CN110686164A - Method for reducing viscosity of crude oil - Google Patents
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- CN110686164A CN110686164A CN201910148971.3A CN201910148971A CN110686164A CN 110686164 A CN110686164 A CN 110686164A CN 201910148971 A CN201910148971 A CN 201910148971A CN 110686164 A CN110686164 A CN 110686164A
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Abstract
The invention relates to the field of crude oil transportation, and provides a method for reducing the viscosity of crude oil, aiming at solving the problem of difficult crude oil transportation caused by the increase of the viscosity of the crude oil at low temperature, overcoming the defects of the existing physical and chemical viscosity reduction technology, particularly improving the problems of viscosity increase and viscosity reduction effect weakening of the existing chemical viscosity reducer at low temperature, so that the viscosity reducer still has good viscosity reduction capability in the low-temperature transportation environment: the cyclosiloxane containing the diethyl siloxane chain or the polymer containing the diethyl siloxane chain is mixed with the crude oil by a common method, so that the viscosity of the crude oil can be obviously reduced, the energy consumption caused by heating and heat preservation in the crude oil conveying process can be reduced, the power of a pump and the resistance of the crude oil in a pipeline are reduced, and the energy consumption in the crude oil conveying process is reduced. The synthesis method is simple, the reaction condition is mild, the product is easy to separate and recycle, the equipment investment is low, the equipment utilization rate is high, and the industrial production is easy to realize.
Description
Technical Field
The invention relates to the field of crude oil transportation, in particular to a method for reducing the viscosity of crude oil.
Technical Field
Crude oil is liquid hydrocarbon or its natural form mixture obtained by direct extraction from underground natural oil reservoir, and after removing water and associated gas compounds such as methane, etc., crude oil usually presents flowing or semi-flowing viscous liquid state. Crude oil is strategic material of each country, and various commodities can be produced after primary and secondary processing, so that the requirements of each department of national economy and each aspect of material life of people are met. Crude oil reserves are unbalanced all over the world, the crude oil reserves in China are small, and the crude oil quality is poor, so in order to meet the huge requirements of various departments of national economy on energy and materials, the crude oil in China is mostly imported to solve the huge gap between the domestic yield and the demanded quantity. Under the influence of multiple factors such as geography, environment and national strategic layout, most crude oil processing enterprises in China such as petrochemical and refining enterprises are not located in coastal cities with oil terminals, so that the transportation of crude oil from the oil terminals or directly from oil production places to related processing enterprises is the primary task for realizing oil processing and utilization, and the long-distance pipeline transportation mode of crude oil is the main mode of crude oil transportation in China.
Crude oil is a complex mixture of various hydrocarbons, aromatic hydrocarbons and heterocyclic aromatic hydrocarbons, and the crude oil produced in different regions has different compositions, resulting in different viscosities of crude oil in different regions. As is well known, the viscosity of the fluid is an important factor affecting the efficiency and energy consumption of pipeline transportation, the greater the viscosity of the fluid is, the greater the resistance loss of the fluid in the pump and the transportation pipeline is, in order to overcome the resistance loss, the power of the pump has to be increased, the intermediate storage tanks are arranged at certain intervals, and the pump is used for transporting the fluid to the next-stage transfer station again, so as to realize the long-distance transportation of the fluid; the greater the viscosity of the fluid, the higher the energy it consumes during delivery. Therefore, reducing the viscosity of crude oil is one of the key technical problems to be overcome in crude oil transportation.
The viscosity of crude oil is reduced along with the rise of temperature, so in order to reduce the resistance loss in the conveying process, reduce the power of a pump and prolong the conveying distance, a heating and heat-insulating mode is usually adopted for a crude oil conveying pipeline, the temperature of the conveyed crude oil is increased, and the viscosity of the crude oil is reduced.
Besides the heating viscosity reduction of crude oil, the physical viscosity reduction technologies such as dilution viscosity reduction, microwave viscosity reduction, magnetic treatment viscosity reduction and the like, and the chemical viscosity reduction technologies such as emulsification viscosity reduction, oil-soluble viscosity reduction, pour point reducer viscosity reduction and the like can be adopted. Diluting and viscosity reduction are carried out by taking some low-viscosity liquid hydrocarbons as diluents to be mixed with thick oil before high-viscosity crude oil enters a pipeline, so that the conveying viscosity of the thick oil is reduced, and the thick oil is conveyed in a mixture form, but the diluting and viscosity reduction has the defects of limited thin oil resources, increased energy consumption, increased conveying load and the like; the microwave viscosity reduction utilizes microwave non-thermal effect to modify the thick oil, changes the chemical components of the thick oil, and irreversibly improves the rheological property of the thick oil so as to achieve the purpose of rapid viscosity reduction, but the microwave viscosity reduction has the problems of uneven macroscopic and microscopic distribution of internal temperature, and easily causes the change of the chemical structure of crude oil components; the magnetic treatment viscosity reduction utilizes the diamagnetism of crude oil and the induced magnetic moment of the magnetization to inhibit the formation and coalescence of wax crystals, so that the wax crystals exist in the thick oil in the form of small particles, the fluidity is enhanced, and the viscosity of the thick oil is reduced. The emulsification and viscosity reduction method is characterized in that a surfactant is added to convert crude oil from a water-in-oil (W/O) type emulsion to an oil-in-water (O/W) type emulsion to achieve the purpose of viscosity reduction, wherein the viscosity reduction mechanism mainly comprises two aspects of emulsification and viscosity reduction, but the emulsification and viscosity reduction has the problems of difficult demulsification, high sewage treatment difficulty, strong selectivity of an emulsifier on crude oil, influence on the emulsification and viscosity reduction effect due to crude oil composition and the like; the oil-soluble viscosity reducer utilizes the strong hydrogen bond forming capability of viscosity reducer molecules, enters between colloid and asphaltene sheet molecules through the penetration or dispersion effect, partially disassembles aggregates formed by plane overlapping and stacking, and constructs new hydrogen bond aggregates which are involved in the random stacking, loose structure, low order degree and small space extension degree of the viscosity reducer molecules, so as to achieve the purpose of reducing the viscosity of crude oil; the molecular structure of the pour point depressant is the same as or similar to that of wax in crude oil, and the pour point depressant can be eutectic with or adsorbed by wax crystals in the nucleation and growth processes of the wax, so that the growth of the wax crystals is prevented, the network structure of the wax is inhibited, and the apparent viscosity of the crude oil is reduced.
