RU2019131826A - Катализатор превращения синтез-газа в спирты - Google Patents
Катализатор превращения синтез-газа в спирты Download PDFInfo
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- RU2019131826A RU2019131826A RU2019131826A RU2019131826A RU2019131826A RU 2019131826 A RU2019131826 A RU 2019131826A RU 2019131826 A RU2019131826 A RU 2019131826A RU 2019131826 A RU2019131826 A RU 2019131826A RU 2019131826 A RU2019131826 A RU 2019131826A
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- catalyst
- catalyst component
- porous oxide
- oxide support
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- 239000003054 catalyst Substances 0.000 title claims 63
- 230000015572 biosynthetic process Effects 0.000 title claims 7
- 238000003786 synthesis reaction Methods 0.000 title claims 7
- 238000006243 chemical reaction Methods 0.000 title claims 3
- 150000001298 alcohols Chemical class 0.000 title claims 2
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 claims 14
- 239000007789 gas Substances 0.000 claims 14
- OKKJLVBELUTLKV-UHFFFAOYSA-N Methanol Chemical compound OC OKKJLVBELUTLKV-UHFFFAOYSA-N 0.000 claims 9
- 229910052739 hydrogen Inorganic materials 0.000 claims 8
- 239000001257 hydrogen Substances 0.000 claims 8
- 238000000034 method Methods 0.000 claims 7
- 239000000377 silicon dioxide Substances 0.000 claims 7
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 claims 6
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 claims 6
- 229910052783 alkali metal Inorganic materials 0.000 claims 6
- 150000001340 alkali metals Chemical class 0.000 claims 6
- 229910052723 transition metal Inorganic materials 0.000 claims 5
- 150000003624 transition metals Chemical class 0.000 claims 5
- UGFAIRIUMAVXCW-UHFFFAOYSA-N Carbon monoxide Chemical compound [O+]#[C-] UGFAIRIUMAVXCW-UHFFFAOYSA-N 0.000 claims 4
- GWEVSGVZZGPLCZ-UHFFFAOYSA-N Titan oxide Chemical compound O=[Ti]=O GWEVSGVZZGPLCZ-UHFFFAOYSA-N 0.000 claims 4
- MCMNRKCIXSYSNV-UHFFFAOYSA-N Zirconium dioxide Chemical compound O=[Zr]=O MCMNRKCIXSYSNV-UHFFFAOYSA-N 0.000 claims 4
- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 claims 4
- 238000001354 calcination Methods 0.000 claims 4
- 229910002091 carbon monoxide Inorganic materials 0.000 claims 4
- 229910052703 rhodium Inorganic materials 0.000 claims 4
- 235000012239 silicon dioxide Nutrition 0.000 claims 4
- OGIDPMRJRNCKJF-UHFFFAOYSA-N titanium oxide Inorganic materials [Ti]=O OGIDPMRJRNCKJF-UHFFFAOYSA-N 0.000 claims 4
- 229910052748 manganese Inorganic materials 0.000 claims 3
- XUIMIQQOPSSXEZ-UHFFFAOYSA-N Silicon Chemical compound [Si] XUIMIQQOPSSXEZ-UHFFFAOYSA-N 0.000 claims 2
- RTAQQCXQSZGOHL-UHFFFAOYSA-N Titanium Chemical compound [Ti] RTAQQCXQSZGOHL-UHFFFAOYSA-N 0.000 claims 2
- QCWXUUIWCKQGHC-UHFFFAOYSA-N Zirconium Chemical compound [Zr] QCWXUUIWCKQGHC-UHFFFAOYSA-N 0.000 claims 2
- 229910052782 aluminium Inorganic materials 0.000 claims 2
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 claims 2
- 238000001035 drying Methods 0.000 claims 2
- 150000002431 hydrogen Chemical class 0.000 claims 2
- 229910052742 iron Inorganic materials 0.000 claims 2
- 229910052744 lithium Inorganic materials 0.000 claims 2
- 239000000203 mixture Substances 0.000 claims 2
- RVTZCBVAJQQJTK-UHFFFAOYSA-N oxygen(2-);zirconium(4+) Chemical compound [O-2].[O-2].[Zr+4] RVTZCBVAJQQJTK-UHFFFAOYSA-N 0.000 claims 2
- 230000035515 penetration Effects 0.000 claims 2
- 239000011148 porous material Substances 0.000 claims 2
- 229910052700 potassium Inorganic materials 0.000 claims 2
