WO2016023776A1 - Procédé de production de gaz de craquage contenant de l'éthylène et tube de craquage à utiliser dans le procédé - Google Patents

Procédé de production de gaz de craquage contenant de l'éthylène et tube de craquage à utiliser dans le procédé Download PDF

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Publication number
WO2016023776A1
WO2016023776A1 PCT/EP2015/067772 EP2015067772W WO2016023776A1 WO 2016023776 A1 WO2016023776 A1 WO 2016023776A1 EP 2015067772 W EP2015067772 W EP 2015067772W WO 2016023776 A1 WO2016023776 A1 WO 2016023776A1
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WO
WIPO (PCT)
Prior art keywords
range
canned
tube
flowed
hydrocarbon
Prior art date
Application number
PCT/EP2015/067772
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German (de)
English (en)
Inventor
Maximilian Walter
Eric Jenne
Natalie GELDER
Original Assignee
Basf Se
Priority date (The priority date 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 date listed.)
Filing date
Publication date
Application filed by Basf Se filed Critical Basf Se
Publication of WO2016023776A1 publication Critical patent/WO2016023776A1/fr

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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
    • C10G9/00—Thermal non-catalytic cracking, in the absence of hydrogen, of hydrocarbon oils
    • C10G9/14—Thermal non-catalytic cracking, in the absence of hydrogen, of hydrocarbon oils in pipes or coils with or without auxiliary means, e.g. digesters, soaking drums, expansion means
    • C10G9/18—Apparatus
    • C10G9/20—Tube furnaces
    • C10G9/203—Tube furnaces chemical composition of the tubes
    • 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
    • C10G9/00—Thermal non-catalytic cracking, in the absence of hydrogen, of hydrocarbon oils
    • C10G9/34—Thermal non-catalytic cracking, in the absence of hydrogen, of hydrocarbon oils by direct contact with inert preheated fluids, e.g. with molten metals or salts
    • C10G9/36—Thermal non-catalytic cracking, in the absence of hydrogen, of hydrocarbon oils by direct contact with inert preheated fluids, e.g. with molten metals or salts with heated gases or vapours

