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1. 发明授权

US07119227B2 Process for catalytic vapor phase oxidation 有权
标题翻译：催化气相氧化工艺
公开(公告)号：US07119227B2
公开(公告)日：2006-10-10
申请号：US10937657
申请日：2004-09-10
申请人： Yasuyuki Sakakura , Shuhei Yada , Kimikatsu Jinno , Hirochika Hosaka , Yoshiro Suzuki
发明人： Yasuyuki Sakakura , Shuhei Yada , Kimikatsu Jinno , Hirochika Hosaka , Yoshiro Suzuki
IPC分类号： C07C51/16
CPC分类号： C07C45/35 , B01J8/067 , B01J2208/00053 , B01J2208/00061 , B01J2208/00088 , B01J2208/00221 , B01J2208/00256 , B01J2208/0053 , B01J2208/025 , B01J2219/0002 , B01J2219/00259 , C07C51/252 , C07C47/22 , C07C57/04
摘要： The present invention provides a process for catalytic vapor phase oxidation which prevents runaway reaction or early deterioration of a catalyst, in the production of (meth)acrylic acid or the like from propylene or isobutylene by the catalytic vapor phase oxidation process using a multi-tubular reactor, which can lead to the production thereof constantly in high yield for a long period of time. Further, the present invention provides a process for catalytic vapor phase oxidation wherein raw material gas is introduced for oxidation into reaction tubes of a multi-tubular reactor which is equipped with, as arranged within the shell of the reactor, a plurality of reaction tubes having a catalyst packed therein and a plurality of baffle plates for changing the direction of the flow of a heating medium introduced into the shell, characterized in that the temperature of the catalyst packed in a reaction tube which is not connected with at least one baffle plate is measured at plural points in the direction of an axis of the reaction tube.
摘要翻译：本发明提供催化气相氧化方法，其通过使用多管状催化气相氧化法从丙烯或异丁烯生产（甲基）丙烯酸等，防止催化剂失控反应或早期劣化反应器，其可以长时间以高产率持续地生产。此外，本发明提供了一种催化气相氧化方法，其中将原料气体引入氧化成多管式反应器的反应管中，该多管式反应器配备有布置在反应器壳体内的多个反应管，其具有填充在其中的催化剂和用于改变引入壳体的加热介质的流动方向的多个挡板，其特征在于，填充在与至少一个挡板相连的反应管中的催化剂的温度为在反应管的轴线方向的多个点处测量。

2. 发明申请

US20050107483A1 Process for catalytic vapor phase oxidation 有权
标题翻译：催化气相氧化工艺
公开(公告)号：US20050107483A1
公开(公告)日：2005-05-19
申请号：US10937657
申请日：2004-09-10
申请人： Yasuyuki Sakakura , Shuhei Yada , Kimikatsu Jinno , Hirochika Hosaka , Yoshiro Suzuki
发明人： Yasuyuki Sakakura , Shuhei Yada , Kimikatsu Jinno , Hirochika Hosaka , Yoshiro Suzuki
IPC分类号： C07C27/04 , B01J8/06 , C07C45/35 , C07C51/25 , C07C27/26
CPC分类号： C07C45/35 , B01J8/067 , B01J2208/00053 , B01J2208/00061 , B01J2208/00088 , B01J2208/00221 , B01J2208/00256 , B01J2208/0053 , B01J2208/025 , B01J2219/0002 , B01J2219/00259 , C07C51/252 , C07C47/22 , C07C57/04
摘要： The present invention provides a process for catalytic vapor phase oxidation which prevents runaway reaction or early deterioration of a catalyst, in the production of (meth)acrylic acid or the like from propylene or isobutylene by the catalytic vapor phase oxidation process using a multi-tubular reactor, which can lead to the production thereof constantly in high yield for a long period of time. Further, the present invention provides a process for catalytic vapor phase oxidation wherein raw material gas is introduced for oxidation into reaction tubes of a multi-tubular reactor which is equipped with, as arranged within the shell of the reactor, a plurality of reaction tubes having a catalyst packed therein and a plurality of baffle plates for changing the direction of the flow of a heating medium introduced into the shell, characterized in that the temperature of the catalyst packed in a reaction tube which is not connected with at least one baffle plate is measured at plural points in the direction of an axis of the reaction tube.
摘要翻译：本发明提供催化气相氧化方法，其通过使用多管状催化气相氧化法从丙烯或异丁烯生产（甲基）丙烯酸等，防止催化剂失控反应或早期劣化反应器，其可以长时间以高产率持续地生产。此外，本发明提供了一种催化气相氧化方法，其中将原料气体引入氧化成多管式反应器的反应管中，该多管式反应器配备有布置在反应器壳体内的多个反应管，其具有填充在其中的催化剂和用于改变引入壳体的加热介质的流动方向的多个挡板，其特征在于，填充在与至少一个挡板相连的反应管中的催化剂的温度为在反应管的轴线方向的多个点处测量。

