DESULFURIZATION PROCESS
The present invention therefore pertains to a process for desulfurizing a sulfur compound-containing liquid fossil fuel. By continuously adding a solution comprising an oxidant to the sulfur compound-containing liquid fossil fuel, it is possible to improve oxidant utilization and achieve higher sulfur removal rate.
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The present invention resides in the field of the desulfurization of petroleum and petroleum-based fuels.
BACKGROUNDThe following discussion of the prior art is provided to place the invention in an appropriate technical context and enable the advantages of it to be more fully understood. It should be appreciated, however, that any discussion of the prior art throughout the specification should not be considered as an express or implied admission that such prior art is widely known or forms part of common general knowledge in the field.
While alternative sources of power are under development and in use in many parts of the world, fossil fuels remain the largest and most widely used source due to their high efficiency, proven performance, and relatively low prices. Fossil fuels take many forms, ranging from petroleum fractions to coal, tar sands, and shale oil, and their uses extend from consumer uses such as automotive engines and home heating to commercial uses such as boilers, furnaces, smelting units, and power plants.
A persistent problem in the processing and use of fossil fuels is the presence of sulfur, notably in the form of organic sulfur compounds, such as mercaptans, thiophenes (T), benzothiophenes (BT), and dibenzothiophenes (DBT). Sulfur has been implicated in the corrosion of pipeline, pumping, and refining equipment and in the premature failure of combustion engines. Sulfur is also responsible for the poisoning of catalysts used in the refining and combustion of fossil fuels. By poisoning the catalytic converters in automotive engines, sulfur is responsible in part for the emissions of oxides of nitrogen (NOx) from diesel-powered trucks and buses. Sulfur is also responsible for the particulate (soot) emissions from trucks and buses since the traps used on these vehicles for controlling these emissions are quickly degraded by high-sulfur fuels. Perhaps the most notorious characteristic of sulfur compounds in fossil fuels is the conversion of the sulfur in these compounds to sulfur dioxide when the fuels are combusted. The release of sulfur dioxide to the atmosphere results in acid rain, a deposition of acid that is harmful to agriculture, wildlife, and human health. Ecosystems of various kinds are threatened with irreversible damage, as is the quality of life.
Applied Thermal Engineering 111 (2017) 1158-1170 reports a study on ultrasound assisted oxidative desulfurization (UAOD) of gas oil. Desired hydrogen peroxide and formic acid was added to the reactor separately.
Fuel, 2011, 90(6), 2158-2164 discloses an ultrasound-assisted oxidative desulfurization process. According to the experimental procedure, oxidant (mixtures of glacial acetic acid and H2O2) was combined with diesel oil in batch mode.
As such, there remains a need to develop a novel process for desulfurizing a fossil fuel, which features an improved oxidant utilization and higher sulfur removal rate.
SUMMARY OF THE INVENTIONAn object of the present invention is to improve the utilization of oxidant and achieve higher sulfur removal rate.
The present invention therefore pertains to a process for desulfurizing a sulfur compound-containing liquid fossil fuel, comprising at least following steps:
-
- adding a solution comprising an oxidant to the sulfur compound-containing liquid fossil fuel and optionally a catalyst to form an oxidation reaction mixture;
- maintaining the reaction mixture under reaction conditions to ensure completion of the oxidation reaction;
- wherein:
- the molar ratio of the oxidant to the sulfur compound in the liquid fossil fuel is from 2:1 to 10:1;
- the concentration of the oxidant in the solution is from 5 wt. % to 70 wt. %; and
- the solution comprising an oxidant is continuously added to the liquid fossil fuel within 0.16 h to 3 h.
Other subjects and characteristics, aspects and advantages of the present invention will emerge even more clearly on reading the detailed description and the examples that follow.
Throughout the description, including the claims, the term “comprising one” should be understood as being synonymous with the term “comprising at least one”, unless otherwise specified, and “between” should be understood as being inclusive of the limits.
As used herein, the terminology “(Cn-Cm)” in reference to an organic group, wherein n and m are both integers, indicates that the group may contain from n carbon atoms to m carbon atoms per group.
