Fuel-based catalyst composition for removing acidified coal

Abstract

The present invention provides a fuel-based catalyst composition for removing oxidized coal containing Ce(III) long-chain carboxylic acid in an organic solvent. A preferred embodiment is a cerium composition for use as a soot reduction catalyst system, which comprises Ce(III) neodecanoate and a carboxylic acid Ce(III) having the general formula RCOO - [wherein R is H or C1-C4 alkyl], Ce(III) neodecanoate, and an organic solvent. A cerium composition is provided.

Description

Technical Field

[0001] The present invention relates to a fuel-based catalyst composition for removing oxidized coal. The object of the present invention is to reduce the emission of fine particles from a diesel engine and improve the function of a diesel particulate filter (DPF).

Background Art

[0002] A diesel engine is an internal combustion engine in which the ignition of fuel is caused by the increase in the temperature of air in a cylinder due to mechanical compression. Diesel engines typically have low exhaust levels of carbon monoxide and hydrocarbons, but the exhaust gas contains certain levels of particulate matter or soot. A diesel particulate filter (DPF) can reduce the amount of soot from the exhaust gas of a diesel engine. The fine particles (soot) are collected on the filter, and the filter is regenerated actively or passively to burn the soot. Considering energy considerations, durability, and system design, an ideal particulate removal unit needs to minimize the regeneration temperature of the soot filter. For this purpose, a soot reduction catalyst, also called a fuel-based catalyst (FBC), has been developed.

[0003] U.S. Patent Application Publication No. 2009 / 004078 discloses a diesel soot filter and method using a catalyst. The diesel soot filter incorporates a porous filter element coated with a catalyst agent. When diesel exhaust gas passes through the porous filter element, the diesel soot from the diesel exhaust gas comes into contact with the catalyst agent and deposits, and the ignition temperature or oxidation temperature of the deposited diesel soot is reduced. The catalyst agent is a mixture of an alkali metal and cerium oxide.

[0004] U.S. Patent Application Publication No. 2007 / 283681 discloses a method for reducing particulate emissions from a diesel engine, which includes operating a diesel engine with a fuel containing a fuel system catalyst comprising a fuel-soluble or dispersible cerium composition and a fuel-soluble or dispersible platinum group metal composition. In this method, a fuel-soluble multi-metal catalyst is used, i.e., a fuel system 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 used at a concentration effective to provide 0.5 to 20 ppm of cerium. The platinum group metal composition is preferably used at a concentration effective to provide 0.0005 to 2 ppm of platinum.

Prior Art Documents

Patent Documents

[0005]

Patent Document 1

Patent Document 2

Summary of the Invention

Problems to be Solved by the Invention

[0006] The present invention provides a solution to at least one of the above problems by providing a fuel system catalyst composition for removing soot, as set forth in claim 1. As a result, it has been shown that the use of the cerium composition enables efficient soot removal and regeneration of a diesel particulate filter.

Means for Solving the Problems

[0007] The present invention further provides a process for preparing a composition according to the general concept of the present invention, a method for operating a diesel engine in which a composition according to the general concept of the present invention is used, and the use of a composition according to the general concept of the present invention for the purpose of soot removal in a diesel particulate filter. [Brief description of the drawings]

[0008] For further guidance and to better understand the teachings of the present invention, the drawings are included, which are intended to aid in the explanation of the invention and are not intended to limit the invention disclosed herein.

[0009] The figures and symbols contained therein have meanings commonly understood by one of ordinary skill in the art to which this invention pertains.

Figure 1

Figure 2

[0010] Unless otherwise defined, all terms used in disclosing the present invention, including technical and scientific terms, have the meanings commonly understood by one of ordinary skill in the art to which this invention belongs. By way of further guidance, definitions of terms are included to better understand the teachings of the present invention.

[0011] As used herein, the following terms have the following meanings: As used herein, "a," "an," and "the" refer to both singular and plural referents unless the context clearly dictates otherwise. By way of example, "a compartment" refers to one or more than one compartment.

[0012] As used herein, "about", when referring to a measurable value such as a parameter, amount, duration, etc., means a variation of ±20% or less, preferably ±10% or less, more preferably ±5% or less, even more preferably ±1% or less, still more preferably ±0.1% or less from the specified value, as long as such variation is appropriate for the practice of the disclosed invention. It should be understood, however, that the value itself to which the modifier "about" refers is also specifically disclosed.

[0013] As used herein, "comprise", "comprising", "comprises", and "comprised of" are synonymous with "include", "including", "includes", or "contain", "containing", "contains", and are inclusive or open-ended terms, specifying the presence of what follows, e.g., elements, and not excluding or precluding the presence of additional, unrecited elements, features, elements, members, steps known in the art or disclosed herein.

[0014] The recitation of numerical ranges by endpoints includes all numbers and fractions subsumed within that range, as well as the recited endpoints. All percentages are understood as weight percentages abbreviated as "wt%", or volume percentages abbreviated as "vol%", unless otherwise defined or unless it is clear from the use and the context in which they are used that a different meaning is intended to a person skilled in the art.

[0015] Accordingly, the term "fuel" is intended to include all fuels effective for operating a diesel engine. The fuel may optionally contain detergents (e.g., 50 - 300 ppm), lubricity additives (e.g., 25 - about 500 ppm), and other additives. Among the fuels suitable for use in the present invention are those typically containing fossil fuels, such as any of the typical petroleum-derived fuels including distillate fuels. The fuel may be a distillate fuel (diesel fuel, e.g., No. 2 diesel fuel, No. 1 diesel fuel, jet fuel, e.g., Jet A, or a similar substance with boiling point and viscosity similar to No. 1 diesel fuel, including ultra-low sulfur diesel fuel (ULSD)); a liquid fuel containing hydrocarbons derived from gaseous or solid fuels; and a fuel of biological origin, such as those containing "monoalkyl ester-based oxygenated fuels", i.e., fatty acid esters, preferably triglycerides, such as methyl or ethyl esters of fatty acids derived from soybean oil, canola oil, and / or tallow, or a blend of one or more fuels selected from the group consisting of "Gas-to-Liquids" fuels derived from biomass, natural gas, coal, or petroleum sources. The term "hydrocarbon fuel" includes all fuels prepared from "distillate fuel" or "petroleum". This includes gasoline, jet fuel, diesel fuel, and various other distillate fuels. The term "distillate fuel" means all products prepared by the distillation of petroleum or petroleum fractions and residues. The term "petroleum" in its ordinary meaning means all materials, including hydrocarbon materials recovered from fossil fuels (regardless of viscosity), and including all materials related to the sources typically included in the meaning of this term.

