Fuel-carried catalyst composition for oxidative soot removal

Abstract

The present invention provides a fuel carried catalyst composition for oxidative soot removal comprising a long chain cerium (III) carboxylate in an organic solvent. A preferred embodiment provides a cerium composition for use as a soot reduction catalyst system, the cerium composition comprising: cerium (III) neodecanoate; a cerium carboxylate (III) wherein the carboxylate has the general formula RCOO-wherein R is H or a C1 to C4 alkyl group; neodecanoic acid; and an organic solvent.

Description

Technical Field

[0001] The present invention relates to a fuel borne catalyst composition for oxidized soot removal. The present invention aims to reduce particulate emissions from diesel engines and improve the function of diesel particulate filters (DPF). Background Art

[0002] A diesel engine is an internal combustion engine in which the ignition of the fuel is caused by the elevated temperature of the air in the cylinder due to mechanical compression. Although diesel engines generally exhibit low exhaust levels of carbon monoxide and hydrocarbons, the exhaust contains certain levels of particulate matter or soot. A diesel particulate filter (DPF) facilitates the reduction of the amount of soot from the exhaust of a diesel engine. The particulates (soot) are collected on the filter, and the filter is actively or passively regenerated to burn the soot. Driven by energy considerations, durability, and system design, an ideal particulate removal unit should minimize the regeneration temperature of the soot filter. To this end, soot reduction catalysts, also known as fuel-borne catalysts (FBCs), have been developed.

[0003] US 2009 / 004078 discloses a catalytic diesel soot filter and method. The diesel soot filter comprises a porous filter element which is coated with a catalyst so that when the diesel exhaust gas is passed through the porous filter element, the diesel soot from the diesel exhaust gas is deposited in contact with the catalyst and the ignition temperature or oxidation temperature of the deposited diesel soot is reduced. The catalyst is a mixture of an alkali metal and cerium oxide.

[0004] US 2007 / 283681 discloses a method for reducing particulate emissions from a diesel engine, the method comprising: operating the diesel engine with a fuel containing a fuel-borne catalyst, the fuel-borne catalyst comprising a fuel-soluble or dispersible cerium composition and a fuel-soluble or dispersible platinum group metal composition. The method employs a fuel-soluble multimetallic catalyst, i.e., a fuel-borne catalyst (FBC) comprising a fuel-soluble or dispersible platinum group metal composition and a fuel-soluble or dispersible cerium composition. The cerium composition is preferably employed in a concentration effective to provide 0.5 ppm to 20 ppm cerium. The platinum group metal composition is preferably employed in a concentration effective to provide 0.0005 ppm to 2 ppm platinum. Summary of the invention

[0005] The present invention provides a solution to at least one of the above problems by providing a fuel-borne catalyst composition for oxidative soot removal according to claim 1. Results show that effective soot removal and regeneration of a diesel particulate filter is achieved using the cerium composition.

[0006] The present invention also provides a method for preparing the composition according to the general inventive concept, a method for operating a diesel engine in which the composition according to the general inventive concept is employed, and the use of the composition according to the general inventive concept in a diesel particulate filter for soot removal purposes. BRIEF DESCRIPTION OF THE DRAWINGS

[0007] By way of further instruction, the accompanying drawings are included to better understand the teachings of the present invention. The drawings are intended to aid in describing the present invention and are not intended to be limitations of the presently disclosed invention.

[0008] The drawings and symbols contained therein have meanings that are generally understood by a person of ordinary skill in the art to which the present invention belongs.

[0009] Figure 1 The soot removal efficiency (expressed as a percentage of the total amount of soot) is shown as a function of oxidation temperature (in °C) for a cerium composition according to the present invention, a cerium composition according to the prior art and a composition containing no soot removal catalyst, respectively.

[0010] Figure 2 The soot removal efficiencies of the cerium composition according to the present invention, the cerium composition according to the prior art, and the composition containing no soot removal catalyst after 10 minutes at 575° C. are respectively shown. DETAILED DESCRIPTION

[0011] Unless otherwise defined, all terms (including technical and scientific terms) used in disclosing the present invention have the meanings commonly understood by those of ordinary skill in the art to which the present invention belongs. By further guidance, term definitions are included to better understand the teachings of the present invention.

[0012] As used herein, the following terms have the following meanings:

[0013] As used herein, "a", "an", and "the" refer to both singular and plural references unless the context clearly dictates otherwise. For example, "a compartment" refers to one or more than one compartment.

[0014] As used herein, "about" in relation to a measurable value such as a parameter, amount, time duration, etc., is intended to encompass + / -20% or less, preferably + / -10% or less, more preferably + / -5% or less, even more preferably + / -1% or less, and still more preferably + / -0.1% or less and variations from the specified value, within which such variations are suitable for performing in the disclosed invention. However, it should be understood that the value to which the modifier "about" refers is itself also specifically disclosed.

[0015] As used herein, "comprising" and "consisting of" are synonymous with "including" or "containing" and are inclusive or open-ended terms that specify the presence of subsequent items, such as components, and do not exclude or preclude the presence of additional non-cited components, features, elements, members, steps known in the art or disclosed herein.

[0016] Numerical ranges recited by endpoints include all numbers and fractions subsumed within the range, as well as the recited endpoints. All percentages are to be understood as weight percentages abbreviated as "wt %" or volume percentages abbreviated as "vol %", unless otherwise defined or unless a different meaning is apparent to one skilled in the art from its use and the context in which it is used.

[0017] Therefore, the term "fuel" is intended to include all those fuels that are effective for operating a diesel engine. The fuel may contain detergents (e.g., 50 ppm to 300 ppm), lubricating additives (e.g., 25 ppm to about 500 ppm) and other additives as needed. Among the fuels suitable for the present invention are those that generally include fossil fuels, such as any typical petroleum-derived fuels, including distillate fuels. The fuel can be a blend of one or more fuels selected from the following: distillate fuels, including diesel fuels, for example, No. 2 diesel fuel, No. 1 diesel fuel, jet fuel (e.g., Jet A, or an analog with a boiling point and viscosity similar to No. 1 diesel fuel), ultra-low sulfur diesel fuel (ULSD); liquid fuels, including hydrocarbons derived from gaseous or solid fuels; and bio-derived fuels, such as those including "monoalkyl ester-based oxygenated fuels", i.e., fatty acid esters (preferably derived from triglycerides (e.g., soybean oil, canola oil and / or tallow) of methyl or ethyl esters of fatty acids), or "gas-to-liquid" fuels derived from biomass, natural gas, coal or petroleum sources. The term "hydrocarbon fuel" is intended to include all those fuels prepared from "distillate fuels" or "petroleum". Gasoline, jet fuel, diesel fuel and various other distillate fuels are included. The term "slip fuel" means all those products prepared by distilling petroleum or petroleum fractions and residues. The term "petroleum" in its ordinary sense is intended to include all those materials recovered from fossil fuels (regardless of the source, which are generally included in the meaning of the term), including hydrocarbon materials (regardless of viscosity).

