A hydrogen production and extraction device and method based on light-guided direct-induction cyclone strengthening

Abstract

The application provides a light guide direct induction type cyclone reinforced hydrogen production and extraction device and method, and relates to the technical field of photocatalytic hydrogen production. The light guide direct induction type cyclone reinforced hydrogen production and extraction device comprises a feeding system, a cyclone reinforced hydrogen production and extraction reactor and a light source direct induction system. The cyclone reactor is vertically arranged, the side wall is provided with a tangential feed inlet, the top is provided with a gas outlet, and the lower and upper parts of the side wall are provided with liquid backflow ports and a reaction liquid outlet. The liquid storage tank of the feeding system is communicated with the tangential feed inlet through a feed pump, the liquid backflow ports and the reaction liquid outlet of the reactor are both communicated with the liquid storage tank to form a closed loop circulation, and the gas outlet is connected with a gas collection device. The light collecting and lighting assembly of the light source direct induction system is coupled with the built-in light guide device of the central axis of the reactor through a light guide transmission assembly to radially guide light energy into the reactor. The application strengthens mass transfer through a cyclone flow field, improves light energy uniformity by using a built-in light guide, realizes the integration of reaction and hydrogen separation, improves hydrogen production efficiency and simplifies the system structure.

Description

Technical Field

[0001] This invention relates to the field of hydrogen production technology, and in particular to a photoconductive direct-drive cyclone-enhanced hydrogen production and extraction device and method. Background Technology

[0002] Hydrogen energy, as a clean and efficient secondary energy source, plays a significant role in alleviating the depletion of fossil fuels and reducing environmental pollution. Photocatalytic water splitting technology, which directly utilizes solar energy to convert water into hydrogen, shows promising application prospects. However, this technology still faces several key challenges in practical application.

[0003] First, regarding mass transfer, photocatalytic hydrogen production typically occurs in a gas-liquid-solid multiphase system. In traditional slurry-bed reactors, particle settling is common, leading to insufficient solid-liquid contact. Hydrogen bubbles also tend to adhere to the catalyst surface or remain in the reaction system, affecting the continuation of the reaction and reducing efficiency. Second, regarding light energy utilization, existing photocatalytic reactors mostly employ external light sources. However, external light source irradiation is affected by absorption, scattering, and light shielding by the reaction liquid, resulting in uneven illumination inside the reactor. Furthermore, the system usually requires a separate gas-liquid separation device, increasing structural complexity and operating energy consumption. While mechanical stirring or gas bubbling can enhance mixing, they require additional energy input and have limited effectiveness in microbubble separation.

[0004] Patent CN119503947A discloses a method and apparatus for photocatalytic cyclone-enhanced hydrogen production from organic wastewater. This apparatus uses a mercury lamp as the light source to illuminate the reaction system. While this method provides stable illumination, it still relies on artificial light sources. If energy is supplied via a "solar energy-electricity-light energy" path, it typically involves multiple stages of conversion, including photovoltaic conversion, electricity transmission or energy storage regulation, and lamp illumination, resulting in a relatively low proportion of effective light energy ultimately used for the photocatalytic reaction. In contrast, directly introducing sunlight into the reactor through a focusing and guiding structure can reduce multi-stage conversion losses and improve light energy utilization efficiency. For example, patent CN117504773A discloses a photocatalytic hydrogen production device that uses a serpentine spherical expansion tube as the photocatalytic reactor and incorporates an ultraviolet lamp as the light source within the device. While the expansion tube structure can extend the residence time of reactants, its enhancement effect on solution turbulence is limited, and a low-velocity region easily forms near the expansion section wall, creating a flow dead zone. This leads to catalyst deposition on the reactor wall, resulting in maintenance difficulties. In the design of photocatalytic reactors, the arrangement of the reaction light source and the optimization of the reactor structure are important research directions for improving system performance. Patent CN117902673A discloses a packed bed photocatalytic reactor, which uses a top-illuminated ultraviolet lamp to excite the photocatalytic reaction attached to the surface of the solid catalyst after removing suspended particles. Although this design reduces light source attenuation, the top-illuminated structure is not conducive to the uniform distribution of light inside the reactor; at the same time, the specific surface area of ​​the packed catalyst particles is relatively low, and large catalyst particles are prone to shading effects, thereby reducing the efficiency of the photocatalytic reaction. Therefore, developing a novel reactor structure that can enhance the mass transfer process of the reaction system, improve light energy utilization efficiency, and couple the photocatalytic reaction with the hydrogen separation process is of great significance for improving the overall performance of photocatalytic hydrogen production systems.

[0005] Patent CN114534666A discloses a continuous photocatalytic hydrogen production reactor and its hydrogen production method. The reactor provides illumination through a light panel below the transparent reaction cabinet, which can achieve a certain degree of continuous hydrogen production. However, it is still an artificial external light supply, which is easily affected by the absorption and scattering of the reaction liquid, resulting in uneven internal illumination. At the same time, hydrogen collection usually still relies on an additional gas-liquid separation structure, making the system relatively complex.

[0006] In addition, patent CN111453696A discloses a concentrating fixed membrane solar photocatalytic hydrogen production device, which gathers sunlight through a concentrating component and introduces it into the reaction area. However, its reaction system mainly relies on the immobilized catalyst, the contact area between the catalyst and the reaction liquid is limited, and the immobilized surface is also prone to local uneven illumination.