Definitions

  • the invention relates to a process for the production of ethylene-containing cracked gas by thermal cracking of a hydrocarbon or hydrocarbon mixture in the presence of water vapor in a can at temperatures in the range of 600 to 1000 ° C and a Spaltgasaustrittstemperatur in the range of 750 to 1000 ° C.
  • the invention further relates to a can for use in a process for the production of ethylene-containing cracking gas by thermal cracking of a hydrocarbon or hydrocarbon mixture in the presence of water vapor.
  • the thermal cracking of hydrocarbons in the presence of water vapor in a canned oven finds widespread use in ethylene plants (steam crackers), in which in addition to the ethylene, other valuable unsaturated compounds such as propylene and butadiene and Pyrolysis gasoline with a high proportion of aromatic hydrocarbons such as benzene, toluene and xylene are won.
  • steam crackers in which in addition to the ethylene, other valuable unsaturated compounds such as propylene and butadiene and Pyrolysis gasoline with a high proportion of aromatic hydrocarbons such as benzene, toluene and xylene are won.
  • aromatic hydrocarbons such as benzene, toluene and xylene
  • residence times for the hydrocarbons in the cans of the can furnace of 0.1 to 0.6 seconds (s) and outlet temperatures of the cracked gases from the cans of more than 750 ° C., generally between 800 and 1000 ° C., are preferred , complied. See, e.g. D. Glietenberg et al., Ullmanns Encyklopadie der ischen Chemie, 4th ed., Volume 8,
  • the canned oven must be turned off and the crevices of the deposits, esp. The coke, freed.
  • the split tubes and associated moldings are usually freed of the deposits with a water vapor / air mixture or even only with air at temperatures of 700 to 1000 ° C, as for example. in EP 36151 A1 (BASF AG).
  • Catalytically active coatings on the inner surface of cans or canned systems which can significantly reduce carbonaceous deposits, especially coke deposits, and convert these deposits, especially coke, into CO and CO2, such as, for example, coke.
  • Camol TM Catalytically active coatings on the inner surface of cans or canned systems which can significantly reduce carbonaceous deposits, especially coke deposits, and convert these deposits, especially coke, into CO and CO2, such as, for example, coke.
  • Highly alloyed surface alumina-forming Cr, Ni and Al-containing steels i.e., Cr-Ni-Al-Fe alloys
  • castings made therefrom by centrifugal casting and molded articles preferably made by molding using the same alloys.
  • Catalytically active coatings e.g. CAMOL TM have the disadvantage of all catalytic processes of being contaminated during operation with impurities, e.g. Sulfur compounds, and indefinite operating conditions in the canned oven lose activity.
  • US 6,488,839 B1 (Inst. Francais du Petrole) relates to the thermal decomposition of hydrocarbons in the presence of steam in pipes under certain boundary conditions such as residence time t, furnace outlet temperature COT, hydraulic diameter DH and pipe length L, with 150 ms ⁇ t ⁇ 2800 ms, 858 ° C ⁇ COT ⁇ 1025 ° C, D H > 34 mm and L> 16 m.
  • the end portion of the tube may also have anti-coking coating and / or internal ribs.
  • US 2003/188850 A1 Honeywell Internat.
  • Inc. teaches a tube assembly for cooling and removing contaminants from an incoming fluid stream, wherein the tube a turbulator having elongated strips and a catalytic coating adhered to at least the strip or the inner surfaces, wherein the catalytic coating is in contact with the fluid flow flowing through the tubes.
  • the object of the present invention while overcoming disadvantages of the prior art, is to provide an improved economical process for the production of ethylene-containing cracked gas.
  • the process should make it possible, by increasing the service life of crevices, to increase the production times for fission gas, e.g. between two decoking phases, to extend.
  • the process should also be particularly advantageous if, in the inlet region of catalytic canned systems, there is a temperature range at which the catalytic coating is not or only insufficiently restored after decoking, i. not or only insufficiently regenerated, can be.
  • the inner surface of the split tube is geometrically modified in the region through which it flows first, whereby carbonaceous deposits in the tube are reduced,
  • a canned tube for use in a process for producing ethylene-containing cracking gas by thermal cracking of a hydrocarbon or hydrocarbon mixture in the presence of water vapor esp.
  • the inner surface of the split tube is geometrically modified in the first area to be flowed, whereby carbonaceous deposits are reduced in the pipe in the production process for fission gas, and the can in the thereafter to be flowed through area on the inner surface of a catalytically active coating has, which reduces carbonaceous deposits in the pipe in the production process for fission gas.