The articles “a”, “an” and “the” are used to refer to one or to more than one (i.e., to at least one) of the grammatical object of the article.
The term “and/or” includes the meanings “and”, “or” and also all the other possible combinations of the elements connected to this term.
It is specified that, in the continuation of the description, unless otherwise indicated, the values at the limits are included in the ranges of values which are given.
Ratios, concentrations, amounts, and other numerical data may be presented herein in a range format. It is to be understood that such a range format is used merely for convenience and brevity and should be interpreted flexibly to include not only the numerical values explicitly recited as the limits of the range, but also all the individual numerical values or sub-ranges encompassed within that range as if each numerical value or sub-range is explicitly recited.
DETAILS OF THE INVENTIONFossil Fuel
Fossil fuel, any of a class of hydrocarbon-containing materials of biological origin occurring within Earth's crust that can be used as a source of energy. Fossil fuels include coal, petroleum, natural gas, oil shales, bitumens, tar sands, and heavy oils.
The liquid fossil fuel desulfurized by the process according to the present invention may have a kinematic viscosity of 0.05 to 700 mm2/s at 50° C., preferably from 0.5 to 500 mm2/s at 50° C. and more preferably 1 to 450 mm2/s at 50° C.
Example of commercial liquid fossil fuel are diesel oil or marine fuel. Marine fuels (cf. DIN ISO 8217), also called bunker fuels, are generally divided into two different classes (Heavy Fuel Oil (HFO) and distillates).
The liquid fossil fuel according to the process of the present invention can notably be a heavy fuel oil, which is normally defined by a density of greater than 900 kg/m3 and a maximum density of 1010 kg/m3 at 15° C., and a kinematic viscosity of more than 180 mm2/s and a maximum viscosity of 700 mm2/s at 50° C. according to ISO 8217. Heavy fuel oils have large percentages of heavy molecules such as long-chain hydrocarbons and aromatics with long-branched side chains and are mainly used as marine fuel. The most commonly used types are IFO180 and IFO 380, with viscosities of 180 mm2/s and 380 mm2/s, respectively.
Advantageously, the liquid fossil fuel may be dissolved in a solvent, which can be an organic solvent, such as decalin, toluene, xylene, mixed aromatic compounds, such as solvesso 150 and solvesso 200 etc.
The weight ratio of the liquid fossil fuel to the solution comprising an oxidant can be from 1:0.001 to 1:4, preferably 1:0.1 to 1:2.
The weight of the fossil oil which can be desulfurized by the process according to the present invention may be preferably in the range of 10 g to 75 million tons and more preferably 20 g to 40 million tons.
Sulfur Compound
The organic sulfur that is present as a naturally-occurring component of fossil (or petroleum-derived) fuels consists of a wide variety of compounds that are primarily hydrocarbons containing one or more sulfur atoms covalently bonded to the remainder of the molecular structure. There are many petroleum-derived compounds containing carbon, hydrogen and sulfur, and some of these compounds contain other heteroatoms as well. The hydrocarbon portions of these compounds may be aliphatic, aromatic, saturated, unsaturated, cyclic, fused cyclic, or otherwise, and the sulfur atoms may be included in the molecular structure as thiols, thioethers, sulfides, disulfides, and the like.
Some of the most refractory of these compounds are sulfur-bearing heterocycles, both aromatic and non-aromatic, ranging from thiophene to fused structures such as substituted and unsubstituted benzothiophene and substituted and unsubstituted dibenzothiophene. Examples are thiophene, 2methylthiophene, benzothiophene, 2-methylbenzothiophene, dibenzothiophene, 4-methyldibenzothiophene, 3-methyldibenzothiophene, 2-methyldibenzothiophene, 4,9-dimethyldibenzothiophene, 4,6-dimethyldibenzothiophene, 1,4,9-trimethyldibenzothiophene and 2,7,8-trimethyl dibenzothiophene. Other examples are analogs in which the methyl groups are replaced by ethyl or other lower alkyl or alkoxy groups or substituted alkyl groups such as hydroxyl-substituted groups.