[0016] Jet A and Diesel No. 1 are considered equivalent for the purposes of the present 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 Oils". Jet A has the designation of ASTM D 1655, "Standard Specification for Aviation Turbine Fuels". The term ultra-low sulfur diesel fuel (ULSD) means No. 1 or No. 2 diesel fuel with a sulfur content of 0.0015 wt% (15 ppm) or less. In some jurisdictions, a low aromatic hydrocarbon content (e.g., less than 10 percent by volume) is required.

[0017] The term "diesel fuel" means "distillate fuel" and includes diesel fuel or other fuels that meet the ASTM definition of diesel fuel, but is not composed of distillates only and may include alcohols, ethers, organic nitro compounds, etc. (e.g., methanol, ethanol, diethyl ether, methyl ethyl ether, nitromethane). Also, emulsions and liquid fuels derived from vegetable or mineral sources such as corn, alfalfa, shale, and coal are within the scope of the present invention. These fuels may also contain other additives known to those skilled in the art, including dyes, cetane improvers, antioxidants such as 2,6-di-tert-butyl-4-methylphenol, corrosion inhibitors, rust inhibitors such as alkylated succinic acids and anhydrides, bactericides, gum inhibitors, metal deactivators, upper cylinder lubricants, anti-icing agents, etc.

[0018] The method of operating a diesel engine according to the present invention uses a cerium catalyst, i.e., a fuel-based catalyst (FBC) containing a preferably fuel-soluble or fuel-dispersible cerium composition. The cerium composition is used at a concentration effective to provide preferably 0.5 to 150 ppm of cerium, more preferably 1 to 100 ppm of cerium, and still more preferably 5 to 50 ppm of cerium. The method can further use a platinum group metal composition at a concentration effective to provide 0.0005 to 2 ppm of platinum. In some embodiments, the treatment regimen can 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 the low level of catalyst is the reduction of ultrafine particles resulting from the emission of carbonaceous soot and metal oxides.

[0019] The cerium composition according to the general inventive concept of the present invention may include one or more chemical enhancers such as those described in U.S. Patent Application Publication No. 2007 / 283681 (but not limited thereto).

[0020] According to the general inventive concept of the present invention, the present invention provides a cerium composition containing Ce(III) long-chain carboxylic acid in an organic solvent. Preferred compositions comprise a Ce(III) content of 1 to 20 wt%, preferably 2 to 18 wt%, more preferably 3 to 16 wt%, still more preferably 5 to 15 wt%, most preferably 6 wt%, 8 wt%, 10 wt%, 12 wt%, 14 wt%, or any value therebetween, based on the total weight of the composition.

[0021] In a preferred embodiment, the general inventive concept of the present invention A. Ce(III) long-chain carboxylic acid, B. long-chain carboxylic acid, and C. an organic solvent, and provides a cerium composition wherein the long-chain carboxylate is the conjugate base of the long-chain carboxylic acid. In a preferred embodiment, the cerium composition also includes Ce(III) short-chain carboxylic acid.

[0022] ​In a preferred embodiment, the present invention provides a cerium composition according to the general inventive concept of the present invention, wherein the cerium(III) long-chain carboxylic acid is a cerium(III) carboxylic acid having a carboxylate group with 6 to 24 carbon atoms, and the cerium(III) short-chain carboxylic acid is a cerium(III) carboxylic acid having a carboxylate group with 1 to 5 carbon atoms. Preferably, the cerium(III) long-chain carboxylic acid is a cerium(III) carboxylic acid having a carboxylate group with 9 to 20 carbon atoms, more preferably 10 to 16 carbon atoms, and the cerium(III) short-chain carboxylic acid is a cerium(III) carboxylic acid having a carboxylate group with 2 to 4 carbon atoms. In some embodiments, the cerium(III) long-chain carboxylic acid can be configured as a mixture of two or more cerium(III) long-chain carboxylic acids. In some embodiments, the long-chain carboxylate is selected from the group comprising saturated carboxylates such as alkyl carboxylates, cycloalkyl carboxylates, and unsaturated carboxylates. The long-chain carboxylate group can include an aliphatic group, an alicyclic group, an aryl group, and an alkylaryl group. Preferably, the cerium(III) long-chain carboxylic acid is composed of an unsaturated carboxylate. The selected cerium(III) long-chain carboxylic acid compounds are cerium(III) naphthenate, cerium(III) octanoate, cerium(III) 2-ethylhexanoate, 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 cerium(III) short-chain carboxylic acid compounds are cerium(III) formate, cerium(III) propionate, and cerium(III) acetylacetonate. Alternatively, cerium(III) acetate can be used. In some embodiments, the cerium(III) short-chain carboxylic acid can be configured as a mixture of two or more cerium(III) short-chain carboxylic acids. 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.

[0023] In a preferred embodiment, in the present invention, the long-chain carboxylic acid Ce(III) is Ce(III) neodecanoate; the short-chain carboxylic acid Ce(III) is a carboxylic acid Ce(III) having the general formula RCOO - [wherein, R is H or C1 - C4 alkyl], and the present invention provides a cerium composition according to the general inventive concept of the present invention, wherein the long-chain carboxylic acid is neodecanoic acid.

[0024] In a preferred embodiment, in the present invention, the long-chain carboxylic acid Ce(III) is present in an amount of 20 - 55% by weight, preferably 30 - 50% by weight, more preferably 40 - 45% by weight, based on the total weight of the composition, and the present invention provides a cerium composition according to the general inventive concept of the present invention. Most preferably, the long-chain carboxylic acid Ce(III) is present in an amount of about 41% by weight, 43% by weight or 45% by weight, or any amount therebetween.

