CN109126661B - Laminated spectral light-splitting solar photocatalytic reaction system - Google Patents
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Abstract
The invention discloses a laminated spectral light-splitting solar photocatalytic reaction system, and belongs to the technical field of solar energy utilization. The system is obtained by depositing sequentially arranged N layers of photocatalytic film materials with gradually decreasing optical band gap values and continuously changing band edge positions on a substrate material layer by layer, wherein N is more than or equal to 3; the two adjacent photocatalytic film materials are connected by a transition layer, a cocatalyst with a surface plasma resonance effect is deposited on the Nth layer, the end face close to the light receiving face is an antireflection film with a porous-pyramid composite structure and a textured light trapping effect, and the material composition of the antireflection film is the same as that of the first layer of photocatalytic film material. The photocatalytic reaction system has the remarkable advantages of wide spectral response and high quantum conversion efficiency, and can greatly improve the utilization rate of solar energy.
Description
Technical Field
The invention relates to a laminated spectral light-splitting solar photocatalytic reaction system, and belongs to the technical field of solar energy utilization.
Background
Among the three common ways of solar energy utilization (photo-thermal conversion, photo-electric conversion and photo-chemical conversion), the photocatalytic technology belongs to the photo-chemical conversion way, the mechanism of which is similar to the photosynthesis in the nature, and is mainly applied to hydrogen production and CO production by decomposing water2The preparation of hydrocarbon by reduction, environmental purification, organic synthesis and other fields. The technology not only increases the supply form and quantity of renewable energy sources, lightens the pollution and damage to the environment, but also can treat the environmental pollution, thereby becoming the field which is very worth paying attention to and developing at present.
The key of the development of the solar photocatalytic technology lies in the development of an efficient, cheap and stable wide-spectral-response semiconductor photocatalytic film material. Subject to the physical constraints of the band structure of natural or artificial materials, the working area of any single kind of semiconductor photocatalytic thin film material cannot match and completely cover the solar spectrum, i.e.: the distribution of the photochemical conversion efficiency of a single material in the solar spectral region is very non-uniform, and its peak conversion efficiency is difficult to match with the solar spectrum, resulting in that most of the energy from the sunlight is transmitted, reflected or converted into heat and wasted in the actual photochemical conversion application. If the wide spectral response is realized by reducing the band gap, the reduction of the redox capability of the semiconductor is usually caused, and simultaneously, the photo-generated electron and hole pairs are easier to combine, and the quantum conversion efficiency is reduced, so that the photocatalytic effect is seriously influenced by simply expanding the spectral response interval in a manner of reducing the band gap of the material, and the method is not preferable.
Disclosure of Invention
In order to solve the technical problems, the invention provides a laminated spectral light-splitting solar photocatalytic reaction system, which overcomes the defects that a single semiconductor photocatalytic film material can only respond to a specific waveband spectrum and the quantum conversion efficiency is low, thereby realizing wide spectral response and high quantum conversion efficiency and greatly improving the utilization rate of solar energy.
The laminated spectral light-splitting solar photocatalytic reaction system is obtained by depositing sequentially arranged N layers of photocatalytic film materials with gradually decreasing optical band gap values and continuously changing band edge positions (valence band tops and guide band bottoms) on a substrate material layer by layer (the substrate material can be positioned on one side of the photocatalytic film materials and also can be positioned among several layers of photocatalytic film materials), wherein N is more than or equal to 3; the two adjacent photocatalytic film materials are connected by a transition layer, a cocatalyst with a surface plasma resonance effect is deposited on the Nth layer, the end face close to the light receiving face is provided with an antireflection film with a porous-pyramid composite structure with a textured light trapping effect, the material composition of the antireflection film is the same as that of the first layer of photocatalytic film material, the antireflection film can simultaneously generate and receive photon-generated carriers and participate in a photocatalytic reaction, and the reflected light on the surface of the system is remarkably reduced or eliminated, so that the light transmission quantity of the system is increased, and the stray light of the system is reduced or eliminated; meanwhile, due to the porous micro-nano structure, more reactive sites can be provided, and the photocatalytic reaction efficiency is higher.