Before desulfurization, the sulfur may be present in an amount of 0.6 to 8.0 wt. %, preferably from 0.8 to 6 wt. % and more preferably 0.8 to 3.5 wt. % in the liquid fossil fuel, relative to the total weight of the liquid fossil fuel, as measured by X-Ray Fluorescence Spectrometer (XRF) following the standard method ISO 8217:2017.
Oxidant
The oxidant is not particularly limited. It can be selected from the group consisting of organic peroxy acid, such as performic acid, peracetic acid; organic peroxide, such as t-butyl hydrogen peroxide; and inorganic peroxide, such as hydrogen peroxide, a perborate, a persulfate and any combination thereof.
Preferred oxidant can be selected in the group consisting of: hydrogen peroxide, performic acid, peracetic acid and combinations thereof.
Preferably, the molar ratio of the oxidant to the sulfur compound in the liquid fossil fuel may be from 2:1 to 8:1 and more preferably from 2.5:1 to 7.5:1.
The solvent for dissolving the oxidant is not particularly limited as long as its presence does not prevent the oxidation reaction. Preferred solvent is water.
The concentration of the oxidant in the solution depends on the specific oxidant. For example, when the oxidant is hydrogen peroxide, the concentration can be preferably from 20 wt. % to 40 wt. %, based on the total weight of the solution. When the oxidant is performic acid, the concentration can be preferably from 5 wt. % to 50 wt. %, based on the total weight of the solution.
In some embodiments, the oxidant is performic acid or peracetic acid. In this embodiment, before being introducing into the liquid fossil fuel, performic acid or peracetic acid is prepared by mixing hydrogen peroxide with formic acid or acetic acid. In a preferred embodiment, an acid can be further comprised in the solution. Said acid can be an organic acid, such as formic acid and acetic acid. The weight ratio of such acid may be present in an amount of 40 to 98 wt. %, preferably from 45 to 98 wt. % in the solution, relative to the total weight of the solution.
In some embodiments, the oxidant is hydrogen peroxide. Advantageously, said oxidation reaction can be carried out in the presence of a polyoxometalate and/or amphiphilic solid particles, which is introduced at the beginning of the oxidation reaction.
As used herein, polyoxometalate is a polyatomic ion, usually an anion, that consists of three or more transition metal, lanthanide metal or actinide metal oxyanions linked together by shared oxygen atoms to form closed 3-dimensional frameworks.
Non-limiting examples of polyoxometalate can notably be Keggin type polyoxometalates (POMs), including H3PWxMo12−xO40 (x=1, 3 or 6), Cs2.5H0.5PW12O40 and H3PW12O40 as described in Catalysis Today 149 (2010) 117-121. Preferable polyoxometalate is H3PW12O40.
In one preferred embodiment, an amphiphilic polyoxometalates, such as vanadium (V)-substituted polyoxometalates [C18H37N(CH3)3]3+x [PMo12−xVxO40] (x=1, 2 or 3) described in China Petroleum Processing and Petrochemical Technology (2012), 14(1), 25-31 or [Cnmim]3PW12O40/SiO2 (n=4, 8 or 16) described in Journal of Molecular Catalysis A: Chemical (2015), 406, 23-30 may be used.
It can be understood by a skilled person that polyoxometalate is used as a catalyst in the oxidation reaction. The amount of polyoxometalate depends on the specific fossil fuel. The weight ratio of polyoxometalate to the liquid fossil fuel may be from 1:100 to 1:30.
The amphiphilic solid particles of the instant invention may notably be particles having an average diameter comprised from 2 to 5000 nm, preferably from 100 to 3000 nm.