Therefore, both the existing physical viscosity reduction technology and the existing chemical viscosity reduction technology have certain technical defects, so that the viscosity reduction effect of crude oil is not ideal, wherein the existing chemical viscosity reduction technology is greatly influenced by the production place of the crude oil and the composition of the crude oil, and in addition, the main components of an emulsifier, an oil-soluble viscosity reducer and a pour point depressant adopted by the existing chemical viscosity reduction technology are mostly compounds or polymers formed by carbon-carbon bonds, and the viscosity of the substances at low temperature is rapidly increased, so that the viscosity reduction capability of the substances originally has is greatly reduced.
Disclosure of Invention
In order to overcome the defects of the existing physical and chemical viscosity reduction technology, particularly the problems of viscosity increase and viscosity reduction effect weakening of the existing chemical viscosity reduction agent at low temperature, the invention provides a method for reducing the viscosity of crude oil, which can obviously reduce the viscosity of the crude oil, can reduce energy consumption caused by heating and heat preservation in the crude oil conveying process, reduce the power of a pump and the resistance of the crude oil in a pipeline, and reduce the energy consumption in the crude oil conveying process.
The invention is realized by the following technical scheme: a method for reducing crude oil viscosity comprises adding a compound containing a diethylsiloxanyl chain (- (C)2H5)2SiO-) cyclic siloxane or diethylsiloxane segment (- (C)2H5)2SiO-) polymer is mixed with crude oil by a common method. The mixed crude oil is cracked into methane, ethane and high-boiling-point substances in the catalytic hydro-reforming and catalytic cracking processes, the methane and the ethane are the products originally existing in the crude oil or the crude oil processed into gasoline and diesel, the boiling point of the organic silicon high-boiling-point substances is higher than that of colloid substances such as asphalt obtained after the crude oil is cracked, and the organic silicon high-boiling-point substances can be used as building materials and other fields together with the asphalt, so that the mixed crude oil contains diethyl silica chain segments (- (C)2H5)2SiO-) cyclic siloxane or diethylsiloxane segment (- (C)2H5)2SiO-) polymer is mixed with the crude oil, and the use of the crude oil is not influenced.
The cyclosiloxane containing the diethyl siloxane chain links is one or more of hexaethylcyclotrisiloxane, octaethylcyclotetrasiloxane, decaethylcyclopentasiloxane and dodecaethylcyclohexasiloxane.
The polymer containing the diethyl siloxane chain links is selected from one of oligomeric siloxane with a structural formula shown in (I) and copolysiloxane with a structural formula shown in (II),
in the formulae (I) and (II), R1、R4Each independently selected from Me and Me3SiO-, Et and Ph; r2、R3、R5、R6Each independently selected from one of Me and Et, wherein Me represents a methyl functional group, Et represents an ethyl functional group, and Ph represents a phenyl functional group; ra、RbAre respectively and independently selected from one of methyl, ethyl, trifluoropropyl and phenyl, and RaAnd RbIs not ethyl or trifluoropropyl at the same time;
in the formula (I), n represents the polymerization degree of the oligomer, and n is 1-100,
in the formula (II), x1Is the degree of polymerization of the diethylsiloxy units, x2By polymerization of other diorganosiloxy units, x1＝1～30，x21 to 100, and x1+x21-120, the structural formula (I) and the structural formula (II) are collectively referred to as ethyl silicone oil for short.
Preferably, the oligomeric siloxanes containing diethylsiloxy units have a viscosity (. eta.) at 20 ℃20) 5 to 500 mPa.s. Copolysiloxanes containing diethylsiloxy units having a viscosity (. eta.) at 20 DEG C20) 5 to 1000 mPa.s.
The mass ratio of the cyclosiloxane containing diethyl siloxane chain or the polymer containing diethyl siloxane chain to the crude oil is 0.000005-0.50: 1, preferably 0.00001-0.01: 1.
The temperature of the mixture of the cyclosiloxane containing diethylsiloxane chain or the polymer containing diethylsiloxane chain and crude oil is-40-60 ℃, and preferably-30-40 ℃.
Compared with the main product dimethyl silicone oil in the current organic silicon industry, the cyclosiloxane, the oligomeric siloxane or the copolysiloxane containing the diethyl siloxane chain link has good compatibility with crude oil, can be rapidly dispersed in the crude oil, and saves the mixing treatment time of the current viscosity reducer and the crude oil; and the cyclosiloxane, the oligomeric siloxane or the copolysiloxane containing the diethyl siloxane chain link is directly mixed with the crude oil, and does not need to be polymerized and then prepared into an aqueous solution for use like an acrylic acid high-grade alkyl ester viscosity reducer, so that the use amount is reduced, the conveying load is reduced, the conveying capacity of a crude oil conveying pipeline is correspondingly improved, the water is prevented from being introduced into the crude oil, the risk of crude oil emulsification is reduced, and the operating cost of subsequent links is saved.
Compared with the prior art, the invention has the beneficial effects that: the viscosity of the crude oil can be obviously reduced, the energy consumption caused by heating and heat preservation in the crude oil conveying process can be reduced, the power of a pump and the resistance of the crude oil in a pipeline are reduced, and the energy consumption in the crude oil conveying process is reduced.
Drawings
FIG. 1 is a trimethylsiloxy terminated poly (dimethyl-diethyl) siloxane copolymer nuclear magnetic hydrogen spectrum;
FIG. 2 is a schematic diagram of the compatibility experiment of the present invention;
FIG. 3 is a graph showing the effect of ethyl silicone oil dosage on crude oil viscosity at different temperatures;
FIG. 4 is a graph of the effect of hexaethylcyclotrisiloxane usage on crude viscosity at different temperatures;
FIG. 5 is a graph showing the effect of comparative example dimethicone dosage on crude viscosity at various temperatures.