[0025] In a preferred embodiment, in the present invention, the short-chain carboxylic acid Ce(III) is present in an amount of 0.1 - 10% by weight, preferably 0.5 - 5% by weight, more preferably 1 - 3% by weight, based on the total weight of the composition, and the present invention provides a cerium composition according to the general inventive concept of the present invention. Most preferably, the short-chain carboxylic acid Ce(III) is present in an amount of about 1% by weight, 2% by weight or 3% by weight, or any amount therebetween.

[0026] In a preferred embodiment, in the present invention, the long-chain carboxylic acid is present in an amount of 1 - 30% by weight, preferably 2 - 30% by weight, more preferably 2 - 20% by weight, based on the total weight of the composition, and the present invention provides a cerium composition according to the general inventive concept of the present invention. Most preferably, the long-chain carboxylic acid is present in an amount of about 2% by weight, 4% by weight, 6% by weight, 8% by weight, or 10% by weight, or any amount therebetween.

[0027] In a preferred embodiment, the present invention provides a cerium composition according to the general inventive concept of the present invention, further comprising an organic solvent. Preferably, the organic solvent is present in an amount of 5 to 78.9% by weight, preferably 15 to 67.5% by weight, more preferably 22 to 57% by weight. Most preferably, the organic solvent is present in an amount of about 25% by weight, 30% by weight, 35% by weight, 40% by weight, or 45% by weight, or any amount therebetween.

[0028] In a first aspect, the present invention is a cerium composition for use as a soot reduction catalyst system, i. Ce(III) neodecanoate, ii. neodecanoic acid, and iii. an organic solvent, and provides a cerium composition.

[0029] In a preferred embodiment, the cerium composition also contains a short-chain carboxylic acid Ce(III) having the general formula RCOO - [wherein, R is H or C1-C4 alkyl]. 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 diesel engines. As a result, it has been shown that the use of the cerium composition enables efficient soot removal and regeneration of diesel particulate filters. Specifically, the cerium composition according to the present invention enables (i) reducing the dosage of the cerium composition in the fuel while generating the same soot activity as compared to the compositions of the prior art, (ii) improving the efficiency of catalytic oxidation by improving the soot conversion rate and exhibiting excellent performance, (iii) regenerating the diesel particulate filter at a relatively low temperature, i.e., 450 °C instead of 600 °C in the absence of a fuel-based catalyst, and (iv) being able to reduce the formation of ash.

[0030] Furthermore, secondary advantages such as a reduction in the time required to reach the regeneration temperature can be obtained, and depending on the dosage of the cerium composition, the regeneration time can be shortened to less than 7 minutes, and even less than 4 minutes. Soot can be removed instantaneously, and a high soot removal efficiency can be obtained. By completely burning the accumulated soot particles, the life of the diesel particulate filter can be extended. Active regeneration can be achieved within 4 minutes at a relatively low temperature of 450°C. Good dispersion of cerium in the soot particles enables high catalytic oxidation.

[0031] The organic solvent further enables good compatibility between the cerium composition and the fuel. The cerium composition forms a stable and homogeneous mixture in the fuel.

[0032] In a preferred embodiment, the present invention provides a cerium composition according to the first aspect of the present invention, i. Ce(III) neodecanoate in an amount of 20 to 55% by weight based on the total weight of the composition, ii. neodecanoic acid in an amount of 1 to 30% by weight based on the total weight of the composition, and iii. an organic solvent in an amount of 15 to 79% by weight based on the total weight of the composition.

[0033] Preferably, the composition comprises i. Ce(III) neodecanoate in an amount of 20 to 55% by weight based on the total weight of the composition, ii. Ce(III) carboxylic acid having the general formula RCOO - [wherein R is H or C1 - C4 alkyl] in an amount of 0.1 to 10% by weight based on the total weight of the composition, iii. neodecanoic acid in an amount of 1 to 30% by weight based on the total weight of the composition, and iv. an organic solvent in an amount of 5 to 78.9% by weight based on the total weight of the composition.

[0034] More preferably, the present invention provides a cerium composition according to the first aspect of the present invention, i. Ce(III) neodecanoate in an amount of 30 to 50% by weight based on the total weight of the composition, ii. neodecanoic acid in an amount of 2 to 30% by weight based on the total weight of the composition, iii. an organic solvent in an amount of 20 to 68% by weight based on the total weight of the composition, to provide a cerium composition.

[0035] Preferably, the cerium composition i. cerium(III) neodecanoate in an amount of 30 to 50% by weight based on the total weight of the composition, ii. preferably, a carboxylic acid cerium(III) having the general formula RCOO - [wherein, R is H or C1 - C4 alkyl] in an amount of 0.5 to 5% by weight based on the total weight of the composition, iii. neodecanoic acid in an amount of 2 to 30% by weight based on the total weight of the composition, and iv. an organic solvent in an amount of 15 to 67.5% by weight based on the total weight of the composition.

[0036] Even more preferably, the present invention provides a cerium composition according to the first aspect of the present invention, i. cerium(III) neodecanoate in an amount of 40 to 45% by weight based on the total weight of the composition, ii. neodecanoic acid in an amount of 2 to 30% by weight based on the total weight of the composition, iii. an organic solvent in an amount of 25 to 58% by weight based on the total weight of the composition.

[0037] Preferably, the cerium composition i. cerium(III) neodecanoate in an amount of 40 to 45% by weight based on the total weight of the composition, ii. a carboxylic acid cerium(III) having the general formula RCOO - [wherein, R is H or C1 - C4 alkyl] in an amount of 1 to 3% by weight based on the total weight of the composition, iii. neodecanoic acid in an amount of 2 to 30% by weight based on the total weight of the composition, and iv. an organic solvent in an amount of 22 to 57% by weight based on the total weight of the composition.

[0038] 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 Ce(III) neodecanoate is from 0.1 to 5.0. Preferably, the molar ratio is from 0.5 to 3.0, more preferably from 1 to 3, and the ratio is about 1.6, 1.8, 2.0, 2.2, 2.4, 2.6 or 2.8, or any value therebetween. The excess neodecanoic acid may be neutralized or partially neutralized.

