CN115504469A - System and method for converting carbon dioxide by using water-assisted plasma and photocatalyst in cooperation manner - Google Patents
System and method for converting carbon dioxide by using water-assisted plasma and photocatalyst in cooperation manner Download PDFInfo
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- CURLTUGMZLYLDI-UHFFFAOYSA-N Carbon dioxide Chemical compound O=C=O CURLTUGMZLYLDI-UHFFFAOYSA-N 0.000 title claims abstract description 60
- 238000000034 method Methods 0.000 title claims abstract description 36
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- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B32/00—Carbon; Compounds thereof
- C01B32/40—Carbon monoxide
Abstract
The invention relates to a system and a method for converting carbon dioxide by using water-assisted plasma and a photocatalyst in a synergistic manner, and belongs to CO 2 The technical field of comprehensive utilization. The invention provides a method for converting carbon dioxide by the cooperation of water-assisted plasma and a photocatalyst, which comprises the following steps: introducing CO 2 CO in the gas collecting bottle 2 Regulating the flow, CO, by means of a gas flowmeter 2 Then enters the bubbler through the air inlet end of the bubbler, heats the temperature of the bubbler and introduces CO 2 CO-regulating the steam flow, CO 2 And carrying water vapor to enter the plasma reaction device filled with the photocatalyst from the air outlet end of the bubbler for reaction, collecting the generated CO through a gas receiving device, and simultaneously adjusting the power of the plasma reaction device by adopting a plasma power generator. The method introduces cheap water vapor into high-energy plasma generated by electric energy and environment-friendly photocatalyst to improve the conductivity of the surface of the photocatalyst, thereby realizing CO together 2 High efficiency conversion to CO.
Description
Technical Field
The invention belongs to CO 2 Comprehensive utilization technical fieldThe patent refers to the field of 'treatment of water, waste water, sewage, or sludge'.
Background
The combustion of fossil fuels such as coal and petroleum in large quantities is accompanied by large quantities of CO while bringing economic effects 2 And (4) discharging. In recent years, CO is used 2 The emission of a large amount of the waste water causes the problems of species decrease, sea level rise, global temperature rise and the like to be increasingly highlighted, so that the waste water is highly valued by countries in the world.
CO 2 Has extremely high thermal stability, only 1.8 percent of the carbon dioxide is decomposed at 2000 ℃, so how to efficiently convert and utilize CO 2 Become a hotspot and a difficulty of the current research. Breaking off CO 2 The energy required by carbon-oxygen bond in molecule is 5.5eV, while the average energy of high-energy particles in low-temperature plasma can reach 10eV, and the high-energy particles are enough to dissociate and activate CO under the conditions of room temperature and normal pressure 2 A molecule. Changing it from stable state to unstable vibration excited state to promote CO 2 The transformation of (3). Individual plasma reforming systems produce products with uncertainty and low selectivity to the target product under different reaction conditions. In order to ensure the certainty of a target product, a photocatalyst absorbing renewable energy source-sunlight can be combined with a plasma conversion system to catalyze CO 2 Generating CO or CH 4 Chemical products with high added value. Although CO is ensured 2 The conversion to high value-added chemical products such as CO and the like is realized, but the conversion efficiency still has a great improvement space. Therefore, to respond to a national call, CO is minimized 2 The emission of the carbon dioxide has very important significance for converting the carbon dioxide into high-value-added chemical products such as CO and the like as much as possible.
Disclosure of Invention
In view of the above, one of the objectives of the present invention is to provide a system for converting carbon dioxide by using water-assisted plasma and a photocatalyst; the invention also aims to provide a method for converting carbon dioxide by using the water-assisted plasma and the photocatalyst.
In order to achieve the purpose, the invention provides the following technical scheme:
1. a system for converting carbon dioxide by using water-assisted plasma and a photocatalyst in a synergistic manner comprises CO connected in sequence 2 The device comprises a gas collecting bottle 1, a gas flowmeter 2, a bubbler 3, a plasma reaction device 4 and a gas receiving device 5, wherein the plasma reaction device 4 is also sequentially connected with a plasma power generator 6 and an oscilloscope 7;
the gas inlet end of the bubbler 3 is connected with the gas flowmeter 2, and the gas outlet end is connected with the plasma reaction device 4.
