CN114522645A - Nano-material multiphase photocatalytic microchannel reactor - Google Patents
Nano-material multiphase photocatalytic microchannel reactor Download PDFInfo
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- CN114522645A CN114522645A CN202210254240.9A CN202210254240A CN114522645A CN 114522645 A CN114522645 A CN 114522645A CN 202210254240 A CN202210254240 A CN 202210254240A CN 114522645 A CN114522645 A CN 114522645A
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J19/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
- B01J19/0093—Microreactors, e.g. miniaturised or microfabricated reactors
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J19/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
- B01J19/0053—Details of the reactor
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J19/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
- B01J19/08—Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor
- B01J19/12—Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor employing electromagnetic waves
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J8/00—Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes
- B01J8/008—Details of the reactor or of the particulate material; Processes to increase or to retard the rate of reaction
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J8/00—Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes
- B01J8/08—Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes with moving particles
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02W—CLIMATE CHANGE MITIGATION TECHNOLOGIES RELATED TO WASTEWATER TREATMENT OR WASTE MANAGEMENT
- Y02W10/00—Technologies for wastewater treatment
- Y02W10/30—Wastewater or sewage treatment systems using renewable energies
- Y02W10/37—Wastewater or sewage treatment systems using renewable energies using solar energy
Abstract
The invention discloses a nano-material multiphase photocatalytic microchannel reactor, which comprises a base body, a transparent upper cover and transparent quartz beads, wherein an accommodating tank is arranged in the base body, a wide-mouth-type upper notch communicated with the accommodating tank is formed in the upper surface of the base body, a gas-liquid-solid turbid liquid inlet communicated with the accommodating tank is formed in one side of the base body, a gas-liquid-solid turbid liquid outlet communicated with the accommodating tank is formed in the other side of the base body, the upper cover is detachably and hermetically fixed to the top of the base body to seal the upper notch and form a transparent optical window, the accommodating tank is filled with the quartz beads serving as fillers, and the quartz beads in the accommodating tank are tightly stacked to form a three-dimensional porous microchannel serving as a gas-solid-liquid three-phase channel and a photocatalytic reaction channel. The size of the size regulation and control microchannel of quartz beads is convenient to clean and easy to clear and block, and the problem that the traditional etching channel is not easy to clean and block and is scrapped is solved.
Description
Technical Field
The invention relates to the technical field of microfluidic heterogeneous catalysis, in particular to a nano-material heterogeneous photocatalytic microchannel reactor.
Background
At present, when microfluidics is used in the field of heterogeneous catalytic reaction, a solid-phase catalyst is fixed in a reactor, and a filter is used for blocking the front and the back of the catalyst to prevent the solid-phase catalyst from flowing. This approach requires that the catalyst particle size must be larger than the pore size of the filter. However, with the advent and extensive use of nanomaterial catalysts, the filters have been unable to achieve a baffling effect. The existing micro-channels are channels etched on a substrate, and due to the small size of the channels, the requirement on a processing process is high, so that the processing cost is high, and meanwhile, the cleaning cost is high and the maintenance is difficult; after the channel is formed, the modification such as diversion or size change cannot be carried out, if the method is applied to different or new heterogeneous catalytic reactions, a reactor needs to be manufactured again (mainly, the channel in the substrate needs to be etched again), but the etching processing period is long, and the experimental progress or the production progress is influenced; when the device is used, the nano catalyst directly enters the micro channel to quickly block the micro channel, and once the micro channel is blocked, the micro channel can not be dredged or repaired basically, so that the whole micro-fluidic device can not be used normally and can be directly scrapped when the micro-fluidic device is serious.