The average diameter of particles can be determined by examining a micrograph of a transmission electron microscopy “TEM” image, measuring the diameter of the particles in the image, and calculating the number average particle size of the measured particles based on magnification of the TEM image. One of ordinary skill in the art will understand how to prepare such a TEM image and determine the particle size based on the magnification. For example, silica particles can be characterized by TEM on a JEOL JEM 2100 microscope operated at 200 kV and equipped with Energy Dispersive Spectroscopy (EDS). The particles to be measured refer to the projection (2D-representation) of the particles on the micrograph. Before performing the measurements, it is necessary to calibrate the image. Size distribution histograms are then plotted as percent silica particles versus silica diameter on the basis of the size measurements obtained from an image processing program, such as ImageJ. The number average is obtained by weighted average method. The measurement should be made on a sufficiently high number of particles, for example at least about 100 particles, preferably at least 300 particles, more preferably at least 1000 particles, still more preferably at least 3000 particles.
The shape or morphology of the amphiphilic solid particle can vary. For example, generally spherical morphologies can be used, as well as particles that are cubic, platy, or acicular (elongated or fibrous), such as sticks or needles. Solid particles are amphiphilic and then comprise solid particles having both hydrophilic and hydrophobic functions. Any amphiphilic solid particles that act as a stabilizer to emulsion may be used in the present invention.
Suitable amphiphilic particles include, for example, inorganic materials, such as water immiscible metal salts or metal hydroxides or metal oxides or mixed metal oxides or clays. Specific non-limiting examples include bentonite, tin oxide, magnesium aluminum silicate, magnesium oxide, titanium oxide, barium sulphate or silicon dioxide, such as is described in U.S. Pat. No. 4,833,060 at col. 4, lines 54-61, the cited portion of which being incorporated herein by reference, and alumina as described in United States Patent Application Publication 2005/0156340.
Said amphiphilic particles can be organic materials, such as graphene, graphite, porous carbons, carbon nanotubes, N-doped carbon materials, graphene. The organic materials can contain functional groups such as —COOH and —SO3H.
Said amphiphilic solid particles can notably be inorganics such as for example made of an oxide, hydroxide or oxy-hydroxide of at least one element chosen from lanthanides, such as cerium, post-transition metals, such as aluminium, transition metals, such as titanium and metalloids, such as silicon.
Some of the elements encompassed by the description above and understood to be metals for the purpose of the present invention, are sometimes also referred to as metalloids. The term metalloid is generally designating an element which has properties between those of metals and non-metals. Typically, metalloids have a metallic appearance but are relatively brittle and have a moderate electrical conductivity. The six commonly recognized metalloids are boron, silicon, germanium, arsenic, antimony, and tellurium.
It can be advantageous that the amphiphilic solid particles of the invention may have a colloidal behaviour, preferably with an inter particular agglomeration rate (number of agglomerated particles/total number of particles) inferior or equal to 5%, more preferably inferior or equal to 2%. In certain embodiments, the solid particles, such as silica and/or alumina particles, are introduced in the form of colloidal dispersion, wherein finely divided solid particles are dispersed within a continuous medium in a manner that prevents them from being filtered easily or settled rapidly.
Preferably, the amphiphilic solid particle is silicon dioxide.
Amphiphilic solid particles can also be organic, obtained from reticulation of polymer chains such as latex particles, polymeric particles with core-shell structures which are composed by amphiphilic chains cross-linked at the core or on the layer of shell.
In a preferred embodiment, amphiphilic solid particles can also be particles linked with hydrophilic and hydrophobic functional groups. The particles linked with hydrophilic and hydrophobic functional groups can have or haven't amphiphilic character. Preferably, the particles linked with hydrophilic and hydrophobic functional groups can be inorganics such as for example made of an oxide, hydroxide or oxy-hydroxide of at least one element chosen from lanthanides, such as cerium, post-transition metals, such as aluminium, transition metals, such as titanium and metalloids, such as silicon.
Hydrophilic functional groups may be neutral (—OH, —COOH as example) or preferentially under their anionic or cationic corresponding forms.
Hydrophobic groups can be organic chains having a hydrophobic nature. Said chains are defined as organic chains having a hydrophobic character such as these chains are soluble in a hydrophobic solvent and less soluble, notably insoluble, in water. Organic chains having a hydrophobic nature may have at least 50% wt, preferentially at least 80% wt of hydrophobic groups such as alkylated groups, or alkoxylated groups.