[0007] In addition, early studies have proposed using multi-channel photocatalytic reaction devices for photocatalytic hydrogen production experiments. For example, patent CN101315357B discloses a multi-channel reaction device for rapid evaluation of photocatalytic hydrogen production activity, which obtains relatively uniform illumination through multiple quartz reaction tubes and a central rotating tube light source. However, this device is mainly used for laboratory catalyst screening, has a complex structure, and relies on multiple stirring and detection systems, making it unsuitable for continuous or large-scale hydrogen production.

[0008] In summary, existing photocatalytic hydrogen production devices still have limitations in terms of reactor structure, light energy introduction, and gas-liquid separation: external light sources easily cause uneven internal light distribution, traditional reactors struggle to simultaneously achieve reaction enhancement and product separation, and often require additional separation devices. Therefore, there is a need for a photocatalytic reaction device that can achieve enhanced mass transfer, optimized light energy distribution, and simultaneous hydrogen separation within the same reactor. Summary of the Invention

[0009] In view of this, the purpose of the present invention is to overcome the shortcomings of the prior art and provide a photoconductive direct-drive cyclone-enhanced hydrogen production and extraction device and method. By optimizing the internal flow field structure of the reactor and the light source introduction method, the mass transfer process of the reaction system is enhanced, the uniformity of light energy distribution inside the reactor is improved, and the efficient separation of generated hydrogen is achieved, thereby improving the overall operating efficiency of the photocatalytic hydrogen production reaction system and simplifying the system structure.

[0010] This invention provides the following technical solution: In a first aspect, embodiments of this application provide a photoconductive direct-draw cyclone-enhanced hydrogen production and extraction device, which includes a feeding system, a cyclone-enhanced hydrogen production and extraction reactor, and a direct-draw system for the light source; The cyclone-enhanced hydrogen production and extraction reactor is a vertically arranged cyclone reactor with a tangential feed inlet on its side wall, a gas outlet at the top, a liquid reflux inlet at the lower part of the side wall, and a reaction liquid outlet at the upper part of the side wall. The feeding system includes a storage tank, a feed pump, and connecting pipes. The storage tank is used to store the reaction liquid. The inlet of the feed pump is connected to the storage tank, and the outlet of the feed pump is connected to the tangential feed inlet of the cyclone reactor via a pipe. The liquid return port of the cyclone reactor is connected to the storage tank via a return pipe, forming a closed-loop circulation channel. The gas outlet of the cyclone reactor is connected to a gas collection device. The direct light source system includes a focusing light-collecting component and a light-guiding transmission component, as well as a built-in light guide device located at the central axis of the swirling reactor. One end of the light guide transmission component is positioned corresponding to the optical focal area of ​​the focusing light-collecting component, and the other end is optically coupled to the input end of the built-in light guide device, for guiding the focused light energy into the interior of the swirling reactor. The built-in light guide device is positioned along the axial direction of the swirling reactor and extends into the internal reaction zone of the swirling reactor, for distributing the light energy radially and laterally into the swirling reactor.

[0011] The embodiments of the present invention have the following advantages: The apparatus provided by this invention enables the photocatalytic reaction and hydrogen gas-liquid separation process to proceed simultaneously within the same device by constructing a stable swirling flow field inside the swirling reactor. After the reaction liquid enters the reactor through the tangential feed inlet, it forms a swirling flow. Under the action of centrifugal force and pressure gradient, the generated hydrogen bubbles gather towards the center of the swirling flow and rise axially before being discharged, achieving in-situ hydrogen separation. For example, under conditions of solar irradiance ≥800 W / m², reaction liquid upward flow velocity 0.06 m / s, and hydraulic residence time 30 s, the apparatus operated continuously for 24 h, achieving an average hydrogen production rate of 42.5 μmol / h, indicating that the apparatus can achieve a stable reaction and gas-liquid separation process within the same reactor.

[0012] Clearly, this invention integrates the feeding system, the cyclone-enhanced hydrogen production and extraction reactor, and the direct light source system into a single design, enabling the reaction, separation, and circulation processes to be completed within the same device. The reaction liquid forms a stable circulation within the system, allowing for continuous feeding and continuous hydrogen production. Under the operating conditions of the example, no catalyst deposition or surface contamination of the light guide device was observed after 24 hours of continuous operation, indicating that the cyclone flow field has a certain self-cleaning effect on the surface of the light guide device, which is beneficial for the long-term stable operation of the device.

[0013] To make the above-mentioned objects, features and advantages of the present invention more apparent and understandable, preferred embodiments are described below in detail with reference to the accompanying drawings. Attached Figure Description

[0014] To more clearly illustrate the technical solutions of the embodiments of the present invention, the accompanying drawings used in the embodiments will be briefly introduced below. It should be understood that the following drawings only show some embodiments of the present invention and should not be regarded as a limitation on the scope. For those skilled in the art, other related drawings can be obtained based on these drawings without creative effort.

[0015] Figure 1 This is a schematic diagram of the structure of a photoconductive direct-drive cyclone-enhanced hydrogen production and extraction device provided by an embodiment of the present invention. Figure 2 This diagram shows a schematic structural view of a swirl reactor provided by an embodiment of the present invention. Figure 3 This diagram illustrates a structural schematic of a swirl reactor provided by an embodiment of the present invention from another perspective; Figure 4 The diagram illustrates the principle flow of a photoconductive direct-drive cyclone-enhanced hydrogen production and extraction method provided by an embodiment of the present invention.