Disclosure of Invention
Therefore, the invention provides a nano material heterogeneous photocatalytic microchannel reactor, provides a new scheme for solving the problem of nano material gas-liquid-solid heterogeneous photocatalytic reaction in the field of microfluidics, is suitable for a reaction system in which a catalyst is a solid-phase nano particle and a reaction raw material is a liquid phase or a gas-liquid coexisting reaction system, and solves the technical problems of high processing cost, high cleaning cost, difficulty in modification, easiness in blocking, difficulty in cleaning and difficulty in maintenance of a microchannel.
In order to achieve the above purpose, the invention provides the following technical scheme:
the utility model provides a heterogeneous photocatalysis microchannel reactor of nano-material, includes base member, transparent upper cover and transparent quartz bead, be equipped with the holding tank in the base member, the upper surface of base member be equipped with notch on the wide-mouthed formula of holding tank intercommunication, one side of base member be equipped with the solid turbid liquid import of gas-liquid of holding tank intercommunication, the opposite side of base member be equipped with the solid turbid liquid export of gas-liquid of holding tank intercommunication, upper cover detachably seal fixation in the top of base member is in order to seal go up the notch and form transparent optical window, quartz bead fills up the holding tank, in the holding tank quartz bead closely piles up and forms three-dimensional porous microchannel in order to regard as gas-solid-liquid three-phase channel and photocatalysis reaction channel, size in order to regulate and control microchannel through the size of regulation and control quartz bead.
Further, the upper cover is detachably connected with the base body.
Further, still be equipped with the coolant liquid runner in the base member, the coolant liquid runner be located the downside of holding tank and with the holding tank does not communicate one side of base member be equipped with the coolant liquid import of coolant liquid runner intercommunication, the opposite side of base member be equipped with the coolant liquid export of coolant liquid runner intercommunication.
Further, still include transparent lower cover, the lower surface of base member be equipped with notch under the wide-mouthed formula of holding tank intercommunication, the lower cover is sealed to be fixed in the bottom of base member is in order to seal notch and formation transparent light window down.
Further, the lower cover is detachably connected with the base body.
The invention has the following advantages:
transparent quartz beads are used as fillers, the quartz beads are tightly packed in the containing cavity to form a three-dimensional porous microchannel, and the size of the microchannel is regulated by regulating the size of the quartz beads, so that compared with an etching channel, the microchannel is easy to manufacture, and is very simple to modify such as changing the channel or changing the size, and only the quartz beads with the other size need to be completely replaced; compared with a planar channel in the existing device, the microchannel formed by stacking the quartz beads is three-dimensional, and is four-way and eight-way, so that gas-liquid-solid suspension is not easy to block when flowing through the reactor; when cleaning, the upper cover is removed, the quartz beads are poured out, and the quartz beads can be cleaned in various ways (such as ultrasonic cleaning), so that the cleaning and maintenance are easy; if the sediment cannot be cleaned, the quartz beads can be directly replaced, the operation is convenient, and the whole device cannot be scrapped (the existing device cannot be scrapped when the blockage cannot be cleaned); when the gas-liquid-solid three-phase suspension passes through the reactor in a flowing mode, the gas-liquid-solid three-phase suspension flows through the three-dimensional porous micro-channel, and the gas-liquid-solid three-phase suspension is dispersed and mixed for multiple times, so that the mass transfer is promoted and the photocatalytic reaction is carried out at the same time; transparent quartz beads with uniform size are regularly arranged (regularly arranged after being filled), the whole reactor has good light transmission effect, light can penetrate through the quartz light window to irradiate the inside of the reactor, and the quartz beads do not influence the absorption of the catalyst to the light; in addition, when a double-sided illumination reactor is adopted, the photocatalytic reaction efficiency is higher.
Drawings
In order to more clearly illustrate the embodiments of the present invention or the technical solutions in the prior art, the drawings used in the description of the embodiments or the prior art will be briefly described below. It should be apparent that the drawings in the following description are merely exemplary, and that other embodiments can be derived from the drawings provided by those of ordinary skill in the art without inventive effort.