[0018] Jet A and No. 1 diesel are considered equivalent for the purposes of this invention, but are covered by different American Society for Testing and Materials (ASTM) specifications. Diesel fuel is covered by ASTM D 975, "Standard Specification for Diesel Fuel Oil." Jet A has the designation ASTM D 1655, "Standard Specification for Aviation Turbine Fuel." The term ultra-low sulfur diesel fuel (ULSD) means No. 1 or No. 2 diesel fuel having a sulfur level no greater than 0.0015 weight percent (15 ppm), and some jurisdictions require a low aromatic content, e.g., less than ten volume percent.

[0019] The term "diesel fuel" means "distillate fuel", including diesel fuel or other fuels that meet the ASTM definition of diesel fuel, even if these fuels are not completely composed of distillates and may contain alcohols, ethers, organic nitro compounds, etc. (e.g., methanol, ethanol, ethyl ether, methyl ethyl ether, nitromethane). Also within the scope of the present invention are emulsions and liquid fuels derived from plant sources or mineral sources such as corn, alfalfa, shale and coal. These fuels may also contain other additives known to those skilled in the art, including dyes, hexadecane improvers, antioxidants (such as 2,6-di-tert-butyl-4-methylphenol), corrosion inhibitors, rust inhibitors (such as alkylated succinic acids and anhydrides), antibacterial agents, anti-gel agents, metal passivators, upper cylinder lubricants, antifreeze agents, etc.

[0020] The method for operating the diesel engine of the present invention employs a cerium catalyst, i.e., a fuel-borne catalyst (FBC), preferably comprising a fuel-soluble or fuel-dispersible cerium composition. The cerium composition is preferably employed in a concentration effective to provide 0.5ppm to 150ppm cerium, more preferably 1ppm to 100ppm cerium, and even 5ppm to 50ppm cerium. The method may also employ a platinum group metal composition effective to provide a concentration of 0.0005ppm to 2ppm platinum. In some embodiments, the treatment scheme may require the use of a higher catalyst concentration initially or at defined intervals or as needed, but not for the entire treatment. The advantage of a low level of catalyst is the reduction of ultrafine particles produced by carbonaceous soot and metal oxide emissions.

[0021] The cerium composition according to the general inventive aspects of the present invention may include one or more chemical enhancers, such as those described, but not limited to, in US 2007 / 283681.

[0022] According to the general inventive aspect of the present invention, the present invention provides a cerium composition comprising a long-chain cerium (III) carboxylate in an organic solvent. A preferred composition comprises cerium (III) in an amount of 1 wt % to 20 wt %, preferably 2 to 18 wt %, more preferably 3 to 16 wt %, even more preferably 5 to 15 wt %, and most preferably 6 wt %, 8 wt %, 10 wt %, 12 wt %, 14 wt % or any value therebetween, relative to the total weight of the composition.

[0023] In a preferred embodiment, according to the general inventive aspect, the present invention provides a cerium composition comprising:

[0024] A. Long chain cerium (III) carboxylate;

[0025] B. long chain carboxylic acids; and

[0026] C. Organic solvents,

[0027] The long-chain carboxylate is a conjugated base of the long-chain carboxylic acid. In a preferred embodiment, the cerium composition further comprises a short-chain carboxylic acid cerium (III).

[0028] In a preferred embodiment, the present invention provides a cerium composition according to the overall invention of the present invention, wherein the long-chain cerium carboxylate (III) is a cerium carboxylate (III) containing a carboxylate group having 6 to 24 carbon atoms, and wherein the short-chain cerium carboxylate (III) is a cerium carboxylate (III) containing a carboxylate group having 1 to 5 carbon atoms. Preferably, the long-chain cerium carboxylate (III) is a cerium carboxylate (III) containing a carboxylate group having 9 to 20 carbon atoms, more preferably 10 to 16 carbon atoms; and the short-chain cerium carboxylate (III) is a cerium carboxylate (III) containing a carboxylate group having 2 to 4 carbon atoms. In some embodiments, the long-chain cerium carboxylate (III) may be included as a mixture of two or more long-chain cerium carboxylates (III). In some embodiments, the long-chain carboxylate is selected from: saturated carboxylates such as alkyl carboxylates, cycloalkyl carboxylates; and unsaturated carboxylates. The long-chain carboxylate group may include aliphatic groups, alicyclic groups, aryl groups, and alkylaryl groups. Preferably, the long-chain carboxylic acid cerium (III) is composed of unsaturated carboxylate. The selected long-chain carboxylic acid cerium (III) compound is: cerium (III) cyclohexane acid, cerium (III) octanoate, 2-ethylhexyl cerium (III), cerium (III) isononanoate, cerium (III) 3,5,5-trimethylhexanoate, cerium (III) versatate, cerium (III) oleate, cerium (III) ricinoleate and other soaps (such as stearate and neodecanoate). The selected short-chain carboxylic acid cerium (III) compound is: cerium (III) formate, cerium (III) propionate and cerium (III) acetylacetonate. Alternatively, cerium (III) acetate can be used. In some embodiments, the short-chain carboxylic acid cerium (III) can be included as a mixture of two or more short-chain carboxylic acid cerium (III). The organic solvent can be a blend of two or more organic solvents. Preferably, the organic solvent is a hydrocarbon solvent containing C10-C13 alkanes.

[0029] In a preferred embodiment, the present invention provides a cerium composition according to the general inventive aspect of the present invention, wherein the long-chain cerium (III) carboxylate is cerium (III) neodecanoate; wherein the short-chain cerium (III) carboxylate is cerium (III) carboxylate, wherein the carboxylate has the general formula RCOO - , wherein R is H or a C1 to C4 alkyl group; and wherein the long chain carboxylic acid is neodecanoic acid.

[0030] In a preferred embodiment, the present invention provides a cerium composition according to the general inventive aspect of the present invention, wherein the long-chain cerium (III) carboxylate is included in an amount of 20% to 55% by weight, preferably 30% to 50% by weight, and more preferably 40% to 45% by weight relative to the total weight of the composition. Most preferably, the long-chain cerium (III) carboxylate is included in an amount of about 41%, 43% or 45% by weight, or any amount therebetween.

[0031] In a preferred embodiment, the present invention provides a cerium composition according to the general inventive aspect of the present invention, wherein the short-chain cerium (III) carboxylate is included in an amount of 0.1% to 10% by weight, preferably 0.5% to 5% by weight, and more preferably 1% to 3% by weight relative to the total weight of the composition. Most preferably, the short-chain cerium (III) carboxylate is included in an amount of about 1%, 2% or 3% by weight, or any amount therebetween.

[0032] In a preferred embodiment, the present invention provides a cerium composition according to the general inventive aspect of the present invention, wherein the long-chain carboxylic acid is included in an amount of 1 wt % to 30 wt %, preferably 2 wt % to 30 wt %, and more preferably 2 wt % to 20 wt % relative to the total weight of the composition. Most preferably, the long-chain carboxylate is included in an amount of about 2 wt %, 4 wt %, 6 wt %, 8 wt % or 10 wt %, or any amount therebetween.