3. 发明授权

US07368601B2 Process for producing (meth)acrylic acids and process for distilling the same 有权
标题翻译：（甲基）丙烯酸的制造方法及蒸馏法
公开(公告)号：US07368601B2
公开(公告)日：2008-05-06
申请号：US11526730
申请日：2006-09-26
申请人： Shuhei Yada , Yasushi Ogawa , Yoshiro Suzuki , Kimikatsu Jinno , Hirochika Hosaka , Kenji Takasaki , Masayasu Goriki
发明人： Shuhei Yada , Yasushi Ogawa , Yoshiro Suzuki , Kimikatsu Jinno , Hirochika Hosaka , Kenji Takasaki , Masayasu Goriki
IPC分类号： C07C51/42
CPC分类号： C07C51/44 , B01D3/14 , B01D3/146 , B01D3/42 , B01D3/4211 , C07C67/54 , C07C57/04 , C07C69/54
摘要： In the stopping and starting operations of a distillation column used for producing (meth)acrylic acids according to the present invention, upon stopping the operation of the distillation column, the heating of a reboiler attached thereto is interrupted and then the reboiler is rapidly cooled; and/or upon starting the operation of the distillation column for production of the (meth)acrylic acids, an inner wall surface of the distillation column is heated to a temperature higher than a condensation temperature of the (meth)acrylic acids and the operation of the distillation column is started under the heated condition. According to the present invention, it is possible to early and safely stop the operation of the distillation column while preventing the occurrence of polymerization within the distillation column, and stably perform an operation for distillation of acrylic monomers for a long period of time.
摘要翻译：在根据本发明的用于生产（甲基）丙烯酸的蒸馏塔的停止和开始操作中，停止蒸馏塔的操作后，连接的再沸器的加热被中断，然后再沸器被快速冷却; 和/或在开始用于生产（甲基）丙烯酸的蒸馏塔的操作时，将蒸馏塔的内壁表面加热到高于（甲基）丙烯酸的冷凝温度的温度和蒸馏塔在加热条件下启动。根据本发明，能够在避免蒸馏塔内发生聚合的同时，早日安全地停止蒸馏塔的运转，并且能够长时间稳定地进行丙烯酸类单体的蒸馏操作。

4. 发明授权

US07188639B2 Storage tank for easily polymerizable compound and method of storage 有权
标题翻译：容易聚合的化合物储存罐和储存方法
公开(公告)号：US07188639B2
公开(公告)日：2007-03-13
申请号：US10840612
申请日：2004-05-07
申请人： Shuhei Yada , Yasushi Ogawa , Yoshiro Suzuki , Kimikatsu Jinno , Hirochika Hosaka , Masayasu Goriki
发明人： Shuhei Yada , Yasushi Ogawa , Yoshiro Suzuki , Kimikatsu Jinno , Hirochika Hosaka , Masayasu Goriki
IPC分类号： F16K49/00 , F17D1/16
CPC分类号： B01J19/00 , B01J2219/00006 , B01J2219/00083 , B01J2219/00247 , B01J2219/00252 , B01J2219/00254 , Y10T137/0391 , Y10T137/6416 , Y10T137/6579 , Y10T137/85978
摘要： A storage tank for an easily polymerizable compound has acceptance piping and delivery piping with a circulation line directly connecting the acceptance piping to the delivery piping or with circulation lines respectively connecting the acceptance piping to the storage tank and the storage tank to the delivery piping. A method of storing an easily polymerizable compound in the storage tank includes circulating the compound in the storage tank through the circulation line(s), where the compound can be (meth)acrylic acid being produced and/or purified with the temperature of purified (meth)acrylic acid being supplied to or removed from the storage tank being regulated to not be higher than the temperature thereof in the tank. A method of joining pipes for-transporting a corrosive liquid using flanges, bolts, and nuts made of a material having resistance to corrosion by the corrosive liquid.
摘要翻译：用于容易聚合的化合物的储罐具有接收管道和输送管道，其具有将接收管线直接连接到输送管线的循环管线或分别将接收管路连接到储罐和储存箱的输送管线的循环管线。将容易聚合的化合物储存在储罐中的方法包括使化合物在储罐中循环通过循环管线，其中化合物可以是纯化的（...）的温度产生和/或纯化的（甲基）丙烯酸甲基）丙烯酸被提供给或从储罐中取出被调节为不高于罐中的温度。使用由腐蚀性液体具有耐腐蚀性的材料制成的法兰，螺栓和螺母来连接输送腐蚀性液体的管道的方法。