[0016] Explanation of key component symbols: 100-Concentrating light-collecting component; 200-Swirl-enhanced hydrogen production and extraction reactor; 210-Gas outlet; 220-Liquid reflux port; 230-Tangential feed inlet; 240-First inner cone; 250-Second inner cone; 300-Storage tank; 400-Flow meter; 500-Feed pump; 600-Light guide rod; 700-Cooling and temperature-regulating jacket. Detailed Implementation

[0017] Embodiments of the present invention are described in detail below. Examples of these embodiments are shown in the accompanying drawings, wherein the same or similar reference numerals denote the same or similar elements or elements having the same or similar functions throughout. The embodiments described below with reference to the accompanying drawings are exemplary and are only used to explain the present invention, and should not be construed as limiting the present invention.

[0018] like Figure 1 , Figure 2 and Figure 3 As shown, in order to solve the above-mentioned technical problems, this application provides a photoconductive direct-drawing cyclone-enhanced hydrogen production and extraction device. The photoconductive direct-drawing cyclone-enhanced hydrogen production and extraction device achieves coordinated operation of reaction, separation and light energy transmission through the structural coupling of the feeding system, the cyclone-enhanced hydrogen production and extraction reactor 200 and the light source direct-drawing system.

[0019] The cyclone-enhanced hydrogen production and extraction reactor 200 is a vertically arranged high-transmittance quartz cyclone reactor. A tangential feed inlet 230 is provided on the reactor sidewall, allowing the reaction liquid to enter tangentially and form a cyclone flow field, which is used to enhance gas-liquid-solid three-phase mass transfer and catalyst suspension. A gas outlet 210 is provided at the top for discharging enriched hydrogen gas. A liquid reflux inlet 220 is provided at the lower part of the sidewall for discharging the degassed liquid phase.

[0020] The feeding system is used for the storage, transportation, and circulation of the reaction solution, and includes a storage tank 300, a feed pump 500, and connecting pipelines. The storage tank 300 stores the reaction solution containing water, sacrificial agent, and photocatalyst particles, and can be configured with cooling, temperature control, and mixing functions; the inlet of the feed pump 500 is connected to the storage tank 300, and the outlet is connected to the tangential feed port 230 via a pipeline, providing power and flow rate for the reaction solution to enter the cyclone reactor.

[0021] The liquid reflux port 220 is connected to the liquid storage tank 300 via a reflux pipe, and the reaction liquid outlet is connected to the liquid storage tank 300 via a return pipe, forming a closed loop; the gas outlet 210 is connected to a gas collection bag or hydrogen storage tank and other gas collection equipment via a gas transmission pipe.

[0022] The direct light source system includes a light-collecting component 100, a light-guiding component, and a built-in light-guiding device for the introduction and distribution of light energy.

[0023] A light-collecting component 100 is installed outside the reactor to collect and converge sunlight or other light sources to form an optical focal area. One end of a light-guiding transmission component is positioned corresponding to the focal area, and the other end extends into the vortex reactor. A built-in light guide device is positioned at the central axis of the reactor and extends axially into the internal reaction zone. The output end of the light-guiding transmission component is optically coupled to the input end of the built-in light guide device, allowing external focused light to be introduced into the reactor via direct docking, socketing, or dielectric coupling.

[0024] The built-in light guide device distributes light energy radially and laterally into the reaction liquid, so that the photocatalyst particles suspended in a swirling manner are exposed to light and undergo photocatalytic hydrogen production.

[0025] During operation, the reaction liquid is driven by the feed pump 500 and enters the cyclone reactor through the tangential feed port 230, forming a cyclone. The photocatalyst particles are suspended and circulated under the action of centrifugal force and turbulence. The direct light source system introduces external light energy through the built-in light guide device and radiates it to the surroundings. The photocatalyst is excited by the light to generate electron-hole pairs, which react with water to produce hydrogen gas. The hydrogen gas bubbles gather in the central low-pressure area and are discharged through the gas outlet 210. The degassed reaction liquid returns to the storage tank 300 through the liquid return port 220, completing the cycle.

[0026] The low-pressure region at the center of the rotating turbulent flow field provides the driving force for gas-liquid separation, while centrifugal force and pressure gradient drive microbubbles to aggregate towards the axis. The high-speed fluid generates a strong shear field, causing the catalyst particles to form velocity gradients and high-speed spins; the enhanced local shear stress on the particle surface can induce nanoscale lattice distortion in the covalent organic framework material, reducing the electron binding energy and promoting the separation of photogenerated carriers.

[0027] In some embodiments, the height-to-diameter ratio of the cyclone reactor is 3:1 to 10:1; The axial direction of the tangential feed inlet 230 is deflected at an angle of 10° to 30° with the tangential direction of the inner wall of the cyclone reactor.

[0028] A high aspect ratio affects swirling stability and gas-liquid separation efficiency. When the ratio is less than 3:1, the axial length and centrifugal force are insufficient, the catalyst is prone to sedimentation, and the bubble residence time is too short. When the ratio is greater than 10:1, the pressure drop along the flow path increases, and a flow field attenuation zone easily appears at the bottom. A ratio of 3:1 to 10:1 can balance swirling intensity, catalyst suspension, bubble coalescence, energy consumption, and equipment cost.

