CN1040609A - 烃类进料的催化裂化方法 - Google Patents

烃类进料的催化裂化方法 Download PDF

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CN1040609A
CN1040609A CN89106511A CN89106511A CN1040609A CN 1040609 A CN1040609 A CN 1040609A CN 89106511 A CN89106511 A CN 89106511A CN 89106511 A CN89106511 A CN 89106511A CN 1040609 A CN1040609 A CN 1040609A
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伊安·埃尔尼斯特·马克思威尔
杰迪普·比斯瓦斯
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    • C—CHEMISTRY; METALLURGY
    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10G—CRACKING HYDROCARBON OILS; PRODUCTION OF LIQUID HYDROCARBON MIXTURES, e.g. BY DESTRUCTIVE HYDROGENATION, OLIGOMERISATION, POLYMERISATION; RECOVERY OF HYDROCARBON OILS FROM OIL-SHALE, OIL-SAND, OR GASES; REFINING MIXTURES MAINLY CONSISTING OF HYDROCARBONS; REFORMING OF NAPHTHA; MINERAL WAXES
    • C10G11/00—Catalytic cracking, in the absence of hydrogen, of hydrocarbon oils
    • C10G11/02—Catalytic cracking, in the absence of hydrogen, of hydrocarbon oils characterised by the catalyst used
    • C10G11/04—Oxides
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    • B01J29/00—Catalysts comprising molecular sieves
    • B01J29/005—Mixtures of molecular sieves comprising at least one molecular sieve which is not an aluminosilicate zeolite, e.g. from groups B01J29/03 - B01J29/049 or B01J29/82 - B01J29/89
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
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    • B01J29/00—Catalysts comprising molecular sieves
    • B01J29/04—Catalysts comprising molecular sieves having base-exchange properties, e.g. crystalline zeolites
    • B01J29/06—Crystalline aluminosilicate zeolites; Isomorphous compounds thereof
    • B01J29/65—Crystalline aluminosilicate zeolites; Isomorphous compounds thereof of the ferrierite type, e.g. types ZSM-21, ZSM-35 or ZSM-38, as exemplified by patent documents US4046859, US4016245 and US4046859, respectively
    • B01J29/66—Crystalline aluminosilicate zeolites; Isomorphous compounds thereof of the ferrierite type, e.g. types ZSM-21, ZSM-35 or ZSM-38, as exemplified by patent documents US4046859, US4016245 and US4046859, respectively containing iron group metals, noble metals or copper
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    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J2229/00—Aspects of molecular sieve catalysts not covered by B01J29/00
    • B01J2229/10—After treatment, characterised by the effect to be obtained
    • B01J2229/26—After treatment, characterised by the effect to be obtained to stabilize the total catalyst structure
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J2229/00—Aspects of molecular sieve catalysts not covered by B01J29/00
    • B01J2229/30—After treatment, characterised by the means used
    • B01J2229/42—Addition of matrix or binder particles

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Abstract

催化裂化烃类进料的方法，包括在催化裂化条件下使烃进料与催化剂组合物接触，催化剂组合物含有孔径大于7nm的沸石I和孔径小于7nm的沸石II，还含有至少一种脱氢金属或金属组分。