5. 发明申请

US20050131254A1 Multitube reactor, vapor phase catalytic oxidation method using the multitube reactor, and start up method applied to the multitube reactor 有权
标题翻译：多管反应器，使用多管反应器的气相催化氧化法，以及应用于多管反应器的启动方法
公开(公告)号：US20050131254A1
公开(公告)日：2005-06-16
申请号：US11049106
申请日：2005-02-03
申请人： Shuhei Yada , Hirochika Hosaka , Masayasu Goriki , Kimikatsu Jinno , Yasushi Ogawa , Yoshiro Suzuki
发明人： Shuhei Yada , Hirochika Hosaka , Masayasu Goriki , Kimikatsu Jinno , Yasushi Ogawa , Yoshiro Suzuki
IPC分类号： B01J8/06 , C07C45/33 , C07C45/35 , C07C51/215 , C07C51/25 , C07C51/16 , B01J8/04
CPC分类号： B01J35/026 , B01J8/06 , B01J8/067 , B01J23/002 , B01J23/8876 , B01J2208/00221 , B01J2208/0053 , B01J2208/00716 , B01J2523/00 , C07C45/33 , C07C45/35 , C07C51/215 , C07C51/252 , F28D7/1607 , F28D2021/0022 , F28F9/026 , F28F9/028 , F28F9/22 , F28F2265/10 , C07C47/22 , C07C57/04 , B01J2523/12 , B01J2523/13 , B01J2523/22 , B01J2523/305 , B01J2523/41 , B01J2523/54 , B01J2523/68 , B01J2523/842 , B01J2523/845 , B01J2523/847
摘要： A multitube reactor, wherein tubes having smaller tolerance between a nominal size and actual sizes are used as reaction tubes to stably perform a high yield reaction for a long period, a catalyst is filled into the reaction tubes so that the catalyst layer peak temperature portions of the reaction tubes are not overlapped with the connection sites thereof with baffles to effectively prevent hot spots from occurring and stably perform a reaction for a long period without the clogging of the reaction tubes, a heat medium and raw material gas are allowed to flow in the direction of a countercurrent and a specified type of catalyst is filled into the reaction tubes so that activity is increased from the inlet of the raw material gas to the outlet thereof to prevent the autooxidation of products so as to prevent equipment from being damaged due to the reaction, and, at the time of starting, gas with a temperature of 100 to 400° C. is led to the outside of the reaction tubes to increase the temperature of the reaction tubes and, a heat medium, which is solid at the room temperature, is heated to circulate to the outside of the reaction tubes to efficiently start up the reactor without affecting the activity of the catalyst.
摘要翻译：使用多管反应器，其中具有公称尺寸和实际尺寸之间的较小公差的管用作反应管以长期稳定地进行高产率反应，将催化剂填充到反应管中，使得催化剂层峰值温度部分反应管不与其连接位置与挡板重叠，以有效地防止热点发生并且长时间稳定地进行反应而不会使反应管堵塞，允许热介质和原料气体流入将反向的方向和特定类型的催化剂填充到反应管中，使得活性从原料气体的入口到其出口增加，以防止产品的自氧化，从而防止设备因为反应，并且在起始时，将温度为100〜400℃的气体导入反应管的外部以增加反应管的温度和在室温下为固体的热介质被加热以循环到反应管的外部，以有效启动反应器而不影响催化剂的活性。