The structures, ratios, sizes, and the like shown in the present specification are only used for matching with the contents disclosed in the specification, so that those skilled in the art can understand and read the present invention, and do not limit the conditions for implementing the present invention, so that the present invention has no technical significance, and any structural modifications, changes in the ratio relationship, or adjustments of the sizes, without affecting the functions and purposes of the present invention, should still fall within the scope covered by the contents disclosed in the present invention.
FIG. 1 is a schematic diagram of a side view of a heterogeneous photocatalytic microchannel reactor made of nanomaterial provided in example 1;
FIG. 2 is a schematic top view of the heterogeneous photocatalytic microchannel reactor with nanomaterial provided in example 1;
FIG. 3 is a schematic cross-sectional view of a microchannel formed by quartz beads in the reactor provided in example 1;
FIG. 4 is a schematic view of another cross-section of a microchannel formed by quartz beads in the reactor provided in example 1;
FIG. 5 is a schematic diagram of a side view structure of another nanomaterial multiphase photocatalytic microchannel reactor provided in example 2.
In the figure: 1-substrate, 2-upper cover, 3-quartz beads, 4-gas-liquid-solid suspension inlet, 5-gas-liquid-solid suspension outlet, 6-cooling liquid flow channel, 7-cooling liquid inlet, 8-cooling liquid outlet and 9-lower cover.
Detailed Description
The present invention is described in terms of particular embodiments, other advantages and features of the invention will become apparent to those skilled in the art from the following disclosure, and it is to be understood that the described embodiments are merely exemplary of the invention and that it is not intended to limit the invention to the particular embodiments disclosed. All other embodiments, which can be derived by a person skilled in the art from the embodiments given herein without making any creative effort, shall fall within the protection scope of the present invention.
In the present specification, the terms "upper", "lower", "left", "right", "middle", and the like are used for clarity of description, and are not intended to limit the scope of the present invention, and changes or modifications in the relative relationship may be made without substantial changes in the technical content.
Example 1
As shown in fig. 1 and 2, example 1 provides a nanomaterial heterogeneous photocatalytic microchannel reactor comprising a substrate 1, a transparent upper cover 2, and transparent quartz beads 3.
The substrate 1 can be a cuboid made of stainless steel, and can also be made of other materials or in other solid geometrical shapes. A recess is as holding the holding tank that packs in the upper surface downward processing of cuboid, also can adopt the overall structure of casting mode processing base member 1 and holding tank. The holding tank is wide-mouthed form at the last notch of base member 1 upper surface, both made things convenient for processing or casting shaping, can increase illumination area or illumination passageway again. A gas-liquid-solid suspension inlet 4 is formed in the left side of the base body 1, is communicated with the containing tank and is a liquid inlet channel for gas-liquid-solid suspension; for connection to a pump or pumping line. A gas-liquid-solid suspension outlet 5 is arranged on the right side of the substrate 1, is communicated with the holding tank and is a liquid discharge channel for gas-liquid-solid suspension (mixed with a product); for connection to a centrifuge or separator or the like. A cooling liquid flow channel 6 is also arranged in the base body 1, and the cooling liquid flow channel 6 is positioned at the lower side of the accommodating groove and is not communicated with the accommodating groove; a cooling liquid inlet 7 communicated with the cooling liquid channel 6 is arranged on the left side of the base body 1, and a cooling liquid outlet 8 communicated with the cooling liquid channel 6 is arranged on the right side of the base body 1; the two coolant ports may be connected to a cooling circulator or a tap water pipe to perform sufficient cooling in a flow form.
The upper cover 2 is made of quartz, for example, a quartz plate, or may be made of a transparent material suitable for other experimental conditions. The upper cover 2 is detachably and hermetically fixed at the top of the base body 1, and seals the upper notch to avoid liquid leakage or air leakage; and simultaneously, a quartz light window is formed, so that light can penetrate and irradiate on the quartz beads 3 in the accommodating groove, and the light can be favorably irradiated to the surface of the catalyst. The upper cover 2 can be fixed on the base 1 by screws or bolts, and a sealing structure or device such as a sealing ring can be arranged between the upper cover 2 and the base 1.
