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WO2008073017A1 - Additif pour mazout ou pétrole brut et composition de mazout ou de pétrole brut contenant cet additif - Google Patents

Additif pour mazout ou pétrole brut et composition de mazout ou de pétrole brut contenant cet additif Download PDF

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Publication number
WO2008073017A1
WO2008073017A1 PCT/SE2007/001072 SE2007001072W WO2008073017A1 WO 2008073017 A1 WO2008073017 A1 WO 2008073017A1 SE 2007001072 W SE2007001072 W SE 2007001072W WO 2008073017 A1 WO2008073017 A1 WO 2008073017A1
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WIPO (PCT)
Prior art keywords
fuel
crude oil
additive
additive according
oil additive
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PCT/SE2007/001072
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English (en)
Inventor
Geoffrey Alan Richards
Original Assignee
Geomar Ab
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Application filed by Geomar Ab filed Critical Geomar Ab
Publication of WO2008073017A1 publication Critical patent/WO2008073017A1/fr

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    • C10L9/00—Treating solid fuels to improve their combustion
    • C10L9/10—Treating solid fuels to improve their combustion by using additives
    • C10L9/12—Oxidation means, e.g. oxygen-generating compounds
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    • C10L1/00—Liquid carbonaceous fuels
    • C10L1/10—Liquid carbonaceous fuels containing additives
    • C10L1/14—Organic compounds
    • C10L1/18—Organic compounds containing oxygen
    • C10L1/182—Organic compounds containing oxygen containing hydroxy groups; Salts thereof
    • C10L1/1822—Organic compounds containing oxygen containing hydroxy groups; Salts thereof hydroxy group directly attached to (cyclo)aliphatic carbon atoms
    • C10L1/1824—Organic compounds containing oxygen containing hydroxy groups; Salts thereof hydroxy group directly attached to (cyclo)aliphatic carbon atoms mono-hydroxy
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    • C10L1/00—Liquid carbonaceous fuels
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    • C10L1/14—Organic compounds
    • C10L1/18—Organic compounds containing oxygen
    • C10L1/182—Organic compounds containing oxygen containing hydroxy groups; Salts thereof
    • C10L1/1822—Organic compounds containing oxygen containing hydroxy groups; Salts thereof hydroxy group directly attached to (cyclo)aliphatic carbon atoms
    • C10L1/1826—Organic compounds containing oxygen containing hydroxy groups; Salts thereof hydroxy group directly attached to (cyclo)aliphatic carbon atoms poly-hydroxy
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    • C10L1/00—Liquid carbonaceous fuels
    • C10L1/10—Liquid carbonaceous fuels containing additives
    • C10L1/14—Organic compounds
    • C10L1/18—Organic compounds containing oxygen
    • C10L1/188—Carboxylic acids; metal salts thereof
    • C10L1/1881—Carboxylic acids; metal salts thereof carboxylic group attached to an aliphatic carbon atom
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    • C10L1/00—Liquid carbonaceous fuels
    • C10L1/10—Liquid carbonaceous fuels containing additives
    • C10L1/14—Organic compounds
    • C10L1/18—Organic compounds containing oxygen
    • C10L1/188—Carboxylic acids; metal salts thereof
    • C10L1/1888—Carboxylic acids; metal salts thereof tall oil
    • C—CHEMISTRY; METALLURGY
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    • C10L1/00—Liquid carbonaceous fuels
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    • C10L1/14—Organic compounds
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    • C10L1/19—Esters ester radical containing compounds; ester ethers; carbonic acid esters
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    • C10L1/00—Liquid carbonaceous fuels
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    • C10L1/18—Organic compounds containing oxygen
    • C10L1/192—Macromolecular compounds
    • C10L1/198—Macromolecular compounds obtained otherwise than by reactions involving only carbon-to-carbon unsaturated bonds homo- or copolymers of compounds having one or more unsaturated aliphatic radicals, each having only one carbon to carbon double bond, and at least one being terminated by an acyloxy radical of a saturated carboxylic acid, of carbonic acid
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    • C10L1/18—Organic compounds containing oxygen
    • C10L1/192—Macromolecular compounds
    • C10L1/198—Macromolecular compounds obtained otherwise than by reactions involving only carbon-to-carbon unsaturated bonds homo- or copolymers of compounds having one or more unsaturated aliphatic radicals, each having only one carbon to carbon double bond, and at least one being terminated by an acyloxy radical of a saturated carboxylic acid, of carbonic acid
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    • C10L1/2431—Organic compounds containing sulfur, selenium and/or tellurium sulfur bond to oxygen, e.g. sulfones, sulfoxides
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Definitions