Description

本发明涉及在催化裂化条件下采用适宜的催化剂与原料接触，对烃类进料进行催化裂化的方法。
催化裂化是工业上大规模采用的精制工艺。本文所述的方法是将重质烃馏分转化成较轻和粘度较小的产物。转化或裂化是在催化剂存在下主要于气相中发生的。例如可将原料转化为汽油。部分进料被转化成每分子4个或4个以下碳原子的气体。该气体由部分烯烃和部分饱和烃组成。
在裂化反应过程中，某些重质物料（例如炭）沉积在催化剂上，这降低了催化剂的催化活性，因此需要再生处理。通常是烧掉催化剂上的积炭实现再生、恢复催化剂活性。催化裂化工艺中三个比较鲜明的步骤是将烃料转化成较轻产物的裂化步骤，将吸附在催化剂上的烃脱除的抽提步骤和从催化剂上烧掉积炭的再生步骤。再生过的催化剂重新用于裂化步骤。
作为催化裂化的催化剂，非晶形基质的沸石是非常有效的，特别是孔径相对较大（即大于0.7nm）的沸石更为适宜。由EP-B-0，131，986可知由大孔径沸石Ⅰ和孔径小于0.7nm的沸石Ⅱ（ZSM-5-型）组成的催化剂组合物，由DE-A-2，149，218还可知其它类似的催化剂组合物。
如上所述，被裂化的部分进料转化成气态馏分，且其中部分是饱和的，内在价值较低。因此，如果将该工艺和/或催化剂改进，使之基本上不形成饱和气态化合物，那将是很有利的。现在令人惊奇地发现，如果催化剂组合物再含有一种脱氢金属或金属组分，可降低饱和气态组分的产率。
为此，本发明提供了催化裂化烃类进料的方法，包括在催化裂化条件下使烃进料与催化剂组合物接触，所述催化剂组合物含有孔径大于0.7nm的沸石Ⅰ和孔径小于0.7nm的沸石Ⅱ，该催化剂组合物还含有至少一种脱氢金属或金属组分。
本发明的令人惊奇之处由US-A-4，100，218可见，该专利描述的是使用孔径小于0.7nm的沸石催化剂由烯烃物流制备液化石油气（饱和的C3-4烃）和汽油的方法，该催化剂可以含有一种金属组分，例如Ⅷ族脱氢金属。由于已知沸石（上述所指为沸石Ⅱ）具有促进烯烃转化为饱和气态烃的活性，因此根据本发明形成了烯烃气态产物是出乎意料的。
脱氢金属或金属组分被施加到沸石催化剂组合物上。可以将脱氢金属（组分）分布于两种沸石之上，这时，脱氢活性表现在对整体进料上。可以相信，当脱氢金属（组分）只分布于沸石Ⅱ上时，只是对于能进入沸石Ⅱ孔的分子才有脱氢活性，即只有线型和或相对较小的分子将受到金属脱氢活性的作用。由于本发明的一个目的是将线型和/或相对小的分子（包括C6-C8环型化合物，例如环烷烃）转化为小分子烯烃或芳烃，因此，仅由沸石Ⅱ含有脱氢金属是可取的。
脱氢金属或金属组分的用量可在宽范围内选取，然而太低的量（即ppm级）所显示的活性太差，不适于工业实施。因此，脱氢金属（组分）的用量以金属计基于沸石Ⅱ宜为0.5-20%（重量）。
可以采用的脱氢金属可从众多的金属中选取。适宜的金属包括Ⅱb族，特别是锌、Ⅲb族，特别是镓。较好的是选取Ⅷ族和/或Ⅵb族金属或金属组分。更为可取的是该金属选自铂、钯、镍、钴、钼、钨和其混合物。当有一种贵金属（如铂或钯）被采用时，Ⅷ族金属以金属态存在为宜，当采用非贵金属（如镍和/或钴和/或钼和/或钨）时，脱氢金属可以氧化态、硫化态或金属态存在。
沸石Ⅰ与沸石Ⅰ和沸石Ⅱ之和的重量百分比可以变化。该重量百分比宜为0.1-30%，更可取的为1-10%。
用于本发明方法的催化剂组合物含有两种沸石。在本发明的一个实施方案中，催化剂组合物包括至少两种裂化组分的物理混合物，一种含有沸石Ⅰ，另一种含有沸石Ⅱ。在这一实施方案中，该组合物由各自含有两种沸石之一的催化剂颗粒的混合物构成。本领域的技术人员不难想到，催化剂颗粒还可含有诸如耐火氧化物一类的基体材料，例如二氧化硅、氧化铝、二氧化硅-氧化铝、氧化镁、氧化钍、二氧化钛和氧化锆。在本发明另一更为可取的实施方案中，该催化剂组合物是在多孔基体材料上含有沸石Ⅰ和沸石Ⅱ的均匀混合物，即每一催化剂颗粒都含有两种沸石。