- 229910052710 silicon Inorganic materials 0.000 claims 2
- 239000010703 silicon Substances 0.000 claims 2
- 229910052708 sodium Inorganic materials 0.000 claims 2
- 229910052719 titanium Inorganic materials 0.000 claims 2
- 239000010936 titanium Substances 0.000 claims 2
- 229910052726 zirconium Inorganic materials 0.000 claims 2
- 229910001928 zirconium oxide Inorganic materials 0.000 claims 2
- 229910052792 caesium Inorganic materials 0.000 claims 1
- 229910052804 chromium Inorganic materials 0.000 claims 1
- 229910052802 copper Inorganic materials 0.000 claims 1
- 239000000463 material Substances 0.000 claims 1
- 229910052751 metal Inorganic materials 0.000 claims 1
- 239000002184 metal Substances 0.000 claims 1
- 238000002156 mixing Methods 0.000 claims 1
- 239000011541 reaction mixture Substances 0.000 claims 1
- 238000011084 recovery Methods 0.000 claims 1
- 229910052701 rubidium Inorganic materials 0.000 claims 1
- 239000000758 substrate Substances 0.000 claims 1
- 229910052725 zinc Inorganic materials 0.000 claims 1
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Claims (38)
1. Катализатор превращения синтез-газа, причем указанный катализатор содержит первый каталитический компонент и второй каталитический компонент, где первый каталитический компонент содержит нанесенный на первую пористую оксидную подложку Rh, Mn, щелочной металл M и Fe, и где второй каталитический компонент содержит нанесенный на второй пористый оксидный материал-носитель Cu и переходный металл, отличный от Cu.
2. Катализатор по п. 1, где в первом каталитическом компоненте,
молярное соотношение Rh, вычисленного как элементарный Rh, и Mn, вычисленного как элементарный Mn, находится в интервале от 0,1 до 10, предпочтительно в интервале от 1 до 8, более предпочтительно в интервале от 2 до 5;
молярное соотношение Rh, вычисленного как элементарный Rh, и Fe, вычисленного как элементарный Fe, находится в интервале от 0,1 до 10, предпочтительно в интервале от 1 до 8, более предпочтительно в интервале от 2 до 5, и
молярное соотношение Rh, вычисленного как элементарный Rh, и щелочного металла M, вычисленного как элементарный M, находится в интервале от 0,1 до 5, предпочтительно в интервале от 0,15 до 3, более предпочтительно в интервале от 0,25 до 2,5.
3. Катализатор по п. 1, где щелочной металл M, содержащийся в первом каталитическом компоненте, представляет собой один или более из Na, Li, K, Rb, Cs, предпочтительно один или более из Na, Li и K, где более предпочтительно, щелочной металл M, содержащийся в первом каталитическом компоненте, содержит, более предпочтительно представляет собой Li.
4. Катализатор по п. 1, где по меньшей мере 99 мас.%, предпочтительно по меньшей мере 99,5 мас.%, более предпочтительно по меньшей мере 99,9 мас.% первого каталитического компонента состоит из Rh, Mn, щелочного металла M, Fe, O, и первой пористой оксидной подложки.
5. Катализатор по п. 1, где первая пористая оксидная подложка содержит диоксид кремния, оксид циркония, оксид титана, оксид алюминия, смесь двух или более из диоксида кремния, оксида циркония, оксида титана, и оксида алюминия, или смешанный оксид двух или более из кремния, циркония, титана и алюминия, где более предпочтительно, первая пористая оксидная подложка содержит диоксид кремния, где в первом каталитическом компоненте, массовое соотношение Rh, вычисленного как элементарный Rh, и первой пористой оксидной подложки, находится предпочтительно в интервале от 0,001:1 до 4000:1, более предпочтительно в интервале от 0,005:1 до 0,200:1, более предпочтительно в интервале от 0,010:1 до 0,070:1.