[0039] 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 has shown improved reactivity with a Ce(III) precursor such as Ce(III) carbonate.

[0040] 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 containing C10 - C13 alkanes.

[0041] 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 monoalcohol ether.

[0042] 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 containing C10 - C13 alkanes and a C6 - C10 aliphatic monoalcohol ether.

[0043] 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 containing C9 - C10 alkanes. Preferably, the hydrocarbon solvent is present in an amount of at least 30% by weight, more preferably at least 40% by weight, and most preferably about 50% by weight, based on the total weight of the organic solvent. The hydrocarbon solvent may include n-alkanes, isoalkanes, and cycloalkanes. The hydrocarbon solvent preferably has the CAS number: 64742 - 48 - 9 and preferably contains less than 2% aromatics.

[0044] 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 containing C10 - C13 alkanes. Preferably, the hydrocarbon solvent is present in an amount of at least 30% by weight, more preferably at least 40% by weight, and most preferably about 50% by weight, based on the total weight of the organic solvent. The hydrocarbon solvent may include paraffins, isoparaffins, and cycloparaffins. The hydrocarbon solvent preferably has the CAS number: 64742 - 48 - 9 and preferably contains less than 2% aromatics.

[0045] In a preferred embodiment, the present invention provides a cerium composition according to the first aspect of the present invention, wherein the organic solvent contains a mixture of C9 - C10 alkanes and C10 - C13 alkanes.

[0046] Preferably, the present invention provides a cerium composition according to the first aspect of the present invention, wherein the organic solvent contains a C6 - C10 aliphatic monoalcohol ether. Preferably, the C6 - C10 aliphatic monoalcohol ether is present in an amount of at least 30% by weight, more preferably at least 40% by weight, and most preferably about 50% by weight, based on the total weight of the organic solvent. Preferably, the organic solvent includes a C1 - C6 alkyl ether of diethylene glycol or dipropylene glycol, more preferably a C1 - C4 alkyl ether of diethylene glycol or dipropylene glycol.

[0047] 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, the hydrocarbon solvent is composed in an amount of 30 wt% - 70 wt% based on the total weight of the organic solvent, and the aliphatic monoalcohol ether is composed in an amount of 70 wt% - 30 wt% based on the total weight of the organic solvent, respectively. More preferably, the hydrocarbon solvent is composed in an amount of 40 wt% - 60 wt%, and the aliphatic monoalcohol ether is composed in an amount of 60 wt% - 40 wt%, respectively. Most preferably, the hydrocarbon solvent is composed in an amount of about 50 wt%, and the aliphatic monoalcohol ether is composed in an amount of about 50 wt%.

[0048] Preferably, the present invention provides a cerium composition according to the first aspect of the present invention, wherein the organic solvent contains one or more saturated and / or unsaturated C5 - C11 esters. A preferred ester can be ethyl lactate.

[0049] 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 saturated and / or unsaturated C12-C30 esters of biological and / or biogenic origin. Preferably, the unsaturated C12-C30 ester is present in an amount of at least 80% by weight, more preferably at least 90% by weight, even more preferably at least 98% by weight, based on the total weight of the organic solvent. In a first preferred embodiment, the unsaturated C12-C30 ester is an ester derived from fatty acids such as rapeseed methyl ester or soybean 2-ethylhexyl ester. Rapeseed methyl ester (RME) is a mixture of methyl esters composed of saturated and unsaturated C16-C22 fatty acids. Technically, rapeseed methyl ester is produced by chemical conversion of rapeseed oil using methanol. In a second preferred embodiment, the unsaturated C12-C30 ester is soybean 2-ethylhexyl ester (also referred to as soybean 2-ethylhexyl ester). The unsaturated C12-C30 ester may be composed as a mixture of two or more ester products.

[0050] 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-alkylpyrrolidone, more preferably C4 N-alkylpyrrolidone. Preferably, the C1-C6 N-alkylpyrrolidone is present in an amount of at least 80% by weight, more preferably at least 90% by weight, even more preferably at least 98% by weight, based on the total weight of the organic solvent. Preferably, the C1-C6 N-alkylpyrrolidone is C4 N-alkylpyrrolidone.

[0051] In a second aspect of the general inventive concept of the present invention, the present invention is a method for preparing a cerium composition, comprising Step a) contacting a long-chain carboxylic acid, preferably in the presence of a short-chain carboxylic acid and / or its hydrate and / or anhydride, with a Ce(III) compound in a non-oxidizing atmosphere, wherein the Ce(III) compound is selected from the group consisting of cerium(III) carbonate, cerium(III) hydroxycarbonate, cerium(III) hydroxide, cerium(III) oxyhydroxide, and / or cerium(III) oxide, and the long-chain carboxylic acid is provided in a stoichiometric excess relative to the amount of the Ce(III) compound, whereby a mixture of cerium(III) long-chain carboxylate and cerium(III) short-chain carboxylate in the long-chain carboxylic acid is obtained, and Step b) adding an organic solvent to the mixture obtained in step a). A method is provided that includes these steps.

[0052] The Ce(III) compound provided in step a) may be provided as it is and / or may contain its hydrate. Preferably, the long-chain carboxylate and the long-chain carboxylic acid are carboxylic acids having 6 to 24 carbon atoms, preferably 9 to 20 carbon atoms, more preferably 10 to 16 carbon atoms. In some embodiments, the long-chain carboxylic acid may be composed of a mixture of two or more long-chain carboxylic acids. In some embodiments, the carboxylic acid is selected from the group including saturated carboxylic acids such as alkyl and cycloalkyl acids, and unsaturated carboxylic acids. The carboxylic acid may contain an aliphatic group, an alicyclic group, an aryl group, and an alkylaryl group. Preferably, the long-chain carboxylic acid is composed of an unsaturated carboxylic acid. The selected long-chain carboxylic acids are naphthenic 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 composed of a hydrate or an 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 may be composed of a mixture of two or more short-chain carboxylic acids. The organic solvent may be a blend of two or more organic solvents.