The quartz beads 3 are used as filler to fill the accommodating tank, and the quartz beads 3 in the accommodating tank are tightly stacked to form a three-dimensional porous microchannel.
The quartz beads 3 are used as fillers, three-dimensional multi-channels with uniform apertures are formed in the reactor, and the multi-channels with different apertures are formed by controlling the sizes of the quartz beads 3. Gas-liquid reaction raw materials and solid-phase catalyst turbid liquid are pumped into the reactor together, the turbid liquid is formed through the multichannel stirring effect, and the gas-liquid-solid turbid liquid flows through the reactor in a uniform mode. The quartz light window is beneficial to the reaction of the suspension liquid under illumination. After the cooling liquid is introduced into the cooling liquid flow passage 6, the effect of cooling and keeping the temperature of the whole reactor constant is achieved. The structure plays a role of three-dimensional turbulence on turbid liquid formed by gas-liquid reaction raw materials and a solid-phase catalyst, the photocatalytic reaction is carried out while mass transfer is carried out, and the high-light-transmittance quartz beads 3 do not influence the absorption of the solid-phase catalyst on light.
As shown in FIGS. 3 and 4, the arrows indicate the flow direction of the gas-liquid-solid suspension. The pore diameters formed by different sizes of the quartz beads 3 are different in size, so that channels with specific pore diameters can be formed by the form of close packing of the quartz beads 3 with uniform sizes, and channels with different size requirements can be formed by using the quartz beads 3 with different sizes (uniform size or non-uniform size), and the channel sizes can be designed according to the size of the nano catalyst.
The method or scheme for using the reactor of this example: 1. filling quartz beads 3 with a target size in the reactor; 2. fixing the upper quartz optical window; 3. introducing cooling circulating water to control the temperature of the whole set of reactor; 4. injecting a mixture of gas-liquid reaction raw materials and a solid-phase catalyst into a reactor by a pump, forming multiple turbulence by stirring and disturbing gas-liquid-solid three-phase suspension in the reactor through quartz beads 3, and simultaneously carrying out a photocatalytic reaction under illumination; 5. pumping the reacted gas-solid-liquid three-phase suspension out of the reactor, centrifugally separating the catalyst, and detecting the gas-liquid phase.
The quartz beads 3 are arranged regularly to form multiple channels with uniform aperture sizes, the multiple channels are formed by layer-by-layer close packing, the high-permeability quartz beads 3 do not influence the absorption of the photocatalyst on light, gas-liquid-solid suspension is injected into a reactor in a syringe pump sample injection mode, and cooling liquid can be sufficiently cooled in a flow mode by adopting a cooling circulator or running water.
Compared with the traditional microfluidic reactor, the reactor has the following advantages:
1. when the traditional microfluidic reactor is used for gas-liquid-solid three-phase catalysis, a solid-phase catalyst is usually fixed in a specific pipeline, and gas-liquid reaction raw materials are easy to block when passing through the catalyst; the reactor of this embodiment adopts quartz bead 3 to form three-dimensional photocatalysis microchannel, forms gas-liquid-solid three-phase turbid liquid through quartz bead 3 to the stirring disturbance effect of gas-liquid raw materials and catalyst, regulates and control the aperture size of microchannel through regulating and controlling 3 sizes of quartz bead, and then regulates and control the mixing and the photocatalytic reaction effect of reactor.
2. The micro-fluidic channels in the three-dimensional space can form cross channels which are four-way and eight-way, gas-liquid-solid three-phase turbid liquid is dispersed and mixed for multiple times, and the planar micro-fluidic mode is difficult to uniformly mix gas, liquid and solid to form turbid liquid.