Hydrophobic groups are preferably alkyl chains comprising 1 to 30 carbon atoms, more preferably from 1 to 8 carbon atoms or alkoxylated groups notably comprising 1 to 10 units of ethylene oxide —CH2CH2O— groups.
The exact nature of the link existing between organic chains and the surface of the solid particles can vary in a large measure and may be for example a covalent bond, or physical adsorption more often including an electrostatic bond, an ionic bond and a hydrogen bond. Covalent bonds can be obtained by grafting or co-condensation.
The grafting rate of the particle surface by hydrophobic groups may be comprised between 5 and 90% of the original amount of hydroxyl groups, preferably between 30 and 70%. This grafting rate may be evaluated by a thermal decomposition of the particles and then calculate the amount of water formed during the decomposition. It is then possible to proceed to an extrapolation of the number of hydroxyl group.
In a preferred embodiment of the invention, the bonds between the organic chains of hydrophobic nature and the surface of the particles are covalent bonds.
In this case, these are usually made covalent bonds between atoms of metal particles and organic chains, usually via oxygen atoms initially present in a hydroxyl metal group of the particle surface.
Preferably, the metal atom of these groups hydroxylated metal surface is an atom of silicon, aluminum, or titanium. In this case, the particles are formed at least partially of silicon oxide, oxy-hydroxide of aluminum and/or titanium oxide, this or these oxide (s) and/or oxy-hydroxide being at least this (s) on the surface. Thus, the particles can then be formed such oxide (s), hydroxide (s) and/or oxy-hydroxide (s) of chemical nature variable, having a surface layer of silicon oxide oxy-aluminum hydroxide and/or titanium oxide, made for example by after-treatment surface.
The organic chains covalently linked are generally introduced by this embodiment of the invention by condensation of a silanol group SiOH on the particle, according to the general reaction:
[particle]-M-OH+OH—Si [organic chain]->[particle]-M-O—Si-[organic chain]
wherein M is Si, Al or Ti.
In this case, the silanol group SiOH usually comes from the acid hydrolysis, neutral, or basic group of an alkoxysilane, for example acid hydrolysis of trimethoxyalkylsilane or triethoxyalkylsilane.
Whatever the exact nature of links implemented to ensure cohesion between the hydrophobic chains and the particle surface, it is preferred that the bonds between the chains and hydrophobic particles are inhomogeneously distributed on the surface of said particles, whereby said particles modified surface have a first area to overall hydrophilic nature and a second area to overall hydrophobic character.
It has to be noticed that according to the nature of hydrophilic and hydrophobic functions at the surface of particles, said amphiphilic solid particles may also act as emulsifier and also catalyst.
The concentration of amphiphilic solid particles can be greater than 0.005 wt %, particularly from 0.005 wt % to 15.000 wt % and more preferably from 0.01 wt % to 5.00 wt % based on the total weight of reaction medium.
Continuous Mode
As previously expressed, the solution comprising the oxidant is continuously added to the liquid fossil fuel.
As used herein, the term “continuously” means the solution is introduced to the liquid fossil fuel at a certain flow rate. The skilled person can calculate the flow rate based on the sulfur content in the liquid fossil fuel, the amount of oxidant required and concentration of the solution comprising the oxidant and the required continuous addition time.
In some embodiments, the solution is continuously added to the liquid fossil fuel within 0.16 h to 1 h.
The flow rate can be 4 g/h to 400 million tons/h, preferably from 6 g/h to 250 million tons/h.
In a preferred embodiment, before the solution is introduced, the liquid fossil oil is pre-mixed with a solvent and/or a catalyst by mechanical stirring and irradiating by bath ultrasound at a proper temperature for a proper time.
Said proper temperature can be from 55 to 85° C. and preferably 50 to 70° C.
Said proper time can be from 1 to 30 mins and preferably 2 to 15 mins.
Reaction Conditions
It shall be understood that the oxidation reaction shall be maintained under proper temperature for a sufficient time so as to ensure completion of the oxidation reaction.
In some embodiments, when the oxidant is performic acid or peracetic acid, the reaction mixture can be maintained at a temperature from 55 to 85° C. for 1 to 5 h under mechanical stirring and/or ultrasound irradiation.