  • the present invention refers to a novel additive for improving the properties of fuel and/or crude oil compositions, said additive composition comprises at least one ferric or ferrous formate.
  • the present invention refers to a fuel and/or crude oil composition comprising an active amount of said additive or an active amount of said ferric or ferrous formate and to the use of said additive or said ferric or ferrous formate in fuel and/or crude oil compositions, such as furnace or marine fuel oil compositions.
  • Heavy oils such as heavy fuel oils (marine fuel oils) and mixtures of heavy fuel oils and heavy distillates (inter fuel oils) are used globally in large quantities, primarily as furnace fuels in industrial plants, power stations, gas turbines and also for internal combustion engines, such as marine engines and land based diesel units.
  • Fuel oils are obtained in the refining of petroleum (crude oils), which essentially comprise of paraffinic, naphthenic and aromatic hydrocarbons some of which have high molecular weight, but also includes residual components from various distillation and thermal cracking processes.
  • the high molecular weight components are typically termed asphaltenes often existing as insoluble aggregated particles randomly dispersed or in the process of sedimenting or flocculating, likewise other compounds having poor or insoluble characteristics (for example oxygen, nitrogen and sulphur compounds), likewise products resulting from aging (sludge), and likewise metallic porfyrins containing vanadium or nickel etc., all of which adversely affect the oil combustion process through intensified soot formation, deposits on metal surfaces of combustion units and plants, corrosion of metal components in combustion units and plants and also undesirable flue gas and stack emissions causing plume, acid rain and thus a negative impact on the environment.
  • asphaltenes often existing as insoluble aggregated particles randomly dispersed or in the process of sedimenting or flocculating
  • other compounds having poor or insoluble characteristics for example oxygen, nitrogen and sulphur compounds
  • sludge products resulting from aging
  • metallic porfyrins containing vanadium or nickel etc. all of which adversely affect the oil combustion process through intensified so
  • metal additives such as metal carboxylates, oxides and hydroxides to improve combustion in boilers, combustion engines and combustion turbines are known and/or have been suggested.
  • These metal additives include species of iron, manganese, copper, alkaline earth metals, such as calcium and barium; cerium, platinum and palladium.
  • additives Besides having a desired effect on the combustion, additives often have undesirable attributes, being themselves sources for atmospheric pollution, being corrosive or having deleterious effects upon the performance of the combustor itself.
  • Manganese generally considered as an effective combustion additive and widely used as a combustion catalyst in boilers with residual oil comprising fuel contaminants, such as vanadium, forms low melting deposits and negates effects of magnesium on control of vanadium, sodium, calcium and potassium deposits.
  • Iron is also regarded as an effective combustion additive while copper is regarded as less effective than either iron or manganese.
  • Calcium forms tenacious deposits with contaminant metals.
  • Barium a known smoke suppressant, forms toxic salts. Cerium is less effective because of its higher elemental weight.
  • Ferrocene Fe(CsHs ⁇ , is probably the best known and most investigated organometallic additive. It is known to be a soot precursor in combustion and have been used for several years. A problem often encountered with Ferrocene is that it tends to leave an oxide deposit on the walls of the combustion chamber that can have severe degrading effects on its long-term performance.
  • FR 2 172 797 describes basic iron salts of organic acids
  • FR 2 632 966 describes a mixture of iron hydroxide and a basic calcium soap as auxiliaries to enhance the combustion of heavy fuel oils.
  • US 4,129,589 recommends highly basic and oil-soluble magnesium salts of sulphonic acids as oil additives.
  • EP 476 196 describes as oil additive, a mixture essentially comprising at least one oil-soluble carbonyl manganese compound and at least one oil-soluble neutral or basic alkali metal or alkaline earth metal salt of an organic acid component.
  • GB 2 091 291 teaches diesel additives comprising calcium sulphonate, naphthenate, carbonate and/or oxide in combination with iron naphthenate, Ferrocene and/or iron oxide.
  • SE 451 197 disclose the use of iron and/or manganese salts of aliphatic carboxylic acids having 3-10 carbon atoms as fuel additives. None of these disclosures teach, disclose or otherwise contemplate the use of iron formates as possible additive in fuel or crude oils and the fact that some disclosures are limited to metal salts of mineral and/or carboxylic acids having three or more carbon atoms negates and teaches away from the use of formates as effective additives in fuel and/or crude oils.