Preferably, the plasma reaction device is a dielectric barrier discharge plasma reaction device.
Preferably, the power of the plasma power generator is set to be 50W or more.
2. A method for the co-operative conversion of carbon dioxide using a water-assisted plasma and a photocatalyst, said method being carried out using said system, said method comprising the steps of:
the flow of carbon dioxide in a carbon dioxide gas collecting bottle 1 is regulated through a gas flowmeter 2, the carbon dioxide enters a bubbler 3 through an air inlet end of the bubbler 3, the bubbler 3 regulates the flow of water vapor, then the carbon dioxide carries the water vapor to enter a plasma reaction device 4 filled with a photocatalyst from an air outlet end of the bubbler 3, and the plasma photocatalytic reaction is carried out to ensure that CO is subjected to the plasma photocatalytic reaction 2 Converted into CO, the generated CO is collected by a gas receiving device 5, while the power of the plasma reaction device 4 is regulated by a plasma power generator 6.
Preferably, the calculation formula of the power in the power of the plasma power generator 6 for adjusting the power of the plasma reaction device 4 is as follows: p = S × f × C,
where P is power, in units of W; s is the integral area of the voltage of the sampling capacitor to the applied voltage in a period, and the unit is V 2 (ii) a f is the discharge frequency in Hz; c is a sampling capacitor with the unit of F;
the voltage and the discharge frequency are detected by an oscilloscope 7.
Preferably, the water vapor is prepared by a bubbling method.
Preferably, the ratio of the flow rate of the carbon dioxide entering the bubbler 3 through the gas inlet end of the bubbler 3 to the flow rate of the steam adjusted by the bubbler 3 is 20: 1.13-50: 2.18.
Preferably, the reaction time of the plasma photocatalytic reaction is more than 10 min.
Preferably, the photocatalyst is a perovskite; the perovskite is Cs 2 SnCl 6 Perovskite.
Preferably, the amount of the photocatalyst is 5mg or more.
Further preferably, the amount of the photocatalyst is 10mg.
The invention has the beneficial effects that: the invention provides a system and a method for converting carbon dioxide by using water-assisted plasma and a photocatalyst in a synergistic manner. When CO is present 2 After the water vapor and the water vapor are simultaneously introduced into a plasma reaction device filled with the photocatalyst, the water vapor can be adsorbed on the surface of the photocatalyst under the action of an external electric field to improve the surface conductivity of the photocatalyst, so that the transfer charge, the discharge charge and the peak-to-peak charge of discharge can be increased, and the occurrence probability of physical and chemical reactions in an air gap is promoted. In addition, the water vapor can increase the micro-discharge times and the micro-discharge time. Thus, CO conversion in plasma with photocatalyst 2 On the basis of the method, the CO can be further promoted by introducing water vapor 2 The conversion of (a). The method introduces cheap steam into high-energy plasma generated by electric energy and environment-friendly photocatalyst to improve the conductivity of the surface of the photocatalyst, thereby realizing CO 2 Efficient conversion to CO.
Additional advantages, objects, and features of the invention will be set forth in part in the description which follows and in part will become apparent to those having ordinary skill in the art upon examination of the following or may be learned from practice of the invention. The objectives and other advantages of the invention will be realized and attained by the structure particularly pointed out in the written description and claims thereof.