When N =3, the first layer of photocatalytic film material is a wide-band-gap photocatalytic film material responding to ultraviolet light; the second layer of photocatalytic film material is a photocatalytic material responding to short-wave visible light; the third layer of photocatalytic film material is a narrow-band-gap photocatalytic film material responding to long-wave visible light; a transition layer is arranged between two adjacent photocatalytic film materials for connection, and a cocatalyst with surface plasma resonance effect is deposited on the third layer and can respond to near infrared light; the end face close to the light receiving face is provided with an antireflection film with a porous-pyramid composite structure and a suede light trapping effect, and the material composition of the antireflection film is the same as that of the first layer of photocatalytic film material; the band gap values of the three layers of semiconductor photocatalytic materials are gradually reduced to form a gradient band gap composite material system, and the conduction band edge position (namely, the conduction band bottom) and the valence band edge position (namely, the valence band top) of the three layers of semiconductor photocatalytic materials are gradually reduced from the first layer of photocatalytic film material to the third layer of photocatalytic film material.
Preferably, the cocatalyst is nano Ag particles, nano Au particles, nano Pt particles or Cu2S nanoparticles, Cu2One of Se nanoparticles; absorbing near infrared light; meanwhile, the cocatalyst and the third layer of semiconductor photocatalytic film form a proper Schottky barrier, which is beneficial to quickly injecting electrons excited by absorbed infrared light into a conduction band of the third layer of semiconductor photocatalysis.
Preferably, the transition layer is obtained by solid solution of photocatalytic materials at two sides, and the mismatch degree of the lattice constant of the material of the transition layer and the photocatalytic materials at two ends is less than 10%; the transition layer is designed to further enable photoproduction electrons and photoproduction holes generated in the semiconductor photocatalysis film material to be more effectively and rapidly transferred; which acts to reduce the lattice mismatch and interface barrier of the semiconductor material at both ends.
Preferably, the substrate material is double-sided connected transparent conductive glass; the conductive glass is designed to comprehensively utilize photoproduction electrons and photoproduction holes generated by the semiconductor photocatalytic material and simultaneously carry out reduction reaction and oxidation reaction; the conductive glass can provide support for a device system, and can be more conveniently applied to actual environments.
The principle of the invention is as follows: as shown in fig. 2, the band gap of the semiconductor photocatalytic thin film material is gradually reduced from one end of the light receiving surface, so that the ultraviolet light-short wave visible light-long wave visible light-near infrared light are sequentially absorbed by the semiconductor materials with different band gaps, thereby realizing full spectrum absorption of the solar spectrum. On the other hand, the band edge positions of the conduction band and the valence band gradually decrease from the first layer of the semiconductor photocatalytic thin film material to the third layer of the semiconductor photocatalytic thin film material. When the light receiving surface is irradiated by sunlight, photoproduction electrons sequentially migrate from the first layer of semiconductor photocatalytic film material to the third layer of semiconductor photocatalytic film material, and a reduction reaction is carried out at one end far away from the light receiving surface; and the photoproduction holes are sequentially transferred from the third layer of semiconductor photocatalytic film material to the first layer of semiconductor photocatalytic film material, and an oxidation reaction is generated at one end of the light receiving surface. Meanwhile, the oxidation reaction and the reduction reaction of photocatalysis can be in different areas, which is more beneficial to the separation of the products of the photocatalysis reaction and the design and optimization of the subsequent photocatalysis devices.
The invention has the beneficial effects that: the solar photocatalytic reaction system realizes wide-spectrum response to solar spectrum by the optimized combination of semiconductor photocatalytic film materials with different band gaps and the coupling of the surface plasma resonance effect of the cocatalyst; meanwhile, the efficient anisotropic migration of photoproduction electrons and photoproduction holes is realized by utilizing the continuous change of energy band positions, so that the quantum conversion efficiency is greatly improved; the system has the obvious advantages of wide spectral response and high quantum conversion efficiency, and can greatly improve the utilization rate of solar energy.
Drawings
FIG. 1 is a graph of the spectral power distribution of solar radiation;
FIG. 2 is a schematic diagram of the laminated spectral light-splitting solar photocatalytic reaction system according to the present invention;
fig. 3 is a schematic structural diagram of a stacked spectral light-splitting solar photocatalytic reaction system according to embodiment 1 of the present invention;
fig. 4 is a schematic structural diagram of a stacked spectral light-splitting solar photocatalytic reaction system according to embodiment 2 of the present invention.
