A system and method for regulating the selectivity of a photocatalytic reaction product using circularly polarized light

Abstract

The present application relates to a kind of system and method for regulating photocatalytic reaction product selectivity using circularly polarized light, belong to photocatalytic reaction regulation technical field.By converting unpolarized light into circularly polarized light of specific handedness, the spin direction of the excited carriers on the surface of the photocatalyst is regulated to match the inherent spin selectivity of the catalyst, thereby achieving efficient regulation of the reaction path and product selectivity.The present application is suitable for water oxidation, selective oxidation of organic matter, selective reduction of CO2, racemate deracemization, biomass-derived conversion and homogeneous asymmetric synthesis, etc., and can switch the main product by changing the polarization state of the incident light, significantly improving the selectivity of the target product, providing a new general and efficient optical regulation method for photocatalytic synthesis and conversion.

Description

Technical Field

[0001] This invention relates to a system and method for controlling the selectivity of photocatalytic reaction products using circularly polarized light, belonging to the field of photocatalytic reaction engineering and technology. Specifically, it relates to a system and method for controlling the spin state of charge carriers in a photocatalytic reaction using circularly polarized light, thereby achieving directional control of the reaction path and product selectivity. Background Technology

[0002] Photocatalysis technology can utilize solar energy to drive chemical reactions, and it holds significant application potential in energy conversion, environmental remediation, and the synthesis of fine chemicals. Traditional photocatalytic reactions typically use unpolarized light as the light source, resulting in randomly distributed spin directions of excited charge carriers. However, many photocatalytic materials, especially those with chiral structures or spin selectivity, exhibit higher transport and utilization efficiencies for charge carriers with specific spin directions. This spin-dependent transport characteristic directly influences the electron transfer process of surface reactions, and may consequently determine the final reaction products.

[0003] If the angular momentum of incident photons can be actively modulated using optical means to convert unpolarized light into circularly polarized light with a specific rotation direction, the spin state of excited charge carriers can be directionally controlled. When the carrier spin direction matches the spin selectivity of the catalyst, the carrier separation and transport efficiency is improved, and the concentration of surface reaction intermediates and reaction pathways may also change, ultimately achieving effective control over the selectivity of reaction products. Currently, research on the systematic application of circularly polarized light to control the selectivity of heterogeneous and homogeneous photocatalytic reaction products is still lacking. Summary of the Invention

[0004] This invention aims to provide a system and method for controlling the selectivity of photocatalytic reaction products using circularly polarized light. The system converts conventional unpolarized light into left- or right-handed circularly polarized light using a polarization optics component. By utilizing the matching relationship between the spin characteristics of the light and the catalyst, the spin state of photogenerated carriers is controlled at the source, thereby achieving efficient and controllable regulation of the reaction pathway and product selectivity for various photocatalytic reactions. This invention is applicable to various reaction systems such as water oxidation, selective oxidation of organic matter, selective reduction of CO2, racemic deracemicization, biomass derivatization, homogeneous asymmetric organic synthesis, water splitting, and methane reforming.

[0005] The technical solution of the present invention includes:

[0006] A system for controlling the selectivity of photocatalytic reaction products using circularly polarized light, the system comprising a solar simulator, a polarization optical system, a reaction vessel, and a product analysis system; The reaction vessel is used to contain the photocatalyst and reactants and to carry out the photocatalytic reaction; A polarizing optical system consists of a linear polarizer and a quarter-wave plate, which can convert unpolarized light into left- or right-hand circularly polarized light. The solar simulator is used to simulate sunlight and output simulated sunlight to a linear polarizer. The linear polarizer polarizes the received simulated sunlight and outputs linearly polarized light to a quarter-wave plate. The quarter-wave plate converts the received linearly polarized light into circularly polarized light and sends it to the reaction vessel. The reactants in the reaction vessel undergo a photocatalytic reaction under the action of circularly polarized light and a photocatalyst. Product analysis systems are used to detect and analyze reaction products and their selectivity; The quarter-wave plate is an achromatic wave plate to reduce wavelength-dependent loss; The photocatalyst is selected from metal oxides, metal nitrides, metal sulfides, organic polymer photocatalysts, organic homogeneous photocatalysts, and organic small molecule photocatalysts, such as TiO2, ZnO, SrTiO3, WO3, BiVO4, chiral CdS, g-C3N4, chiral metal-organic framework materials, chiral conjugated organic framework materials, and 3DPAFIPN.