Detailed Description
The present invention is further illustrated by the following examples, which are not intended to limit the scope of the invention, and the starting materials used in the examples are commercially available or can be prepared by conventional methods.
Preparation example 1: trimethylsiloxy-terminated poly (dimethyl-diethyl) siloxane copolymers
61.2g of hexaethylcyclotrisiloxane (D)3 Et) Adding into a 250mL three-neck flask with mechanical stirring, temperature control device, nitrogen bottom-inserting tube and reflux condensing device, heating to 50 deg.C, and adding into trace N2Dehydrating for 1h under protection; then adding 5.5g of dried solid super acid into a three-neck flask mixed with the materials, raising the temperature to 80 ℃, carrying out ring opening reaction for 4h, then adding 48.8g of octamethyltrisiloxane (MDM) for carrying out end-capping reaction for 3h, then cooling the materials in the kettle to room temperature, filtering to remove the solid super acid catalyst, transferring the filtrate into a reduction reaction kettle, gradually raising the vacuum degree of the system to-100 kPa under the protection of trace nitrogen, then gradually raising the temperature to 220 ℃ and maintaining the temperature for 8h to remove low-boiling-point substances in the reaction system, after the reduction is finished, cooling the materials of the system to room temperature under the protection of nitrogen, collecting the materials and weighing to obtain 75.9g of trimethylsiloxy end-capped poly (dimethyl-diethyl) siloxane copolymer.
The resulting trimethylsiloxy-terminated poly (dimethyl-diethyl) siloxane copolymer had a viscosity of 42.5mPa.s at 20 ℃ as measured by a Brookfield DV2TRVTJO type rotational viscometer, a number average molecular weight Mn of 1419, a weight average molecular weight Mw of 2379, and a polydispersity index PDI of 1.67 as measured by GPC. From the results of nuclear magnetic analysis and the structural formula of the polymer, the polymerization degree x1 of diethylsiloxy units in the copolymer was calculated to be 3.80, and the polymerization degree x2 of dimethylsiloxy units was calculated to be 1.
Test example 1
Nuclear magnetic hydrogen spectrum of prepared trimethylsiloxy-terminated poly (dimethyl-diethyl) siloxane copolymer (b) ((b))1HNMR) as shown in fig. 1, the mass fraction of ethyl groups in the silicone oil was calculated to be 32.7%.
Preparation example 2: trimethylsiloxy-terminated polydiethylsiloxane oligomers
61.2g of hexaethylcyclotrisiloxane (D)3 Et) Adding into a 250mL three-neck flask with mechanical stirring, a temperature control device, a nitrogen bottom inserting tube and a reflux condensing device, raising the temperature to 60 ℃, and then adding into a trace amount of N2Under the protection of-dehydration under vacuum of 100kPa for 0.5 h; then adding 8.0g of dried solid super acid into a three-neck flask mixed with the materials, raising the temperature to 80 ℃, carrying out ring opening reaction for 3h, then adding 34.0g of hexamethyldisiloxane (MM) for carrying out end-capping reaction for 5h, then cooling the materials in the kettle to room temperature, filtering to remove the solid super acid catalyst, transferring the filtrate into a reduction reaction kettle, gradually raising the vacuum degree of the system to-100 kPa under the protection of trace nitrogen, then gradually raising the temperature to 220 ℃ and maintaining the temperature for 6h to remove low-boiling-point substances in the reaction system, after the reduction is finished, cooling the materials of the system to room temperature under the protection of nitrogen, collecting the materials and weighing to obtain 60.6g of the trimethyl siloxy end-capped polydiethylsiloxane oligomer.
The resulting trimethylsiloxy-terminated polydiethylsiloxane oligomer had a viscosity of 46.9mpa.s at 20 ℃ as measured by a brookfield DV2TRVTJO type rotational viscometer, a number average molecular weight Mn of 1846, a weight average molecular weight Mw of 2964, and a polydispersity index PDI of 1.61 as measured by GPC. NMR spectra of Trimethylsiloxy-terminated polydiethylsiloxane oligomers (A)1H NMR) to obtain the mass fraction of ethyl in the silicone oil to be 35.8%, and the polymerization degree n of the oligomer to be 16.5 is obtained by calculation according to the nuclear magnetic molecular result and the structural formula of the polymer.
Preparation example 3: trimethylsiloxy-terminated poly (dimethyl-diethyl) siloxane copolymers
60g of octamethylcyclotetrasiloxane, 28.7g of hexaethylcyclotrisiloxane (D)3 Et) Adding into a 250mL three-neck flask with mechanical stirring, a temperature control device, a nitrogen bottom inserting tube and a reflux condensing device, heating to 55 ℃, and then adding into a trace amount of N2Dehydrating under the protection of-100 kPa for 1.5 h; then 5.4g of dried solid super acid is added into a three-neck flask mixed with the materials, the temperature is raised to 85 ℃, ring opening reaction is carried out for 2h, then 20.0g of octamethyltrisiloxane (MDM) is added for end capping reaction for 6h, then the materials in the kettle are cooled to room temperature, solid super acid catalyst is removed by filtration, and the filtrate is transferred to a three-neck flaskIn a depletion reaction kettle, under the protection of trace nitrogen, the vacuum degree of the system is gradually increased to-100 kPa, then the temperature is gradually increased to 218 ℃ and maintained at the temperature for 5 hours to remove low-boiling-point substances in the reaction system, after the depletion is finished, the system material is cooled to room temperature under the protection of nitrogen, and the material is collected and weighed to obtain 69.6g of trimethylsiloxy-terminated poly (dimethyl-diethyl) siloxane copolymer.
The resulting trimethylsiloxy-terminated poly (dimethyl-diethyl) siloxane copolymer had a viscosity of 122.3mPa.s at 20 ℃ as measured by a Brookfield DV2TRVTJO type rotational viscometer, and the trimethylsiloxy-terminated polydiethylsiloxane oligomer had a number average molecular weight Mn of 3871, a weight average molecular weight Mw of 6423, and a polydispersity index PDI of 1.65 as measured by GPC. Nuclear magnetic hydrogen spectrum of poly (dimethyl-diethyl) siloxane copolymer terminated by trimethylsiloxy group(s) ((ii))1H NMR) was calculated to give a mass fraction of ethyl groups in the silicone oil of 14.45%, and from the results of nuclear magnetic analysis and the structural formula of the polymer, the degree of polymerization x1 of diethylsiloxy units in the copolymer was calculated to be 9.35, and the degree of polymerization x2 of dimethylsiloxy units was calculated to be 36.25.