Drawings
For the purposes of promoting a better understanding of the objects, aspects and advantages of the invention, reference will now be made to the following detailed description taken in conjunction with the accompanying drawings in which:
FIG. 1 shows the CO-conversion of water-assisted plasma with a photocatalyst 2 The system of (1);
FIG. 2 shows the photocatalyst Cs observed under a scanning electron microscope 2 SnCl 6 The microstructure of (a);
FIG. 3 shows the CO-conversion of water-assisted plasma and photocatalyst in example 2 2 The system lissajous figure;
FIG. 4 shows the CO conversion by the cooperation of the plasma and the photocatalyst in comparative example 1 2 The system lissajous figure;
FIG. 5 shows the CO conversion by plasma alone in comparative example 3 2 The system lissajous figure;
FIG. 6 shows the CO conversion of water-assisted plasma and photocatalyst in example 2 2 Voltage current diagram of time discharge;
FIG. 7 shows the CO-conversion of plasma with photocatalyst in comparative example 1 2 Voltage current diagram of time discharge;
FIG. 8 shows the CO conversion by plasma alone in comparative example 3 2 Voltage current diagram of time discharge;
wherein 1 is CO 2 A gas collection bottle; 2 is a gas flowmeter; 3 is a bubbler; 4 is a plasma reaction device; 5 is a gas receiving device; 6 is a plasma power generator; and 7 is an oscilloscope.
Detailed Description
The embodiments of the present invention are described below with reference to specific embodiments, and other advantages and effects of the present invention will be easily understood by those skilled in the art from the disclosure of the present specification. The invention is capable of other and different embodiments and of being practiced or of being carried out in various ways, and its several details are capable of modification in various respects, all without departing from the spirit and scope of the present invention. It should be noted that the drawings provided in the following embodiments are only for illustrating the basic idea of the present invention in a schematic way, and the features in the following embodiments and embodiments may be combined with each other without conflict.
Example 1
CO is carried out by adopting a system (shown in figure 1) for converting carbon dioxide by using water-assisted plasma and photocatalyst in a synergistic way 2 The transformation is specifically as follows:
CO 2 CO in the gas collecting bottle 2 The flow is adjusted by a gas flowmeter, enters the bubbler through the gas inlet end of the bubbler, and the bubbler adjusts the flow of water vapor to convert CO into CO 2 The flow rate entering the bubbler through the gas inlet end of the bubbler and the flow ratio of the water vapor regulated by the bubbler are regulated to be 50.18, and the carbon dioxide carrying the water vapor enters the reactor filled with 5mg of photocatalyst Cs from the gas outlet end of the bubbler 2 SnCl 6 The dielectric barrier discharge plasma reaction device performs plasma photocatalytic reaction for 10min, generated CO is collected by the gas receiving device, and meanwhile, the power of the plasma reaction device is adjusted to 60W by the plasma power generator.
Example 2
5mg of the photocatalyst Cs in example 1 2 SnCl 6 Changed to 10mg of photocatalyst Cs 2 SnCl 6 The rest of the procedure was the same as in example 1.
Example 3
5mg of the photocatalyst Cs in example 1 2 SnCl 6 Changed to 15mg of photocatalyst Cs 2 SnCl 6 The rest of the procedure was the same as in example 1.
Example 4
The plasma photocatalytic reaction in example 2 was changed from 10min to 40min, and the remaining steps were the same as in example 2.
Example 5
The power of the plasma reaction apparatus in example 2 was set to 60W to 50W, and the remaining steps were the same as in example 2.
Example 6
CO in example 2 2 The flow rate into the bubbler through the gas inlet end of the bubbler and the flow rate of the water vapor adjusted by the bubbler are adjusted to 50.18 to 20 to 1.13, and the rest steps are the same as in example 2.
Example 7
Will be described in example 2CO 2 The ratio of the flow rate into the bubbler through the inlet end of the bubbler to the flow rate of the water vapor adjusted by the bubbler was adjusted to 50.18 to 35 to 1.72, and the rest of the procedure was the same as in example 2.
Comparative example 1
CO 2 CO in gas collecting bottle 2 The flow rate is adjusted to 50mL/min by a gas flowmeter and the photocatalyst Cs filled with 10mg is introduced 2 SnCl 6 In the dielectric barrier discharge plasma reaction device, plasma photocatalytic reaction is carried out for 10min, the generated CO is collected by the gas receiving device, and meanwhile, the power of the plasma reaction device is adjusted to 60W by the plasma power generator.
Comparative example 2
The photocatalyst Cs in comparative example 1 was added 2 SnCl 6 By conversion to non-photocatalyst Al 2 O 3 The rest of the procedure was the same as in comparative example 1.