[0033] In a preferred embodiment, the present invention provides a cerium composition according to the general inventive aspect of the present invention, wherein the composition further comprises an organic solvent. Preferably, the organic solvent is included in an amount of 5 wt % to 78.9 wt %, preferably in an amount of 15 wt % to 67.5 wt %, and more preferably in an amount of 22 wt % to 57 wt %. Most preferably, the organic solvent is included in an amount of about 25 wt %, 30 wt %, 35 wt %, 40 wt % or 45 wt %, or any amount therebetween.

[0034] In a first aspect, the present invention provides a cerium composition for use as a soot reduction catalyst system, the cerium composition comprising:

[0035] i. Cerium (III) neodecanoate;

[0036] ii. neodecanoic acid; and

[0037] iii. Organic solvents.

[0038] In a preferred embodiment, the cerium composition further comprises a short-chain cerium (III) carboxylate, wherein the carboxylate has the general formula RCOO -, wherein R is H or a C1 to C4 alkyl group. The inventors have found that the cerium composition according to the first aspect of the present invention can be advantageously used as a soot reduction catalyst system in a diesel engine. The results show that effective soot removal and regeneration of a diesel particulate filter is achieved using the cerium composition. Specifically, it was found that the cerium composition according to the present invention achieves: (i) a lower dosage of the cerium composition in the fuel compared to the prior art composition, while producing similar soot activity; (ii) increased catalytic oxidation efficiency in terms of higher soot conversion, thereby achieving excellent performance; (iii) regeneration of the diesel particulate filter at a relatively low temperature, i.e., at 450°C instead of 600°C, in the absence of a fuel-borne catalyst; and (iv) less ash formation.

[0039] In addition, depending on the dosage of the cerium composition, secondary advantages are achieved, such as a reduction in the time to reach the regeneration temperature, and a reduction in the regeneration time to less than 7 minutes or even less than 4 minutes can be achieved. Instant soot removal can be achieved, and high soot removal efficiency is possible. Complete combustion of accumulated soot particles enables an extended life of the diesel particulate filter. Active regeneration can be achieved in less than 4 minutes at a relatively low temperature of 450°C. High catalytic oxidation can be achieved by good dispersion of cerium in the soot particles.

[0040] The organic solvent also achieves good compatibility of the cerium composition with the fuel. The cerium composition forms a stable, uniform mixture in the fuel.

[0041] In a preferred embodiment, the present invention provides a cerium composition according to the first aspect of the present invention, the cerium composition comprising:

[0042] i. cerium (III) neodecanoate in an amount of 20 wt % to 55 wt % relative to the total weight of the composition;

[0043] ii. neodecanoic acid in an amount of 1 wt % to 30 wt % relative to the total weight of the composition; and

[0044] iii. an organic solvent in an amount of 15 to 79 wt % relative to the total weight of the composition.

[0045] Preferably, the composition comprises:

[0046] i. cerium (III) neodecanoate in an amount of 20 wt % to 55 wt % relative to the total weight of the composition;

[0047] ii. a cerium (III) carboxylate, wherein the carboxylate has the general formula RCOO - , wherein R is H or a C1 to C4 alkyl group, and the amount of the carboxylate radical is 0.1 wt % to 10 wt % relative to the total weight of the composition;

[0048] iii. neodecanoic acid in an amount of 1 wt % to 30 wt % relative to the total weight of the composition; and

[0049] iv. an organic solvent in an amount of 5 to 78.9 wt % relative to the total weight of the composition.

[0050] More preferably, the present invention provides a cerium composition according to the first aspect of the present invention, the cerium composition comprising:

[0051] i. cerium (III) neodecanoate in an amount of 30 wt % to 50 wt % relative to the total weight of the composition;

[0052] ii. neodecanoic acid in an amount of 2 wt % to 30 wt % relative to the total weight of the composition; and

[0053] iii. an organic solvent in an amount of 20 to 68 wt % relative to the total weight of the composition.

[0054] Preferably, the cerium composition comprises:

[0055] i. cerium (III) neodecanoate in an amount of 30 wt % to 50 wt % relative to the total weight of the composition;

[0056] ii. preferably a cerium (III) carboxylate, wherein the carboxylate has the general formula RCOO - , wherein R is H or a C1 to C4 alkyl group, and the amount of the carboxylate radical is 0.5 wt % to 5 wt % relative to the total weight of the composition;

[0057] iii. neodecanoic acid in an amount of 2 wt % to 30 wt % relative to the total weight of the composition; and

[0058] iv. an organic solvent in an amount of 15 to 67.5 wt % relative to the total weight of the composition.

[0059] Even more preferably, the present invention provides a cerium composition according to the first aspect of the present invention, the cerium composition comprising:

[0060] i. cerium (III) neodecanoate in an amount of 40% to 45% by weight relative to the total weight of the composition;

[0061] ii. neodecanoic acid in an amount of 2 wt % to 30 wt % relative to the total weight of the composition; and

[0062] iii. an organic solvent in an amount of 25 to 58 wt % relative to the total weight of the composition.

[0063] Preferably, the cerium composition comprises:

[0064] i. cerium (III) neodecanoate in an amount of 40% to 45% by weight relative to the total weight of the composition;

[0065] ii. a cerium (III) carboxylate, wherein the carboxylate has the general formula RCOO - , wherein R is H or a C1 to C4 alkyl group, and the amount of the carboxylate radical is 1 wt % to 3 wt % relative to the total weight of the composition;

[0066] iii. neodecanoic acid in an amount of 2 wt % to 30 wt % relative to the total weight of the composition; and

[0067] iv. an organic solvent in an amount of 22 to 57 wt % relative to the total weight of the composition.

[0068] In a preferred embodiment, the present invention provides a cerium composition according to the first aspect of the present invention, wherein the molar ratio of neodecanoic acid to cerium (III) neodecanoate is between 0.1 and 5.0. Preferably, the molar ratio is between 0.5 and 3.0, and more preferably between 1 and 3, the ratio being about 1.6, 1.8, 2.0, 2.2, 2.4, 2.6 or 2.8, or any value therebetween. The excess amount of neodecanoic acid may be neutralized or partially neutralized.

[0069] In a preferred embodiment, the present invention provides a cerium composition according to the first aspect of the present invention, wherein the carboxylate is selected from the group consisting of formate, acetate and propionate. The selected carboxylate exhibits improved reactivity with a cerium (III) precursor such as cerium (III) carbonate.

[0070] In a preferred embodiment, the present invention provides a cerium composition according to the first aspect of the present invention, wherein the organic solvent is a hydrocarbon solvent comprising a C10-C13 alkane.

[0071] In a preferred embodiment, the present invention provides a cerium composition according to the first aspect of the present invention, wherein the organic solvent is a C6-C10 aliphatic monohydric alcohol ether.

[0072] In a preferred embodiment, the present invention provides a cerium composition according to the first aspect of the present invention, wherein the organic solvent is a mixture of a hydrocarbon solvent comprising a C10-C13 alkane and a C6-C10 aliphatic monohydric alcohol ether.

[0073] Preferably, the present invention provides a cerium composition according to the first aspect of the present invention, wherein the organic solvent is a hydrocarbon solvent comprising C9-C10 alkanes. Preferably, the hydrocarbon solvent is included in an amount of at least 30% by weight relative to the total weight of the organic solvent, more preferably at least 40% by weight, and most preferably about 50% by weight. The hydrocarbon solvent may comprise normal alkanes, isoalkanes and cycloalkanes. The hydrocarbon solvent preferably has a CAS number: 64742-48-9 and preferably comprises less than 2% of aromatic compounds.