[0007] A method for controlling the selectivity of photocatalytic reaction products using circularly polarized light, comprising the following steps: The photocatalyst and reactants are placed in a reaction vessel; The simulated sunlight output from the solar simulator is sent to a linear polarizer. The linear polarizer polarizes the received simulated sunlight and outputs linearly polarized light to a quarter-wave plate. The quarter-wave plate converts the received linearly polarized light into circularly polarized light and sends it to the reaction vessel. The reactants in the reaction vessel undergo a photocatalytic reaction under the synergistic effect of circularly polarized light, a photocatalyst, and a co-catalyst. The composition and selectivity of the products were detected by a product analysis system and compared with the results under unpolarized light conditions.

[0008] The polarization direction of the circularly polarized light matches the spin selectivity direction of the photocatalyst, which is used to regulate the carrier spin state and thus affect the reaction path and product selectivity. The photocatalytic reactions include, but are not limited to: water oxidation to produce hydrogen peroxide or oxygen; selective oxidation of organic matter to produce high-value chemicals; selective reduction of carbon dioxide; selective deracemosis of racemic compounds; selective conversion of biomass and its derivatives; homogeneous asymmetric organic photocatalytic reactions; water splitting reactions; and methane reforming reactions.

[0009] This invention relates to a system and method for controlling the selectivity of photocatalytic reaction products using circularly polarized light, belonging to the field of photocatalytic reaction control technology. By converting unpolarized light into circularly polarized light with a specific spin direction, the spin direction of excited carriers on the photocatalyst surface is controlled to match the inherent spin selectivity of the catalyst, thereby achieving efficient control over the reaction pathway and product selectivity. This invention is applicable to various reactions such as water oxidation, selective oxidation of organic matter, selective reduction of CO2, racemic deracemicization, biomass derivatization, and homogeneous asymmetric synthesis. By changing the polarization state of the incident light, the main product can be switched, significantly improving the selectivity of the target product, providing a universal and efficient new optical control method for photocatalytic synthesis and conversion.

[0010] The solar simulator is an AM 1.5G solar simulator; The output of simulated sunlight needs to be calibrated to 100 mW·cm using a standard silicon cell. - ², and recalibrate after switching polarization states to ensure consistent light intensity; The selected photocatalyst and reactants are placed in a transparent reactor. For example, for water oxidation, the TiO2 composite material can be dispersed in deionized water; for CO2 reduction, the chiral CuAu / g-C3N4 composite material can be added to a CO2-saturated aqueous solution; for homogeneous asymmetric synthesis, the organic substrate, photosensitizer, additives, and solvent are mixed in proportion. The reaction system is purged with gas or sealed as needed.

[0011] First, a photocatalytic reaction is carried out under unpolarized light. The composition of the products is analyzed using gas chromatography, high-performance liquid chromatography (with a chiral column), mass spectrometry, and circular dichroism spectroscopy to obtain the baseline conversion rate and selectivity. Then, a polarization module is inserted, and the angle of the quarter-wave plate is adjusted to generate circularly polarized light with a specific rotation direction (left-handed or right-handed). The reaction is carried out again under the same light intensity, and the products are analyzed.

[0012] By comparing reaction results under unpolarized light and circularly polarized light with different rotation directions, the effect of circularly polarized light on the regulation of reaction pathways and product selectivity can be evaluated. For example, in the water oxidation reaction, the changes in the selectivity of hydrogen peroxide and oxygen can be observed; in CO2 reduction, the differences in the selectivity of CO and CH4 can be compared; and in asymmetric synthesis, the enantiomeric excess value (ee) of the product can be determined.

[0013] Through the above technical solution, the present invention achieves the following beneficial effects: This invention provides a universal optical control strategy applicable to a wide range of photocatalytic reaction systems. Product selectivity can be controlled simply by switching the polarization state of the incident light, without altering the catalyst structure or reaction conditions, making the operation straightforward. This opens up new avenues for the synthesis of highly selective, high-value-added products from photocatalytic reactions, possessing significant scientific importance and application potential. Attached Figure Description

[0014] Figure 1 This is a schematic diagram of the system composition of the present invention, which utilizes circularly polarized light to regulate the selectivity of photocatalytic reaction products; Figure 2 This is a schematic diagram illustrating the process by which a polarization optical system converts unpolarized light into left- or right-hand circularly polarized light. Figure 3 This is a schematic diagram illustrating the mechanism by which circularly polarized light and catalyst spin-selectivity match regulate reaction pathways and product selectivity. Detailed Implementation

[0015] The present invention will be described in detail below with reference to several application examples, but these examples are merely illustrative and do not constitute a limitation on the scope of protection of the present invention. Any other similar systems based on the concept of the present invention that utilize circularly polarized light to modulate the selectivity of photocatalytic reactions are also within the scope of protection of the present invention.