沸石Ⅰ的孔径大于0.7nm，适用的沸石Ⅰ的孔径可大到1.2nm。适宜的沸石Ⅰ包括八面沸石和沸石L。八面沸石（包括沸石X和Y）较为可取，其中沸石Y更为可取。沸石可以呈酸性态，即沸石基本上不含任何碱金属离子的状态。可以将上述的脱氢金属载于沸石之上。较好的是，沸石Ⅰ含有稀土金属。可用任何常规方法将稀土金属掺加到沸石上，其中离子交换是特别适用的方法。
沸石Ⅱ的孔径小于0.7nm，并可小至0.4nm。适宜的沸石Ⅱ包括结晶二氧化硅、磷酸硅铝、磷酸铬、硅酸镓、硅酸铁、磷酸铝、硅铝酸钛、硅酸硼、铝磷酸钛和硅铝酸铁。可以应用于本发明的方法其孔径为0.4-0.7nm的沸石Ⅱ的实例包括SAPO-4和SAPO-11（见US-A-4，440，871），ALPO-11（见US-A-4，310，440），TAPO-11（见US-A-4，500，651），TASO-45（见EP-A-229，295），硅酸硼（见US-A-4，254，297），诸如毛沸石、镁碱沸石一类的硅酸铝，
Figure 891065113_IMG1
和ZSM型沸石，例如ZSM-5、ZSM-11、ZSM-12、ZSM-35、ZSM-23和ZSM-38。较好的是，沸石选自具有ZSM-5结构的结晶金属硅酸盐、镁碱沸石、毛沸石和其混合物。适宜的具有ZSM-5结构的结晶金属硅酸盐的实例有硅酸铝、硅酸镓、硅酸铁、硅酸钪、硅酸铑和/或硅酸铬（见GB-B-2，110，559）。这些硅酸盐的孔径在0.5-0.6nm的范围内。
沸石Ⅱ不宜呈酸性态，这可以通过使脱氢金属（组分）占据可能能的酸位来实现。还可以使沸石Ⅱ呈它的碱金属形式。通过在沸石Ⅱ上防止出现大量酸位，可以降低过度裂化较小分子的危险。
本发明所用催化剂组合的制备可用任何常规方法完成，例如离子交换、（共）沉积、浸渍、（共）研磨等。适宜的方法是，经一种或多种常规方法制备含有脱氢金属的沸石Ⅱ，将这种负载沸石与基体材料和沸石Ⅱ制成催化剂颗粒。
本发明的方法在催化裂化条件下进行，即在方法的进行中不添加氢。较好的是使用向上的或向下的移动催化床，以常规的塞摩福（Thermofor）催化裂化或流化催化裂化过程为宜。工艺条件宜为温度400-650℃，特别是450-600℃，压力1-10巴，特别是1-7.5巴，重量的空速1-250kg/kg·h，特别是5-150kg/kg·h，催化剂组合物/进料重量比1-25、特别是1.5-20。
可用于本发明方法的进料包括常规的催化裂化原料，例如（减压）瓦斯油，脱沥青残油以及常压或减压渣油。一般说来，常规的催化裂化原料含有沸点至少为330℃的烃类。本发明的一个优点在于有可能在原料中包括附加的含2-5个碳原子的烃。这些较小的分子将被脱氢以得到有更高价值的烯烃。因此，本发明的方法可以有利地利用含有沸点至少为330℃的烃类和2-5个碳原子的烃类的原料来进行。原料可由气态（C2-5）烃、石脑油、煤油、粗柴油、减压馏分和减压渣油的混合物组成。较好的是，原料由上述的常规催化裂化原料和气态C2-5烃的混合物组成。原料中含有2-5个碳原子的烃的量宜为沸点至少为330℃的烃和C2-5烃总重的1-20%。
分子中含有2-5个碳原子的烃可从多种来源获得。适宜的来源包括直馏液化石油气，加氢处理和/或加氢裂化的气态产物，烷基化或催化脱蜡的废物流等。C2-5烃最好含有液化石油气馏分，即丙烷和/或丁烷。
可取的是，含有2-5个碳原子的烃至少部分来自本发明方法中所获得的循环物流。本发明的方法产生烯烃，但仍有一部分饱和化合物未被转化。将未转化的烃分离之后，很容易将其循环至本发明的方法中。