[0074] Preferably, the present invention provides a cerium composition according to the first aspect of the present invention, wherein the organic solvent is a hydrocarbon solvent comprising C10-C13 alkanes. Preferably, the hydrocarbon solvent is included in an amount of at least 30% by weight relative to the total weight of the organic solvent, more preferably at least 40% by weight, and most preferably about 50% by weight. The hydrocarbon solvent may include paraffins, isoparaffins and cycloparaffins. The hydrocarbon solvent preferably has CAS number: 64742-48-9 and preferably contains less than 2% of aromatic compounds.

[0075] In a preferred embodiment, the present invention provides a cerium composition according to the first aspect of the present invention, wherein the organic solvent comprises a mixture of C9-C10 alkanes and C10-C13 alkanes.

[0076] Preferably, the present invention provides a cerium composition according to the first aspect of the present invention, wherein the organic solvent comprises a C6-C10 aliphatic monoalcohol ether. Preferably, the C6-C10 aliphatic monoalcohol ether is included in an amount of at least 30 wt %, more preferably at least 40 wt %, and most preferably about 50 wt % relative to the total weight of the organic solvent. Preferably, the organic solvent comprises a C1-C6 alkyl ether of diethylene glycol or dipropylene glycol, and more preferably comprises a C1-C4 alkyl ether of diethylene glycol or dipropylene glycol.

[0077] Preferably, the present invention provides a cerium composition according to the first aspect of the present invention, wherein the organic solvent is a mixture of a hydrocarbon solvent containing C10-C13 alkanes and a C6-C10 aliphatic monoalcohol ether, respectively, wherein the hydrocarbon solvent is contained in an amount of 30 wt % to 70 wt % relative to the total weight of the organic solvent, and wherein the aliphatic monoalcohol ether is contained in an amount of 70 wt % to 30 wt % relative to the total weight of the organic solvent. More preferably, the hydrocarbon solvent is contained in an amount of 40 wt % to 60 wt %, and the aliphatic monoalcohol ether is contained in an amount of 60 wt % to 40 wt %, respectively. Most preferably, the hydrocarbon solvent is contained in an amount of about 50 wt %, and the aliphatic monoalcohol ether is contained in an amount of about 50 wt %.

[0078] Preferably, the present invention provides a cerium composition according to the first aspect of the present invention, wherein the organic solvent comprises one or more saturated and / or unsaturated C5-C11 esters. The preferred ester may be ethyl lactate.

[0079] Preferably, the present invention provides a cerium composition according to the first aspect of the present invention, wherein the organic solvent comprises one or more saturated and / or unsaturated C12-C30 esters, more preferably bio-based and / or bio-derived saturated and unsaturated C12-C30 esters. Preferably, the unsaturated C12-C30 ester is contained in an amount of at least 80% by weight relative to the total weight of the organic solvent, more preferably in an amount of at least 90% by weight, and even more preferably in an amount of at least 98% by weight. In a first preferred embodiment, the unsaturated C12-C30 ester is rapeseed methyl ester, or an ester derived from a fatty acid such as soybean 2-ethylhexyl ester. Rapeseed methyl ester (RME) is a mixture of methyl esters consisting of saturated and unsaturated C16 to C22 fatty acids. Technically, rapeseed methyl ester is produced by chemically converting rapeseed oil using methanol. In a second preferred embodiment, the unsaturated C12-C30 ester is soybean 2-ethylhexyl ester, also known as soybean 2-ethylhexyl ester. The unsaturated C12-C30 ester may be included as a mixture of two or more ester products.

[0080] Preferably, the present invention provides a cerium composition according to the first aspect of the present invention, wherein the organic solvent comprises C1-C6 n-alkyl pyrrolidone, more preferably C4 n-alkyl pyrrolidone. Preferably, the C1-C6 n-alkyl pyrrolidone is contained in an amount of at least 80 wt %, more preferably at least 90 wt %, and even more preferably at least 98 wt % relative to the total weight of the organic solvent. Preferably, the C1-C6 n-alkyl pyrrolidone is C4 n-alkyl pyrrolidone.

[0081] In a second aspect of the general inventive concept of the present invention, the present invention provides a method for preparing a cerium composition, the method comprising the following steps:

[0082] step a) contacting a long-chain carboxylic acid, preferably in the presence of a short-chain carboxylic acid and / or a hydrate and / or anhydride thereof, with a cerium(III) compound under a non-oxidizing atmosphere, wherein the cerium(III) compound is selected from cerium(III) carbonate, cerium(III) hydroxycarbonate, cerium(III) hydroxide, cerium(III) oxyhydroxide and / or cerium(III) oxide, and wherein the long-chain carboxylic acid is provided in a stoichiometric excess relative to the amount of the cerium(III) compound, thereby obtaining a mixture of long-chain cerium(III) carboxylic acids and short-chain cerium(III) carboxylates in the long-chain carboxylic acid; and

[0083] Step b) An organic solvent is added to the mixture obtained in step a).

[0084] The cerium (III) compound provided in step a) may be provided as such, and / or may comprise a hydrate thereof. Preferably, the long-chain carboxylate radical and the long-chain carboxylic acid are carboxylic acids having 6 to 24 carbon atoms, preferably 9 to 20 carbon atoms, and more preferably 10 to 16 carbon atoms. In some embodiments, the long-chain carboxylic acid may be included as a mixture of two or more long-chain carboxylic acids. In some embodiments, the carboxylic acid is selected from: saturated carboxylic acids such as alkyl acids and cycloalkyl acids; and unsaturated carboxylic acids. The carboxylic acid may contain aliphatic groups, alicyclic groups, aryl groups and alkylaryl groups. Preferably, the long-chain carboxylic acid is composed of unsaturated carboxylic acids. The selected long-chain carboxylic acids are: cycloalkane acid, octanoic acid, 2-ethylhexanoic acid, isononanoic acid, 3,5,5-trimethylhexanoic acid, versatic acid, oleic acid, ricinoleic acid, stearic acid and neodecanoic acid. Preferably, the short-chain carboxylic acid contains 1 to 5 carbon atoms, more preferably 2 to 4 carbon atoms. Preferably, the short-chain carboxylic acid is a saturated carboxylic acid. In some embodiments, the short-chain carboxylic acid is included as a hydrate or anhydride of a short-chain carboxylic acid. The selected short-chain carboxylic acids are: formic acid, acetic acid, propionic acid, butyric acid and acetic anhydride. In some embodiments, the short-chain carboxylic acid can be included as a mixture of two or more short-chain carboxylic acids. The organic solvent can be a blend of two or more organic solvents.

[0085] The inventors have found that when attempting to prepare long-chain carboxylic acid cerium (III) in the absence of a short-chain carboxylic acid, complete conversion of the starting product cerium (III) cannot be achieved and a clear solution is not obtained. Therefore, the presence of a short-chain carboxylic acid improves the reaction and the purification of the reaction product.