[0016] like Figure 1 As shown, a system for controlling the selectivity of photocatalytic reaction products using circularly polarized light is disclosed. The system includes a solar simulator, a polarization optical system, a reaction vessel, and a product analysis system. The reaction vessel is used to contain the photocatalyst and reactants and to carry out the photocatalytic reaction; A polarizing optical system consists of a linear polarizer and a quarter-wave plate, which can convert unpolarized light into left- or right-hand circularly polarized light. like Figure 2 As shown, the solar simulator is used to simulate sunlight and outputs simulated sunlight to a linear polarizer. The linear polarizer polarizes the received simulated sunlight and outputs linearly polarized light to a quarter-wave plate. The quarter-wave plate converts the received linearly polarized light into circularly polarized light and sends it to the reaction vessel. The reactants in the reaction vessel undergo a photocatalytic reaction under the action of circularly polarized light and a photocatalyst. Product analysis systems are used to detect and analyze reaction products and their selectivity; The quarter-wave plate is an achromatic waveplate to reduce wavelength-dependent loss.

[0017] Example 1: Circularly polarized light modulates the selectivity of water oxidation pathway In this embodiment, 50 mg of TiO2 catalyst was added to 50 mL of deionized water and irradiated with AM 1.5G simulated sunlight (100 mW / cm²) for 2 hours to investigate the regulatory effect of different polarized light on the reaction pathway. When irradiated with unpolarized light, oxygen is mainly produced, with an oxygen production rate of approximately 120 μmol·g. - ¹·h - ¹, the H₂O₂ selectivity is less than 10%. When the light source is adjusted to left-handed circularly polarized light and photochirality is controlled by a combination of polarizers and quarter-wave plates, a significant enhancement of the hydrogen peroxide generation pathway can be observed, with H₂O₂ selectivity increasing to 72%–78%, and the H₂O₂ concentration in the solution reaching 0.9–1.2 mM. Under the same conditions, when irradiated with right-handed circularly polarized light, the reaction reverts to a four-electron process, with oxygen as the main product, a selectivity exceeding 80%, and the H₂O₂ content in the system below 0.2 mM.

[0018] This embodiment illustrates an optically polarization-tunable catalytic reaction pathway, demonstrating that the choice of reaction path is photochiral dependent. This example proves the ability of circularly polarized light to modulate homogeneous chiral photoreactions, and this method can be extended to other reaction systems such as water oxidation, charge separation, and the construction of peroxy systems.

[0019] Example 2: Selective Production of High-Value Chemicals by Controlled Alcohol Oxidation Using Circularly Polarized Light In this embodiment, 30 mg of a Pt / TiO2 composite material with 1 wt% Pt was used as a catalyst and dispersed in 50 mL of an aqueous solution containing 1 vol% methanol. The effect of polarized light on product selectivity was studied under visible light irradiation for 3 hours.

[0020] Under non-polarized light irradiation, the system produces a variety of products such as formaldehyde, formic acid, and CO2, with unsatisfactory selectivity.

[0021] When the light is adjusted to left-handed circularly polarized light, formaldehyde becomes the main product, with a selectivity of 92–95% and a formation rate of approximately 60–80 μmol·g. - ¹·h - ¹; When the light source is changed to right-handed circularly polarized light, methanol is further oxidized to formic acid, with a yield of 55–70 μmol·g⁻¹. - ¹·h - ¹, the selectivity of formic acid reaches 88%–90%.

[0022] This method can be extended to various alcohol systems such as ethanol and n-propanol, and exhibits similar polarization-induced product distribution modulation behavior. This example demonstrates the potential of circularly polarized light in homogeneous chiral catalysis and photoinduced selectivity modulation, and the method can be extended to other homogeneous photocatalytic systems such as alcohol oxidation and alkane functionalization.