The frequency of ultrasound may be in the ranges of 2 KHz to 2 MHz.
In some embodiments, when the oxidant is hydrogen peroxide, the reaction mixture can be maintained at a temperature from 55 to 85° C. for 1 to 5 h under mechanical stirring and/or ultrasound irradiation.
The following examples are included to illustrate embodiments of the invention. Needless to say, the invention is not limited to describe examples.
EXPERIMENTAL PARTMaterials
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- Maritime fuel (RMG380) with sulfur content 2.5 wt. %, cas: 68476-33-5, SINOPEC;
- H2O2 (30 wt. %), cas: 7722-84-1, Sinopharm;
- H3PW12O40·xH2O (regent grade), cas: 12501-23-4, J&K;
- Functionalized SiO2 (R805), CAS: 92 797-60-9, Evonik;
- Formic acid (98%), cas: 64-18-6, J&K.
In a typical procedure, maritime fuel (RMG380) in decalin (30 g with 40 wt. % fuel oil) was added into three-necked glassware equipped with a cooling condenser. After premixing fuel by mechanical stirring (450 rpm) and irradiating by bath ultrasound (Ultrasonic Elma-100H) at 60° C. for 5 mins, then the pre-formed performic acid solution ((formic acid (4.08 ml) and H2O2 (30 wt. %, 4.08 ml)) was continuously added into the fuel with a flowrate of 1.12 ml/min. The reaction was carried out under mechanical stirring and irradiation for 2 hours at 60° C. The sulfone yield is shown in Table 1.
The sulfides and sulfones before and after oxidation were analyzed by X-ray photoelectron spectroscopy (XPS). In practice, liquid samples were dropped on aluminum foil to dry and then perform XPS analysis. The spectra were recorded using an Al monochromated X-ray source (1486.6 eV, 15 kV, 15 mA) in the CAE mode. The adventitious C is binding energy (284.8 eV) was used as an internal reference. The spectra were devoluted by Advantage software. The S 2p spectra have splitting into 2p3/2 (˜167 eV) and 2p1/2 (˜168 eV) (3/2 is more intense than 1/2) for sulfone, into 2p3/2 (˜163 eV) and 2p1/2 (˜164 eV) for sulfide. As shown in
The experimental procedure is similar as example 1, except that performic acid was added in two portions with the same volume.
In a typical procedure, maritime fuel (RMG380) in decalin (30 g with 40 wt. % fuel oil) and H3PW12O40 (0.2940 g) and SiO2 (0.0317 g) were added into three-necked glassware equipped with a cooling condenser. After premixing fuel by mechanical stirring (450 rpm) and irradiating by bath ultrasound (Ultrasonic Elma-100H) at 60° C. for 5 mins, then H2O2 (30 wt. %, 4.08 ml) was continuously added into the fuel with flowrate of 0.56 ml/min. The reaction was carried out under mechanical stirring and irradiation for 2 hours at 60° C. The sulfones and sulfides in oxidized fuel without solid adsorption were analyzed by X-ray photoelectron spectroscopy (XPS). The sulfone yield was calculated through peak fitting using Advantage software (Sulfone yield %=weight of sulfones/weight of sulfides*100%). The sulfone yield is shown in Table 2.
Example 3In a typical procedure, maritime fuel (RMG380) in decalin (30 g with 40 wt. % fuel oil) and H3PW12O40 (0.2940 g) and SiO2 (0.0317 g) were added into three-necked glassware equipped with a cooling condenser. After premixing fuel by mechanical stirring (450 rpm) and irradiating by bath ultrasound (Ultrasonic Elma-100H) at 60° C. for 5 mins, then H2O2 (30 wt. %, 6.12 ml) was continuously added into the fuel with flowrate of 0.84 ml/min. The reaction was carried out under mechanical stirring and irradiation for 2 hours at 60° C. The sulfones and sulfides in oxidized fuel without solid adsorption were analyzed by X-ray photoelectron spectroscopy (XPS) as shown by
Claims
1. A process for desulfurizing a sulfur compound-containing liquid fossil fuel, comprising at least following steps: wherein:
- adding a solution comprising an oxidant to the sulfur compound-containing liquid fossil fuel and optionally a catalyst to form an oxidation reaction mixture;
- maintaining the reaction mixture under reaction conditions to ensure completion of an oxidation reaction;
- a molar ratio of the oxidant to the sulfur compound in the liquid fossil fuel is from 2:1 to 10:1;
- a concentration of the oxidant in the solution is from 5 wt. % to 70 wt. %; and
- the solution comprising the oxidant is continuously added to the liquid fossil fuel within 0.16 h to 3 h.