Preparation example 4: trimethylsiloxy-terminated poly (dimethyl-diethyl) siloxane copolymers
59.3g of octamethylcyclotetrasiloxane and 15.3g of hexaethylcyclotrisiloxane (D)3 Et) And 12.4g octamethyltrisiloxane (MDM) were added at room temperature to a 250mL three-necked flask with mechanical stirring, temperature control, nitrogen bottom-insertion tube and reflux condenser, the temperature was raised to 65 ℃ and then the mixture was cooled to a minimum of N2Dehydrating for 2.0h under the protection of-100 kPa vacuum; then adding 4.3g of dried solid super acid into a three-neck flask mixed with the above materials, raising the temperature to 150 ℃, reacting for 4h, then cooling the materials in the kettle to room temperature, filtering to remove the solid super acid catalyst, transferring the filtrate into a reduction reaction kettle, gradually increasing the vacuum degree of the system to-100 kPa under the protection of trace nitrogen, then gradually heating to 200 ℃ and maintaining for 4h at the temperature to remove low-boiling-point substances in the reaction system, after the reduction is finished, cooling the bulk materials to room temperature under the protection of nitrogen,the material was collected and weighed to give 60.1g of trimethylsiloxy-terminated poly (dimethyl-diethyl) siloxane copolymer.
The resulting trimethylsiloxy-terminated poly (dimethyl-diethyl) siloxane copolymer had a viscosity of 91.0mPa.s at 20 ℃ as measured by a Brookfield DV2TRVTJO type rotational viscometer, and the trimethylsiloxy-terminated polydiethylsiloxane oligomer had a number average molecular weight Mn of 9515, a weight average molecular weight Mw of 22744, and a polydispersity index PDI of 2.39 as measured by GPC. Nuclear magnetic hydrogen spectrum of poly (dimethyl-diethyl) siloxane copolymer terminated with trimethylsiloxy group (1H NMR) was calculated to give a mass fraction of ethyl groups in the silicone oil of 15.68%, and from the results of nuclear magnetic analysis and the structural formula of the polymer, the degree of polymerization x1 of diethylsiloxanyl units in the copolymer was calculated to be 14.96, and the degree of polymerization x2 of dimethylsiloxasiloxanyl units was calculated to be 29.30.
Example 1(1)
1.9877g of the trimethylsiloxy-terminated poly (dimethyl-diethyl) siloxane copolymer (ethyl silicone oil for short) prepared in preparation example 1 and 8.0g of light crude oil imported from Saudi Arabia were mixed and homogenized at room temperature.
Example 1(2)
2.0125g of the trimethylsiloxy-terminated polydiethylsiloxane oligomer (abbreviated as ethylsilicone oil) prepared in preparation example 2 were mixed homogeneously with 8.0g of a light crude oil imported from Saudi Arabia at room temperature.
Example 1(3)
1.9907g of the trimethylsiloxy-terminated poly (dimethyl-diethyl) siloxane copolymer (ethyl silicone oil for short) prepared in preparation example 3 was mixed with 8.0g of light crude oil imported from Saudi Arabia at room temperature to be homogenized.
Example 1(4)
1.9883g of the trimethylsiloxy-terminated poly (dimethyl-diethyl) siloxane copolymer (ethyl silicone oil for short) prepared in preparation example 4 and 8.0g of light crude oil imported from Saudi Arabia were mixed and homogenized at room temperature.
Example 2
2.0089g of hexaethylcyclotrisiloxane (abbreviated as ethylcyclo) was mixed with 8.0g of light crude oil imported from Saudi Arabia at room temperature.
Comparative example 1
2.0134g of viscosity (. eta.) was mixed20) Trimethylsiloxy-terminated polydimethylsiloxane (abbreviated as dimethylsilicone oil) at 50mPa.s was mixed uniformly with 8.0g of crude oil at room temperature.
Test example 2: compatibility test
After the mixed crude oil prepared in example 1 (including 1(1), 1(2), 1(3), 1(4)) and example 2 and comparative example 1 is left for 2 days, samples are respectively obtained, as shown in fig. 2(a), 2(b) and 2(c), as can be seen from fig. 2(a), different ethyl silicone oils respectively prepared in preparation examples 1 to 4 are completely miscible with the crude oil, and the compatibility is good; as can be seen from FIG. 2(b), hexaethylcyclotrisiloxane is completely miscible with crude oil and has good compatibility; as can be seen from FIG. 2(c), the dimethicone oil has some delamination from the crude oil and is less compatible than ethylsilicone oil and hexaethylcyclotrisiloxane.
Example 3 example 34
Clear and transparent light crude oil containing no impurities was taken out at room temperature, and the trimethylsiloxy-terminated poly (dimethyl-diethyl) siloxane copolymer (ethyl silicone oil for short) prepared in preparation example 1 was added thereto, and the mass ratios of ethyl silicone oil/crude oil shown in Table 1 were mixed uniformly.
Test example 3: trimethylsiloxy terminated poly (dimethyl-diethyl) siloxane copolymer viscosity reduction experiment (1) crude oil viscosity as a function of temperature
The viscosity of the light crude oil was measured at-20 to 40 ℃ using a rotational viscometer of DV2TRVTJO type with a spindle suitable for the viscosity measurement range, and the results are shown in FIG. 3 (a).
(2) Variation of ethyl silicone oil viscosity with temperature
The viscosity of the ethyl silicone oil synthesized in preparation example 1 was measured as a function of temperature using a rotational viscometer of the DV2TRVTJO type with a spindle having an appropriate viscosity measurement range at a temperature ranging from-20 to 50 ℃ and the results are shown in FIG. 3 (b).