[0053] The inventors attempted to prepare Ce(III) long-chain carboxylate in the absence of short-chain carboxylic acid and found that complete conversion of the starting product Ce(III) could not be achieved and a clear solution could not be obtained. Therefore, the presence of short-chain carboxylic acid improves the reaction and the purification of the reaction product.

[0054] In a preferred embodiment, the present invention is a method for preparing a cerium composition according to the general inventive concept of the present invention, wherein the long-chain carboxylic acid is neodecanoic acid; the short-chain carboxylic acid is a carboxylic acid having the general formula RCOOH [wherein R is H or C1-C4 alkyl]; the long-chain carboxylic acid Ce(III) is neodecanoic acid Ce(III); and the short-chain carboxylic acid Ce(III) has the general formula RCOO - [wherein R is H or C1-C4 alkyl].

[0055] In a second aspect, the present invention is a method for preparing a cerium composition, comprising Step a): contacting neodecanoic acid with a Ce(III) compound in a non-oxidizing atmosphere in the presence of an organic acid having the general formula RCOOH [wherein R is H or C1-C4 alkyl], and / or its hydrate and / or anhydride, wherein the Ce(III) compound is selected from the group consisting of cerium(III) carbonate, cerium(III) hydroxycarbonate, cerium(III) hydroxide, cerium(III) oxyhydroxide, and / or cerium(III) oxide, and the neodecanoic acid is provided in a stoichiometric excess relative to the amount of the Ce(III) compound, thereby obtaining a mixture of cerium(III) neodecanoate and cerium(III) carboxylate in the neodecanoic acid, and Step b): adding an organic solvent to the mixture obtained in step a).

[0056] The inventors have found that when a stoichiometric excess of neodecanoic acid is used, the conversion of a Ce(III) compound to neodecanoic acid Ce(III) proceeds more readily, and the excess neodecanoic acid does not interfere with the effect of a fuel-based catalyst composition for use in reducing soot by a catalyst, while no significant adverse effects are observed. The inventors have also discovered that the use of a carboxylic acid having 1 to 5 carbon atoms facilitates the conversion of the Ce(III) compound. The short-chain carboxylic acid is presumed to improve the solubility of the Ce(III) compound in the reaction mixture. The inventors have also found that it is preferable to add an organic solvent after contacting the long-chain carboxylic acid with the Ce(III) compound in the presence of the short-chain carboxylic acid.

[0057] 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 (e.g., NaOH or KOH).

[0058] In a preferred embodiment, the Ce(III) compound is selected from the group consisting of Ce(III) carbonate, Ce(III) hydroxycarbonate, Ce(III) hydroxide, Ce(III) oxyhydroxide, and / or Ce(III) oxide, and more preferably is selected from the group consisting of Ce(III) carbonate, Ce(III) hydroxycarbonate, and / or their hydrates.

[0059] In a preferred embodiment, the organic acid is selected from the group consisting of 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. A combination of two or more organic acids can be advantageously used.

[0060] In a preferred embodiment, the present invention provides a method according to a second aspect of the present invention, wherein the neodecanoic acid is contacted with the Ce(III) compound at a temperature of 60°C to 180°C in the presence of the organic acid. More preferably, the neodecanoic acid is contacted with the Ce(III) compound at a temperature of 80°C to 120°C, more preferably 90°C to 100°C, in the presence of the organic acid. Preferably, the neodecanoic acid is contacted with the Ce(III) compound with vigorous stirring.

[0061] In a preferred embodiment, the present invention provides a method according to a second aspect of the present invention, wherein the organic solvent is added to the mixture obtained in step a) at a temperature of 100°C to 200°C. More preferably, the organic solvent is added to the mixture obtained in step a) at a temperature of 120°C to 160°C, more preferably 130°C to 150°C. Preferably, the organic solvent is added with vigorous stirring.

[0062] In a preferred embodiment, the present invention provides a method according to a second aspect of the present invention, wherein the mixture obtained in step a) is filtered, and an organic solvent is further added to the filtrate. The solvent is added to obtain Ce at a predetermined concentration.

[0063] In a preferred embodiment, the present invention provides a method according to a second aspect of the present invention for preparing a cerium composition according to the first aspect of the present invention.

[0064] In a third aspect, the present invention provides a method for reducing particulate emissions from a diesel engine, wherein a fuel composition containing fuel, neodecanoic acid Ce(III), and a carboxylic acid Ce(III) having the general formula RCOO - [wherein R is H or C1-C4 alkyl] is supplied to the diesel engine.

[0065] More specifically, the method according to the third aspect of the present invention is a method for reducing particulate emissions from a diesel engine, comprising the steps of operating a diesel engine with a fuel containing a fuel system catalyst containing a fuel-soluble or fuel-dispersible cerium composition, passing exhaust containing cerium oxide generated by combustion of the fuel and 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 raising the temperature to a temperature of 300°C to 700°C, more preferably a temperature of 350°C to 650°C, even more preferably a temperature of 400°C to 600°C, most preferably 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 of 400°C to 500°C. Preferably, the cerium composition further contains neodecanoic acid. Preferably, the cerium composition further contains an organic solvent. More preferably, the cerium composition is a fuel system 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 contains neodecanoic acid.

[0066] In a fourth aspect, the present invention provides the use of a cerium composition according to the first aspect of the present invention as a soot reduction catalyst composition.

[0067] In a particularly preferred embodiment, the present invention provides the following: A cerium composition for use as a soot reduction catalyst system, i. Ce(III) neodecanoate, ii. A carboxylic acid Ce(III) having the general formula RCOO - [wherein R is H or C1-C4 alkyl], iii. Neodecanoic acid, and iv. An organic solvent,

[0068] More specifically, it is the aforementioned cerium composition, i. Cerium(III) neodecanoate in an amount of 20 to 55% by weight based on the total weight of the composition, ii. Cerium(III) carboxylic acid having the general formula RCOO - [wherein, R is H or C1-C4 alkyl] in an amount of 0.1 to 10% by weight based on the total weight of the composition, iii. Neodecanoic acid in an amount of 1 to 30% by weight based on the total weight of the composition, and iv. An organic solvent in an amount of 5 to 78.9% by weight based on the total weight of the composition, a cerium composition.