6. 发明申请

US20070021631A1 Gas-phase catalytic oxidation process and process for producing (meth) acrolein or (meth) acrylic acid 审中-公开
标题翻译：气相催化氧化工艺及制备（甲基）丙烯醛或（甲基）丙烯酸的方法
公开(公告)号：US20070021631A1
公开(公告)日：2007-01-25
申请号：US11527451
申请日：2006-09-27
申请人： Shuhei Yada , Yasushi Ogawa , Yoshiro Suzuki , Hirochika Hosaka , Kimikatsu Jinno
发明人： Shuhei Yada , Yasushi Ogawa , Yoshiro Suzuki , Hirochika Hosaka , Kimikatsu Jinno
IPC分类号： C07C51/16 , C07C45/28
CPC分类号： C07C51/215 , C07C45/33 , C07C45/35 , C07C51/252 , C07C47/22 , C07C57/04
摘要： (1) In a gas-phase catalytic oxidation process for conducting gas-phase catalytic oxidation reaction using a fixed bed multipipe type reactor having reaction tubes filled with a catalyst while feeding a reaction raw gas thereinto, the catalyst is filled in each of the reaction tubes of the fixed bed multipipe type reactor to form two or more catalyst layers having different catalytic activities from each other in a direction of the oxidation reaction, and the catalyst layer disposed nearest to a reaction raw gas inlet of the reaction tube has a higher catalytic activity than that of the next catalyst layer adjacent thereto, or (2) in a process for producing (meth)acrolein or (meth)acrylic acid by subjecting a raw material of the (meth)acrolein or (meth)acrylic acid, and molecular oxygen or a molecular oxygen-containing gas to gas-phase catalytic oxidation reaction using a fixed bed multipipe type reactor having two or more catalyst layers in an axial direction of each of reaction tubes provided in the reactor, a difference between maximum and minimum reaction peak temperatures of the respective catalyst layers in the axial direction of the reaction tube is not more than 20° C. According to these processes, formation of hot spots in the catalyst can be efficiently prevented.
摘要翻译：（1）在使用固定床多管式反应器进行气相催化氧化反应的气相催化氧化反应器中，在反应管中装入催化剂，同时向其中加入反应原料气体，在每个反应中填充催化剂固定床多管式反应器的管，在氧化反应的方向上形成具有彼此不同的催化活性的两个以上的催化剂层，最靠近反应管的反应原料气体入口设置的催化剂层具有较高的催化剂活性高于与其相邻的下一催化剂层的活性，或（2）在（甲基）丙烯醛或（甲基）丙烯酸的原料和分子量氧或含分子氧的气体进行气相催化氧化反应，使用在每个反应管的轴向上具有两个以上催化剂层的固定床多管型反应器在反应器中设置反应管的轴向方向上的各催化剂层的最大和最小反应峰值温度之间的差不超过20℃。根据这些方法，可以有效地形成催化剂中的热点防止了

7. 发明申请

US20070256921A1 Process for producing (meth) acrylic acids and process for distilling the same 审中-公开
标题翻译：（甲基）丙烯酸的制造方法及蒸馏法
公开(公告)号：US20070256921A1
公开(公告)日：2007-11-08
申请号：US11812716
申请日：2007-06-21
申请人： Shuhei Yada , Yasushi Ogawa , Yoshiro Suzuki , Kimikatsu Jinno , Hirochika Hosaka , Kenji Takasaki , Masayasu Goriki
发明人： Shuhei Yada , Yasushi Ogawa , Yoshiro Suzuki , Kimikatsu Jinno , Hirochika Hosaka , Kenji Takasaki , Masayasu Goriki
IPC分类号： B01D3/00
CPC分类号： C07C51/44 , B01D3/14 , B01D3/146 , B01D3/42 , B01D3/4211 , C07C67/54 , C07C57/04 , C07C69/54
摘要： In the stopping and starting operations of a distillation column used for producing (meth)acrylic acids according to the present invention, upon stopping the operation of the distillation column, the heating of a reboiler attached thereto is interrupted and then the reboiler is rapidly cooled; and/or upon starting the operation of the distillation column for production of the (meth)acrylic acids, an inner wall surface of the distillation column is heated to a temperature higher than a condensation temperature of the (meth)acrylic acids and the operation of the distillation column is started under the heated condition. According to the present invention, it is possible to early and safely stop the operation of the distillation column while preventing the occurrence of polymerization within the distillation column, and stably perform an operation for distillation of acrylic monomers for a long period of time.
摘要翻译：在根据本发明的用于生产（甲基）丙烯酸的蒸馏塔的停止和开始操作中，停止蒸馏塔的操作后，连接的再沸器的加热被中断，然后再沸器被快速冷却; 和/或在开始用于生产（甲基）丙烯酸的蒸馏塔的操作时，将蒸馏塔的内壁表面加热到高于（甲基）丙烯酸的冷凝温度的温度和蒸馏塔在加热条件下启动。根据本发明，能够在避免蒸馏塔内发生聚合的同时，早日安全地停止蒸馏塔的运转，并且能够长时间稳定地进行丙烯酸类单体的蒸馏操作。