  • the present invention accordingly refers to a fuel or crude oil additive composition
  • a fuel or crude oil additive composition comprising at least one ferric and/or ferrous formate as sole organometallic component or in combination with for instance a calcium carboxylate.
  • Said ferric and/or ferrous formate is suitably present in an amount of for instance between 0.5 and 99.5% by weight of said oil additive and in addition thereto at least one solvent, dispersant, stabiliser, anti-caking agent and/or other auxiliary agent per se known in the art.
  • Embodiments of said fuel or crude oil additive may additionally comprise at least one carboxylate, mineral salt, oxide or hydroxide of calcium, such as calcium formate and/or calcium sulphonate in a weight ratio Fe to Ca of for instance between 0.5 to 99.5 and 99.5 to 0.5% by weight calculated as metal, and/or at least one organic or inorganic metal compound, carboxylate, mineral salt, oxide and/or hydroxide, other than said ferric and/or ferrous formate and other than said calcium carboxylate or mineral salt, such as ferrous fumarate.
  • carboxylate, mineral salt, oxide or hydroxide of calcium such as calcium formate and/or calcium sulphonate in a weight ratio Fe to Ca of for instance between 0.5 to 99.5 and 99.5 to 0.5% by weight calculated as metal
  • organic or inorganic metal compound, carboxylate, mineral salt, oxide and/or hydroxide, other than said ferric and/or ferrous formate and other than said calcium carboxylate or mineral salt, such as ferrous fumarate such as ferrous
  • These preferred additional organic or inorganic compounds include species comprising iron, cerium, barium, beryllium, calcium, magnesium, copper, silver, zinc, cadmium, titanium, zirconium, molybdenum, chromium, tungsten, cobalt, nickel, lanthanum and/or ytterbium as active metal.
  • species comprising iron, cerium, barium, beryllium, calcium, magnesium, copper, silver, zinc, cadmium, titanium, zirconium, molybdenum, chromium, tungsten, cobalt, nickel, lanthanum and/or ytterbium as active metal.
  • Particularly preferred are carboxylates, mineral salts, oxides and hydroxides of barium, beryllium, calcium, magnesium, copper, zinc, zirconium, molybdenum, iron, nickel, cerium and ytterbium.
  • Further embodiments of said fuel or crude oil additive include fluid components comprising an active amount of at least one asphaltene dispersant and/or stabiliser in an amount of for instance between 0.1 and 50% by weight based on said metal compounds and/or fluid components comprising an active amount of at least one anionic, cationic and/or nonionic surfactant in an amount of 1-10%, such as 2-5%, by weight of said additive.
  • Asphaltenes are colloidal dispersed components present in for instance crude oil and may precipitate due to changes in temperature, pressure, oil composition and/or when coming onto contact with other fluids and gases, sediment and sludge are formed in oil tanks and fuel lines.
  • asphaltenes do not combust completely under normal conditions, resulting in loss of potential combustible energy and increase in unburned hydrocarbons in the fly ash.
  • a typical and well known in the art solution to above problems is the use of an asphaltene inhibitor or more commonly an asphaltene dispersant/stabiliser.
  • Suitable asphaltene dispersants/stabilisers can be exemplified by the Protea ® RF-series supplied by System Separation, Sweden.
  • a fluid additive including water based additives comprising one or more anionic, cationic and/or nonionic surfactants, according to the present invention is suitably prepared by mixing together the individual components according to specific requirements with or without the use of a solvent or dispersing medium, such as a hydrocarbon process solvent or oil and/or a glycol.
  • a solvent or dispersing medium such as a hydrocarbon process solvent or oil and/or a glycol.
  • Suitable solvents include rape seed methyl ester and other biodegradable solvents and suitable dispersants include tall oil fatty acid adducts.
  • Preparation of said additive is suitably carried out at atmospheric pressure and at a temperature of for instance 15-100°C, such as 20-70°C.
  • Yet further embodiments of the fuel and/or crude oil additive of the present invention include dry powders or granules additionally comprising an active amount of at least one anti-caking agent, such as a magnesium and/or calcium salt of an oxidised microwax, a phenolic resin, a fatty acid derivative, an amide and/or an amide wax.
  • at least one anti-caking agent such as a magnesium and/or calcium salt of an oxidised microwax, a phenolic resin, a fatty acid derivative, an amide and/or an amide wax.
  • a powder form fuel and/or crude oil additive according to the present invention is preferably prepared by first milling included metal compound(s) to a particle size of preferably less than for instance 100 microns, using any suitable milling equipment.
  • metal compound(s) and processing aid(s) such as an anti-caking agent selected from the group consisting of for instance a magnesium and/or calcium salt of an oxidised microwax, a phenolic resin, a fatty acid derivative, an amide and/or an amide wax, to a desired composition, it is preferable to mill the components individually prior to blending.