  • the canned tube according to the invention and the crevice tube used in the method according to the invention therefore does not have the catalytically active coating on the inner surface in the region to be flowed through initially, but only in the region to be flowed thereafter.
  • the inner surface of the can is geometrically not modified in the area to be flowed thereafter (in contrast to the inner surface of the can in the area to be flowed through first).
  • Suitable starting hydrocarbons for the thermal cracking are ethane, propane, butane, liquefied petroleum gas (LPG), gasoline fractions such as mineral spirits, e.g. Light gasoline having the boiling range of about 30 to 150 ° C, gasoline (full-range naphtha), e.g. Gasoline with the boiling range of about 30 to 180 ° C, heavy gasoline, e.g. Heavy gasoline with the boiling range of about 150 to 220 ° C, kerosene, e.g. Kerosene with the boiling range of about 200 to 260 ° C, gas oils such as light gas oil, e.g. light gas oil having the boiling range of about 200 to 360 ° C, heavy gas oil, e.g. heavy gas oil with the boiling range of approx. 310 to 430 ° C, and vacuum distillates. Furthermore, mixtures or combinations of the suitable starting hydrocarbons can be used for the thermal cracking.
  • LPG liquefied petroleum gas
  • gasoline fractions such as mineral spirits
  • Preferred hydrocarbons for the production of ethylene-containing cracked gases are gases such as ethane, propane and mixtures containing ethane and propane, LPG, gasoline fractions, kerosene, bionaphtha, condensates, which are e.g. are obtained from gas fields, and / or gas oils and mixtures thereof.
  • the split tubes to be modified partly geometrically and partly to be provided internally with a catalytically active coating may be straight tubes or curved tubes, such as tube coils.
  • the term 'split tube' in particular also includes molded parts connected to the split tube, such as Y-pieces, collectors, reversal bends, reducers.
  • Canned pipe plus connected moldings are also called canned system.
  • Canned systems can be provided e.g. 1 to 20 reversal bends (or even more), especially e.g. 1 to 1 1 reverse bends, and corresponding to 2 to 21 (or correspondingly more), especially 2 to 12, passports.
  • Passes in an initially traversed area can also be divided into several, e.g. 2 to 25, parallel tubes and possibly reversal bends be divided.
  • the Linde PYROCRACK® 4-2 Canned Pipe System (Fig. 2) consists of 6 passports and 5 reversing bends, with 4 passages divided into 2 parallel pipes in an initially flown-through area.
  • crevices and canned systems described herein in the previous three paragraphs are conventional, non-geometrically modified crevices and canned systems.
  • the total length of the canned pipe is measured from the crevice pipe entrance to the crevasse pipe outlet, thus also over the total length of a canned pipe system.
  • When sizing the length only one pipe counts in parallel pipes connecting later in the run (e.g., via Y-pieces or collectors).
  • the decisive factor is the shortest possible path length via the split-tube system.
  • the can is preferably heated indirectly in the canned oven, ie. the split tube is not heated directly by a flame, but indirectly via the heat radiation of a flame.
  • the thermal cleavage of the hydrocarbon or hydrocarbon mixture is preferably carried out at temperatures in the range of 600 to 1000 ° C, especially 700 to 1000 ° C.
  • the thermal cleavage of the hydrocarbon or hydrocarbon mixture is preferably carried out in the first flow-through range at temperatures in the range of 600 to 800 ° C and in the thereafter flowed through at temperatures in the range of 700 to 1000 ° C.
  • the outlet temperatures of the cracked gas from the split tube are 750 to 1000 ° C, preferably 780 to 950 ° C, in particular 800 to 900 ° C.
  • the residence times in the can are particularly 0.05 to 1 second (s), preferably 0.08 to 0.6 s, in particular 0.1 to 0.3 s.
  • the heat loads of the cans in the canned oven are preferably 64 kW / m 2 h to 128 kW / m 2 h (40,000 to 80,000 kcal / m 2 h), preferably 58 kW / m 2 h to 81 kW / m 2 h (50,000 to 70,000 kcal / m 2 h).
  • the weight ratio of water vapor to the hydrocarbon used or to the hydrocarbon mixture used is in the thermal cracking particularly in the range of 0.1 to 1, preferably in the range of 0.2 to 0.8, and more particularly in the range of 0.3 to 0th , 7th
  • the pressure in the can is in the thermal cleavage especially 1, 5 to 5 bar, especially 1, 6 to 2.5 bar.
  • the inner surface of the split tube is geometrically modified in the first area through which it flows.
  • the geometric modification causes changed flow conditions, e.g. increased turbulent flow of the gas to be split in the pipe, whereby carbonaceous deposits are reduced in the pipe.
  • This can e.g. by internals, such as baffles, spirals (e.g., uninterrupted spirals or spirals with successive breaks), ribs, coils, can be achieved in the can.
  • the geometric modification may also include additional bends, possibly in combination with internals, of the can (as compared to a conventional can). Examples of such bends are helically shaped tubes, helical shaped tubes, and wavy shaped tubes.