[0023] Example 3: Circularly polarized light modulates the orientation of CO2 reduction products In this embodiment, 40 mg of chiral 3 wt% CuAu / g-C3N4 material was added to 50 mL of CO2 saturated aqueous solution, and CO2 photoreduction reaction was carried out under 450 nm wavelength illumination.

[0024] When irradiated with unpolarized light, the product is a mixture of CO and CH4, with CO accounting for approximately 55% and CH4 accounting for approximately 45%.

[0025] When irradiated with left-handed circularly polarized light, CO2 generation was further enhanced, with selectivity increasing to 80–83% and a generation rate reaching 4.5 μmol·g⁻¹. - ¹·h - ¹; When irradiated with right-handed circularly polarized light, the system tends to produce more reactive methane, with a CH4 selectivity of 76–78% and a formation rate of approximately 4.0 μmol·g. - ¹·h - ¹.

[0026] This example demonstrates that CO2 reduction can be controlled by optical chirality to produce switchable product outcomes. This example illustrates the regulatory significance of circularly polarized light in CO2 conversion systems, and the method can be extended to other systems such as CO2-to-alcohol, CO2-to-methanol, and multi-electron reduction systems.

[0027] Example 4: Circularly polarized light modulates the deracerotation selectivity of racemic bodies 25 mg of chiral g-C3N4 was added to a 20 mM DL-lactic acid aqueous solution, and enantiomeric separation was performed under visible light irradiation. After 6 hours of irradiation with right-handed circularly polarized light, D-lactic acid preferentially underwent oxidation or cleavage, and the residual L-lactic acid ee value in the solution reached 85%. However, when irradiated with left-handed circularly polarized light in the same system, the separation direction was completely reversed, and L-lactic acid was more likely to be consumed, with the residual D-lactic acid ee reaching 82%.

[0028] This experiment demonstrates that the combined action of polarized light and a chiral catalyst can achieve molecular-level optical resolution control in a system, and can be extended to racemic amino acid systems such as alanine and valine. This example proves the controllability of circularly polarized light in homogeneous chiral photoresolution reactions, and this method can be extended to a wider range of optical molecular resolution systems.

[0029] Example 5: Circularly polarized light modulates the conversion pathway of biomass derivatives In this embodiment, the biomass model molecule 2-phenoxy-1-phenylethanol was used as the reaction substrate. 30 mg of chiral conjugated organic framework material was added to 25 mL of acetonitrile / water mixture and irradiated for 4 hours to investigate the modulating effect of polarized light on the product network. Under left-handed circularly polarized light irradiation, the system mainly produced phenylacetylbenzene (AP) and phenylethanol (PHOL), with a total selectivity of approximately 70%. Under right-handed circularly polarized light irradiation, the main products shifted to hydrogen and acetophenone (PP-ONE), with a total selectivity of approximately 78%.

[0030] This result demonstrates that polarized light not only affects single reaction pathways but can also adjust the orientation of product networks in complex organic conversion systems. This example illustrates the regulatory significance of circularly polarized light in biomass catalytic conversion systems, and its potential applications can be extended to lignin cleavage and platform molecule-oriented preparation.

[0031] Example 6: Controlling the selectivity of homogeneous asymmetric organic photocatalytic reactions (taking α-C(sp³)–H carboxylation as an example) In this embodiment, a solution of 0.2 mmol benzylamine, 3 mol% 3DPAFIPN photosensitizer, 20 mol% hexamethylenetetramine, 10 mol% Cs₂CO₃, and 2 mL DMAc was mixed under nitrogen protection and irradiated with CO₂ at 450 nm visible light for 12 hours to obtain the photocarboxylation product. Under conventional illumination, the product showed no significant enantiomeric advantage. However, irradiation with left-handed circularly polarized light yielded an S-configuration α-amino acid with an ee value of 26% and a yield of 65–70%. Irradiation with right-handed circularly polarized light yielded an R-configuration α-amino acid with an ee value of approximately 24% and a yield of 62–68%.

[0032] This system demonstrates the ability of optical chirality as a stereocontrolling factor in homogeneous chiral photocatalysis. This example proves the ability of circularly polarized light to modulate homogeneous asymmetric photosynthesis, and can be extended to other systems such as asymmetric cycloaddition, photoisomerization, and radical rearrangement.

