EP3390574A1 - Process for converting mixed waste plastic into liquid fuels by catalytic cracking - Google Patents
Process for converting mixed waste plastic into liquid fuels by catalytic crackingInfo
- Publication number
- EP3390574A1 EP3390574A1 EP16809849.9A EP16809849A EP3390574A1 EP 3390574 A1 EP3390574 A1 EP 3390574A1 EP 16809849 A EP16809849 A EP 16809849A EP 3390574 A1 EP3390574 A1 EP 3390574A1
- Authority
- EP
- European Patent Office
- Prior art keywords
- waste plastic
- catalyst
- mixed waste
- weight
- reactor
- Prior art date
- Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
- Withdrawn
Links
Classifications
-
- 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
- C10G1/00—Production of liquid hydrocarbon mixtures from oil-shale, oil-sand, or non-melting solid carbonaceous or similar materials, e.g. wood, coal
- C10G1/10—Production of liquid hydrocarbon mixtures from oil-shale, oil-sand, or non-melting solid carbonaceous or similar materials, e.g. wood, coal from rubber or rubber waste
-
- 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
- C10G1/00—Production of liquid hydrocarbon mixtures from oil-shale, oil-sand, or non-melting solid carbonaceous or similar materials, e.g. wood, coal
- C10G1/08—Production of liquid hydrocarbon mixtures from oil-shale, oil-sand, or non-melting solid carbonaceous or similar materials, e.g. wood, coal with moving catalysts
- C10G1/086—Characterised by the catalyst used
-
- 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
- C10G2300/00—Aspects relating to hydrocarbon processing covered by groups C10G1/00 - C10G99/00
- C10G2300/10—Feedstock materials
- C10G2300/1003—Waste materials
-
- 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
- C10G2300/00—Aspects relating to hydrocarbon processing covered by groups C10G1/00 - C10G99/00
- C10G2300/70—Catalyst aspects
- C10G2300/701—Use of spent catalysts
Definitions
- the present invention relates to a process for converting mixed waste plastic into liquid fuels by catalytic cracking.
- the process comprises the steps of introducing mixed waste plastic and a catalyst comprising an amorphous-type catalyst within a reactor; allowing at least a portion of the mixed waste plastic to be converted to liquid fuels within the reactor; and removing a product stream containing said liquid fuels from the reactor.
- the volatile compounds can be either relatively high boiling liquid hydrocarbons useful as fuel oils or fuel oil supplements or light to medium boiling
- hydrocarbons useful as gasoline-type fuels or as other chemicals are hydrocarbons useful as gasoline-type fuels or as other chemicals.
- Catalytic cracking of mixed waste plastic is a process well known to the person skilled in the art.
- US 5,216,149 discloses a method for controlling the pyrolysis of a complex waste stream of plastics to convert such stream into useful high-value monomers or other chemicals, by identifying catalyst and temperature conditions that permit decomposition of a given polymer in the presence of others, without substantial decomposition of the other polymers.
- K.-H. Lee, et al. disclose in Polymer Degradation and Stability 84 (2004) 123-127 the liquid-phase catalytic degradation of mixtures of waste high-density polyethylene and polystyrene over spent FCC catalyst.
- the effect of the mixing proportions of polyethylene to polystyrene was studied and the authors found that an increase of polystyrene content in the reactants showed an increase of gasoline fraction and a decrease in kerosene and diesel fraction in the obtained liquid product.
- the fraction of aromatic components in the liquid product dramatically increased to 70 % and more even at a polystyrene content of only about 40 %. This finding is confirmed in the publication of K.-H.
- the present inventors found that this and other problems as described below can surprisingly by solved by selecting a certain ratio of polystyrene to polyolefm in the mixed waste plastic and increasing the ratio of catalyst comprising an amorphous-type catalyst to waste plastic in the reactor.
- the present invention therefore relates to a process for converting mixed waste plastic into liquid fuels by catalytic cracking, the process comprising :
- the mixed waste plastic contains from 5 to 50 % by weight of polystyrene and from 50 to 95 % by weight of polyolefm, each based on the total weight of polystyrene and polyolefm in the mixed waste plastic, and in that the weight ratio of catalyst to mixed waste plastic in the reactor is above 1 : 10.