[0029] The deflection angle is used to optimize the tangential velocity component. If it is too small, the wall impact is large and the energy dissipation is fast; if it is too large, it is difficult to form an effective rotating flow field. 10° to 30° can balance the rotational kinetic energy and the axial propulsion velocity, form a stable vortex core and enhance the enrichment of hydrogen bubbles.

[0030] In some embodiments, the cyclone reactor is equipped with a double inner cone cyclone separation structure, including a first inner cone 240 and a second inner cone 250 arranged coaxially. The first inner cone 240 is located at the upper part, and the second inner cone 250 is located at the lower part, forming an annular cyclone channel between them, so that the reaction liquid forms a cyclone, the catalyst particles remain suspended and circulate, hydrogen bubbles gather towards the central low-pressure zone and are discharged through the gas outlet 210, and the liquid is returned through the liquid return port 220.

[0031] After the reaction liquid enters through the tangential feed port 230, it forms a swirling flow. Under the action of centrifugal force and turbulent shear, the photocatalyst particles spiral downward along the wall and turn back upward from the bottom, forming a circulating flow pattern to avoid bottom deposition and dead zones.

[0032] During the rotation, hydrogen bubbles migrate toward the swirling center axis under the action of radial pressure gradient force, forming a central gas nucleus, and rise axially, passing through the central through hole of the first inner cone 240 and being discharged from the top gas outlet 210.

[0033] The degassed heavy phase liquid is blocked by the first inner cone 240, flows down its inner wall, flows downward through the annular swirling channel, and is discharged from the side wall liquid return port 220 and returned to the feeding system.

[0034] The double inner cone structure forms a two-stage guided separation. The first inner cone 240 shortens the gas discharge path and prevents gas accumulation at the top; the second inner cone 250 guides and stabilizes the flow, reducing the disturbance of the bottom reflux liquid to the central gas core, thereby improving the gas-liquid separation efficiency and maintaining liquid circulation.

[0035] In this embodiment, the feeding system is equipped with a cooling and temperature-regulating jacket 700 on the basis of the storage tank 300 and the feed pump 500 for reaction environment control and stable slurry delivery.

[0036] A cooling and temperature-regulating jacket 700 is installed outside the storage tank 300, which is connected to the subsequent equipment. It is used to store the reaction liquid containing water, sacrificial agent and photocatalyst particles, and regulates the temperature through temperature control components such as jackets or coils to prevent the reaction liquid from overheating due to photothermal effect.

[0037] The outlet of the storage tank 300 is connected to the inlet of the feed pump 500. Its internal swirling chamber or stirring structure is used to homogenize the reaction liquid containing photocatalyst particles, prevent sedimentation before transportation, and ensure that the slurry entering the swirling reactor has a uniform concentration. Alternatively, a swirling channel can be formed inside the storage tank 300 to achieve swirling mixing.

[0038] The feed pump 500 is the power source of the system, and its outlet is connected to the tangential feed port 230 through a connecting pipe.

[0039] A flow meter 400 and / or a pressure gauge are installed on the pipeline between the outlet of the feed pump 500 and the tangential feed port 230.

[0040] The flow meter 400 is used to monitor the flow rate of the reaction liquid entering the cyclone reactor, which facilitates the adjustment of pump speed and control of the upward flow velocity and hydraulic residence time.

[0041] Pressure gauges are used to monitor pipeline pressure, ensure that the system operating pressure is within a safe range, and help determine whether a blockage has occurred.

[0042] The reaction solution is homogenized in the storage tank 300, then pressurized by the feed pump 500, and tangentially injected into the cyclone reactor after being metered by the flow meter 400. The cooling and temperature control jacket 700, in conjunction with the storage tank 300, can reduce local overheating and uneven catalyst distribution, thereby improving operational stability and the ability to maintain hydrogen production efficiency.

[0043] In some embodiments, the upper end of the liquid storage tank 300 is connected to the gas outlet 210, the lower end of the liquid storage tank is connected to the liquid return port 220, and the upper end of the liquid storage tank 300 is provided with an exhaust port to discharge hydrogen gas.

[0044] In this embodiment, the solar concentrating and collecting component 100 is used for solar energy capture and concentration, including a solar concentrating structure and a solar tracking component.

[0045] Solar concentrators focus incident sunlight to a focal point or focal line region through reflection or refraction. Specifically, they can be: A parabolic reflective focusing structure includes a parabolic reflector and a light receiver located at its focal point, wherein the light receiver is connected to the light guide transmission component.

[0046] The Fresnel lens focusing structure includes a Fresnel lens assembly and a light receiving end located in its focal region, the light receiving end being connected to a light guiding transmission assembly. The optical focal region is the location of the light input end of the light guiding transmission assembly, used to ensure the input light flux. To reduce the impact of apparent solar motion on receiving efficiency, the focusing light-collecting assembly 100 is equipped with a solar tracking assembly.

[0047] The solar tracking assembly includes a support structure, an azimuth drive mechanism, a pitch drive mechanism, and a control unit, with the solar concentrator structure mounted on the support structure.