Comparative example 3
The photocatalyst in comparative example 1 was removed and the remaining procedure was the same as in comparative example 1.
Comparative example 4
10mg of photocatalyst Cs 2 SnCl 6 Adding into a photocatalytic testing device (Labsolar-III, beijing Perf ect Light Technology Co. Ltd. China), and introducing CO 2 And the pressure is kept at 90kPa, and the light is irradiated for 3 hours for carrying out the photocatalytic reduction of CO 2 And (4) reacting.
Comparative example 5
10mg of non-photocatalyst Al 2 O 3 Adding into a photocatalytic testing device (Labsolar-III, beijing Perf ect Light Technology Co. Ltd. China), and introducing CO 2 And the pressure is kept at 90kPa, and the light is irradiated for 3h for carrying out the photocatalytic reduction of CO 2 And (4) reacting.
The production of CO per minute of example 1 and comparative examples 1 to 5 was compared and tested in the following manner.
Method for testing and calculating CO yield per minute:
1. in the photocatalysis: after the illumination for 3 hours, the content of CO is detected by a gas chromatograph, and the yield is averaged to minutes to obtain the generation rate of CO.
2. In plasma photocatalysis: when the plasma discharge reaction is stable, gas collection is started, and no carbon deposition and CO deposition occur in the plasma reactor 2 The carbon in the reaction solution exists in the form of gas, the gas generated under each reaction condition is collected in the same time, 100 mu L of gas is collected and injected into a gas chromatographic column to detect the gas components and the content. The amount of CO in 100. Mu.L of gas was averaged up to minute to obtain the CO generation rate.
The results of tests comparing the yields of CO per minute of examples 1 to 7 with those of comparative examples 1 to 5 are shown in Table 1:
TABLE 1 CO production per minute under different catalytic conditions
As can be seen from Table 1, the current power, the reaction time and the CO 2 And H 2 When the flow ratio of O is fixed, only the dosage of the catalyst is changed, and when the dosage of the catalyst is respectively 5mg, 10mg and 15mg, the water-assisted plasma and the photocatalyst are used for synergistically converting CO 2 The amount of carbon monoxide converted per minute corresponds to 5.06X 10 4 μmol、6.02×10 4 μ mol and 5.84X 10 4 Mu mol, it can be seen that the water-assisted plasma and the photocatalyst synergistically convert CO 2 The optimal dosage of the catalyst is 10mg; when the power, the reaction time and the catalyst dosage are constant, only CO is changed 2 And H 2 Flow ratio of O when CO 2 And H 2 The flow ratio of O is 20:1.13, 35 2 The amount of CO converted per minute corresponds to 7.56X 10 4 μmol、6.64×10 4 μ mol, and 6.02X 10 4 Mu mol; when the reaction time, the amount of catalyst and CO 2 And H 2 When the flow rate ratio of O is constant, only the power is changed, and when the power is set to be 50W and 60W, the water-assisted plasma and the photocatalyst are cooperated to convert CO 2 The amount of CO converted per minute was 5.78X 10 4 And 6.02X 10 4 (ii) a Current power, catalyst amount and CO 2 And H 2 When the flow ratio of O is constant, only the reaction time is changed, but when the reaction time is 10min and 40min, the water-assisted plasma and the photocatalyst are used for cooperatively converting CO 2 The amount of CO converted per minute was 6.09X 10, respectively 4 And 6.02X 10 4 . Power, reaction time, catalyst amount and CO 2 CO conversion by water-assisted plasma and photocatalyst corresponding to different flow ratio of water vapor 2 The amount of CO change was also different, thus indicating that the water-assisted plasma and the photocatalyst synergistically converted CO 2 The reaction conditions of (a) have a crucial influence on the reaction. In addition, the plasma and the photocatalyst synergistically convert CO 2 The amount of CO converted per minute was 4X 10 4 Mu mol; synergistic conversion of CO by plasma and non-photocatalyst 2 The amount of CO converted per minute was 3.71X 10 4 Mu mol; plasma alone CO conversion 2 The amount of CO converted per minute was 2.70X 10 4 Mu mol; photocatalyst alone conversion of CO 2 The amount of CO converted per minute was 13.14X 10 -4 Mu mol; non-photocatalysts not