[0086] In a preferred embodiment, the present invention provides a method for preparing a cerium composition according to the general inventive aspect of the present invention, wherein the long-chain carboxylic acid is neodecanoic acid; wherein the short-chain carboxylic acid is a carboxylic acid having the general formula RCOOH, wherein R is H or a C1 to C4 alkyl group; wherein the long-chain carboxylic acid cerium (III) is neodecanoate cerium (III); and wherein the short-chain carboxylic acid cerium (III) has the general formula RCOO - , wherein R is H or C1 to C4 alkyl.

[0087] In a second aspect, the present invention provides a method for preparing a cerium composition, the method comprising the following steps:

[0088] step a) contacting neodecanoic acid with a cerium(III) compound, preferably in the presence of an organic acid of the general formula RCOOH and / or its hydrate and / or anhydride, under a non-oxidizing atmosphere, wherein R is H or a C1 to C4 alkyl group, wherein the cerium(III) compound is selected from cerium(III) carbonate, cerium(III) hydroxycarbonate, cerium(III) hydroxide, cerium(III) oxyhydroxy and / or cerium(III) oxide, and wherein the neodecanoic acid is provided in a stoichiometric excess relative to the amount of the cerium(III) compound, thereby obtaining a mixture of cerium(III) neodecanoate and cerium(III) carboxylate in the neodecanoic acid; and

[0089] Step b) An organic solvent is added to the mixture obtained in step a).

[0090] The present inventors have found that when a stoichiometric excess of neodecanoic acid is used, the conversion of the cerium (III) compound to cerium (III) neodecanoate proceeds more easily, and the excess neodecanoic acid does not hinder the effectiveness of the fuel-borne catalyst composition for catalytic soot reduction, while no significant negative side effects are observed. The present inventors have also found that the use of carboxylic acids having 1 to 5 carbon atoms is beneficial to the conversion of the cerium (III) compound. It is speculated that short-chain carboxylic acids increase the solubility of the cerium (III) compound in the reaction mixture. The present inventors have also found that the organic solvent is preferably added after the long-chain carboxylic acid is contacted with the cerium (III) compound in the presence of the short-chain carboxylic acid.

[0091] In a preferred embodiment, the excess amount of neodecanoic acid or the excess amount of the long chain carboxylic acid can be neutralized or partially neutralized using a reactive base such as NaOH or KOH.

[0092] In a preferred embodiment, the cerium (III) compound is selected from: cerium (III) carbonate, cerium (III) hydroxycarbonate, cerium (III) hydroxide, cerium (III) oxyhydroxy and / or cerium (III) oxide, and more preferably selected from: cerium (III) carbonate, cerium (III) hydroxycarbonate and / or their hydrates.

[0093] In a preferred embodiment, the organic acid is selected from formic acid, acetic acid, propionic acid and butyric acid, more preferably the organic acid is formic acid, acetic acid, propionic acid, and most preferably the organic acid is acetic acid. Combinations of two or more organic acids may be advantageously used.

[0094] In a preferred embodiment, the present invention provides a method according to the second aspect of the present invention, wherein the neodecanoic acid is contacted with the cerium (III) compound in the presence of the organic acid at a temperature between 60° C. and 180° C. More preferably, the neodecanoic acid is contacted with the cerium (III) compound in the presence of the organic acid at a temperature between 80° C. and 120° C., and more preferably at a temperature between 90° C. and 100° C. Preferably, the neodecanoic acid is contacted with the cerium (III) compound under vigorous agitation.

[0095] In a preferred embodiment, the present invention provides a method according to the second aspect of the present invention, wherein the organic solvent is added to the mixture obtained in step a) at a temperature between 100° C. and 200° C. More preferably, the organic solvent is added to the mixture obtained in step a) at a temperature between 120° C. and 160° C., and more preferably at a temperature between 130° C. and 150° C. Preferably, the organic solvent is added under vigorous stirring.

[0096] In a preferred embodiment, the present invention provides a method according to the second aspect of the present invention, wherein the mixture obtained in step a) is filtered and wherein a further organic solvent is added to the filtrate. The solvent is added to obtain a predetermined concentration of cerium.

[0097] In a preferred embodiment, the present invention provides a method according to the second aspect of the present invention for preparing the cerium composition according to the first aspect of the present invention.

[0098] In a third aspect, the present invention provides a method for reducing particulate emissions from a diesel engine, wherein the diesel engine is fed a fuel composition comprising a fuel, cerium (III) neodecanoate and a cerium (III) carboxylate, wherein the carboxylate has the general formula RCOO - , wherein R is H or C1 to C4 alkyl.

[0099] More specifically, the method according to the third aspect of the invention relates to a method for reducing particulate emissions from a diesel engine, the method comprising the steps of: operating a diesel engine with a fuel containing a fuel-borne catalyst comprising a fuel-soluble or fuel-dispersible cerium composition; passing exhaust gas produced by the combustion of the fuel and containing cerium oxide released from the fuel by combustion through a diesel particulate filter to collect particulate matter in the diesel particulate filter; and regenerating the diesel particulate filter by increasing the temperature to a temperature between 300°C and 700°C, more preferably to a temperature elevated to between 350°C and 650°C, even more preferably between 400°C and 600°C, and most preferably to a temperature of about 400°C, 425°C, 450°C, 475°C, 500°C, 525°C, 550°C or 575°C, or any temperature therebetween. Most preferably, the diesel particulate filter is regenerated at a temperature between 400°C and 500°C. Preferably, the cerium composition further comprises neodecanoic acid. Preferably, the cerium composition further comprises an organic solvent. More preferably, the cerium composition is a fuel-borne catalyst composition according to the first aspect of the present invention. In a preferred embodiment, the present invention provides a method according to the third aspect of the present invention, wherein the fuel composition further comprises neodecanoic acid.

[0100] In a fourth aspect, the present invention provides use of a cerium composition according to the first aspect of the present invention as a soot reduction catalyst composition.

[0101] In a particularly preferred embodiment, the present invention provides:

[0102] A cerium composition for use as a soot reduction catalyst system, the cerium composition comprising:

[0103] i. Cerium (III) neodecanoate;

[0104] ii. a cerium (III) carboxylate, wherein the carboxylate has the general formula RCOO - , wherein R is H or C1 to C4 alkyl;

[0105] iii. neodecanoic acid; and

[0106] iv. Organic solvents.

[0107] More specifically, the aforementioned cerium composition comprises:

[0108] i. cerium (III) neodecanoate in an amount of 20 wt % to 55 wt % relative to the total weight of the composition;

[0109] ii. a cerium (III) carboxylate, wherein the carboxylate has the general formula RCOO -, wherein R is H or a C1 to C4 alkyl group, and the amount of the carboxylate radical is 0.1 wt % to 10 wt % relative to the total weight of the composition;

[0110] iii. neodecanoic acid in an amount of 1 wt % to 30 wt % relative to the total weight of the composition; and

[0111] iv. an organic solvent in an amount of 5 to 78.9 wt % relative to the total weight of the composition.