  • the area through which flow passes first preferably has a length in the range of 15 to 60%, in particular 20 to 55%, very particularly 25 to 50%, in each case based on the total length of the can.
  • the area through which flows thereafter directly adjoins the region through which flow has taken place.
  • This results in the preferred length of the area flowed through thereafter from the above-mentioned lengths for the area through which the first flow passes (total length 100%).
  • between the two areas is a conventional range, for example over a length of> 0 to 20% (based on the total length of the can), without geometric modification and without catalytically active coating.
  • the length of the first area flowed through increases with the residence time of the cracked gas in the can.
  • the area through which flow first flows preferably has a length in the range from 15 to 40%, in particular from 20 to 40%, very particularly from 25 to 40%, based in each case on Total length of the can, on and has at residence times in the range of> 0.60 s (eg to 1 s) of the first flow-through range preferably has a length in the range of> 40 to 60%, especially> 40 to 55%, especially> 40 up to 50%, in each case based on the total length of the can.
  • the concentration of hydrogen in the can in the location or in the region between the geometrically modified part and the catalytically active coated part is preferably in the range of 2 to 5% by volume, especially 3 to 4% by volume.
  • the inner surface of the split tube is geometrically modified in the region through which it flows first, and in the region through which it flows, it has a catalytically active coating on the inner surface.
  • the catalytically active coating which is applied in particular after the production of the can and before its use for thermal hydrocarbon cleavage on its inner surface, compared to a conventional can, a reduction of carbonaceous deposits in the pipe.
  • Such catalytic cracking tubes and canned systems also called “steam cracker furnace tubes with catalytic surface coatings" are also available on the market, see, for example, the above-mentioned Catalyzed-Assisted Manufacture of Olefin (CAMOL) systems also referred to as a "catalytic coating", “catalyst layer” or as a “catalyst”; the catalyst is present as a layer on the inner surface of the can.
  • the layer preferably has a thickness in the range of 0.05 to 5 mm, more preferably in the range from 0.1 to 3 mm, especially in the range of 0.2 to 2 mm.
  • the catalytically active coating of the can contains as active component one or more metals of subgroups VIB, VI IB, VIII of the Periodic Table (Chemical Abstracts Service group notation), e.g. Cr, Mo, W, Mn, Re, Co, Ni.
  • these metals are present in the coating in oxidized form (oxidation number is> 0, especially in the range of 1 to 8, e.g., 2 to 7).
  • Mn manganese
  • CAMOL TM coatings as e.g. in the BASF publication "CAMOL TM Catalytic Coatings for Steam cracker furnace tubes", BF-9657 3/12. These are the so-called “Low-Catalytic Gasification (LCG) Coating” and the so-called “High-Catalytic Gasification (HCG) Coating”.
  • LCG Low-Catalytic Gasification
  • HCG High-Catalytic Gasification
  • Examples Figure 1 shows schematically a canned oven including an inventive canned system with convection zone and radiation zone and quench cooler for the cracked gas.
  • the canned system is located in the radiation zone.
  • a mixture of up to 2.2 t / h of a gasoline fraction (naphtha) having a boiling range of 40 to 180 ° C and 1, 0 t / h steam were passed per canned system and at a crevice tube outlet temperature thermally split up to 840 ° C.
  • a canned system consists of 18 parallel, vertical inlet tubes, which are flowed through from top to bottom and merged into a manifold. From there, the fission gas is led out of the furnace in 2 parallel, vertical outlet pipes, which are flowed through from bottom to top.
  • the canned system is constructed analogously to a selective 2-pass canned system with the designation SRT®-V from CB & I (Lummus); see. Fig. 3.
  • SRT®-V from CB & I (Lummus); see. Fig. 3.
  • the cracked gas from each of two split-tube systems is cooled in a downstream split-gas cooler.
  • the split tubes were provided with a geometrical modification applied internally to the surface, namely an uninterrupted inner spiral in the straight tube sections, namely MERT (not a MERT), both in the front region of the can system, which was flowed through first, and in the subsequently flowed through section of the can system.
  • Modification such as sMERT, xMERT), as described in the publication M. Györffy et al., MERT Performance and technology update, 2009 AIChE Spring National Meeting (April 26-30, 2009).
  • the manually measured pipe wall temperature at the outlet of the canned system could be 930 to 960 ° C.
  • the tube wall temperature at the measured point in the last flowed through region of the crevice tube system could finally rise to up to 1100 ° C. after several months of running time, the highest tube wall temperature used for the material at this point of the canned tube system.