  • Suitable embodiments of the additive of the present invention include for instance formulations having: i) Fe(E) and/or Fe( ⁇ T)formate as only active metal compound, ii) Fe(II) and/or Fe(IE)formate and Ca-carboxylate or mineral salt, such as Ca-formate or Ca-sulphonate, as active metal compounds in a weight ratio calculated as metals of between 0.5% to 99.5% and 99.5% to 0.5%, such as Fe 30% and Ca 70% or Fe 70% and Ca 30% by weight, iii) Fe( ⁇ ) and/or Fe(III)formate and Mg-carboxylate, mineral salt, oxide or preferably hydroxide as active metal compounds in a weight ratio calculated as metals of between 0.5% to 99.5% and 99.5% to 0.5%, such as Fe 5% and Mg 95% for boiler applications and Fe 50% and Mg 50% for marine and land based diesel application with a preferred dosage of 1 part by weight of the additive to 3000 parts by weight of a fuel and/or crude oil, preferably
  • a preferred dosage of the additives according to the present invention is suitably found between 0.5 and 5000 ppm, such as 40-60, 0.5-500, 50-200, 2-2000 or 100-1000 ppm, based on the fuel and/or crude oil.
  • formulations are based on the actual active metal combinations.
  • the solids content of liquid combinations can only be limited by the dispersant system adopted and the practical viscosity enabling a dosage pump to operate efficiently.
  • Formulations having a low active metal content are often more applicable to marine and land based diesel engines where dosage requirements take into consideration the type of dosage pump and effective dosage range and also the importance of the additive distribution in the fuel.
  • the present invention does not prevent addition of further metal compounds as mentioned previously and/or whole or partial replacement of carboxylates mentioned with other metallic salts whether over-based or not.
  • the present invention refers to a fuel or crude oil composition
  • a fuel or crude oil composition comprising a fuel and/or crude oil and at least one additive as disclosed above in an amount of for instance between 0.5 and 5000 ppm, such as 40-60, 0.5-500, 50-200, 2-2000 or 100-1000 ppm.
  • Said fuel and/or crude oil composition is in especially preferred embodiments a furnace or marine fuel oil composition.
  • the present invention refers the use of a fuel or crude oil additive as disclosed above and to the use of a ferric or ferrous formate in particular in furnace and marine fuel oil compositions for obtaining for instance improved combustion properties, such as reduced smoke and/or particulate emission and/or reduced soot formation, in fuel or crude oil compositions.
  • the additive according to the present invention and fuel or crude oil compositions comprising said additive have particularly desired characteristics and even synergistic effects of particular component combinations, such as ferric and/or ferrous formate combined with a calcium compound as disclosed above and ferric and/or ferrous formate combined with a cerium and magnesium compound as disclosed above.
  • ferric or ferrous formate in accordance with the present invention yields, moreover, a highly effective combustion enhancer, ensuring for instance complete combustion of fuels and simultaneous decrease in soot formation, hi addition substantial environmental benefits are achieved with reduced flue gas particle emissions and it is, furthermore, possible to obtain biodegradable additives.
  • Additives additionally comprising for example cerium and or magnesium can reduce combustion unit deposits and corrosion.
  • the present invention vary from combinations known in the of metal compounds as combustion additives/combustion improvers in that overbased metal salts are not used, although combinations comprising overbased metal salts may be permitted. Instead so called all organic metal salts and combinations of all organic metal salts together with inorganic metal salts are used. Enhancement of the combustion additive/combustion improver for liquid products can be achieved by the use of said solvents, dispersants and/or stabilisers providing a more complete combustion and heavy fuel oil stability.
  • Example are fuel oil compositions comprising an additive composition according to the present invention thermogravimetrically and calorimetrically analyses and compared with an oil composition without additive composition and oil compositions comprising ferrous fumarate and Ferrocene, resp., as combustion additive composition. The results are given in Graphs 1-3.
  • the fuel oil used complied with the Venezuelan fuel oil specification and was provided by Ramonwolves Power Plant, Maracaibo, Venezuela.
  • Sample 1 200 ppm of ferrous formate.
  • Sample 2 200 ppm of ferric formate.
  • Sample 3 200 ppm of ferrous formate + 200 ppm of calcium formate.
  • Sample 4 200 ppm of ferrous formate + 200 ppm of calcium sulphonate.
  • Sample 5 (Reference 1): 200 ppm of ferrous fumarate.
  • Sample 6 (Reference 2): 200 ppm of Ferrocene. Control: Blank sample without additive.