[0069] More specifically, it is the aforementioned cerium composition, i. Cerium(III) neodecanoate in an amount of 40 to 45% by weight based on the total weight of the composition, ii. Cerium(III) carboxylic acid having the general formula RCOO - [wherein, R is H or C1-C4 alkyl] in an amount of 1 to 3% by weight based on the total weight of the composition, iii. Neodecanoic acid in an amount of 2 to 30% by weight based on the total weight of the composition, and iv. An organic solvent in an amount of 22 to 57% by weight based on the total weight of the composition, a cerium composition.

[0070] More specifically, the aforementioned cerium composition wherein the molar ratio of neodecanoic acid to cerium(III) neodecanoate is 0.1 to 5.0.

[0071] More specifically, the aforementioned cerium composition wherein the carboxylate is selected from the group consisting of formate, acetate, and propionate.

[0072] More specifically, the aforementioned cerium composition wherein the organic solvent is a hydrocarbon solvent containing C10-C13 alkanes.

[0073] More specifically, the aforementioned cerium composition wherein the organic solvent is a C6-C10 aliphatic monoalcohol ether.

[0074] More specifically, the cerium composition in which the organic solvent contains one or more biological and / or bio-derived saturated and / or unsaturated C12-C30 esters.

[0075] A method for preparing a cerium composition, i. Neodecanoic acid is contacted with a Ce(III) compound in a non-oxidizing atmosphere in the presence of an organic acid having the general formula RCOOH [wherein R is H or C1-C4 alkyl], and / or its hydrate and / or anhydride, and the Ce(III) compound is selected from the group consisting of Ce(III) carbonate, Ce(III) hydroxycarbonate, Ce(III) hydroxide, Ce(III) oxyhydroxide, and / or Ce(III) oxide, and / or their hydrates, and the neodecanoic acid is provided in a stoichiometric excess relative to the amount of the Ce(III) compound, whereby a mixture of Ce(III) neodecanoate and Ce(III) carboxylate in neodecanoic acid is obtained, and, ii. A step of adding an organic solvent to the mixture obtained in step a). A method comprising this step.

[0076] More specifically, the above-described method in which the neodecanoic acid is contacted with the Ce(III) compound at a temperature of 60°C to 180°C in the presence of the organic acid.

[0077] More specifically, the above-described method in which the organic solvent is added to the mixture obtained in step a) at a temperature of 100°C to 200°C.

[0078] More specifically, the above-described method in which the mixture obtained in step a) is filtered and the organic solvent is added to the filtrate.

[0079] A method for reducing particulate emissions from a diesel engine, comprising a fuel, Ce(III) neodecanoate, and a general formula RCOO -A method comprising the steps of operating a diesel engine using a fuel composition comprising a cerium(III) carboxylate having [[R is H or C1-C4 alkyl]], neodecanoic acid, and an organic solvent; passing exhaust containing cerium oxide produced by combustion of the fuel and 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 raising the temperature to a temperature of 350°C to 600°C.

[0080] More specifically, the above-described method, wherein the diesel particulate filter is regenerated by raising the temperature to a temperature between 350°C and 500°C.

Examples

[0081] The following examples are intended to clarify the present invention and are not intended to limit the scope of the present invention.

[0082] Example 1 The reactor was flushed with nitrogen gas to create an inert atmosphere. 804 g of neodecanoic acid and 8.8 g of acetic acid (80% aqueous solution) were placed in the reactor, the contents of the reactor were stirred, and heated to 95°C. While maintaining the temperature at 95°C, 400 g of cerium(III) carbonate was gradually added to the reactor over 2.5 hours. Finally, 8.8 g of acetic acid (80% aqueous solution) 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 the cerium(III) carbonate was converted. Next, 348 mL of D60 was gradually added to the reactor over 6 hours at a temperature of 140°C under an inert atmosphere of nitrogen. D60 is an organic solvent mainly containing C10-C12 paraffins and naphthenes and having a very low aromatic content. Trace amounts of water can also be further removed by vacuum distillation. After cooling to about 100°C, the reaction mixture was filtered, and D60 was further added to the filtrate until the Ce content reached about 10% by weight. The resulting composition had a density of 1.0 g / mL.

[0083] Example 2 Using cerium(III) hydroxide as the cerium salt instead of cerium(III) carbonate, the procedure of Example 1 was repeated.

[0084] Example 3 Using formic acid instead of acetic acid, the procedure of Example 1 was repeated.

[0085] Example 4 The cerium composition obtained by the process according to Example 1 was introduced into the fuel at 0.2 g / L to produce 24 ppm of Ce. The soot removal tests are shown in FIGS. 1 and 2.

[0086] Example 5 The cerium composition obtained by the process according to Example 1 was introduced into the fuel at 1.0 g / L to produce 120 ppm of Ce. The soot removal tests are shown in FIGS. 1 and 2.

[0087] Example 6 The reactor was flushed with nitrogen gas to create an inert atmosphere. 803.4 g of neodecanoic acid and 8.6 g of propionic acid were placed into the reactor, the contents of the reactor were stirred, and heated to 95 °C. While maintaining the temperature at 95 °C, 400 g of cerium(III) carbonate was gradually added to the reactor over 1.5 hours. Finally, 8.6 g of propionic acid was added, and the reaction mixture was heated at 95 °C for 2 hours, followed by heating at 140 °C for 6 hours while distilling off water. Trace amounts of water can also be further removed by vacuum distillation. Next, 347 mL of D60 was gradually added to the reactor over 3 hours at a temperature of 140 °C under an inert nitrogen atmosphere. While distilling off water, the reaction mixture was held at 140 °C for an additional 6 hours. Trace amounts of water can also be further removed by vacuum distillation. After cooling to approximately 100 °C, the reaction mixture was filtered, and D60 was further added to the filtrate until the Ce content was approximately 10 wt%. The resulting composition has a density of 1.0 g / mL. More than 99% of the added cerium(III) carbonate was converted.