  • the differential pressure of the flow nozzles in the inlet of the can system could be reduced to the minimum applied differential pressure limit of 0.3 bar.
  • the hydrocarbon stream was interrupted by the canned oven and the canned systems separated from the rest of the process and freed from the coke by means of oxygen.
  • a temperature in the range of 760 to 825 ° C and a pressure of 1, 05 to 3 bar over a total period of 60 hours at the beginning of a steam / air mixture passed into the gap tubes, which in the further course by reducing the amount of steam was changed so that the amount of air in the mixture of initially 10 wt .-% increased to 70 wt .-%.
  • a canned system consists of 18 parallel, vertical inlet tubes, which are flowed through from top to bottom and merged into a manifold. From there, the fission gas is led out of the furnace in 2 parallel, vertical outlet pipes, which are flowed through from bottom to top.
  • the canned system is constructed analogously to a selective 2-pass canned system with the designation SRT®-V from CB & I (Lummus); see. Fig. 3.
  • SRT®-V from CB & I (Lummus); see. Fig. 3.
  • the cracked gas from each of two split-tube systems is cooled in a downstream split-gas cooler.
  • the split tubes were internally provided with a catalytically active coating containing manganese as described in the BASF publication "CAMOL TM catalytic coatings for steam cracker furnace tubes", BF-9657 3/12.
  • a combination of Low-Catalytic Gasification (LCG) Coating in the front, first-flow area and High-Catalytic Gasification (HCG) Coating in the rear, last-flowed area of the can system were used.
  • the manually measured pipe wall temperature at the outlet of the canned system was 940 to 980 ° C.
  • the tube wall temperature at the measured location in the canned system eventually increased to 1 100 ° C after several months running time, the highest tube wall temperature used for the material and coating of this canned system.
  • the differential pressure of the flow nozzles in the inlet of the can system could be reduced to the minimum applied differential pressure limit of 0.3 bar.
  • one of the criteria 'wall temperature' or 'differential pressure' could be decisive for the interruption of the production operation and the initiation of the decoking procedure.
  • the hydrocarbon stream was interrupted by the canned oven and the canned systems separated from the process and freed from coke by oxygen.
  • a mixture of up to 2.2 t / h of a gasoline fraction (naphtha) with a boiling range of 40 to 180 ° C and 1, 0 t / h steam are passed per canned system and at a split tube outlet temperature of up to 840 ° C thermally split.
  • a canned system consists of 18 parallel, vertical inlet tubes, which are flowed through from top to bottom and merged into a manifold. From there, the fission gas is led out of the furnace in 2 parallel, vertical outlet pipes, which are flowed through from bottom to top.
  • the canned system is constructed analogously to a selective 2-pass canned system with the designation SRT®-V from CB & I (Lummus); see. Fig. 3.
  • SRT®-V from CB & I (Lummus); see. Fig. 3.
  • the cracked gas from each of two split-tube systems is cooled in a downstream split-gas cooler.
  • the split tubes are geometrically modified in the front, first through-flow region of the can system as described above in Comparative Example 1.
  • the geometric modification of the gap tubes in the inlet area comprises a length of 30% of the total length of the can system.
  • the canned system is inside with a catalytically active coating containing manganese and tungsten, namely 'High Catalytic Gasification (HCG) Coating', as described in the BASF publication "CAMOL TM catalytic coatings for steam cracker furnace tubes", BF-9657 3/12.
  • HCG High Catalytic Gasification
  • the tube wall temperature at the measured point in the last flowed through area of the canned system can finally increase after several months running time up to 1 100 ° C, the highest applied to the material and the coating at this point of the canned pipe wall temperature.
  • the differential pressure of the flow nozzles in the inlet of the can system can be reduced to the minimum applied differential pressure limit of 0.3 bar.
  • the hydrocarbon stream is interrupted by the canned oven and the canned systems separated from the rest of the process and freed from the coke by means of oxygen.
  • the hydrocarbon stream is interrupted by the canned oven and the canned systems separated from the rest of the process and freed from the coke by means of oxygen.
  • a temperature in the range of 760 to 825 ° C and a pressure of 1, 05 to 3 bar over a total period of 60 hours at the beginning of a water vapor / air mixture passed into the gap tubes, which in the further course by reducing the amount of steam is changed so that the amount of air in the mixture of initially 10 wt .-% to 70 wt .-% increases.