[0048] The azimuth drive mechanism rotates the focusing structure around the vertical axis to track changes in the hour angle; the pitch drive mechanism oscillates the focusing structure around the horizontal axis to track changes in the declination angle. A control unit, such as a PLC or microcontroller, connects to the two drive mechanisms and can incorporate a solar position algorithm or connect to a photoelectric sensor to align the optical axis with the sun and stabilize the focal point or focal line at a preset position.

[0049] The solar tracking component can use a commercial dual-axis solar tracking system, such as the US Nextracker (now Nextpower) system, or the Chinese Arctech Solar SkyLine or SkySmart series, which can rotate around the azimuth and elevation axes to track the solar diurnal and seasonal changes.

[0050] Solar tracking components can improve the problem of reduced light collection efficiency of fixed concentrators during non-midday hours. Compared with fixed installations, the concentrator 100 equipped with a dual-axis tracking system can increase the average daily solar energy collection and improve the system's energy self-sufficiency and overall hydrogen production efficiency.

[0051] In some embodiments, the optical transmission component is a quartz fiber bundle, a quartz light guide rod 600, or a light guide tube structure, wherein the quartz fiber bundle consists of 10 to 500 quartz optical fibers, and the diameter of a single optical fiber is 0.2 to 3 mm.

[0052] In these embodiments, the optical transmission component is used to transmit the focused optical energy, and it may take the form of a quartz fiber bundle, a quartz light guide rod 600, or a light guide tube structure.

[0053] A quartz fiber bundle consists of 10 to 500 high-purity quartz fibers, with a single fiber diameter preferably between 0.2 and 3 mm. It is flexible and easy to bend and lay. Combining multiple fibers can increase the light-receiving end area and reduce the requirements for focal alignment accuracy.

[0054] For example, a fiber bundle consisting of 3,000 quartz optical fibers with a diameter of 1 mm is selected, which has an average transmittance of over 85% in the 400 to 700 nm wavelength band, and can transmit light energy collected by the condenser to the inside of the reactor.

[0055] The quartz light guide rod 600 or light guide tube structure is a solid or hollow quartz columnar component, which has high mechanical strength, thermal shock resistance and low end face coupling loss, and is suitable for short-distance, high light throughput transmission.

[0056] The input end of the light guide transmission component is positioned in the optical focal area of ​​the light-collecting component 100, and the output end is optically coupled to the input end of the built-in light guide device through a sealed interface, such as direct end-face bonding or connection with a light-transmitting medium, to guide the external high-energy beam into the reaction core area.

[0057] The aforementioned fiber bundle or light guide rod 600 can ensure light flux input while taking into account transmission flexibility and installation convenience, enabling remote direct optical energy transmission.

[0058] In this embodiment, the built-in light guide device is located at the central axis of the cyclone reactor. As a light energy release component, it can be a high-transmittance quartz light guide rod 600 or an optical fiber light guide structure.

[0059] If the insertion depth is less than 20%, the illumination is mainly concentrated in the upper part, resulting in uneven axial light distribution; if it is greater than 80%, the light guide device will block the swirling core region, affecting the formation of the central low-pressure zone and the axial discharge of bubbles, and increasing fluid resistance. Controlling the insertion length between 20% and 80% of the axial height can balance the light field distribution and the stability of the swirling flow field.

[0060] To address the difficulty in light extraction caused by total internal reflection of quartz materials, the surface of the built-in light guide device is equipped with a light scattering structure, including a frosted rough surface, a laser-etched microstructure, or a high-refractive-index light scattering coating.

[0061] When a high-energy beam is transmitted within the light guide device, the light scattering structure disrupts the total internal reflection condition, causing some of the light energy to be scattered radially into the swirling reaction zone by diffuse reflection or lateral refraction.

[0062] The built-in light guide device works in conjunction with the swirling flow field to allow the photocatalyst particles to periodically pass through high light intensity regions along a spiral trajectory; combined with lateral scattering, the catalyst can receive light at different positions, alleviating the light penetration limitation and light shielding effect of externally illuminated reactors.

[0063] In this embodiment, a light guide interface is provided on the top or side wall of the cyclone reactor for a sealed connection between the built-in light guide device and the reactor.

[0064] The optical fiber interface includes a sealing sleeve, a compression flange, and a seal, forming a pressure-resistant and corrosion-resistant sealed connection assembly.

[0065] The sealing sleeve is fixedly embedded in the reactor wall, and is hollow inside to allow the built-in light guide device to pass through. The outer wall is welded or flanged to seal the reactor wall.

[0066] The seal is located between the outer wall of the built-in light guide device and the inner wall of the sealing sleeve, serving as a dynamic / static sealing barrier.

[0067] Considering the acid sacrificial agent and long-term ultraviolet radiation, the sealing components should be made of corrosion-resistant elastic sealing materials, specifically: silicone rubber sealing rings, fluororubber sealing rings, or polytetrafluoroethylene sealing rings.

[0068] During installation, the built-in light guide device passes through the sealing sleeve, compresses the flange seal, and fits the outer wall of the light guide device to achieve airtight isolation. This structure can prevent leakage of reaction liquid and entry of external impurity gases, and allows for axial fine adjustment of the light guide device.

[0069] This optical guide interface is used to solve the leakage problem at the connection between the quartz optical guide device and the metal or glass reactor.

[0070] In this embodiment, to reduce the radial illumination dead angle of the reactor, an auxiliary lighting structure is provided on the outer wall and periphery of the swirl reactor cylinder.