6. Катализатор по п. 1, где первый каталитический компонент имеет удельную площадь поверхности по БЭТ в интервале от 250 до 500 м²/г, предпочтительно в интервале от 320 до 450 м²/г, общий объем проникновения в интервале от 0,1 до 5 мл/г, предпочтительно в интервале от 0,5 до 3 мл/г, и средний диаметр пор в интервале от 0,001 до 0,5 микрометров, предпочтительно в интервале от 0,01 до 0,05 микрометров.
7. Катализатор по п. 1, где во втором каталитическом компоненте, переходный металл отличный от Cu, представляет собой один или более из Cr и Zn, предпочтительно Zn, где молярное соотношение Cu, вычисленного как элементарный Cu, и переходного металла отличного от Cu, предпочтительно Zn, вычисленного как элементарный металл, предпочтительно как Zn, предпочтительно находится в интервале от 0,1 до 5, более предпочтительно в интервале от 0,2 до 4, более предпочтительно в интервале от 0,3 до 1,0.
8. Катализатор по п. 1, где по меньшей мере 99 мас.%, предпочтительно по меньшей мере 99,5 мас.%, более предпочтительно по меньшей мере 99,9 мас.% второго каталитического компонента состоит из Cu, переходного металла отличного от Cu, O, и второй пористой оксидной подложки.
9. Катализатор по п. 1, где вторая пористая оксидная подложка содержит диоксид кремния, оксид циркония, оксид титана, оксид алюминия, смесь двух или более из диоксида кремния, оксида циркония, оксида титана, и оксида алюминия, или смешанный оксид двух или более из кремния, циркония, титана и алюминия, где более предпочтительно, вторая пористая оксидная подложка содержит диоксид кремния, где предпочтительно по меньшей мере 99 мас.%, более предпочтительно по меньшей мере 99,5 мас.%, более предпочтительно по меньшей мере 99,9 мас.% второй пористой оксидной подложки состоит из диоксида кремния, где массовое соотношение Cu, вычисленного как элементарный Cu, и второй пористой оксидной подложки находится в интервале от 0,001 до 0,5, предпочтительно в интервале от 0,005 до 0,25, более предпочтительно в интервале от 0,01 до 0,20.
10. Катализатор по п. 1, где второй каталитический компонент имеет удельную площадь поверхности по БЭТ в интервале от 100 до 500 м²/г, предпочтительно в интервале от 200 до 350 м²/г, общий объем проникновения в интервале от 0,1 до 10 мл/г, предпочтительно в интервале от 0,5 до 5 мл/г, и средний диаметр пор в интервале от 0,001 до 5 микрометров, предпочтительно в интервале от 0,01 до 2,5 микрометров.
11. Катализатор по п. 1, где массовое соотношение первого каталитического компонента и второго каталитического компонента находится в интервале от 1 до 10, предпочтительно в интервале от 1,5 до 8; более предпочтительно в интервале от 2 до 6.
12. Катализатор по любому из пп. 1-11, где по меньшей мере 99 мас.%, предпочтительно по меньшей мере 99,5 мас.%, более предпочтительно по меньшей мере 99,9 мас.% катализатора состоит из первого каталитического компонента и второго каталитического компонента.
13. Трубка реактора для превращения синтез-газа, содержащая слой катализатора, который содержит катализатор по любому из пп. 1-12.
14. Трубка реактора по п. 13, предпочтительно расположенная вертикально, содержащая две или более зон слоя катализатора, где первая зона слоя катализатора расположена сверху второй зоны слоя катализатора, где первая зона слоя катализатора содержит, предпочтительно состоит из катализатора по любому из пп. 1-12, и где вторая зона слоя катализатора содержит, предпочтительно состоит из второго каталитического компонента по любому из пп. 1 и 7-10.