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  • Chemical & Material Sciences (AREA)
  • Oil, Petroleum & Natural Gas (AREA)
  • Engineering & Computer Science (AREA)
  • Organic Chemistry (AREA)
  • Combustion & Propulsion (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • General Chemical & Material Sciences (AREA)
  • Health & Medical Sciences (AREA)
  • Emergency Medicine (AREA)
  • Solid Fuels And Fuel-Associated Substances (AREA)
  • Liquid Carbonaceous Fuels (AREA)

Abstract

L'invention concerne un additif pour mazout et/ou pétrole brut, qui comprend au moins un formate ferrique ou ferreux et au moins un solvant, un dispersant, un stabilisant, un agent anti-agglomérant et/ou un agent auxiliaire connu dans la technique actuelle, auxquels s'ajoute(nt) éventuellement un ou plusieurs composés métalliques organiques ou inorganiques complémentaires. Le formate ferrique ou ferreux est présent dans l'additif en quantité appropriée comprise entre 0,5 et 99,5 % en poids.
PCT/SE2007/001072 2006-12-14 2007-12-03 Additif pour mazout ou pétrole brut et composition de mazout ou de pétrole brut contenant cet additif WO2008073017A1 (fr)

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SE0602692-6 2006-12-14

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Cited By (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
WO2010092401A1 (fr) * 2009-02-16 2010-08-19 Innospec Limited Améliorations à ou relatives à la combustion du charbon
CN104130818A (zh) * 2013-12-25 2014-11-05 吉林市东燃新能源科技有限责任公司 油页岩半焦活化剂及制备方法和应用

Citations (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
GB2091291A (en) * 1981-01-15 1982-07-28 Drew Chem Corp Combustion additive for diesel fuel oil comprising Ca and Fe salts
SE451197B (sv) * 1980-11-28 1987-09-14 Ruhrchemie Ag Anvendning av jern- och/eller mangan av alifatiska karboxylsyror med 3 till 10 kolatomer i flytande brenslen som forbrenningshjelpmedel
US20050060929A1 (en) * 2003-09-05 2005-03-24 Rinaldo Caprotti Stabilised diesel fuel additive compositions

Patent Citations (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
SE451197B (sv) * 1980-11-28 1987-09-14 Ruhrchemie Ag Anvendning av jern- och/eller mangan av alifatiska karboxylsyror med 3 till 10 kolatomer i flytande brenslen som forbrenningshjelpmedel
GB2091291A (en) * 1981-01-15 1982-07-28 Drew Chem Corp Combustion additive for diesel fuel oil comprising Ca and Fe salts
US20050060929A1 (en) * 2003-09-05 2005-03-24 Rinaldo Caprotti Stabilised diesel fuel additive compositions

Cited By (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
WO2010092401A1 (fr) * 2009-02-16 2010-08-19 Innospec Limited Améliorations à ou relatives à la combustion du charbon
CN102348787A (zh) * 2009-02-16 2012-02-08 英诺斯派有限公司 煤的燃烧或有关煤的燃烧的改进
AU2010212620B2 (en) * 2009-02-16 2014-06-19 Innospec Limited Improvements in or relating to the combustion of coal
US8845767B2 (en) 2009-02-16 2014-09-30 Innospec Limited Methods of treating coal to improve combustion and reduce carbon content of fly ash
CN104130818A (zh) * 2013-12-25 2014-11-05 吉林市东燃新能源科技有限责任公司 油页岩半焦活化剂及制备方法和应用

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