further contains unreacted iodine, and the process is further, A step of separating the unreacted iodine from the product stream as solid iodine, A step of heating the solid iodine to produce liquid iodine, The process according to [1], further comprising the step of returning the liquid iodine to the reaction material stream. [9] The product stream further contains unreacted hydrogen, and the process involves an additional, A step of separating the hydrogen from the product stream, The process according to [8], further comprising the step of returning the separated hydrogen to the reaction material stream.

[10] Separating the hydrogen from the product stream is Compressing the aforementioned product flow, The process according to [9], comprising flash cooling the compressed product flow.

Claims

1. A process for producing hydrogen iodide, To provide a gas-phase reaction material stream containing hydrogen and iodine, The reaction material stream is reacted in the presence of a catalyst containing at least one of nickel, cobalt, and iron to produce hydrogen iodide (HI) and unreacted iodine (I). ２ ), and unreacted hydrogen (H ２ This involves generating a product stream containing ) and To separate unreacted iodine, In some cases, this involves condensing the flow containing hydrogen iodide (HI), In some cases, unreacted hydrogen (H ２ ) to remove or regenerate the flow including, A process that includes this.

2. The process according to claim 1, wherein the catalyst comprises nickel.

3. The process according to claim 1, wherein the catalyst is supported on a carrier containing alumina.

4. The process according to claim 2, wherein the catalyst is supported on a carrier containing alumina.

5. Separating unreacted iodine is further important. Cooling the unreacted iodine, The unreacted iodine is separated from the product stream as solid iodine, The process according to claim 1, including the process described in claim 1.

6. The process involves heating the solid iodine to produce liquid iodine, The process involves evaporating the aforementioned liquid iodine, The evaporated iodine is returned to the reaction material stream, The process according to claim 5, further comprising:

7. The unreacted hydrogen is separated from the product stream, The separated hydrogen is returned to the reaction material stream, The process according to claim 1, further comprising the additional step of

8. Separating the unreacted hydrogen from the product stream is Compressing the aforementioned product flow, The compressed product flow is flash-cooled, The process according to claim 7, including the process described in claim 7.

9. The process according to claim 1, comprising reacting the hydrogen and the iodine in a gas-phase reactant stream in a molar ratio of 2:1 to 5:

1.

10. The process according to claim 1, comprising reacting hydrogen with iodine at a reaction temperature of 200°C to 500°C in the presence of a catalyst.

11. The process according to claim 1, comprising reacting hydrogen and iodine for a contact time of 2 to 100 seconds.

12. The process according to claim 1, further comprising the additional step of forming an organic iodide using the hydrogen iodide.

13. The process according to claim 1, further comprising the additional step of forming an iodoalkane using the hydrogen iodide.

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