[0112] More specifically, the aforementioned cerium composition comprises:

[0113] i. cerium (III) neodecanoate in an amount of 40% to 45% by weight relative to the total weight of the composition;

[0114] ii. a cerium (III) carboxylate, wherein the carboxylate has the general formula RCOO - , wherein R is H or a C1 to C4 alkyl group, and the amount of the carboxylate radical is 1 wt % to 3 wt % relative to the total weight of the composition;

[0115] iii. neodecanoic acid in an amount of 2 wt % to 30 wt % relative to the total weight of the composition; and

[0116] iv. an organic solvent in an amount of 22 to 57 wt % relative to the total weight of the composition.

[0117] More specifically, in the aforementioned cerium composition, the molar ratio of neodecanoic acid to cerium (III) neodecanoate is between 0.1 and 5.0.

[0118] More specifically, in the aforementioned cerium composition, the carboxylate is selected from the group consisting of formate, acetate and propionate.

[0119] More specifically, in the aforementioned cerium composition, the organic solvent is a hydrocarbon solvent containing C10-C13 alkane.

[0120] More specifically, in the aforementioned cerium composition, the organic solvent is a C6-C10 aliphatic monohydric alcohol ether.

[0121] More specifically, the aforementioned cerium composition, wherein the organic solvent comprises one or more bio-based and / or bio-derived, saturated and / or unsaturated C12-C30 esters.

[0122] A method for preparing a cerium composition, the method comprising the following steps:

[0123] i. contacting neodecanoic acid with a cerium (III) compound in the presence of an organic acid of the general formula RCOOH and / or its hydrate and / or anhydride under a non-oxidizing atmosphere, wherein R is H or a C1 to C4 alkyl group, wherein the cerium (III) compound is selected from cerium (III) carbonate, cerium (III) hydroxycarbonate, cerium (III) hydroxide, cerium (III) oxyhydroxide and / or cerium (III) oxide and / or their hydrates, and wherein the neodecanoic acid is provided in a stoichiometric excess relative to the amount of the cerium (III) compound, thereby obtaining a mixture of cerium (III) neodecanoate and cerium (III) carboxylate in neodecanoic acid; and i. contacting neodecanoic acid with a cerium (III) compound in the presence of an organic acid of the general formula RCOOH and / or its hydrate and / or anhydride, wherein R is H or a C1 to C4 alkyl group, wherein the cerium (III) compound is selected from cerium (III) carbonate, cerium (III) hydroxycarbonate, cerium (III) hydroxide, cerium (III) oxyhydroxide and / or cerium (III) oxide and / or their hydrates, and wherein the neodecanoic acid is provided in a stoichiometric excess relative to the amount of the cerium (III) compound, thereby obtaining a mixture of cerium (III) neodecanoate and cerium (III) carboxylate in neodecanoic acid; and

[0124] ii. adding an organic solvent to the mixture obtained in step a).

[0125] More specifically, the aforementioned method, wherein the neodecanoic acid is contacted with the cerium (III) compound in the presence of the organic acid at a temperature between 60°C and 180°C.

[0126] More specifically, the aforementioned process, wherein the organic solvent is added to the mixture obtained in step a) at a temperature between 100°C and 200°C.

[0127] More specifically, the aforementioned process, wherein the mixture obtained in step a) is filtered, and wherein the organic solvent is added to the filtrate.

[0128] A method for reducing particulate emissions from a diesel engine, the method comprising the steps of: operating the diesel engine with a fuel composition comprising: a fuel, cerium (III) neodecanoate and a cerium (III) carboxylate, wherein the carboxylate has the general formula RCOO - , wherein R is H or a C1 to C4 alkyl group; neodecanoic acid; and an organic solvent; passing exhaust gas produced by combustion of a fuel and containing cerium oxide released from the fuel through a diesel particulate filter to collect particulate matter in the diesel particulate filter; and regenerating the diesel particulate filter by increasing the temperature to a temperature between 350° C. and 600° C.

[0129] More specifically, the aforementioned method, wherein the diesel particulate filter is regenerated by increasing the temperature to a temperature between 350°C and 500°C.

[0130] Example

[0131] The following examples are intended to further illustrate the present invention but are not intended to limit the scope of the present invention.

[0132] Example 1

[0133] The reactor was purged with nitrogen to provide an inert atmosphere. 804 g of neodecanoic acid and 8.8 g of acetic acid (80% solution in water) were added to the reactor, and the reactor contents were stirred and heated to 95 ° C. Over a period of 2.5 hours, 400 g of cerium carbonate (III) was gradually added to the reactor while maintaining the temperature at 95 ° C. Finally, 8.8 g of acetic acid (80% solution in water) was added, and the reaction mixture was heated at 95 ° C for 2 hours, and then at 140 ° C for 4 hours. Water was removed by vacuum distillation. More than 96% of cerium carbonate (III) was converted. Then, under an inert atmosphere of nitrogen, 348 mL of D60 was gradually added to the reactor at a temperature of 140 ° C over a period of 6 hours. D60 is an organic solvent mainly comprising C10-C12 paraffins and cycloalkanes, with very low aromatic content. Trace amounts of water can be further removed by vacuum distillation. After cooling to about 100° C., the reaction mixture was filtered out, and D60 was further added to the filtrate until a cerium content of about 10 wt % was reached. The obtained composition had a density of 1.0 g / mL.

[0134] Example 2

[0135] The procedure of Example 1 was repeated, wherein cerium (III) hydroxide was used as the cerium salt instead of cerium (III) carbonate.

[0136] Example 3

[0137] The procedure of Example 1 was repeated, using formic acid instead of acetic acid.

[0138] Example 4

[0139] The cerium composition obtained by the method according to Example 1 was added to the fuel at a dosage of 0.2 g / L to generate 24 ppm cerium. The soot removal test is shown in Figure 1 and Figure 2 middle.

[0140] Example 5

[0141] The cerium composition obtained by the method according to Example 1 was added to the fuel at a dosage of 1.0 g / L to generate 120 ppm cerium. The soot removal test is shown in Figure 1 and Figure 2 middle.

[0142] Example 6

[0143] Reactor is purged with nitrogen to provide inert atmosphere. 803.4 g neodecanoic acid and 8.6 g propionic acid are added to the reactor, and the reactor contents are stirred and heated to 95 ° C. In the period of 1.5 hours, 400 g cerium carbonate (III) is gradually added to the reactor, while the temperature is maintained at 95 ° C. Finally, 8.6 g propionic acid is added, and the reaction mixture is heated at 95 ° C for 2 hours, and then at 140 ° C for 6 hours, while distilling out water. Trace amounts of water can be further removed by vacuum distillation. Then, under the inert atmosphere of nitrogen, 347 mL D60 is gradually added to the reactor at a temperature of 140 ° C in the period of 3 hours. The reaction mixture is maintained at 140 ° C for another 6 hours, while distilling out water. Trace amounts of water can be further removed by vacuum distillation. After being cooled to about 100 ° C, the reaction mixture is filtered out, and D60 is further added to the filtrate until the cerium content of about 10 weight % is reached. The composition obtained has a density of 1.0 g / mL. +99% of the added cerium(III) carbonate was converted.