[0071] The swirl reactor shell is made of highly transparent quartz material, which has transmittance in the ultraviolet-visible light band. It serves as both a pressure-bearing shell and an optical window for external light energy to enter the reaction zone.

[0072] A ring-shaped optical fiber assembly is arranged circumferentially on the outer side of the quartz outer wall. This assembly is composed of multiple turns of quartz optical fiber, arranged close to or near the quartz outer wall, and connected to the focusing light-collecting assembly 100 or an auxiliary artificial light source through branch optical paths.

[0073] After receiving light energy, the ring fiber optic assembly distributes it and enters the reactor interior radially through the outer wall of the quartz in a multi-point incident manner. The light propagates towards the central region through refraction and scattering.

[0074] The ring fiber optic assembly and the centrally built-in light guide device together form a bidirectional lighting structure: The central illumination comes from the side-scattered light from the built-in light guide device, which mainly illuminates the core area of ​​the vortex. The peripheral illumination comes from the coupled light from the outer wall of the ring fiber assembly, which mainly illuminates the ring area near the reactor wall to compensate for insufficient illumination caused by attenuation or blockage of the central light.

[0075] The swirling flow field causes the photocatalyst particles to move in a spiral circulation between the central region and the outer wall region. The bidirectional illumination allows the catalyst to receive light on both the inner and outer sides, reducing the dark area at the edge of a single central light source.

[0076] like Figure 4 As shown, this application also provides a photoconductive direct-drive cyclone-enhanced hydrogen production and extraction method, applied to the apparatus of any of the above embodiments, including the following steps: S100: Water, sacrificial agent and photocatalyst particles are mixed to form a homogeneous reaction solution.

[0077] In these embodiments, the sacrificial agent is selected from one or more of methanol, ethanol, and ascorbic acid to capture holes and inhibit photocorrosion of the photocatalyst; the photocatalyst is selected from one or more of cadmium sulfide, graphitic carbon nitride, and titanium dioxide, and the catalyst particle size is selected to be 20 to 600 nm.

[0078] The above components are added to the storage tank 300 of the feeding system and homogenized using a cyclone mixer. The mass concentration of the photocatalyst in the reaction solution is controlled to be between 50 mg / L and 1.2 g / L to ensure that the slurry has good dispersion stability.

[0079] S200: The reaction liquid is fed into the cyclone-enhanced hydrogen production and extraction reactor 200 through the tangential feed port 230 by the feed pump 500. The reaction liquid forms a stable cyclone flow field in the cyclone-enhanced hydrogen production and extraction reactor 200, so that the photocatalyst particles are kept suspended and circulated.

[0080] In these embodiments, the reaction liquid is tangentially injected into the reactor at a deflection angle of 10° to 30°, forming a high-speed rotating flow field constrained by the reactor wall. The centrifugal force and turbulent shear force generated by this flow field work together to force the photocatalyst particles to remain suspended and circulate within the reactor, effectively preventing particle settling and scaling on the reactor wall.

[0081] By adjusting the feed pump frequency to 500, the upward flow velocity of the reaction liquid in the cyclone reactor is controlled to be 0.01 to 5 m / s, and the hydraulic residence time is 30 to 60 s, to ensure sufficient reaction time.

[0082] S300: Light energy is introduced into the internal reaction zone of the swirling enhanced hydrogen production and extraction reactor 200 through the light source direct attraction system via the built-in light guide device. The light energy is radially and laterally scattered from the surface of the light guide device into the swirling liquid layer, irradiating the photocatalyst particles and causing a photocatalytic hydrogen production reaction.

[0083] In these embodiments, sunlight is focused by the light-collecting component 100 and transmitted through a quartz fiber bundle or light guide rod 600 to a built-in light guide device at the central axis position. The light is then radially scattered into the swirling liquid layer via a frosted surface, etched microstructure, or light-scattering coating. Suspended photocatalyst particles are excited by light to generate electron-hole pairs, which then undergo a redox reaction with water molecules to produce hydrogen gas.

[0084] S400: Under the action of centrifugal force, the generated hydrogen bubbles gather in the low-pressure area at the center of the vortex and are discharged along the axis through the gas outlet 210; the liquid after the reaction is returned to the storage tank 300 of the feeding system through the liquid return port 220 to participate in the next cycle and achieve continuous operation.

[0085] In these embodiments, the generated hydrogen bubbles have a low density and migrate and coalesce towards the low-pressure region (gas nucleus) at the center of the swirl under the action of radial pressure gradient force. They then move upward along the axial direction and are discharged through the gas outlet 210 at the top of the reactor, entering the gas collection device.

[0086] After degassing, the reaction liquid returns to the storage tank 300 of the feeding system through the liquid return port 220 on the side wall; it then rejoins the cycle from S100 to S300, achieving continuous and stable operation of the device.

[0087] During the implementation of the above method, the swirling flow field not only enhances mass transfer, but also achieves a self-cleaning effect on the surface of the built-in light guide device through fluid scouring, preventing catalyst adhesion and light blocking.

[0088] In some embodiments, the sacrificial agent in step 100 is selected from one or more of methanol, ethanol and ascorbic acid; the photocatalyst is selected from one or more of cadmium sulfide, graphitic carbon nitride and titanium dioxide, and the photocatalyst particle size is 20 to 600 nm.