- the gasoline fraction contains compounds having a low boiling point of for example below 216°C. This fraction includes compounds having 5 to 11 carbon atoms.
- the kerosene and diesel fraction has a higher boiling point of for example 216°C to 359°C. This fraction generally contains compounds having 12 to 21 carbon atoms.
- the even higher boiling fraction is generally designated as wax (Heavy Cycle Oil or HCO).
- the compounds are hydrocarbons which optionally comprise heteroatoms, such as N, O, etc.
- "Liquid fuels" in the sense of the present invention therefore are fuels like gasoline and diesel but may also be used as other valuable chemicals or solvents.
- a plastic is mostly constituted of a particular polymer and the plastic is generally named by this particular polymer.
- a plastic contains more than 25 % by weight of its total weight of the particular polymer, preferably more than 40 % by weight and more preferably more than 50 % by weight.
- Other components in plastic are for example additives, such as fillers, reinforcers, processing aids, plasticizers, pigments, light stabilizers, lubricants, impact modifiers, antistatic agents, inks, antioxidants, etc.
- a plastic comprises more than one additive.
- LDPE polyethylene
- PP polypropylene
- PS polystyrene
- Mixed plastics mostly constituted of polyolefm and polystyrene are preferred.
- concentration of the polyolefm and the polystyrene in the mixed plastic is above 50 % by weight, more preferably above 75 % by weight, each based on the total weight of the dry mixed plastic.
- the mixed plastic may be constituted of polyolefm and polystyrene.
- the mixed plastic contains less than 99.5 % by weight, more preferably less than 99 % by weight of polyolefm and polystyrene, based on the total weight of the dry mixed plastic.
- plastics such as polyvinylchloride, polyvinylidene chloride, polyethylene terephthalate, polyurethane (PU), acrylonitrile-butadiene-styrene (ABS), nylon and fluorinated polymers are less desirable. If present in the waste plastic, they are preferably present in a minor amount of less than 50 % by weight, preferably less than 30 % by weight, more preferably less than 20 % by weight, even more preferably less than 10 % by weight of the total weight of the dry waste plastic.
- the individual content of any less desirable plastic is less than 5 % by weight, more preferably less than 2 % by weight based on the total weight of the dry waste plastic.
- the plastics waste starting material comprises one or more thermoplastic polymers and is essentially free of thermosetting polymers.
- thermosetting polymers of less than 15, preferably less than 10 and even more preferably less than 5 wt % of the composition.
- waste plastic contains other non-desired components, namely foreign material, such as paper, glass, stone, metal, etc.
- the weight of the waste plastic or the weight of the polystyrene and polyolefm in the mixed waste plastic, this weight relates to the weight of the dry plastic without any foreign material being admixed with the plastic.
- the weight includes any components in the plastic, such as the above described additives.
- the present inventors found that when using a catalyst comprising an amorphous-type catalyst, the addition of polystyrene to polyolefm raw material increases the reaction rate of the de-polymerization reaction of the polyolefins. There is, however, an optimum polystyrene to polyolefm ratio that maximizes the rate kinetic constant of the polyolefin's de-polymerization reaction.
- the increase of rate kinetic constant is a significant advantage for an industrial process as it allows higher conversions as well as higher productivity.
- the rate kinetic constant of the polyolefin's de- polymerization reaction has a maximum when the mixed waste plastic contains about 20 % by weight of polystyrene based on the total weight of polystyrene and polyolefm in the mixed waste plastic. Still good values are achieved if the mixed waste plastic contains from 5 to 50 % by weight of polystyrene, preferably from 5 to 40 % by weight, more preferably from 5 to 30 % by weight and even more preferably from 10 to 30 % by weight of polystyrene, each based on the total weight of polystyrene and polyolefm in the mixed waste plastic. Most preferably, the mixed waste plastic contains from 15 to 25 % by weight, such as about 20 % by weight of polystyrene based on the total weight of polystyrene and polyolefm in the mixed waste plastic.