8. 发明申请

US20070021633A1 Process for producing (meth)acrylic acids and process for distilling the same 有权
标题翻译：（甲基）丙烯酸的制造方法及蒸馏法
公开(公告)号：US20070021633A1
公开(公告)日：2007-01-25
申请号：US11526730
申请日：2006-09-26
申请人： Shuhei Yada , Yasushi Ogawa , Yoshiro Suzuki , Kimikatsu Jinno , Hirochika Hosaka , Kenji Takasaki , Masayasu Goriki
发明人： Shuhei Yada , Yasushi Ogawa , Yoshiro Suzuki , Kimikatsu Jinno , Hirochika Hosaka , Kenji Takasaki , Masayasu Goriki
IPC分类号： C07C51/42
CPC分类号： C07C51/44 , B01D3/14 , B01D3/146 , B01D3/42 , B01D3/4211 , C07C67/54 , C07C57/04 , C07C69/54
摘要： In the stopping and starting operations of a distillation column used for producing (meth)acrylic acids according to the present invention, upon stopping the operation of the distillation column, the heating of a reboiler attached thereto is interrupted and then the reboiler is rapidly cooled; and/or upon starting the operation of the distillation column for production of the (meth)acrylic acids, an inner wall surface of the distillation column is heated to a temperature higher than a condensation temperature of the (meth)acrylic acids and the operation of the distillation column is started under the heated condition. According to the present invention, it is possible to early and safely stop the operation of the distillation column while preventing the occurrence of polymerization within the distillation column, and stably perform an operation for distillation of acrylic monomers for a long period of time.
摘要翻译：在根据本发明的用于生产（甲基）丙烯酸的蒸馏塔的停止和开始操作中，停止蒸馏塔的操作后，连接的再沸器的加热被中断，然后再沸器被快速冷却; 和/或在开始用于生产（甲基）丙烯酸的蒸馏塔的操作时，将蒸馏塔的内壁表面加热到高于（甲基）丙烯酸的冷凝温度的温度和蒸馏塔在加热条件下启动。根据本发明，能够在避免蒸馏塔内发生聚合的同时，早日安全地停止蒸馏塔的运转，并且能够长时间稳定地进行丙烯酸类单体的蒸馏操作。