[0088] Example 7 The reactor was flushed with nitrogen gas to create an inert atmosphere. 803.5 g of neodecanoic acid was placed into the reactor, the contents of the reactor were stirred, and heated to 95 °C. While maintaining the temperature at 95 °C, 400 g of cerium(III) carbonate was gradually added to the reactor over 2.5 hours. While distilling water, the reaction mixture was heated at 95 °C for 2 hours and then at 140 °C for 4 hours. Trace amounts of water can also be further removed by vacuum distillation. Next, 346 mL of D60 was gradually added to the reactor over 2 hours at a temperature of 140 °C under an inert nitrogen atmosphere. While distilling water, the reaction mixture was held at 140 °C for an additional 6 hours. Trace amounts of water can also be further removed by vacuum distillation. After cooling to approximately 100 °C, the reaction mixture was filtered. The resulting filtrate had a Ce content of approximately 9.7 wt% and a density of ±1.0 g / mL. 81% of the added cerium(III) carbonate was converted.

[0089] Example 8 The reactor was flushed with nitrogen gas to create an inert atmosphere. 672.7 g of 2-ethylhexanoic acid and 8.8 g of acetic acid (80% aqueous solution) were placed into the reactor, the contents of the reactor were stirred, and heated to 95 °C. While maintaining the temperature at 95 °C, 400 g of cerium(III) carbonate was gradually added to the reactor over 2.5 hours. Finally, 8.8 g of acetic acid (80% aqueous solution) 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. Next, 430 mL of D60 was gradually added to the reactor over 2 hours at a temperature of 140 °C under an inert nitrogen atmosphere. While distilling water, the reaction mixture was held at 140 °C for an additional 6 hours. Trace amounts of water can also be further removed by vacuum distillation. After cooling to approximately 100 °C, 316 mL of D60 was further added. The resulting composition had 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.

[0090] Example 9 The reactor was flushed with nitrogen gas to create an inert atmosphere. 672.7 g of 2-ethylhexanoic acid was placed into the reactor, the contents of the reactor were stirred, and heated to 95 °C. While maintaining the temperature at 95 °C, 400 g of cerium(III) carbonate was gradually added to the reactor over 2.5 hours. 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. Next, 430 mL of D60 was gradually added to the reactor over 2 hours at a temperature of 140 °C under an inert nitrogen atmosphere. While distilling off water, the reaction mixture was held at 140 °C for an additional 6 hours. Trace amounts of water can also be further removed by vacuum distillation. An additional 290 mL of D60 was added and the reaction mixture was filtered. The resulting composition had a density of 0.97 g / mL. Less than 92 wt% of the cerium(III) carbonate was converted.

[0091] Example 10 The reactor was flushed with nitrogen gas to create an inert atmosphere. 758 g of Versatic™ Acid 913 and 8.8 g of acetic acid (80% aqueous solution) were placed into the reactor, the contents of the reactor were stirred, and heated to 95 °C. Versatic™ Acid 913 is a mixture of tertiary carboxylic acids having C6 - C13, with C9 being the main component. While maintaining the temperature at 95 °C, 400 g of cerium(III) carbonate was gradually added to the reactor over 2 hours. Finally, 8.8 g of acetic acid (80% aqueous solution) 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. Next, 348 mL of D60 was gradually added to the reactor over 1.5 hours at a temperature of 140 °C under an inert nitrogen atmosphere. After an additional 9 hours at 140 °C, the reaction mixture was cooled to approximately 100 °C and the reaction mixture was filtered off. A filtrate having a Ce content of approximately 9.7 wt% was obtained. More than 79% of the cerium(III) carbonate was converted.

[0092] Example 11 The reactor was flushed with nitrogen gas to create an inert atmosphere. 336.3 g of caprylic acid, 401.7 g of capric acid, and 8.8 g of acetic acid (80% aqueous solution). While maintaining the temperature at 95 °C, 400 g of cerium(III) carbonate was gradually added to the reactor over 1.5 hours. Finally, 8.8 g of acetic acid (80% aqueous solution) 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 off water. The residual water was removed by vacuum distillation. Next, 348 mL of D60 was gradually added to the reactor over 2 hours at a temperature of 140 °C under an inert atmosphere of nitrogen. After an additional 6.5 hours at 140 °C, 400 mL of D60 was added, and the reaction mixture was filtered. A filtrate having a Ce content of about 9.6 wt% was obtained and solidified upon cooling. More than 99% of the cerium(III) carbonate was converted.

[0093] Example 12 The reactor was flushed with nitrogen gas to create an inert atmosphere. 737.2 g of isononanoic acid and 8.8 g of acetic acid (80% aqueous solution). While maintaining the temperature at 95 °C, 400 g of cerium(III) carbonate was gradually added to the reactor over 2 hours. Finally, 8.8 g of acetic acid (80% aqueous solution) was added, and the reaction mixture was heated at 95 °C for 2 hours and then at 140 °C for 7 hours. The water was removed by vacuum distillation. Next, 430 mL of D60 was gradually added to the reactor over 1.5 hours at a temperature of 140 °C under an inert atmosphere of nitrogen. After an additional 6 hours at 140 °C, the reaction mixture was cooled to about 100 °C, 277 mL of D60 was further added, and the reaction mixture was filtered. A filtrate that solidified upon standing at room temperature was obtained with a Ce content of 9.77 wt%. More than 97% of the cerium(III) carbonate was converted. D60 was further added to the filtrate until a Ce content of about 9.5 wt% was achieved, which is the metal concentration at which the filtrate remains liquid at room temperature.

[0094] Comparative Example 1 Cerium dioxide nanoparticle material (8 - 10 nm) was introduced into the fuel at 0.35 g / L to produce 24 ppm of Ce. The soot removal test is shown in FIGS. 1 and 2.

[0095] Comparative Example 2 Cerium dioxide nanoparticle material (8 - 10 nm) was introduced into the fuel at 1.5 g / L to produce 120 ppm of Ce. The coal removal tests are shown in FIGS. 1 and 2.

[0096] Comparative Example 3 The coal removal catalyst system was not introduced. The coal removal tests are shown in FIGS. 1 and 2.