- the concentration of aromatic compounds in the gasoline and diesel fractions is low. It was even found that the quality of the diesel obtained with the process of the invention meets EN 590:2009+Al (version of February 2010) specification. In particular, the concentration of poly-aromatic compounds in the diesel fraction is low.
- the inventors found that the gasoline quality in particular at a concentration of about 20 % by weight of polyolefm in the mixed waste plastic is increased with respect to an increase in Research Octane Number (RON) and Motor Octane Number (MON).
- RON Research Octane Number
- MON Motor Octane Number
- the process of the present invention therefore is also characterized in that the weight ratio of catalyst to mixed waste plastic in the reactor is above 1 : 10.
- the weight ratio of catalyst to mixed waste plastic in the reactor is above 1 :9, more preferably above 1 :8, more preferably above 1 :7, more preferably above 1 :6, more preferably above 1 :5, more preferably above 1 :4 and even more preferably above 1 :3, such as above 1 :2.
- a particularly preferred weight ratio of catalyst to mixed waste plastic in the reactor is about 1 : 1.5.
- the weight ratio of catalyst to mixed waste plastic in the reactor can be below 10: 1, preferably below 7: 1.
- the weight ratio of catalyst to mixed waste plastic in the reactor can be for example in the range of from l :9 to 10: 1, preferably from 1 :8 to 10: 1, preferably from 1 :7 to 10: 1, preferably from 1 :6 to 10: 1, preferably from 1 :5 to 10: 1, preferably from 1 :4 to 10: 1, preferably from 1 :3 to 10: 1 and even more preferably from 1 :2 to 10: 1 or from 1 :2 to 7:1.
- the catalyst used in the process of the present invention comprises an amorphous-type catalyst.
- the catalyst predominantly is an amorphous-type catalyst.
- the catalyst consists of an amorphous-type catalyst.
- the catalyst additionally comprises a further catalyst, in particular a zeolite-type catalyst.
- amorphous-type catalyst is to be understood as an amorphous solid, such as an amorphous powder.
- amorphous solids are known to the skilled person.
- Amorphous solids lack crystallinity, namely the long-range order characteristic of a crystal. This feature may be observed via X-ray diffraction analysis by the lack of sharp Bragg reflexes.
- an amorphous-type catalyst may comprise a certain amount of crystalline solids.
- the amorphous-type catalyst comprises less than 50 % by weight, more preferably less than 25 % by weight, even more preferably less than 10 % by weight, such as less than 5 % by weight or less than 2 % or even less than 1 % by weight of crystalline solids, each based on the total weight of the catalyst.
- the term "predominantly" defines a catalyst which is a mixture of an amorphous-type catalyst and a non-amorphous- type catalyst, such as a zeolite-type catalyst, but wherein the catalyst comprises more than 50 % by weight of the amorphous-type catalyst based on the total weight of the catalyst.
- the catalyst comprises more than 60 %, more preferably more than 70 %, even more preferably more than 80 % and most preferably more than 90 % of the amorphous-type catalyst.
- the catalyst can comprise a single amorphous-type catalyst or a mixture of two or more amorphous-type catalysts.
- FCC catalysts are well known to the person skilled in the art.
- the amorphous-type catalyst may comprise silica, alumina, kaolin, or a mixture thereof.
- Silica in particular in the form of sand, is well known for FCC catalytic applications.
- Preferred amorphous-type catalysts comprise at least 60 % by weight, preferably at least 70 % by weight and even more preferably at least 80 % by weight of silica- equivalent of an oxidic compound based on silicon like silica (Si0 2 ), kaolin, etc.
- the catalyst additionally comprises a zeolite-type catalyst, this may be selected from crystalline microporous zeolites which are known to the person skilled in the art and which are commercially available. Preferred examples for zeolite-type catalysts are described in WO 2010/135273, the content of which is incorporated herein by reference.
- zeolite-type catalysts include but are not limited to ZSM-5, ZSM-11, ZSM-22, ZSM-23, ZSM-35, ZSM-48, ZSM-50, TS-1, TS-2, SSZ-46, MCM-22, MCM-49, FU-9, PSH-3, ITQ-1, EU-1, NU-10, silicalite-1, silicalite-2, boralite-C, boralite-D, BCA, and mixtures thereof.