[0033] Example 7: Circularly polarized light enhances the photocatalytic efficiency of methanol-to-hydrogen production. In this embodiment, 40 mg of 1 wt% Pt / TiO2 was added to 50 mL of methanol-water solution and irradiated for 2 hours to evaluate the effect of polarized light on hydrogen production performance. Under unpolarized light irradiation, the hydrogen production rate was 180 μmol·g⁻¹. - ¹·h - ¹, while the hydrogen production rate increased to 260 μmol·g when irradiated with right-handed circularly polarized light. - ¹·h - ¹, the increase is about 45%, while the change is not obvious under left-handed circularly polarized light, and the hydrogen production rate is about 190 μmol·g. - ¹·h - ¹.

[0034] This result demonstrates that the coupling between the carrier spin structure and the catalyst may affect the reaction efficiency. This example illustrates the regulatory significance of circularly polarized light in photocatalytic hydrogen production systems, and this effect can be extended to ZnO, SrTiO3, chiral CdS, g-C3N4, and chiral MOF / COF systems.

[0035] Example 8: Circularly polarized light enhances photocatalytic oxygen production efficiency In this embodiment, 1 wt% BiVO4 / CoPi composite material was used as the catalyst. 30 mg of the catalyst was added to 50 mL of an aqueous solution containing the hole sacrificial agent Na2S2O8. Under non-polarized light irradiation, the oxygen production rate was 110 μmol·g. - ¹·h - ¹, while the oxygen production rate can be increased to 165 μmol·g when irradiated with left-handed circularly polarized light. - ¹·h - ¹, the improvement reaches 50%. This system is also applicable to the photocatalytic oxygen generation process of WO3, g-C3N4, and their composites. This example demonstrates the regulatory significance of circularly polarized light in photocatalytic oxygen generation systems, which can be extended to other oxidant systems and electronic structure regulation processes.

[0036] Example 9: Circularly polarized light enhances Z-scheme pure water splitting efficiency In this embodiment, a Z-scheme water splitting system was constructed, consisting of SrTiO3:Rh as the hydrogen production component and BiVO4 as the oxygen production component. The total catalyst amount was 60 mg, and the overall water splitting rate was 95 μmol·g under unpolarized light irradiation. - ¹·h - ¹, while under right-handed circularly polarized light irradiation, the overall activity increased to 150 μmol·g. - ¹·h -¹, representing an improvement of 58%. This change is attributed to the enhanced carrier migration efficiency across the interface and spin-matching effect promoted by polarized light. This example demonstrates the potential for modulation of circularly polarized light in composite photocatalytic systems, which can be extended to multi-level energy-matching and tandem catalytic systems.

[0037] Example 10: Circularly polarized light-induced methane coupling to generate high-value chemicals In this embodiment, a Pd / TiO2 composite material was used as a photocatalyst to study the selective regulation of the methane coupling reaction. 40 mg of 1 wt% Pd / TiO2 was added to 50 mL of deionized water or dilute ethanol solution, and a methane / oxygen or methane / air mixture was introduced to 1 atm. The reaction was then carried out under 450 nm light for 6 hours. Under unpolarized light irradiation, the system mainly produced ethane, a small amount of ethanol, and carbon oxides, with an ethane yield of approximately 2.5 μmol·g. - ¹·h - ¹. Irradiation with left-handed circularly polarized light significantly improves the activation efficiency of methane C–H and the efficiency of radical coupling, increasing the ethane yield to 4.0–4.5 μmol·g. - ¹·h - ¹, trace amounts of C2 oxygen-containing products such as ethanol were also detected, indicating that the coupling depth was controlled; however, under right-handed circularly polarized light irradiation, the system was more prone to deep oxidation and chain scission, with ethane selectivity decreasing to 1.5–2.0 μmol·g. - ¹·h - ¹, while the proportion of deep oxide species such as acetaldehyde and formic acid increased significantly.

[0038] This system reveals that circularly polarized light can influence the C–C coupling and oxidation competition processes of methane, modulating the migration of surface-active species, radical lifetime, and oxygen insertion depth through photochirality, thereby determining the direction of high-value products. This example demonstrates the regulatory potential of circularly polarized light in alkane activation and coupling systems, applicable to the directional coupling processes of ethane, propane, and longer-chain alkanes.