15. Трубка реактора по п. 13 или 14, где объем первой зоны слоя катализатора относительно объема второй зоны слоя катализатора находится в интервале от 0 до 100, предпочтительно в интервале от 0,01 до 50, более предпочтительно в интервале от 0,5 до 5.
16. Применение катализатора по любому из пп. 1-12, при необходимости в комбинации со вторым каталитическим компонентом по любому из пп. 1 и 7-10, для превращения синтез-газа, содержащего водород и монооксид углерода, предпочтительно для превращения синтез-газа, содержащего водород и монооксид углерода, в один или более спиртов, предпочтительно один или более из метанола и этанола.
17. Способ превращения синтез-газа, содержащего водород и монооксид углерода, в один или более из метанола и этанола, причем указанный способ включает
(i) обеспечение потока газа, который содержит поток синтез-газа, содержащий водород и монооксид углерода;
(ii) обеспечение катализатора по любому из пп. 1-12 и при необходимости второго каталитического компонента по любому из пп. 1 и 7-10;
(iii) приведение потока газа, обеспеченного на стадии (i), в контакт с катализатором, обеспеченным на стадии (ii), и при необходимости вторым каталитическим компонентом, получая поток реакционной смеси, содержащей один или более из метанола и этанола.
18. Способ по п. 17, где перед стадией (iii), катализатор, обеспеченный на стадии (i), восстанавливают, где восстановление катализатора предпочтительно включает приведение катализатора в контакт с потоком газа, содержащим водород, где предпочтительно по меньшей мере 95 об.%, предпочтительно по меньшей мере 98 об.%, более предпочтительно по меньшей мере 99 мас.% потока газа состоит из водорода, где поток газа, содержащий водород, приводят в контакт с катализатором при температуре потока газа предпочтительно в интервале от 250 до 350°C, более предпочтительно в интервале от 275 до 325°C, и где поток газа, содержащий водород, приводят в контакт с катализатором при давлении потока газа предпочтительно в интервале от 10 до 100 бар(абсолютное), предпочтительно в интервале от 20 до 80 бар(абсолютное).
19. Способ получения катализатора по любому из пп. 1-12, включающий
(a) обеспечение первого каталитического компонента по любому из пп. 1-6;
(b) обеспечение второго каталитического компонента по любому из пп. 1 и 7-10;
(c) смешивание первого каталитического компонента, обеспеченного на стадии (a), и второго каталитического компонента, обеспеченного на стадии (b).
20. Способ по п. 19, где обеспечение первого каталитического компонента согласно стадии (a) включает получение первого каталитического компонента способом, включающим
(a.1) обеспечение источника первой пористой оксидной подложки, предпочтительно включающее подвергание источника первой пористой оксидной подложки кальцинированию;
(a.2) обеспечение источника Rh, источника Mn, источника щелочного металла, предпочтительно Li, и источника Fe;
(a.3) импрегнирование предпочтительно кальцинированного источника первой пористой оксидной подложки, полученной на стадии (a.1), источниками, обеспеченными на стадии (a.2);
(a.4) кальцинирование импрегнированного источника первой пористой оксидной подложки, предпочтительно после сушки,
и где обеспечение второго каталитического компонента согласно стадии (b) включает получение второго каталитического компонента способом, включающим
(b.1) обеспечение источника второй пористой оксидной подложки, предпочтительно включающее подвергание источника второй пористой оксидной подложки кальцинированию;
(b.2) обеспечение источника Cu, источника переходного металла отличного от Cu, предпочтительно Zn;
(b.3) импрегнирование предпочтительно кальцинированного источника второй пористой оксидной подложки, полученного на стадии (a.1), источниками, обеспеченными на стадии (a.2);
(b.4) кальцинирование импрегнированного источника второй пористой оксидной подложки, предпочтительно после сушки.
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