- the catalyst can be fresh catalyst, equilibrated catalyst (such as spent catalyst), or a mixture thereof.
- the mixed waste plastic and the catalyst comprising the amorphous-type catalyst can be introduced within the reactor simultaneously or subsequently. Furthermore, the mixed waste plastic and the catalyst comprising the amorphous- type catalyst can be introduced within the reactor batchwise or continuously.
- the rotary kiln is a cylindrical vessel, inclined slightly to the horizontal, which is rotated slowly about its axis. The material to be processed is fed into the upper end of the cylinder. As the kiln rotates, material gradually moves down towards the lower end, and may undergo a certain amount of stirring and mixing.
- a fluid gas or liquid
- a circulating fluidized bed also called transport reactor
- the catalyst and the fluid flow co-currently at high speed.
- a cyclone system is used to separate the fluid, which can undergo downstream processing, from the solid, which is recirculated to the reactor.
- These reactors can be either upflow for risers, or downflow for downers.
- the whole process is conducted continuously.
- the reactor in presence of the catalyst, at least a portion of the mixed waste plastic is converted to liquid fuels.
- This conversion preferably takes place at an elevated temperature of for example above 350°C, preferably above 400°C, more preferably above 410°C.
- the conversion tales place at a temperature in the range of above 410°C to 500°C, more preferably in the range of from 420°C to 470°C, such as about 450°C.
- the temperature was increased to the reaction temperature at a heating rate of 10°C/min, and the collection of gases and nitrogen in the corresponding gas sampling bag was started.
- the circulation of the gaseous products was commuted to another pair of glass traps and corresponding gas sampling bag. This was considered as the zero reaction time.
- liquid and gaseous products were collected in a pair of glass traps and their associated gas sampling bag, respectively.
- the reactor was cooled to room temperature. During this cooling step, liquids and gases were also collected.
- reaction products were classified into 3 groups : i) gases, ii) liquid hydrocarbons and iii) residue (waxy compounds, ashes and coke accumulated on the catalyst). Quantification of the gases was done by gas chromatography (GC) using nitrogen as the internal standard, while quantification of liquids and residue was done by weight.
- GC gas chromatography
- the detailed hydrocarbon analysis (DHA) GC method allowed the determination of the PIONA (paraffins, iso-paraffins, olefins, naphthenes, aromatics) components in the gasoline fraction of the last withdrawn sample (C5-C11 : Boiling point ⁇ 216.1°C; what includes C5-C6 in the gas sample and C5-C11 in the liquid samples), and GCxGC allowed the determination of saturates (everything that is not aromatic), mono-, di- and tri-aromatics in the diesel fraction of the last withdrawn liquid samples (C12-C21; 216.1 ⁇ BP ⁇ 359°C).
- PIONA paraffins, iso-paraffins, olefins, naphthenes, aromatics
- the experiment was carried out following the general procedure described above.
- the raw material was pure HDPE (labelled 0 % PS).
- Reaction temperature was set at 450°C.
- 20 g of silica were used.
- Catalyst to plastic weight ratio was equal to 20/30.
- the raw material is a mixture containing 95 wt. % HDPE and 5 wt. % PS (labelled 5 % PS).
- Reaction temperature was set at 450°C.
- 20 g of silica have been used.
- Catalyst to plastic weight ratio was equal to 20/30.
- the raw material was a mixture containing 90 wt. % HDPE and 10 wt. % PS (labelled 10 % PS).
- Reaction temperature was set at 450°C.
- 20 g of silica were used.
- Catalyst to plastic weight ratio was equal to 20/30.
- the raw material was a mixture containing 80 wt. % HDPE and 20 wt. % PS (labelled 20 % PS).
- Reaction temperature was set at 450°C.
- 20 g of silica were used.
- Catalyst to plastic weight ratio was equal to 20/30.
- the raw material was a mixture containing 50 wt. % HDPE and 50 wt. % PS (labelled 50 % PS).
- Reaction temperature was set at 450°C.
- 20 g of silica were used.
- Catalyst to plastic weight ratio was equal to 20/30.