[0039] Example 11: Circularly polarized light-induced asymmetric selective oxidation of alkanes In this embodiment, 40 mg of chiral Au-TiO2 was added to 50 mL of deionized water, and a methane / oxygen mixture was bubbled through to 1 atm. The reaction was carried out under 450 nm light irradiation for 6 hours. Under unpolarized light irradiation, methane was mainly converted into a mixture of methanol, formaldehyde, and carbon oxide, with a methanol selectivity of approximately 35%. Under left-handed circularly polarized light irradiation, methanol formation was significantly enhanced, with the product selectivity increasing to 72–75% and a formation rate of approximately 8 μmol·g. - ¹·h -¹, but when the system is irradiated with right-handed circularly polarized light under the same conditions, it tends to undergo deep oxidation, with a significant increase in the proportion of formaldehyde and formic acid, and a decrease in methanol selectivity to 28–32%.

[0040] This system illustrates how optical chirality and co-catalysts work together to regulate C–H activation and the direction of deep product oxidation. This example demonstrates that circularly polarized light can be used to selectively control the oxidation of methane, and that methane conversion depends on a co-catalyst. Different co-catalysts, such as oxides, halides, metal coordination compounds, and supported photosensitizers, can produce different selectivities. The patent protection scope includes a wider range of co-catalysts and their combinations. This system also demonstrates the universal applicability of this strategy to alkane oxidation, extending it to systems with low C–H activity, such as ethane, propane, and n-hexane, to achieve chiral light-induced selective product formation.

[0041] Example 12: Circularly polarized light modulates the pollutant degradation process In this embodiment, 50 mg of commercial titanium dioxide (P25-TiO2) was added to 50 mL of an aqueous solution containing 10 ppm of the typical pollutant methyl orange (MO), and irradiated under air conditions for 2 hours under a combined visible and ultraviolet light source. The degradation rate of MO was approximately 65% ​​under unpolarized light irradiation, while the degradation rate increased to 85–88% after irradiation with left-handed circularly polarized light, exhibiting faster photogenerated hole oxidation degradation kinetics. Under the same system, when irradiated with right-handed circularly polarized light, the reaction pathway shifted towards the generation of reactive oxygen species (•OH and •O2). - The degradation rate can reach 82%, but the selectivity of intermediates in solution is different, resulting in more aromatic ring breakage byproducts.

[0042] This system reveals that circularly polarized light not only affects the degradation rate but also modulates the selectivity and fragmentation strategies of pollutant oxidation, demonstrating its potential function in wastewater treatment and environmental remediation systems. This system can be further extended to volatile organic compound (VOC) air purification, volatile aldehyde and ketone degradation, and catalytic air disinfection systems, enabling controllable environmental remediation applications through polarized light-induced reaction pathways. The patent protection scope covers the above and similar systems.

[0043] Example 13: Circularly polarized light enhances photoelectrochemical oxidation process and high-value conversion This embodiment was conducted in a three-electrode photoelectrochemical system, in which a TiO2 or BiVO4 photoanode supported on an FTO substrate was placed in an electrolyte containing 10 mM ethanol or other oxidizable organic compounds, and photo-assisted electrolysis was performed under a bias voltage of 0.6–1.2 V (vs Ag / AgCl). Under unpolarized light, the system exhibited a conventional photocurrent response, with ethanol mainly oxidized to acetaldehyde and acetic acid. When irradiated with left-handed circularly polarized light, the photocurrent density increased by approximately 30–45%, and the product distribution favored the more selective acetaldehyde or higher-value C2 products. When irradiated with right-handed circularly polarized light, the oxidation depth was enhanced, the system favored the production of acetic acid, and exhibited stronger electron extraction efficiency.

[0044] This result indicates that circularly polarized light not only affects photocatalytic systems but also influences charge transfer and product distribution at the photoelectrocatalytic-photoelectrochemical interface, providing a regulatory pathway for high-value conversion, such as... Figure 3 As shown. This system is also applicable to various organic substrate oxidation processes, and can be combined with semiconductor electrodes, cocatalyst layers, MOF / COF modification layers, or chiral interface materials to achieve broader control, indicating that circularly polarized light can be extended to all the above-mentioned photocatalytic and photoelectrochemical reaction systems. The scope of patent protection includes the above and similar systems.