(3) Change in viscosity of light crude oil blended with Ethyl Silicone oil
The light crude oil mixed with ethyl silicone oil prepared in examples 3 to 11 was placed in a sample measuring tube of a rotational viscometer of DV2TRVTJO type, appropriate rotors and shear rates were selected, the temperature of an external cryostat was set, the viscosity of the ethyl silicone oil/crude oil mixture was measured after the temperature in the sample measuring tube reached the set value, and the measurement results were recorded after the viscosity values stabilized, as shown in table 1.
Fig. 3(c) shows the effect of the amount of ethyl silicone oil on the viscosity of crude oil at-20 ℃, and as can be seen from fig. 3(c), the addition of a small amount of diethyl silicone oil has a very significant viscosity-reducing effect on the viscosity of crude oil; fig. 3(d) shows the effect of reducing the amount of ethyl silicone oil on the viscosity of crude oil at-20 ℃, and it can be seen that the addition of a small amount of ethyl silicone oil can effectively reduce the viscosity of crude oil;
fig. 3(e) effect of ethyl silicone oil content on crude oil viscosity at-18 ℃;
FIG. 3(f) Effect of ethyl silicone oil content on crude oil viscosity at-16 deg.C;
FIG. 3(g) Effect of ethyl silicone oil content on crude oil viscosity at-13 deg.C; analyzing the experimental data and as can be seen from fig. 3(a), the viscosity of the crude oil decreases rapidly with increasing temperature; on the other hand, while the temperature is raised, a certain mass of ethyl silicone oil is added, so that the viscosity of the crude oil can be further reduced, but as the temperature is raised, the addition of the ethyl silicone oil in a similar proportion has a reduction trend on the reduction effect of the viscosity of the crude oil, and under the condition, the use amount of the ethyl silicone oil is increased, so that the reduction effect of the viscosity of the crude oil can be enhanced;
FIG. 3(h) Effect of ethyl silicone oil content on crude oil viscosity at-10 deg.C; FIG. 3(i) Effect of increasing ethyl silicone oil content on crude oil viscosity at-10 deg.C;
fig. 3(j) effect of ethyl silicone oil content on crude oil viscosity at 0 ℃; fig. 3(k) effect of ethyl silicone oil content on crude oil viscosity at 10 ℃; FIG. 3(1) Effect of ethyl silicone oil content on crude oil viscosity at 30 deg.C.
As can be seen, the addition of ethyl silicone oil can reduce the viscosity of the crude oil at different temperatures, but the influence of ethyl silicone oil on the viscosity of the crude oil is gradually reduced as the temperature is increased.
TABLE 1
Example 35 example 92
Crude oil blends were prepared as described in example 3, using hexaethylcyclotrisiloxane in place of the ethylsilicone oil prepared in preparation 1, and were homogeneously mixed with crude oil in various mass ratios as shown in tables 2 to 8.
Test example 4: viscosity reduction experiment of hexaethylcyclotrisiloxane on crude oil
(1) Viscosity of hexaethylcyclotrisiloxane as a function of temperature
The melting point of hexaethylcyclotrisiloxane is 14 deg.C, and when the temperature is lower than this value, hexaethylcyclotrisiloxane will crystallize and its viscosity cannot be measured. The viscosity of m-hexaethylcyclotrisiloxane at 20-50 ℃ was measured using a rotational viscometer of the DV2TRVTJO type with a spindle suitable for the viscosity measurement range, and the results are shown in FIG. 4 (a).
(2) Effect of hexaethylcyclotrisiloxane amount on crude oil viscosity
When the hexaethylcyclotrisiloxane/crude oil mass ratio increased from 0 to 0.4038 at-20 ℃, the viscosity of the crude oil decreased from 11230mpa.s to 1707mpa.s, the effect of hexaethylcyclotrisiloxane/crude oil mass ratio on crude oil viscosity is shown in table 2, and fig. 4(b) is the effect of hexaethylcyclotrisiloxane usage on crude oil viscosity (T-20 ℃).
Table 2:
| hexaethylcyclotrisiloxane/crude oil mass ratio | viscosity/mPa.s | Viscosity reduction amplitude/%) | Temperature of | |
| 0 | 11230 | 0 | -20 | |
| Example 35 | 0.0054 | 10680 | 4.9 | -20 |
| Example 36 | 0.0101 | 10340 | 7.93 | -20 |
| Example 37 | 0.0206 | 8617 | 23.27 | -20 |
| Example 38 | 0.0323 | 6875 | 38.78 | -20 |
| Example 39 | 0.0418 | 5580 | 50.31 | -20 |
| Example 40 | 0.0533 | 4758 | 57.63 | -20 |
| EXAMPLE 41 | 0.0497 | 5483 | 51.18 | -20 |
| Example 42 | 0.1002 | 3331 | 70.34 | -20 |
| Example 43 | 0.1516 | 2760 | 75.42 | -20 |
| Example 44 | 0.2023 | 2103 | 81.27 | -20 |
| Example 45 | 0.3028 | 1900 | 83.08 | -20 |
| Example 46 | 0.4034 | 1707 | 84.8 | -20 |
When the hexaethylcyclotrisiloxane/crude oil mass ratio increased from 0 to 0.3061 at-10 ℃, the viscosity of the crude oil decreased from 616mpa.s to 271mpa.s, the effect of hexaethylcyclotrisiloxane/crude oil mass ratio on crude oil viscosity is shown in table 3, and fig. 4(c) is the effect of hexaethylcyclotrisiloxane usage on crude oil viscosity (T-10 ℃).