[0144] Example 7

[0145] Reactor is purged with nitrogen to provide inert atmosphere.803.5 g of neodecanoic acid are added to the reactor, and the reactor contents are stirred and heated to 95 ° C. In the period of 2.5 hours, 400 g of cerium carbonate (III) are gradually added to the reactor, while the temperature is maintained at 95 ° C. The reaction mixture is heated at 95 ° C for 2 hours, and then at 140 ° C for 4 hours, while distilling out water. Trace amounts of water can be further removed by vacuum distillation. Then, under the inert atmosphere of nitrogen, 346 mL of D60 is gradually added to the reactor at a temperature of 140 ° C in the period of 2 hours. The reaction mixture is maintained at 140 ° C for another 6 hours, while distilling out water. Trace amounts of water can be further removed by vacuum distillation. After being cooled to about 100 ° C, the reaction mixture is filtered out. The filtrate obtained has a cerium content of about 9.7 weight % and a density of + / -1.0 g / mL. 81% of the added cerium carbonate (III) is converted.

[0146] Example 8

[0147] The reactor was purged with nitrogen to provide an inert atmosphere. 672.7 g of 2-ethylhexanoic acid and 8.8 g of acetic acid (80% solution in water) were added to the reactor, and the reactor contents were stirred and heated to 95 ° C. Over a period of 2.5 hours, 400 g of cerium carbonate (III) was gradually added to the reactor while maintaining the temperature at 95 ° C. Finally, 8.8 g of acetic acid (80% solution in water) was added, and the reaction mixture was heated at 95 ° C for 2 hours, and then at 140 ° C for 4 hours. Water was removed by vacuum distillation. Then, under an inert atmosphere of nitrogen, 430 mL of D60 was gradually added to the reactor at a temperature of 140 ° C over a period of 2 hours. The reaction mixture was maintained at 140 ° C for another 6 hours while distilling out water. Trace amounts of water can be further removed by vacuum distillation. After cooling to about 100 ° C, 316 mL of D60 was further added. The composition obtained has a density of 0.97 g / mL and a cerium content of 10.6 wt %. More than 99% of the cerium(III) carbonate was converted.

[0148] Example 9

[0149] Reactor is purged with nitrogen to provide inert atmosphere.672.7g 2-ethylhexanoic acid is added to reactor, and reactor contents are stirred and heated to 95°C.In the period of 2.5 hours, 400 g cerium carbonate (III) is gradually added to reactor, while temperature is maintained at 95°C.Reaction mixture is heated at 95°C for 2 hours, and then at 140°C for 4 hours.Water is removed by vacuum distillation.Then, under the inert atmosphere of nitrogen, 430mL D60 is gradually added to reactor at a temperature of 140°C in the period of 2 hours.Reaction mixture is maintained at 140°C for another 6 hours, while water is distilled out.Trace water can be further removed by vacuum distillation.Add another 290mL D60 and filter reaction mixture.The composition obtained has a density of 0.97g / mL.Cerium carbonate (III) less than 92% by weight is converted.

[0150] Example 10

[0151] The reactor was purged with nitrogen to provide an inert atmosphere. 758 g of tertiary carbon ™ Acid 913 and 8.8 g of acetic acid (80% solution in water) were added to the reactor and the reactor contents were agitated and heated to 95°C. ™Acid 913 is a mixture of tertiary carboxylic acids of C6 to C13, wherein C9 is a major component. Over a 2-hour period, 400 g of cerium carbonate (III) are gradually added to the reactor while maintaining the temperature at 95 ° C. Finally, 8.8 g of acetic acid (80% solution in water) are added, and the reaction mixture is heated at 95 ° C for 2 hours, and then at 140 ° C for 7 hours. Water is removed by vacuum distillation. Then, under an inert atmosphere of nitrogen, 348 mL of D60 is gradually added to the reactor at a temperature of 140 ° C over a 1.5-hour period. After another 9 hours at 140 ° C, the reaction mixture is cooled to about 100 ° C and the reaction mixture is filtered out. Obtaining a filtrate of about 9.7 % by weight of cerium content. More than 79% of cerium carbonate (III) is converted.

[0152] Embodiment 11

[0153] The reactor was purged with nitrogen to provide an inert atmosphere. 336.3 g of octanoic acid, 401.7 g of capric acid and 8.8 g of acetic acid (80% solution in water). Over a period of 1.5 hours, 400 g of cerium carbonate (III) was gradually added to the reactor while maintaining the temperature at 95 ° C. Finally, 8.8 g of acetic acid (80% solution in water) was added, and the reaction mixture was heated at 95 ° C for 2 hours, and then at 140 ° C for 6.5 hours, while distilling out water. Residual water was removed by vacuum distillation. Then, under an inert atmosphere of nitrogen, 348 mL of D60 was gradually added to the reactor at a temperature of 140 ° C over a period of 2 hours. After another 6.5 hours at 140 ° C, 400 mL of D60 was added and the reaction mixture was filtered out. The filtrate solidified when cooling with a cerium content of about 9.6% by weight was obtained. More than 99% of cerium carbonate (III) was converted.

[0154] Example 12

[0155] The reactor was purged with nitrogen to provide an inert atmosphere. 737.2 g isononanoic acid and 8.8 g acetic acid (80% solution in water). Over a 2-hour period, 400 g cerium carbonate (III) was gradually added to the reactor while maintaining the temperature at 95 ° C. Finally, 8.8 g acetic acid (80% solution in water) was added, and the reaction mixture was heated at 95 ° C for 2 hours, and then at 140 ° C for 7 hours. Water was removed by vacuum distillation. Then, under an inert atmosphere of nitrogen, 430 mL D60 was gradually added to the reactor at a temperature of 140 ° C over a 1.5-hour period. After another 6 hours at 140 ° C, the reaction mixture was cooled to about 100 ° C, 277 mL D60 was further added and the reaction mixture was filtered out. The filtrate solidified when standing at room temperature with a cerium content of 9.77% by weight was obtained. More than 97% of cerium carbonate (III) was converted. D60 was further added to the filtrate until a cerium content of about 9.5 wt% was reached, ie, a metal concentration at which the filtrate remained liquid at room temperature.

[0156] Comparative Example 1

[0157] Ceria nanoparticle material (8nm to 10nm) was added to the fuel at a dosage of 0.35g / L to generate 24ppm cerium. Soot removal tests are shown in Figure 1 and Figure 2 middle.

[0158] Comparative Example 2

[0159] Ceria nanoparticle material (8nm to 10nm) was added to the fuel at a dosage of 1.5g / L to generate 120ppm cerium. Soot removal tests are shown in Figure 1 and Figure 2 middle.

[0160] Comparative Example 3

[0161] No soot removal catalyst system was dosed. Soot removal tests are shown in Figure 1 and Figure 2 middle.

[0162] Figure 1 The soot removal efficiency (expressed as a percentage of the total soot) is shown as a function of oxidation temperature. The results show that the soot reduction additive according to the present invention achieves a higher soot conversion at any temperature tested. Figure 1It is shown that when a cerium-based soot removal catalyst is used, the soot removal efficiency is significantly improved at any temperature. A higher loading of the soot removal catalyst composition achieves higher soot removal. Importantly, the cerium composition according to the present invention exhibits significantly improved soot removal activity and achieves high soot removal efficacy, even at lower temperatures such as 450°C to 475°C, or even as low as 400°C to 425°C.