having photocatalytic reduction of CO 2 The ability of the cell to perform. CO-conversion with plasma and photocatalyst 2 Compared with the prior art, the power is 60W, the reaction time is 10min, the dosage of the catalyst is 10mg, and CO is 2 And H 2 The flow ratio of O is 50 2 In the catalytic reaction of (2), introduction of water vapor causes CO 2 The amount of carbon monoxide converted per minute increased by 50.5%; and CO-conversion of CO by plasma and non-photocatalyst 2 In contrast, the introduction of water vapor results in CO 2 The amount of CO converted per minute was increased by 62.26%; CO conversion separate from plasma 2 In contrast, CO conversion by water-assisted plasma and photocatalyst 2 The amount of CO converted per minute increased 122.96%; photocatalyst alone conversion of CO 2 In contrast, CO conversion by water-assisted plasma and photocatalyst 2 The amount of CO converted per minute was 4.6X 10 of that 7 And (4) multiplying. It can be seen that a high-energy plasma, an environmentally friendly photocatalyst, and inexpensive water vapor generated from electrical energy are usedThe combined action can realize CO 2 High efficiency conversion to CO.
For prepared Cs 2 SnCl 6 The microstructure of the photocatalyst was measured by scanning electron microscopy and the results are shown in FIG. 2. From FIG. 2, it can be seen that Cs 2 SnCl 6 The photocatalyst has an irregular morphology.
CO conversion in example 2, comparative example 1 and comparative example 3, respectively 2 The energy efficiency of (2) was measured, and the experimental results are shown in fig. 3, 4 and 5, respectively. As can be seen from the figure, the water-assisted plasma and the photocatalyst synergistically convert CO 2 System (figure 3), CO-conversion of CO by plasma and photocatalyst 2 System (FIG. 4), plasma independent CO conversion 2 The peak-to-peak charge of the system (FIG. 5) was 532nC, 492nC, 420nC, respectively; the discharge charges were 276nC, 240nC, 220nC, respectively. Therefore, the introduction of the photocatalyst increases peak-to-peak charges and discharge charges, and is beneficial to the occurrence of physicochemical reactions in a discharge air gap; the introduction of water vapor further improves the peak-to-peak charge and the discharge charge of the reaction; further improve CO 2 Conversion rate and energy efficiency.
The voltage current during the plasma discharge reaction in example 2, comparative example 1 and comparative example 3 was measured, and the experimental results are shown in fig. 6, fig. 7 and fig. 8, respectively. Comparing FIG. 7 with FIG. 8, it can be seen that the photocatalyst is coupled with the plasma to convert CO 2 CO conversion by plasma alone 2 Has more discharge times and stronger discharge intensity. This shows that the introduction of the photocatalyst can obviously improve the micro-discharge times, thereby improving the CO 2 The conversion of (a). Comparing fig. 6 and fig. 7, it can be seen that the times and intensity of micro-discharges in the negative half period of the discharge are obviously better than those without introducing water vapor when water vapor is introduced into the photocatalyst-filled plasma reaction device. Thus, CO conversion in plasma with photocatalysis 2 On the basis of the method, the CO can be further promoted by introducing water vapor 2 The conversion of (a).
In summary, the present invention provides a synergistic conversion of water-assisted plasma and photocatalystA system and method for converting carbon dioxide. Under the action of an external electric field, water vapor can be adsorbed on the surface of the photocatalyst to improve the surface conductivity of the photocatalyst, transfer charges, discharge charges and peak-to-peak charges in plasma discharge reaction are increased, the occurrence probability of physicochemical reaction in an air gap is promoted, and the micro-discharge frequency and the micro-discharge time can be increased. CO-conversion with plasma and photocatalyst 2 In contrast, the introduction of water vapor results in CO 2 The amount of CO converted per minute increased by 50.5%. The method combines high-energy plasma generated by electric energy, environment-friendly photocatalyst and cheap steam to realize CO 2 Efficient conversion to CO.