3. Transparent quartz beads 3 with uniform size are used as fillers and are regularly stacked and arranged in the matrix, so that the light transmittance can be enhanced, and the photocatalytic reaction is realized while the mass transfer is carried out.
4. The quartz beads 3 are used as filler, so that the quartz beads are convenient to disassemble and replace, and chemical sediments generated in the reaction process are convenient to clean.
The reactor of the embodiment can not only solve the limitation of the traditional micro-fluidic, but also realize the photocatalytic reaction while the gas-liquid-solid mass transfer, thereby greatly improving the photocatalytic reaction activity.
Example 2
As shown in fig. 5, example 2 provides another nanomaterial heterogeneous photocatalytic microchannel reactor, whose structure is substantially the same as that of example 1, except that: the accommodating groove is a through groove, and the lower notch of the accommodating groove is wide-mouthed and is positioned on the lower surface of the substrate 1; the quartz light window is characterized by further comprising a transparent lower cover 9, the lower cover 9 can be a cover plate made of quartz materials, the lower cover 9 is fixed at the bottom of the base body 1 in a sealing mode to seal a lower notch and form a quartz light window, sealing is generally carried out in the mode of a sealing ring and a sealing gasket, and the lower cover 9 can also be made of other transparent materials meeting experimental requirements; the lower cover 9 is detachably connected to the base body 1, for example, by screws or bolts. In addition, a cooling liquid flow channel is reserved at the bottom of the reactor, and the constant temperature function of the reactor is reserved.
The reactor of embodiment 2 not only has all the advantages of the reactor of embodiment 1, but also adopts the design of a double-sided quartz light window, and when the double-sided light is irradiated, the whole reactor is made of quartz, and the irradiation mode is favorable for the photocatalyst to fully absorb the light.
Although the invention has been described in detail above with reference to a general description and specific examples, it will be apparent to one skilled in the art that modifications or improvements may be made thereto based on the invention. Accordingly, such modifications and improvements are intended to be within the scope of the invention as claimed.
Claims (5)
1. The utility model provides a heterogeneous photocatalysis microchannel reactor of nano-material, its characterized in that, includes base member, transparent upper cover and transparent quartz bead, be equipped with the holding tank in the base member, the upper surface of base member be equipped with notch on the wide-mouthed formula of holding tank intercommunication, one side of base member be equipped with the solid turbid liquid import of gas-liquid of holding tank intercommunication, the opposite side of base member be equipped with the solid turbid liquid export of gas-liquid of holding tank intercommunication, upper cover detachably seal fixation in the top of base member is in order to seal go up the notch and form transparent optical window, the quartz bead is filled up the holding tank, in the holding tank the quartz bead closely piles up and forms three-dimensional porous microchannel in order to regard as gas-solid three-phase channel and photocatalysis reaction channel, size in order to regulate and control microchannel through the size of regulation and control quartz bead.
2. The heterogeneous photocatalytic microchannel reactor of claim 1, wherein the cover is removably attached to the substrate.
3. The nano-material multiphase photocatalytic microchannel reactor according to claim 1 or 2, wherein a cooling liquid flow channel is further disposed in the substrate, the cooling liquid flow channel is located at a lower side of the accommodating tank and is not communicated with the accommodating tank, a cooling liquid inlet communicated with the cooling liquid flow channel is disposed at one side of the substrate, and a cooling liquid outlet communicated with the cooling liquid flow channel is disposed at the other side of the substrate.
4. The heterogeneous photocatalysis microchannel reactor of nano-material according to claim 1 or 2, further comprising a transparent lower cover, wherein the lower surface of the substrate is provided with a wide-mouthed lower notch communicated with the accommodating groove, and the lower cover is hermetically fixed at the bottom of the substrate to close the lower notch and form a transparent light window.
5. The heterogeneous photocatalytic microchannel reactor of claim 4, wherein the lower cover is removably attached to the substrate.
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