[0163] Figure 2 The soot removal efficiency of the cerium composition according to the present invention, the cerium composition according to the prior art and the composition without soot removal catalyst after 10 minutes at 575° C. is shown respectively. The results show that the soot reduction additive according to the present invention ensures the formation of a smaller amount of ash compared to cerium dioxide nanoparticles. Figure 2 It is shown that for the cerium composition according to the invention, high soot removal efficiency is achieved even at lower catalyst loadings. All soot removal catalyst compositions perform better than soot removal without the soot removal catalyst. Further experiments under the same conditions show that for Example 4, a regeneration time of less than 7 minutes is achieved; for Example 5, a regeneration time of less than 4 minutes is achieved. Thus, the compositions of the invention achieve higher soot conversion and improved regeneration kinetics.

[0164] Further experiments showed that during the soot removal operation, for the cerium composition according to Example 4, about 0.8 g of ash was generated per g of cerium, while for the composition according to Comparative Example 1, about 1.4 g of ash was generated per g of metal; and for the cerium composition according to Example 5, about 0.8 g of ash was generated per g of metal, while for the composition according to Comparative Example 2, about 1.1 g of ash was generated per g of metal.

Claims

1. A cerium composition for use as a soot reduction catalyst, the cerium composition comprising a long-chain cerium (III) carboxylate in an organic solvent, wherein the long-chain carboxylate has the general formula R L COO - , where R L It is a C6 to C24 alkyl group. 2 . The cerium composition according to claim 1 , comprising cerium (III) in an amount of 1% to 20% by weight, preferably 5% to 15% by weight, relative to the total weight of the composition.

3. The cerium composition according to claim 1 or 2, comprising: i. A long-chain cerium (III) carboxylate, wherein the long-chain carboxylate has the general formula R L COO - , where R L is C6 to C24 alkyl; ii. Optionally a cerium (III) carboxylate, wherein the carboxylate has the general formula RCOO - , wherein R is H or C1 to C4 alkyl; iii. a long chain carboxylic acid, wherein the long chain carboxylic acid is a conjugate acid of the long chain carboxylate; and iv. Organic solvents.

4. The cerium composition according to claim 3, comprising: i. a long-chain cerium (III) carboxylate in an amount of 20% to 55% by weight relative to the total weight of the composition; ii. cerium (III) carboxylate in an amount of 0.1 wt % to 10 wt % relative to the total weight of the composition; iii. a long chain carboxylic acid in an amount of 1 wt % to 30 wt % relative to the total weight of the composition; and iv. an organic solvent in an amount of 5 wt % to 78.9 wt % relative to the total weight of the composition.

5. The cerium composition according to claim 4, comprising: i. a long-chain cerium (III) carboxylate in an amount of 40% to 45% by weight relative to the total weight of the composition; ii. cerium (III) carboxylate in an amount of 1 wt % to 3 wt % relative to the total weight of the composition; iii. a long chain carboxylic acid in an amount of 2% to 30% by weight relative to the total weight of the composition; and iv. an organic solvent in an amount of 22 to 57 wt % relative to the total weight of the composition. 6 . The cerium composition according to claim 3 , wherein the long-chain carboxylate radical and the long-chain carboxylic acid are respectively composed of a mixture of two or more long-chain carboxylates and long-chain carboxylic acids.

7. The cerium composition according to any one of claims 3 to 6, wherein the molar ratio of the long-chain carboxylic acid to the long-chain carboxylic acid cerium (III) is between 0.1 and 5.

0.

8. The cerium composition according to any one of claims 3 to 7, wherein the carboxylate RCOO - Selected from: formate, acetate and propionate. 9 . The cerium composition according to claim 1 , wherein the organic solvent is a hydrocarbon solvent comprising a C10-C13 alkane.

10. The cerium composition according to any one of claims 1 to 8, wherein the organic solvent is a C6-C10 aliphatic monohydric alcohol ether.

11. The cerium composition according to any one of claims 1 to 8, wherein the organic solvent comprises one or more bio-based and / or bio-derived, saturated and / or unsaturated C12-C30 esters.

12. A method for preparing a cerium composition, the method comprising the following steps: Step a) making a compound having the general formula R L COO - A long-chain carboxylic acid is contacted with a cerium (III) compound under a non-oxidizing atmosphere, wherein R L is a C6 to C24 alkyl group, wherein the cerium (III) compound is selected from cerium (III) carbonate, cerium (III) hydroxycarbonate, cerium (III) hydroxide, cerium (III) oxyhydroxide, and / or cerium (III) oxide, and / or hydrates thereof, thereby obtaining a long-chain cerium (III) carboxylate; and Step b) An organic solvent is added to the product obtained in step a).

13. The method according to claim 12, wherein the long-chain carboxylic acid is contacted with the cerium (III) compound in the presence of an organic acid having the general formula RCOOH and / or its hydrate and / or anhydride under a non-oxidizing atmosphere, wherein R is H or a C1 to C4 alkyl group.

14. The method according to claim 12 or 13, wherein the long-chain carboxylic acid is provided in a stoichiometric excess relative to the amount of the cerium (III) compound.

15. The method according to any one of claims 12 to 14, wherein the long chain carboxylic acid is contacted with the cerium (III) compound at a temperature between 60°C and 180°C.

16. The method according to any one of claims 12 to 15, wherein the long-chain carboxylic acid is contacted with the cerium (III) compound in the presence of the organic acid.

17. The process according to any one of claims 12 to 16, wherein the organic solvent is added to the product obtained in step a) at a temperature between 100°C and 200°C.

18. The process according to any one of claims 12 to 17, wherein the product obtained in step a) is filtered, and wherein the organic solvent is added to the filtrate.

19. A method for reducing particulate emissions from a diesel engine, the method comprising the steps of: A diesel engine is operated using a fuel composition comprising a fuel, a long-chain cerium (III) carboxylate in an organic solvent, wherein the long-chain carboxylate has the general formula R L COO - , where R L is C6 to C24 alkyl; passing exhaust gas produced by combustion of the fuel and containing cerium oxide released from the fuel by combustion through a diesel particulate filter to collect particulate matter in the diesel particulate filter; as well as The diesel particulate filter is regenerated by increasing the temperature to a temperature between 350°C and 600°C.

20. The method of claim 19, wherein the method comprises the step of operating a diesel engine with a fuel composition comprising: a fuel; a long-chain cerium (III) carboxylate, wherein the long-chain carboxylate has the general formula R L COO - , where R L is a C6 to C24 alkyl group; optionally a long chain carboxylic acid having the general formula R L COOH; optionally a cerium (III) carboxylate, wherein the carboxylate has the general formula RCOO - , wherein R is H or a C1 to C4 alkyl group; and an organic solvent.

21. A method according to claim 19 or 20, wherein the diesel particulate filter is regenerated by increasing the temperature to a temperature between 350°C and 500°C.

22. Use of a cerium composition according to any one of claims 1 to 11 as a soot reduction catalyst composition and / or for regenerating a diesel particulate filter.

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