TABLE 3
| Hexaethylcyclotrisiloxane/crude oil mass ratio | viscosity/mPa.s | Viscosity reduction amplitude/%) | Temperature of | |
| 0 | 616 | 0 | -10 | |
| Example 47 | 0.0051 | 594 | 3.57 | -10 |
| Example 48 | 0.0096 | 584 | 5.19 | -10 |
| Example 49 | 0.0199 | 553 | 10.23 | -10 |
| Example 50 | 0.031 | 535 | 13.15 | -10 |
| Example 51 | 0.0427 | 522 | 15.26 | -10 |
| Example 52 | 0.0544 | 505 | 18.02 | -10 |
| Example 53 | 0.1055 | 450 | 26.95 | -10 |
| Example 54 | 0.1558 | 408 | 33.77 | -10 |
| Example 55 | 0.2061 | 354 | 42.53 | -10 |
| Example 56 | 0.255 | 302.1 | 50.96 | -10 |
| Example 57 | 0.3061 | 271 | 56.01 | -10 |
When the hexaethylcyclotrisiloxane/crude oil mass ratio increased from 0 to 0.4302 at 0 ℃, the viscosity of the crude oil decreased from 164.3mpa.s to 73.25mpa.s, the effect of hexaethylcyclotrisiloxane/crude oil mass ratio on crude oil viscosity is shown in table 4, and fig. 4(d) is the effect of hexaethylcyclotrisiloxane dosage on crude oil viscosity (T0 ℃).
TABLE 4
When the hexaethylcyclotrisiloxane/crude oil mass ratio increased from 0 to 0.4299 at T ═ 10 ℃, the viscosity of the crude oil decreased from 75.5mpa.s to 37.25mpa.s, the effect of hexaethylcyclotrisiloxane/crude oil mass ratio on crude oil viscosity is shown in table 5, and fig. 4(e) is the effect of hexaethylcyclotrisiloxane dosage on crude oil viscosity (T ═ 10 ℃).
TABLE 5
| Hexaethylcyclotrisiloxane/crude oil mass ratio | viscosity/mPa.s | Viscosity reduction amplitude/%) | Temperature of | |
| 0 | 75.5 | 0 | 10 | |
| Example 69 | 0.0528 | 59.5 | 21.19 | 10 |
| Example 70 | 0.1124 | 57.25 | 24.17 | 10 |
| Example 71 | 0.1773 | 53 | 29.8 | 10 |
| Example 72 | 0.2511 | 48.5 | 35.76 | 10 |
| Example 73 | 0.3347 | 44.5 | 41.06 | 10 |
| Example 74 | 0.4299 | 37.25 | 50.66 | 10 |
When the hexaethylcyclotrisiloxane/crude oil mass ratio increased from 0 to 0.429 at T ═ 20 ℃, the viscosity of the crude oil decreased from 39mpa.s to 23.5mpa.s, the effect of hexaethylcyclotrisiloxane/crude oil mass ratio on the crude oil viscosity is shown in table 6, and fig. 4(f) is the effect of hexaethylcyclotrisiloxane dosage on the crude oil viscosity (T ═ 20 ℃).
TABLE 6
When the hexaethylcyclotrisiloxane/crude oil mass ratio increased from 0 to 0.4286 at 30 ℃, the viscosity of the crude oil decreased from 20.79mpa.s to 15.3mpa.s, the effect of hexaethylcyclotrisiloxane/crude oil mass ratio on crude oil viscosity is shown in table 7, and fig. 4(g) is the effect of hexaethylcyclotrisiloxane usage on crude oil viscosity (T30 ℃).
TABLE 7
| Hexaethylcyclotrisiloxane/crude oil mass ratio | viscosity/mPa.s | Viscosity reduction amplitude/%) | Temperature of | |
| 0 | 20.79 | 0 | 30 | |
| Example 81 | 0.0526 | 20.44 | 1.68 | 30 |
| Example 82 | 0.1111 | 20.26 | 2.55 | 30 |
| Example 83 | 0.1766 | 18.98 | 8.71 | 30 |
| Example 84 | 0.2505 | 17.12 | 17.65 | 30 |
| Example 85 | 0.3335 | 16 | 23.04 | 30 |
| Example 86 | 0.4286 | 15.3 | 26.41 | 30 |
When the hexaethylcyclotrisiloxane/crude oil mass ratio increased from 0 to 0.4287 at 40 ℃, the viscosity of the crude oil decreased from 15.68mpa.s to 11.68mpa.s, the effect of hexaethylcyclotrisiloxane/crude oil mass ratio on crude oil viscosity is shown in table 8, and fig. 4(h) is the effect of hexaethylcyclotrisiloxane usage on crude oil viscosity (T40 ℃).
TABLE 8
The data of the crude oil viscosity measured at different temperatures along with the change of the hexaethylcyclotrisiloxane/crude oil mass ratio show that the crude oil viscosity is gradually reduced along with the addition of the hexaethylcyclotrisiloxane; the lower the temperature is, the more remarkable the influence of hexaethylcyclotrisiloxane on the viscosity of the crude oil is, and the better the viscosity reduction effect of the crude oil is after hexaethylcyclotrisiloxane is added.
Example 93 example 102
Clear and transparent light crude oil without impurities is taken out at room temperature, the trimethyl siloxy terminated polydiethylsiloxane oligomer (ethyl silicone oil for short) prepared in preparation example 2 is added, and the mass ratio of ethyl silicone oil/crude oil is shown in table 9 and is uniformly mixed.
The light crude oil mixed with ethyl silicone oil prepared in example 93-example 102 was placed in a sample measuring tube of a rotational viscometer of the DV2TRVTJO type, the appropriate spindle and shear rate were selected, the temperature of an external cryostat was set, the viscosity of the ethyl silicone oil/crude oil mixture was measured after the temperature in the sample measuring tube reached the set value, and the measurement results were recorded after the viscosity values stabilized, as shown in Table 9.
TABLE 9
| Ethyl silicone oil/crude oil mass ratio | Viscosity reduction amplitude/%) | Temperature of | |
| Example 93 | 0.005 | 13.11 | -20 |
| Example 94 | 0.01 | 26.84 | -20 |
| Example 95 | 0.02 | 38.45 | -20 |
| Example 96 | 0.035 | 61.12 | -20 |
| Example 97 | 0.04 | 63.31 | -20 |
| Example 98 | 0.05 | 72.67 | -20 |
| Example 99 | 25×10-6 | 11.61 | -20 |
| Example 100 | 48×10-6 | 15.47 | -20 |
| Example 101 | 72×10-6 | 19.86 | -20 |
| Example 102 | 99×10-6 | 22.74 | -20 |
Example 103 to example 112
Clear and transparent light crude oil containing no impurities was taken out at room temperature, and trimethylsiloxy-terminated poly (dimethyl-diethyl) siloxane oligomer (ethyl silicone oil for short) prepared in preparation example 3 was added thereto, and the mass ratio of ethyl silicone oil/crude oil was as shown in Table 10, followed by uniform mixing.