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  • Chemical & Material Sciences (AREA)
  • Oil, Petroleum & Natural Gas (AREA)
  • Physics & Mathematics (AREA)
  • Thermal Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • General Chemical & Material Sciences (AREA)
  • Organic Chemistry (AREA)
  • Production Of Liquid Hydrocarbon Mixture For Refining Petroleum (AREA)

Abstract

L'invention concerne un procédé de production de gaz de craquage contenant de l'éthylène par craquage thermique d'un hydrocarbure ou d'un mélange d'hydrocarbures en présence de vapeur d'eau dans un tube de craquage à des températures dans la plage de 600 à 1000 °C et une température de sortie du gaz de craquage dans la plage de 750 à 1000 °. La surface intérieure du tube de craquage est modifiée géométriquement dans la zone traversée en premier par le courant, les dépôts contenant du carbone dans le tube étant ainsi réduits, et le tube de craquage possède, sur la surface intérieure dans la zone qui est ensuite traversée par le courant, un revêtement à activité catalytique qui réduit les dépôts contenant du carbone dans le tube. L'invention concerne également un tube de craquage destiné à utiliser dans le procédé.
PCT/EP2015/067772 2014-08-13 2015-08-03 Procédé de production de gaz de craquage contenant de l'éthylène et tube de craquage à utiliser dans le procédé WO2016023776A1 (fr)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
EP14180863 2014-08-13
EP14180863.4 2014-08-13

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WO2016023776A1 true WO2016023776A1 (fr) 2016-02-18

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Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
EP3490704A4 (fr) * 2016-07-29 2020-03-25 BASF Qtech Inc. Revêtements catalytiques, leurs procédés de fabrication et d'utilisation

Citations (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US6488839B1 (en) * 1999-05-11 2002-12-03 Institut Francais Du Petrole Process and furnace for steam-cracking a feedstock that contains ethane and/or propane
US20030188850A1 (en) * 2002-04-09 2003-10-09 Honeywell International Inc., Tubular catalytic aircraft precooler
US20060102327A1 (en) * 2002-11-15 2006-05-18 Masahiro Inui Cracking tube having helical fins
US20130337999A1 (en) * 2012-06-01 2013-12-19 Basf Corporation Catalytic surfaces and coatings for the manufacture of petrochemicals

Patent Citations (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US6488839B1 (en) * 1999-05-11 2002-12-03 Institut Francais Du Petrole Process and furnace for steam-cracking a feedstock that contains ethane and/or propane
US20030188850A1 (en) * 2002-04-09 2003-10-09 Honeywell International Inc., Tubular catalytic aircraft precooler
US20060102327A1 (en) * 2002-11-15 2006-05-18 Masahiro Inui Cracking tube having helical fins
US20130337999A1 (en) * 2012-06-01 2013-12-19 Basf Corporation Catalytic surfaces and coatings for the manufacture of petrochemicals

Cited By (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
EP3490704A4 (fr) * 2016-07-29 2020-03-25 BASF Qtech Inc. Revêtements catalytiques, leurs procédés de fabrication et d'utilisation
US10894251B2 (en) 2016-07-29 2021-01-19 Basf Qtech Inc. Catalytic coatings, methods of making and use thereof

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