9. 发明申请

US20050209482A1 Storage tank for easily polymerizable compound and method of storage 有权
标题翻译：容易聚合的化合物储存罐和储存方法
公开(公告)号：US20050209482A1
公开(公告)日：2005-09-22
申请号：US11133184
申请日：2005-05-20
申请人： Shuhei Yada , Yasushi Ogawa , Yoshiro Suzuki , Kimikatsu Jinno , Hirochika Hosaka , Masayasu Goriki
发明人： Shuhei Yada , Yasushi Ogawa , Yoshiro Suzuki , Kimikatsu Jinno , Hirochika Hosaka , Masayasu Goriki
IPC分类号： B01J4/00 , B01J19/00 , B65D90/00 , C07C51/42 , C07C51/50 , C07C57/04 , C07C67/48 , F16L23/00 , F17D1/08 , G05D7/00
CPC分类号： B01J19/00 , B01J2219/00006 , B01J2219/00083 , B01J2219/00247 , B01J2219/00252 , B01J2219/00254 , Y10T137/0391 , Y10T137/6416 , Y10T137/6579 , Y10T137/85978
摘要： The storage tank of the invention for an easily polymerizable compound is a storage tank having an acceptance piping and a delivery piping and is characterized by having a circulation line which directly connects the acceptance piping to the delivery piping or having circulation lines which respectively connect the acceptance piping to the storage tank and the storage tank to the delivery piping; the method of storing of the invention is characterized by storing an easily polymerizable compound in the storage tank while circulating the compound in the storage tank through the circulation line(s); the method of pipe jointing and apparatus therefor of the invention are a method of jointing pipes fitted to a handling apparatus in a production apparatus, storage apparatus, or the like for the purpose of transporting a corrosive liquid, the method being characterized in that the pipes are jointed with flanges, bolts, and nuts made of a material having resistance to corrosion by the corrosive liquid; the process for (meth)acrylic acid compound production of the invention is a process for producing and/or purifying a (meth)acrylic acid compound, and is characterized in that the temperature of a purified (meth)acrylic acid compound obtained which is being supplied to a storage tank is regulated so as to be not higher than the temperature of the purified (meth)acrylic acid compound residing in the storage tank; and the process of the invention for producing an easily polymerizable compound which is a (meth)acrylic acid compound is characterized in that the temperature of a (meth)acrylic acid compound-containing liquid which has been discharged as an off-specification product and is being supplied to a storage tank is regulated so as to be not higher than the temperature of the off-specification liquid stored in the storage tank.
摘要翻译：用于易聚合化合物的本发明的储罐是具有接受管道和输送管道的储罐，其特征在于，具有将接收管道直接连接到输送管道的循环管线或具有分别连接接收的循环管线管道到储罐和储罐到输送管道; 本发明的储存方法的特征在于，通过在循环管道中使化合物在储罐中循环而将容易聚合的化合物储存在储罐中; 本发明的管接头方法及其设备是在制造装置，储存装置等中装配于处理装置的管道的输送腐蚀性液体的方法，其特征在于，管道与由腐蚀性液体具有腐蚀性的材料制成的法兰，螺栓和螺母接合; 本发明的（甲基）丙烯酸化合物的制造方法是（甲基）丙烯酸化合物的制造和/或纯化方法，其特征在于，得到的纯化的（甲基）丙烯酸化合物的温度为调节供给到储罐的温度不高于存储在储罐中的纯化的（甲基）丙烯酸化合物的温度; 本发明的制备作为（甲基）丙烯酸化合物的易聚合性化合物的方法的特征在于，作为脱离规格的产品排出的（甲基）丙烯酸化合物的液体的温度为被调节为不高于储存在储罐中的不合格液体的温度。

10. 发明申请

US20080234522A1 Method for vapor phase catalytic oxidation 有权
公开(公告)号：US20080234522A1
公开(公告)日：2008-09-25
申请号：US12081916
申请日：2008-04-23
申请人： Shuhei Yada , Masayasu Goriki , Hirochika Hosaka , Kimikatsu Jinno , Teruo Saito , Yoshiro Suzuki
发明人： Shuhei Yada , Masayasu Goriki , Hirochika Hosaka , Kimikatsu Jinno , Teruo Saito , Yoshiro Suzuki
IPC分类号： C07C45/33 , C07C45/35 , C07C51/25 , B01J8/02
CPC分类号： B01J8/003 , B01J8/0085 , B01J8/067 , B01J23/002 , B01J23/28 , B01J23/31 , B01J23/8876 , B01J35/026 , B01J2208/00212 , B01J2208/00221 , B01J2208/00513 , B01J2208/00539 , B01J2208/00663 , B01J2208/00752 , B01J2523/00 , C07C45/33 , C07C45/35 , C07C51/252 , C07C47/22 , C07C57/04 , B01J2523/12 , B01J2523/13 , B01J2523/305 , B01J2523/41 , B01J2523/54 , B01J2523/68 , B01J2523/842 , B01J2523/845 , B01J2523/847
摘要： An object of the present invention is to provide a method for vapor phase catalytic oxidation which is almost free of variations in reaction states in respective reaction tubes of the fixed bed multi-tube heat-exchanger type reactor.Provided is a method for vapor phase catalytic oxidation for obtaining a reaction product gas by using a fixed bed multi-tube heat-exchanger type reactor provided with a plurality of reaction tubes and by feeding a raw material gas inside the reaction tubes packed with a catalyst, wherein the method comprises: adjusting pressure losses of the respective reaction tubes so that the pressure losses of the respective reaction tubes after catalyst packing is within ±20% of an average pressure loss of the reaction tubes by: packing an inert substance at a raw material gas inlet portion of the reaction tubes or removing and re-packing the catalyst packed, for a reaction tube having a pressure loss lower than the average pressure loss of the reaction tubes; and removing and re-packing the catalyst packed, for a reaction tube having a pressure loss higher than the average pressure loss of the reaction tubes.

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