Claims (20)

1、催化裂化烃类进料的方法，包括在催化裂化条件下使进料与催化剂组合物接触，所述催化剂组合物含有孔径大于0.7nm的沸石I和孔径小于0.7nm的沸石Ⅱ，该组合物还含有至少一种脱氢金属或金属组分。
2、根据权利要求1的方法，其中只有沸石Ⅱ含有脱氢金属或金属组分。
3、根据权利要求1或2的方法，其中在催化剂组合物中脱氢金属或金属组分的含量为沸石Ⅱ重量的0.5-20%。
4、根据权利要求1-3的任一方法，其中脱氢金属选自Ⅵb族和/或Ⅷ族。
5、根据权利要求4的方法，其中脱氢金属选自铂、钯、镍、钴铁、钨、钼和其混合物。
6、根据权利要求1-5的任一方法，其中在催化剂组合物中沸石Ⅰ相对于沸石Ⅰ和Ⅱ的总重的百分比为0.1-30%。
7、根据权利要求1-6的任一方法，其中催化剂组合物包括含有沸石Ⅰ的催化剂颗粒和含有沸石Ⅱ的催化剂颗粒的物理混合物。
8、根据权利要求1-6的任一方法，其中催化剂组合物含有于多孔基质上均匀混合的沸石Ⅰ和Ⅱ。
9、根据权利要求1-8的任一方法，其中催化剂组合物中的沸石Ⅰ包括八面沸石。
10、根据权利要求9的方法，其中八面沸石是沸石Y。
11、根据权利要求9或10的方法，其中八面沸石含有稀土金
12、根据权利要求1-11的任一方法，其中沸石Ⅱ选自具有ZSM-5结构的结晶金属硅酸盐、镁碱沸石、毛沸石及其混合物。
13、根据权利要求1-11的任一方法，其中沸石Ⅱ基本上呈其碱金属形式。
14、根据权利要求1-13的任一方法，所述方法在没有添加氢的条件下进行。
15、根据权利要求1-14的任一方法，所述方法在向上或向下移动的催化床中进行。
16、根据权利要求1-15的任一方法，所述方法在温度为400-650℃，压力为1-10巴，空速为1-250kg/kg·h和催化剂组合物/进料重量比为1-25的条件下进行。
17、根据权利要求1-16的任一方法，其中烃进料含有沸点至少为330℃的烃类和C2-5烃。
18、根据权利要求17的方法，其中进料中C2-5烃的含量为沸点至少为330℃的烃和C2-5烃总重的1-20%。
19、根据权利要求1-18的任一方法，其中C2-5烃至少部分来自本方法中得到的循环物流。
20、根据权利要求1-18的任一方法，其中C2-5烃包括液化石油气馏分。
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CN101171082B (zh) * 2005-04-29 2012-09-05 格雷斯公司 用在部分燃烧FCC工艺中的减少NOx的组合物
CN101503632B (zh) * 2003-11-06 2013-01-23 格雷斯公司 流化裂化催化剂及降低流化裂化期间NOx排放量的方法

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MY106601A (en) 1995-06-30
AU4021289A (en) 1990-03-01
KR900003338A (ko) 1990-03-26
DE68901960T2 (de) 1992-12-10
GR3005150T3 (zh) 1993-05-24
AU616791B2 (en) 1991-11-07
CA1333576C (en) 1994-12-20
DE68901960D1 (de) 1992-08-06
US4976847A (en) 1990-12-11
IN174290B (zh) 1994-10-29
KR0137029B1 (ko) 1998-04-24
JPH02113090A (ja) 1990-04-25
ES2033079T3 (es) 1993-03-01
EP0355928B1 (en) 1992-07-01
EP0355928A1 (en) 1990-02-28
BR8904248A (pt) 1990-04-10
SG45193G (en) 1993-06-25
JP2707140B2 (ja) 1998-01-28
CN1021970C (zh) 1993-09-01

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