Finally, the above embodiments are only intended to illustrate the technical solutions of the present invention and not to limit the present invention, and although the present invention has been described in detail with reference to the preferred embodiments, it will be understood by those skilled in the art that modifications or equivalent substitutions may be made on the technical solutions of the present invention without departing from the spirit and scope of the technical solutions, and all of them should be covered by the claims of the present invention.
Claims (10)
1. A system for converting carbon dioxide by using water-assisted plasma and a photocatalyst in a synergistic manner is characterized in that: the system comprises sequentially connected CO 2 The device comprises a gas collecting bottle (1), a gas flowmeter (2), a bubbler (3), a plasma reaction device (4) and a gas receiving device (5), wherein the plasma reaction device (4) is also sequentially connected with a plasma power generator (6) and an oscilloscope (7);
the gas inlet end of the bubbler (3) is connected with the gas flowmeter (2), and the gas outlet end of the bubbler is connected with the plasma reaction device (4).
2. The system of claim 1, wherein the water-assisted plasma and the photocatalyst are used for the co-conversion of carbon dioxide, and the system comprises: the plasma reaction device (4) is a dielectric barrier discharge plasma reaction device.
3. The system of claim 1, wherein the water-assisted plasma and the photocatalyst are used for the co-conversion of carbon dioxide, and the system comprises: the power of the plasma power generator (6) is set to be more than 50W.
4. A method for converting carbon dioxide by the cooperation of water-assisted plasma and a photocatalyst is characterized in that: the method is carried out by using the system of any one of claims 1 to 3, and comprises the following steps:
introducing CO 2 CO in the gas collecting bottle (1) 2 The flow is adjusted by the gas flowmeter (2), enters the bubbler (3) through the air inlet end of the bubbler (3), the bubbler (3) adjusts the flow of water vapor, and then CO 2 The vapor carried by the gas enters a plasma reaction device (4) filled with photocatalyst from the gas outlet end of the bubbler (3) for plasma photocatalytic reaction to lead CO to be generated 2 The CO is converted into CO, the generated CO is collected by a gas receiving device (5), and the power of the plasma reaction device (4) is adjusted by a plasma power generator (6).
5. The method of claim 4, wherein the water-assisted plasma and the photocatalyst are used in combination to convert carbon dioxide, and the method comprises the following steps: the calculation formula of the power in the power of the plasma power generator (6) for adjusting the plasma reaction device (4) is as follows: p = S × f × C,
where P is power, in units of W; s is the integral area of the voltage of the sampling capacitor to the applied voltage in a period, and the unit is V 2 (ii) a f is the discharge frequency in Hz; c is a sampling capacitor with the unit of F;
the voltage and the discharge frequency are detected by an oscilloscope (7).
6. The method of claim 4, wherein the water-assisted plasma and the photocatalyst are used for the co-transformation of carbon dioxide, and the method comprises the following steps: the water vapor is prepared by a bubbling method.
7. The synergistic conversion of water-assisted plasma and photocatalyst as claimed in claim 4A method for converting carbon dioxide, characterized by: said CO 2 The flow rate entering the bubbler (3) through the air inlet end of the bubbler (3) is regulated by the bubbler (3) to be 20: 2.18.
8. The method of claim 4, wherein the water-assisted plasma and the photocatalyst are used for the co-transformation of carbon dioxide, and the method comprises the following steps: the reaction time of the plasma photocatalytic reaction is more than 10 min.
9. The method of claim 4, wherein the water-assisted plasma and the photocatalyst are used in combination to convert carbon dioxide, and the method comprises the following steps: the photocatalyst is perovskite; the perovskite is Cs 2 SnCl 6 Perovskite.
10. The method of claim 4, wherein the water-assisted plasma and the photocatalyst are used for the co-transformation of carbon dioxide, and the method comprises the following steps: the dosage of the photocatalyst is more than 5 mg.
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Citations (16)
| Publication number | Priority date | Publication date | Assignee | Title |
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