[0089] In step 200, the feed direction of the tangential feed inlet 230 forms an angle of 10° to 30° with the tangential direction of the inner wall of the cyclone-enhanced hydrogen production and extraction reactor 200. The feed flow rate of the reaction liquid maintains the upward flow velocity of the liquid in the cyclone-enhanced hydrogen production and extraction reactor 200 at 0.02 to 0.15 m / s, and the hydraulic residence time is 30 to 60 s.

[0090] By adjusting the frequency of the feed pump 500, the upward flow velocity of the liquid inside the cyclone-enhanced hydrogen production and extraction reactor 200 is maintained between 0.02 and 0.15 m / s. This flow velocity range is the key interval for the cyclone reactor to achieve a semi-aerated state, providing sufficient centrifugal force for gas-liquid separation while preventing excessively high flow rates from causing bubbles to escape due to entrainment in the liquid phase.

[0091] The hydraulic residence time of the reaction liquid in the cyclone-enhanced hydrogen production and extraction reactor 200 is controlled to be 30 to 60 s. This time range ensures that water molecules have sufficient time to contact the active sites of the catalyst and complete the redox reaction. For example, when the flow rate is set to 0.06 m / s, the hydraulic residence time is approximately 30 s, at which point the hydrogen production rate reaches its peak.

[0092] Example 1: Basic device and its operational performance This embodiment provides a specific implementation of an integrated hydrogen production and extraction device using a light-guided direct-drive cyclone-enhanced hydrogen production and extraction system.

[0093] The device mainly consists of a feeding system, a cyclone-enhanced hydrogen production and extraction reactor 200, a direct light source system, and a built-in light guide device. Its main structural parameters and operating conditions are shown in the table below.

[0094]

[0095] Under standard test conditions (direct solar radiation intensity ≥800 W / m²), the system operated continuously for 24 hours. The results showed: The average hydrogen production rate reached 42.5 μmol / h, and the hydrogen purity reached 99.9%. The swirling flow field was stable, and the catalyst particles remained uniformly suspended without sedimentation. The surface of the light guide rod 600 remained clean under the swirling flow, with no catalyst adhesion observed. This demonstrates that the insertion length range (50% to 70%) can balance light energy utilization and flow field stability, and the height-to-diameter ratio of 8:1 is suitable for the reaction and separation processes.

[0096] Example 2: Engineering Scale-up and Hybrid Light Source Optimization Scheme Based on Example 1, this embodiment has scaled up the device for engineering purposes and optimized the light source system and feeding system, making it suitable for industrial scenarios.

[0097]

[0098] During the 30-day continuous operation test, the system demonstrated excellent stability: The average hydrogen production rate reached 68.3 μmol / h, with a maximum of 75.6 μmol / h. The purity of the discharged hydrogen consistently remained above 99.2%. The catalyst remained well suspended, with no sedimentation. The bidirectional illumination structure and optimized flow field parameters significantly improved the light energy utilization efficiency, verifying the reliability of the device at scale and providing sufficient technical basis for industrial application.

[0099] In all examples shown and described herein, any specific values ​​should be interpreted as merely exemplary and not as limitations; therefore, other examples of exemplary embodiments may have different values.

[0100] It should be noted that similar labels and letters in the following figures indicate similar items. Therefore, once an item is defined in one figure, it does not need to be further defined and explained in subsequent figures.

[0101] The above-described embodiments are merely illustrative of several implementations of the present invention, and while the descriptions are specific and detailed, they should not be construed as limiting the scope of the invention. It should be noted that those skilled in the art can make various modifications and improvements without departing from the concept of the present invention, and these modifications and improvements all fall within the scope of protection of the present invention.

Claims

1. A photoconductive direct-drive cyclone-enhanced hydrogen production and extraction device, characterized in that, The light-guided direct-drive cyclone-enhanced hydrogen production and extraction device includes a feeding system, a cyclone-enhanced hydrogen production and extraction reactor, and a direct-drive light source system. The cyclone-enhanced hydrogen production and extraction reactor is a vertically arranged cyclone reactor with a tangential feed inlet at the lower part of its sidewall, a gas outlet at the top, and a liquid reflux inlet at the upper part of its sidewall. The feeding system includes a storage tank, a feed pump, and connecting pipes. The storage tank is used to store the reaction liquid. The inlet of the feed pump is connected to the storage tank, and the outlet of the feed pump is connected to the tangential feed inlet of the cyclone reactor via a pipe. The liquid return port of the cyclone reactor is connected to the storage tank via a return pipe, forming a closed-loop circulation channel. The gas outlet of the cyclone reactor is connected to a gas collection device. The direct light source system includes a focusing light-collecting component and a light-guiding transmission component, as well as a built-in light guide device located at the central axis of the swirling reactor. One end of the light guide transmission component is positioned corresponding to the optical focal area of ​​the focusing light-collecting component, and the other end is optically coupled to the input end of the built-in light guide device, for guiding the focused light energy into the interior of the swirling reactor. The built-in light guide device is positioned along the axial direction of the swirling reactor and extends into the internal reaction zone of the swirling reactor, for radially and laterally distributing the light energy into the swirling reactor. The cyclone reactor is equipped with a double-inner-cone cyclone separation structure, which includes a first inner cone and a second inner cone. The first and second inner cones are coaxially arranged inside the cyclone reactor. The first inner cone is located in the upper region of the cyclone reactor, and the second inner cone is located in the lower region of the cyclone reactor. The apexes of the first and second inner cones are opposite to each other. An annular cyclone channel is formed between the first and second inner cones, so that the reaction liquid enters the cyclone reactor through the tangential feed port and forms a cyclone flow field. The photocatalyst particles in the reaction liquid are kept suspended and circulated under the action of centrifugal force and turbulence. The generated hydrogen bubbles converge towards the center of the cyclone and are discharged through the gas outlet. The separated liquid is returned through the liquid return port. The built-in light guide device is a quartz light guide rod or an optical fiber light guide structure, and its length extending into the reaction zone inside the swirling reactor is 20% to 80% of the axial height of the swirling reactor. The surface of the built-in light guide device is provided with a light scattering structure, which is a frosted rough surface, an etched microstructure, or a light scattering coating, used to scatter the light energy transmitted inside the light guide device radially and laterally to the swirling reaction zone.