The light crude oil mixed with ethyl silicone oil prepared in example 103 to example 112 was placed in a sample measuring tube of a rotational viscometer of the DV2TRVTJO type, appropriate spindle and shear rate were selected, the temperature of an external cryostat was set, the viscosity of the ethyl silicone oil/crude oil mixture was measured after the temperature in the sample measuring tube reached the set value, and the measurement results were recorded after the viscosity values stabilized, as shown in table 10.
| Ethyl silicone oil/crude oil mass ratio | Viscosity reduction amplitude/%) | Temperature of | |
| Example 103 | 0.005 | 12.23 | -20 |
| Example 104 | 0.01 | 25.31 | -20 |
| Example 105 | 0.02 | 36.79 | -20 |
| Example 106 | 0.035 | 59.54 | -20 |
| Example 107 | 0.04 | 62.64 | -20 |
| Example 108 | 0.05 | 71.59 | -20 |
| Example 109 | 26×10-6 | 11.21 | -20 |
| Example 110 | 51×10-6 | 14.97 | -20 |
| Example 111 | 71×10-6 | 18.91 | -20 |
| Example 112 | 103×10-6 | 21.91 | -20 |
Example 113 example 122
Clear and transparent light crude oil containing no impurities was taken out at room temperature, and the trimethylsiloxy-terminated poly (dimethyl-diethyl) siloxane oligomer (ethyl silicone oil for short) prepared in preparation example 4 was added thereto, and the mass ratio of ethyl silicone oil/crude oil was as shown in Table 11, followed by uniform mixing.
The light crude oil mixed with ethyl silicone oil prepared in example 113 to example 122 was placed in a sample measuring tube of a rotational viscometer of the DV2TRVTJO type, appropriate spindle and shear rate were selected, the temperature of an external cryostat was set, the viscosity of the ethyl silicone oil/crude oil mixture was measured after the temperature in the sample measuring tube reached the set value, and the measurement results were recorded after the viscosity values stabilized, as shown in table 11.
TABLE 11
Example 123 example 133
Crude oil blends were prepared as described in example 3, replacing ethyl silicone oil prepared in preparation example 1 with octaethylcyclotetrasiloxane and homogeneously mixed with crude oil in various mass ratios as shown in Table 12.
When the octamethylcyclotetrasiloxane/crude oil mass ratio increased from 0 to 0.4000 at-20 ℃, the viscosity of the crude oil decreased from 11230mpa.s to 1958mpa.s, and the effect of the octaethylcyclotetrasiloxane/crude oil mass ratio on the viscosity of the crude oil is shown in table 12.
Table 12:
| octaethylcyclotetrasiloxane to crude oil mass ratio | viscosity/mPa.s | Viscosity reduction amplitude/%) | Temperature of | |
| 0 | 11230 | 0 | -20 | |
| Example 123 | 0.0050 | 10710 | 4.63 | -20 |
| Example 124 | 0.0100 | 10410 | 7.3 | -20 |
| Example 125 | 0.0201 | 8655 | 22.93 | -20 |
| Example 126 | 0.0305 | 6920 | 38.38 | -20 |
| Example 127 | 0.0402 | 5670 | 49.51 | -20 |
| Example 128 | 0.0500 | 4862 | 56.71 | -20 |
| Example 129 | 0.1000 | 5623 | 49.93 | -20 |
| Example 130 | 0.1500 | 3471 | 69.09 | -20 |
| Example 131 | 0.2000 | 2906 | 74.12 | -20 |
| Example 132 | 0.3000 | 2264 | 79.84 | -20 |
| Example 133 | 0.4000 | 1958 | 82.56 | -20 |
Examples 134 to 144
Crude oil blends were prepared as described in example 3, substituting decaethylcyclopentasiloxane for the ethyl silicone oil prepared in preparation 1, and homogeneously mixed with crude oil in various mass ratios as shown in Table 13.
When the decaethylcyclopentasiloxane/crude oil mass ratio increased from 0 to 0.4000 at-20 ℃, the viscosity of the crude oil decreased from 11230mpa.s to 2164mpa.s, and the effect of the decaethylcyclopentasiloxane/crude oil mass ratio on the viscosity of the crude oil is shown in table 13.
Table 13:
| decaethylcyclopentasiloxane/crude oil mass ratio | viscosity/mPa.s | Viscosity reduction amplitude/%) | Temperature of | |
| 0 | 11230 | 0 | -20 | |
| Example 134 | 0.0050 | 10980 | 2.23 | -20 |
| Example 135 | 0.0100 | 10560 | 5.97 | -20 |
| Example 136 | 0.0200 | 8823 | 21.43 | -20 |
| Example 137 | 0.0300 | 7061 | 37.12 | -20 |
| Example 138 | 0.0402 | 5734 | 48.94 | -20 |
| Example 139 | 0.0500 | 4994 | 55.53 | -20 |
| Example 140 | 0.1000 | 5762 | 48.69 | -20 |
| Example 141 | 0.1500 | 3605 | 67.9 | -20 |
| Example 142 | 0.2000 | 2994 | 73.34 | -20 |
| Example 143 | 0.3000 | 2431 | 78.35 | -20 |
| Example 144 | 0.4000 | 2164 | 80.73 | -20 |
Example 145 example 155
The crude oil mixture was prepared as described in example 3, substituting dodecaethylcyclohexasiloxane for the ethylsilicone oil prepared in preparation example 1, and uniformly mixed with crude oil at various mass ratios shown in Table 14.
When the mass ratio of dodecaethylcyclohexasiloxane/crude oil at T ═ 20 ℃ was increased from 0 to 0.4000, the viscosity of the crude oil was reduced from 11230mpa.s to 2286mpa.s, and the effect of the dodecaethylcyclohexasiloxane/crude oil mass ratio on the viscosity of the crude oil is shown in table 14.