[0045] In summary, the above embodiments fully demonstrate the broad applicability and effectiveness of using circularly polarized light to modulate the selectivity of photocatalytic reaction products. Those skilled in the art can select appropriate photocatalysts and polarization conditions according to the specific reaction system to achieve efficient and highly selective synthesis of the target product. Any variations, substitutions, or extensions based on the core idea of ​​this invention—namely, using circularly polarized light to modulate carrier spin to influence the catalytic reaction pathway and selectivity—should be included within the scope of protection of this invention.

Claims

1. A system for controlling the selectivity of photocatalytic reaction products using circularly polarized light, characterized in that: The system includes a solar simulator, a polarization optics system, and a reaction vessel; A polarizing optical system consists of a linear polarizer and a quarter-wave plate, which can convert unpolarized light into left- or right-hand circularly polarized light. The solar simulator is used to simulate sunlight and outputs simulated sunlight to a linear polarizer. The linear polarizer polarizes the received simulated sunlight and outputs linearly polarized light to a quarter-wave plate. The quarter-wave plate converts the received linearly polarized light into circularly polarized light and sends it to the reaction vessel. The reactants in the reaction vessel undergo a photocatalytic reaction under the action of circularly polarized light and a photocatalyst.

2. The system for controlling the selectivity of photocatalytic reaction products using circularly polarized light according to claim 1, characterized in that: The system also includes a product analysis system, which is used to detect and analyze the reaction products and their selectivity.

3. The system for controlling the selectivity of photocatalytic reaction products using circularly polarized light according to claim 1, characterized in that: The quarter-wave plate is an achromatic wave plate.

4. The system for controlling the selectivity of photocatalytic reaction products using circularly polarized light according to claim 1, characterized in that: The photocatalyst is selected from metal oxides, metal nitrides, metal sulfides, organic polymer photocatalysts, organic homogeneous photocatalysts, and organic small molecule photocatalysts; A co-catalyst is also added when the photocatalytic reaction is carried out in the reaction vessel; The co-catalysts are copper, gold, platinum, ruthenium, and magnetic elements iron, cobalt, and nickel.

5. A system for controlling the selectivity of photocatalytic reaction products using circularly polarized light according to claim 4, characterized in that: The metal oxides are TiO2, ZnO, SrTiO3, WO3, or BiVO4; The metal sulfide is chiral CdS; The organic polymer photocatalyst is carbon nitride (g-C3N4), chiral metal-organic framework (MOF) or chiral conjugated organic framework (COF); The organic homogeneous photocatalyst is 3DPAFIPN.

6. A method for controlling the selectivity of photocatalytic reaction products using circularly polarized light, characterized in that... The steps include: The photocatalyst and reactants are placed in a reaction vessel; The simulated sunlight output from the solar simulator is sent to a linear polarizer. The linear polarizer polarizes the received simulated sunlight and outputs linearly polarized light to a quarter-wave plate. The quarter-wave plate converts the received linearly polarized light into circularly polarized light and sends it to the reaction vessel. The reactants in the reaction vessel undergo a photocatalytic reaction under the action of circularly polarized light and a photocatalyst.

7. A method for controlling the selectivity of photocatalytic reaction products using circularly polarized light according to claim 6, characterized in that: The photocatalytic reactions include, but are not limited to: water oxidation to produce hydrogen peroxide or oxygen, selective oxidation of organic matter to produce high-value chemicals, selective reduction of carbon dioxide, selective deracemosis of racemic compounds, selective conversion of biomass and its derivatives, homogeneous asymmetric organic photocatalytic reactions, water splitting reactions, and methane reforming reactions.

8. A method for controlling the selectivity of photocatalytic reaction products using circularly polarized light according to claim 6, characterized in that: The solar simulator is an AM 1.5G solar simulator.

9. A method for controlling the selectivity of photocatalytic reaction products using circularly polarized light according to claim 6, characterized in that: The output of simulated sunlight needs to be calibrated to 100 mW·cm using a standard silicon cell. - ², and recalibrate after switching polarization states to ensure consistent light intensity.

10. A method for controlling the selectivity of photocatalytic reaction products using circularly polarized light according to claim 8, characterized in that: The selected photocatalyst and reactants are placed in a transparent reactor; For the water oxidation reaction, the TiO2 composite material is dispersed in deionized water; For the CO2 reduction reaction, the chiral CuAu / g-C3N4 composite material was added to a CO2 saturated aqueous solution; For homogeneous asymmetric synthesis, the organic substrate, photosensitizer, additives and solvent are mixed in proportion, and the reaction system is purged or sealed as needed.

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