- Reaction temperature was set at 450°C.
- 20 g of silica were used.
- Catalyst to plastic weight ratio was equal to 20/30.
- Figure 5 shows the effect of the polystyrene loading on the quality of the gasoline fraction (P : paraffins, I : iso-paraffins, O : olefins, N : naphthenes, A : aromatics, U : unidentified).
- Figure 5 additionally shows the RON and MON of the gasoline fractions obtained with different polystyrene loadings. Surprisingly, both RON and MON increase if the amount of polystyrene in the mixed waste plastic is increased from 0 % to 20 %.
- Figure 6 shows the effect of the polystyrene loading on the quality of the diesel fraction (S : saturated, MA : monoaromatic, DA : diaromatic, TA :
- PA polyaromatic
Landscapes
- Chemical & Material Sciences (AREA)
- Engineering & Computer Science (AREA)
- Oil, Petroleum & Natural Gas (AREA)
- Life Sciences & Earth Sciences (AREA)
- Wood Science & Technology (AREA)
- Chemical Kinetics & Catalysis (AREA)
- General Chemical & Material Sciences (AREA)
- Organic Chemistry (AREA)
- Separation, Recovery Or Treatment Of Waste Materials Containing Plastics (AREA)
- Production Of Liquid Hydrocarbon Mixture For Refining Petroleum (AREA)
Abstract
Description
Claims
Applications Claiming Priority (2)
Application Number | Priority Date | Filing Date | Title |
---|---|---|---|
EP15201124 | 2015-12-18 | ||
PCT/EP2016/081304 WO2017103015A1 (en) | 2015-12-18 | 2016-12-15 | Process for converting mixed waste plastic into liquid fuels by catalytic cracking |
Publications (1)
Publication Number | Publication Date |
---|---|
EP3390574A1 true EP3390574A1 (en) | 2018-10-24 |
Family
ID=54936878
Family Applications (1)
Application Number | Title | Priority Date | Filing Date |
---|---|---|---|
EP16809849.9A Withdrawn EP3390574A1 (en) | 2015-12-18 | 2016-12-15 | Process for converting mixed waste plastic into liquid fuels by catalytic cracking |
Country Status (4)
Country | Link |
---|---|
US (1) | US20190002765A1 (en) |
EP (1) | EP3390574A1 (en) |
CN (1) | CN107922850A (en) |
WO (1) | WO2017103015A1 (en) |
Families Citing this family (1)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
CN114133951B (en) * | 2021-12-14 | 2023-04-18 | 青海天创新能源科技有限公司 | Method for preparing fuel oil by depolymerizing waste plastics by using catalyst |
Family Cites Families (5)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
CN1150968A (en) * | 1995-11-23 | 1997-06-04 | 杨亚力 | Method and equipment for treat waste plastic hydrocarbon |
CN102744101B (en) * | 2012-08-02 | 2014-07-09 | 新疆大学 | Catalyst used for preparing gasoline through splitting of waste plastic and preparation method and using method thereof |
WO2014040634A1 (en) * | 2012-09-14 | 2014-03-20 | Outotec Oyj | Method and apparatus for recycling plastic wastes |
WO2015128033A1 (en) * | 2014-02-25 | 2015-09-03 | Saudi Basic Industries Corporation | Process for converting mixed waste plastic (mwp) into valuable petrochemicals |
CN104479721B (en) * | 2014-12-29 | 2017-12-12 | 金妙英 | A kind of preparation technology that fuel oil is produced using waste plastic |
-
2016
- 2016-12-15 EP EP16809849.9A patent/EP3390574A1/en not_active Withdrawn
- 2016-12-15 WO PCT/EP2016/081304 patent/WO2017103015A1/en active Application Filing
- 2016-12-15 CN CN201680051675.6A patent/CN107922850A/en active Pending
- 2016-12-15 US US16/062,702 patent/US20190002765A1/en not_active Abandoned
Also Published As
Publication number | Publication date |
---|---|
WO2017103015A1 (en) | 2017-06-22 |
US20190002765A1 (en) | 2019-01-03 |
CN107922850A (en) | 2018-04-17 |
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