Table 14:
| decadiethyl cyclohexasiloxane/crude oil mass ratio | viscosity/mPa.s | Viscosity reduction amplitude/%) | Temperature of | |
| 0 | 11230 | 0 | -20 | |
| Example 145 | 0.0050 | 10920 | 2.76 | -20 |
| Example 146 | 0.0100 | 10610 | 5.52 | -20 |
| Example 147 | 0.0200 | 8850 | 21.19 | -20 |
| Example 148 | 0.0300 | 7180 | 36.06 | -20 |
| Example 149 | 0.0402 | 5864 | 47.78 | -20 |
| Example 150 | 0.0500 | 5026 | 55.24 | -20 |
| Example 151 | 0.1000 | 5906 | 47.41 | -20 |
| Example 152 | 0.1500 | 3784 | 66.3 | -20 |
| Example 153 | 0.2000 | 3055 | 72.8 | -20 |
| Example 154 | 0.3000 | 2593 | 76.91 | -20 |
| Example 155 | 0.4000 | 2286 | 79.64 | -20 |
Comparative example 2
(1) Change of viscosity of dimethicone with temperature
Selecting trimethylsiloxy end-blocked polydimethylsiloxane (abbreviated as dimethicone, eta) with a viscosity number similar to that of the ethyl silicone oil synthesized in preparation example 12050mpa.s), using a rotational viscometer model DV2TRVTJ0, and matching the appropriate viscosity measurement rangeThe rotor (2) was measured for the change in viscosity of the dimethylsilicone fluid at-20 to 40 ℃ depending on the temperature, and the results are shown in FIG. 5 (a).
(2) Effect of Dimethicone on crude oil viscosity
The procedure of preparing a crude oil mixture as described in example 3 was followed, except that the ethyl silicone oil prepared in example 1 was replaced with a commercially available dimethyl silicone oil having a viscosity of 50mPa.s at 20 ℃ and mixed with crude oil at various mass ratios, and then the viscosities of the hexaethylcyclotrisiloxane/crude oil mixtures were measured at-20 ℃, -10 ℃, 0 ℃, 10 ℃, 20 ℃, 30 ℃ and 40 ℃ respectively, as shown in FIGS. 5(b) to 5 (h).
As can be seen from fig. 5(b) to 5(e) (corresponding to the temperature range of-20 ℃ to 10 ℃), the viscosity of the simethicone/crude oil mixture is gradually reduced with the increase of the mass ratio of the simethicone/crude oil between-20 ℃ and 10 ℃, and the influence of the addition of the simethicone on the viscosity of the crude oil is more obvious when the temperature is lower; however, when the temperature is increased, as shown in FIGS. 5(f) to 5(h) (corresponding to the temperature range of 20 ℃ to 40 ℃), the viscosity of the dimethicone/crude oil mixture increases with the increase in the dimethicone/crude oil quality ratio, indicating that the addition of dimethicone did not reduce the viscosity of the crude oil, and the trend was completely opposite to that of the example of the present invention.
Because the viscosity-temperature coefficient of the dimethyl silicone oil is small, the viscosity of the dimethyl silicone oil does not change greatly along with the temperature, and the viscosity of the crude oil changes remarkably along with the temperature, the dimethyl silicone oil mainly plays a role in diluting the viscosity of the crude oil at low temperature; after the temperature is increased, the viscosity of the simethicone does not change greatly, but the viscosity of the crude oil is reduced rapidly, and when the viscosity of the crude oil is lower than that of the simethicone at the temperature, the viscosity of the simethicone/crude oil mixture is increased along with the increase of the mass ratio of the simethicone to the crude oil, which shows that the simethicone cannot effectively reduce the viscosity of the crude oil.
Comparative example 1 shows that since dimethylsilicone oil is also poorly compatible with crude oil, dimethylsilicone oil does not have the effect of lowering the viscosity of crude oil as in ethylsilicone oil and hexaethylcyclotrisiloxane.
Because crude oil contains volatile substances, there may be errors in the measurement process,without altering the addition of a compound containing a diethylsiloxy unit (- (C)2H5)2SiO-) cyclic siloxane or diethylsiloxane segment (- (C)2H5)2The polymer of SiO-) has the reduced viscosity tendency of crude oil.
Claims (7)
1. A method for reducing the viscosity of crude oil, characterized in that cyclosiloxane containing diethylsiloxy units or a polymer of diethylsiloxy units is mixed with the crude oil.
2. The method for reducing the viscosity of crude oil according to claim 1, wherein the cyclosiloxane containing diethylsiloxane chain units is one or more selected from hexaethylcyclotrisiloxane, octaethylcyclotetrasiloxane, decaethylcyclopentasiloxane, and dodecaethylcyclohexasiloxane.
3. The method of claim 1, wherein the polymer containing diethylsiloxane chain units is selected from the group consisting of an oligomericsiloxane of formula (I) and a copolysiloxane of formula (II),
in the formulae (I) and (II), R1、R4Each independently selected from Me and Me3SiO-, Et and Ph; r2、R3、R5、R6Each independently selected from one of Me and Et; ra、RbAre respectively and independently selected from one of methyl, ethyl, trifluoropropyl and phenyl, and RaAnd RbIs not ethyl or trifluoropropyl at the same time;
wherein n is 1 to 100,
in the formula (II) x1＝1～30，x21 to 100, and x1+x2＝1～120。
4. The method for reducing the viscosity of crude oil according to claim 3, wherein the viscosity of the oligomeric siloxane containing diethylsiloxane chain units at 20 ℃ is 5 to 500 mPa.s.
5. The method for reducing the viscosity of crude oil according to claim 3, wherein the viscosity of the copolysiloxane containing diethylsiloxane chain units at 20 ℃ is 5 to 1000 mPa.s.
6. The method for reducing the viscosity of crude oil according to any one of claims 1 to 5, wherein the mass ratio of the cyclic siloxane containing diethyl siloxane chain segments or the polymer containing diethyl siloxane chain segments when mixed with the crude oil is 0.000005-0.50: 1.
7. The method for reducing the viscosity of crude oil according to claim 6, wherein the temperature of the mixture of the cyclic siloxane containing diethylsiloxane chain segments or the polymer containing diethylsiloxane chain segments and the crude oil is-40 to 60 ℃.
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