[0097] FIG. 1 shows the coal removal efficiency expressed as a percentage of the total amount of coal as a function of oxidation temperature. The results show that the coal reduction additive according to the present invention enables higher coal conversion at any temperature tested. FIG. 1 shows that the use of a Ce - based coal removal catalyst significantly improves the coal removal efficiency at any temperature. By increasing the loading amount of the coal removal catalyst composition, the coal removal effect is improved. Importantly, the cerium composition according to the present invention exhibits significantly improved coal removal activity, enabling high coal removal efficiency even at lower temperatures such as 450°C - 475°C or even at lower temperatures around 400°C - 425°C.

[0098] FIG. 2 shows the coal removal efficiency after 10 minutes at 575°C for the cerium composition according to the present invention, the cerium composition according to the prior art, and the composition without a coal removal catalyst, respectively. As a result, it was shown that the coal reduction additive according to the present invention ensures the formation of less ash compared to cerium dioxide nanoparticles. FIG. 2 shows that the cerium composition according to the present invention achieves high coal removal efficiency even with a low catalyst loading. All coal removal catalyst compositions exhibit performance superior to coal removal without a coal removal catalyst. Further experiments under the same conditions showed that in Example 4, a regeneration time of less than 7 minutes was achieved; in Example 5, a regeneration time of less than 4 minutes was achieved. Therefore, the composition of the present invention enables a higher coal conversion rate and an improved regeneration rate.

[0099] According to further experiments, during the coal removal operation, for the cerium composition according to Example 4, about 0.8 g of ash is generated per 1 g of cerium, while for the composition according to Comparative Example 1, about 1.4 g of ash is generated per 1 g of metal; and for the cerium composition according to Example 5, about 0.8 g of ash is generated per 1 g of metal, while for the composition according to Comparative Example 2, about 1.1 g of ash is generated per 1 g of metal.

Claims

1. General formula R Ｌ COO － [wherein, R Ｌ is C6-C24 alkyl] A cerium composition containing a long-chain carboxylic acid Ce(III) having the formula in an organic solvent and used as a soot reduction catalyst.

2. The cerium composition according to claim 1, comprising a Ce(III) content of 1 to 20% by weight, preferably 5 to 15% by weight, based on the total weight of the composition.

3. i. General formula R Ｌ COO － [wherein, R Ｌ is C6-C24 alkyl] long-chain carboxylic acid Ce(III), ii. Optionally, a cerium(III) carboxylic acid having the general formula RCOO － [wherein R is H or C1-C4 alkyl] iii. A long-chain carboxylic acid which is the conjugate acid of the long-chain carboxylate, and iv. An organic solvent, the cerium composition according to claim 1 or 2.

4. i. A long-chain carboxylic acid Ce(III) in an amount of 20 to 55% by weight based on the total weight of the composition, ii. A carboxylic acid Ce(III) in an amount of 0.1 to 10% by weight based on the total weight of the composition, iii. A long-chain carboxylic acid in an amount of 1 to 30% by weight based on the total weight of the composition, and iv. An organic solvent in an amount of 5 to 78.9% by weight based on the total weight of the composition, the cerium composition according to claim 3.

5. i. A long-chain carboxylic acid Ce(III) in an amount of 40 to 45% by weight based on the total weight of the composition, ii. A carboxylic acid Ce(III) in an amount of 1 to 3% by weight based on the total weight of the composition, iii. A long-chain carboxylic acid in an amount of 2 to 30% by weight based on the total weight of the composition, and iv. An organic solvent in an amount of 22 to 57% by weight based on the total weight of the composition, the cerium composition according to claim 4.

6. The cerium composition according to any one of claims 3 to 5, wherein the long-chain carboxylate and the long-chain carboxylic acid each consist 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 Ce(III) is 0.1 to 5.

0.

8. The carboxylate RCOO － The cerium composition according to any one of claims 3 to 7, wherein the carboxylate RCOO is selected from the group consisting of formate, acetate, and propionate.

9. The cerium composition according to any one of claims 1 to 8, wherein the organic solvent is a hydrocarbon solvent containing C10 - C13 alkanes.

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

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

12. A method for preparing a cerium composition, comprising Step a) A long-chain carboxylic acid having the general formula R Ｌ COO － wherein R Ｌ is C6-C24 alkyl] is contacted with a Ce(III) compound in a non-oxidizing atmosphere, and the Ce(III) compound is selected from the group consisting of Ce(III) carbonate, Ce(III) hydroxycarbonate, Ce(III) hydroxide, Ce(III) oxyhydroxide, and / or Ce(III) oxide, and / or hydrates thereof, whereby a Ce(III) long-chain carboxylic acid is obtained, and Step b) A step of adding an organic solvent to the product obtained in step a).

13. The method according to claim 12, wherein the long-chain carboxylic acid is brought into contact with a Ce(III) compound in a non-oxidizing atmosphere in the presence of an organic acid having the general formula RCOOH [wherein R is H or C1-C4 alkyl], and / or a hydrate and / or an anhydride thereof.

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

15. The method according to any one of claims 12 to 14, wherein the long-chain carboxylic acid is brought into contact with the Ce(III) compound at a temperature of 60°C to 180°C.

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

17. The method 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 of 100°C to 200°C.

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

19. A method for reducing particulate emissions from a diesel engine, comprising a fuel and a cerium (III) long-chain carboxylic acid having the general formula R Ｌ COO － wherein R Ｌ is C6-C24 alkyl], operating a diesel engine using a fuel composition containing the same, passing exhaust gas containing cerium oxide generated by combustion of the fuel and 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 raising the temperature to a temperature of 350°C to 600°C.

20. The method according to claim 19, comprising a fuel and a general formula R Ｌ COO － [wherein, R Ｌ is C6-C24 alkyl] and a long-chain carboxylic acid Ce(III), and optionally a long-chain carboxylic acid having a general formula R Ｌ COOH, and optionally a carboxylic acid Ce(III) having a general formula RCOO － [R is H or C1-C4 alkyl], and an organic solvent, and operating a diesel engine using a fuel composition containing the same.

21. The method according to claim 19 or 20, wherein the diesel particulate filter is regenerated by raising the temperature to a temperature of 350°C to 500°C.

22. Use of the 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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