2. The process according to claim 1, wherein the sulfur compound-containing liquid fossil fuel is dissolved in a solvent.
3. The process according to claim 1, wherein the liquid fossil fuel has a kinematic viscosity of 0.05 to 700 mm2/s at 50° C.
4. The process according to claim 1, wherein the sulfur is present in an amount of 0.6 to 8.0 wt. % in the liquid fossil fuel, relative to a total weight of the liquid fossil fuel, as measured by X-Ray Fluorescence Spectrometer following a standard method ISO 8217:2017.
5. The process according to claim 1, wherein the oxidant is selected from a group consisting of: hydrogen peroxide, performic acid, peracetic acid and combinations thereof.
6. The process according to claim 1, wherein the molar ratio of the oxidant to the sulfur compound in the liquid fossil fuel is from 2:1 to 8:1.
7. The process according to claim 1, wherein a weight ratio of the liquid fossil fuel to the solution is from 1:0.001 to 1:4.
8. The process according to claim 1, wherein the oxidant is performic acid and a concentration of performic acid is from 5 wt. % to 50 wt. %, based on a total weight of the solution.
9. The process according to claim 8, wherein formic acid is comprised in the solution and a weight ratio of formic acid is present in an amount of 40 to 98 wt. %, relative to a total weight of the solution.
10. The process according to claim 1, wherein the oxidant is hydrogen peroxide at a concentration ranging from 20 wt. % to 40 wt. %, based on a total weight of the solution.
11. The process according to claim 10, wherein the oxidation reaction is carried out in the presence of a polyoxometalate.
12. The process according to claim 11, wherein a weight ratio of polyoxometalate to the liquid fossil fuel is from 1:100 to 1:30.
13. The process according to claim 1, wherein the liquid fossil fuel has a kinematic viscosity from 0.5 to 500 mm2/s at 50° C.
14. The process according to claim 1, wherein the liquid fossil fuel has a kinematic viscosity from 1 to 450 mm2/s at 50° C.
15. The process according to claim 1, wherein the sulfur is present in an amount from 0.8 to 6 wt. % in the liquid fossil fuel, relative to a total weight of the liquid fossil fuel, as measured by X-Ray Fluorescence Spectrometer following a standard method ISO 8217:2017.
16. The process according to claim 1, wherein the sulfur is present in an amount from 0.8 to 3.5 wt. % in the liquid fossil fuel, relative to a total weight of the liquid fossil fuel, as measured by X-Ray Fluorescence Spectrometer following a standard method ISO 8217:2017.
17. The process according to claim 1, wherein the molar ratio of the oxidant to the sulfur compound in the liquid fossil fuel is from 2.5:1 to 7.5:1.
18. The process according to claim 1, wherein a weight ratio of the liquid fossil fuel to the solution is from 1:0.1 to 1:2.
19. The process according to claim 8, wherein formic acid is comprised in the solution and a weight ratio of formic acid is present in an amount of 45 to 98 wt. % in the solution, relative to the total weight of the solution.
Type: Application
Filed: Dec 23, 2020
Publication Date: Feb 29, 2024
Applicant: Solvay SA (Brussels)
Inventors: Wenjuan Zhou (Shanghai), Andrew Willson (Brussels), Nuno Formiga (Brussels), Francois Dabeux (Brussels), Zhen Yan (Shanghai), Stephane Streiff (Aubervilliers)
Application Number: 18/259,039