2. The photoconductive direct-drive cyclone-enhanced hydrogen production and extraction device according to claim 1, characterized in that, The height-to-diameter ratio of the cyclone reactor is 3:1 to 10:1; The axial direction of the tangential feed inlet is deflected at an angle of 10° to 30° from the tangential direction of the inner wall of the cyclone reactor.

3. The photoconductive direct-drive cyclone-enhanced hydrogen production and extraction device according to claim 1, characterized in that, The feeding system also includes a cooling and temperature regulating jacket, which covers the outside of the storage tank. The cooling and temperature regulating jacket is used to regulate the temperature of the reaction liquid. The storage tank forms a swirling flow channel for homogenizing and mixing the reaction liquid containing photocatalyst particles. The outlet of the feed pump is connected to the tangential feed inlet, and a flow meter and / or pressure gauge are provided on the connecting pipe between the outlet of the feed pump and the tangential feed inlet.

4. The photoconductive direct-drive cyclone-enhanced hydrogen production and extraction device according to claim 3, characterized in that, The solar concentrating light-collecting component includes a solar concentrating structure and a solar tracking component; the solar concentrating structure is one or a combination of a parabolic reflector, a Fresnel lens, a parabolic trough linear concentrating structure, and a plane reflector array, and the optical focal point or focal line region of the solar concentrating structure constitutes the optical focal point region; The solar tracking component includes a support structure, an azimuth drive mechanism, a pitch drive mechanism, and a control unit. The solar concentrating structure is mounted on the support structure. The control unit is electrically connected to the azimuth drive mechanism and the pitch drive mechanism, respectively, to drive the concentrating structure to perform dual-axis attitude adjustment according to the sun's movement trajectory, so that the optical axis of the concentrating structure remains aligned with the sun.

5. The photoconductive direct-drive cyclone-enhanced hydrogen production and extraction device according to claim 4, characterized in that, The optical transmission component is a quartz fiber bundle, a quartz light guide rod, or a light guide tube structure. The quartz fiber bundle consists of 10 to 500 quartz fibers, with a single fiber diameter of 0.2 to 3 mm.

6. The photoconductive direct-drive cyclone-enhanced hydrogen production and extraction device according to claim 5, characterized in that, The built-in light guide device is inserted into the light guide interface opened on the top or side wall of the cyclone reactor. The light guide interface includes a sealing sleeve, a compression flange, and a seal. A seal made of corrosion-resistant elastic sealing material is provided between the outer wall of the built-in light guide device and the sealing sleeve. The seal is selected from one or more combinations of silicone rubber sealing rings, fluororubber sealing rings, and polytetrafluoroethylene sealing rings.

7. The photoconductive direct-drive cyclone-enhanced hydrogen production and extraction device according to claim 1, characterized in that, The outer wall of the cyclone reactor is made of high-transmittance quartz material. A ring-shaped optical fiber assembly is arranged circumferentially on the outer side of the quartz outer wall. The ring-shaped optical fiber assembly is optically connected to the direct light source system and is used to radially couple external light energy into the reactor interior through the quartz outer wall. Together with the central built-in light guide device, it forms a bidirectional lighting structure.

8. A method for hydrogen production and extraction using a photoconductive direct-drive cyclone-enhanced system, characterized in that, The method, applied to the photoconductive direct-drive cyclone-enhanced hydrogen production and extraction apparatus as described in any one of claims 1 to 7, includes the following steps: S100: Mix water, sacrificial agent and photocatalyst particles to form a homogeneous reaction solution; S200: The reaction liquid is fed into the cyclone-enhanced hydrogen production and extraction reactor through the tangential feed port by the feed pump. The reaction liquid forms a stable cyclone flow field in the cyclone-enhanced hydrogen production and extraction reactor, so that the photocatalyst particles are kept suspended and circulated. S300: Light energy is introduced into the internal reaction zone of the swirling enhanced hydrogen production and extraction reactor through the built-in light guide device via the direct light source system. The light energy is radially and laterally scattered from the surface of the light guide device into the swirling liquid layer, irradiating the photocatalyst particles and causing a photocatalytic hydrogen production reaction. S400: Under the action of centrifugal force, the generated hydrogen bubbles converge towards the center of the vortex and are discharged along the axial direction through the gas outlet; the reacted liquid is returned to the storage tank of the feeding system through the liquid return port to participate in the next cycle, realizing continuous operation.

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