Detailed Description
In order to make the objects, technical solutions and advantages of the present invention clearer, the following detailed description of embodiments of the present invention is provided with reference to the accompanying drawings; examples of these preferred embodiments are illustrated in the accompanying drawings; the embodiments of the invention shown in the drawings and described in accordance with the drawings are exemplary only, and the invention is not limited to these embodiments. It should be noted that, in order to avoid obscuring the present invention with unnecessary details, only the structures and processing steps closely related to the scheme according to the present invention are shown in the drawings, and other details not so related to the present invention are omitted.
Example 1
The invention relates to a laminated spectral light-splitting solar photocatalytic reaction system, wherein N =3, wherein a first layer of photocatalytic film material is a wide-band-gap photocatalytic film material responding to ultraviolet light; the second layer of photocatalytic film material is a wide-band-gap photocatalytic material responding to short-wave visible light; the third layer of photocatalytic film material is a narrow-band-gap photocatalytic film material responding to long-wave visible light; a transition layer is arranged between two adjacent photocatalytic film materials for connection, and cocatalyst nano material particles with surface plasma resonance effect are deposited on the third layer and can respond to near infrared light; the end face close to the light receiving face is provided with an antireflection film with a porous-pyramid composite structure and a textured light trapping effect, and the material composition of the antireflection film is the same as that of the first layer of photocatalytic film material (shown in figure 3); the band gap values of the three layers of semiconductor photocatalytic materials are gradually reduced to form a gradient band gap composite material system, and the conduction band edge position (namely, the conduction band bottom) and the valence band edge position (namely, the valence band top) of the three layers of semiconductor photocatalytic materials are gradually reduced from the first layer of photocatalytic film material to the third layer of photocatalytic film material (as shown in fig. 3).
The first semiconductor photocatalytic film material is a wide-bandgap photocatalytic film material responsive to ultraviolet light, and in this example, a gallium nitride-zinc oxide solid solution (GaN) is selected1-x(ZnO)x(x = 0.05) (corresponding to a basic band gap value of 2.9 eV); the second layer of semiconductor photocatalytic film material is a photocatalytic film material responding to short visible light, and cadmium sulfide CdS (corresponding to a basic band gap value of-2.5 eV) is selected in the embodiment; the third layer of semiconductor photocatalytic film material is a photocatalytic film material responding to long visible light and narrow band gap, and iron oxide Fe is selected in the embodiment2O3(corresponding to a basic band gap value of 2.1 eV).
Position of the bottom of the conduction band and the top of the valence band of the semiconductor materialThe first layer of semiconductor photocatalytic film material (i.e., gallium nitride-zinc oxide solid solution (GaN)1-x(ZnO)x(x = 0.05): 1.2V/1.7V), a second layer of semiconductor photocatalytic thin film material (i.e., cadmium sulfide CdS: -0.7V/1.8V) to a third layer of semiconductor photocatalytic film material (i.e., iron oxide Fe2O3: -0.2V/1.9V).
In this embodiment, the design and control of the transition layer mainly consider the matching of the lattice constant and the matching of the energy band position, and can be controlled by the composition of the solid solution. The difference of the valence band top positions of the three selected photocatalytic materials is very small, and the photoproduction cavity can smoothly follow Fe without further regulation and control2O3The valence band through CdS and finally to (GaN)1-x(ZnO)x(x = 0.05). However, the difference of the positions of the bottoms of the guide belts is large, and the photo-generated electrons can be smoothly transmitted by regulation and control. Meanwhile, the crystal structures of the three photocatalytic materials are wurtzite structures. Thus, the transition layer can be designed using a fibrous mineral solid solution. In this embodiment, the transition layer between the first and second semiconductor photocatalytic film materials is selected (GaN)1-x(ZnO)x(x = 0.25) solid solution (lattice constant close to (GaN)1-x(ZnO)xA crystal constant of (x = 0.05); the belt edge position: -0.95V/1.75V); CdS is selected as transition layer between the second and third layers of semiconductor photocatalytic film materials1-xSex(x = 0.30) solid solution (lattice constant close to that of CdS; band edge position: -0.45V/1.85V).
In this embodiment, the end surface near one end of the light receiving surface is an antireflection film with a porous-pyramid composite structure (the surface of the film has a pyramid composite structure with compact arrangement, and the surface is a porous structure), and the material composition is selected from (GaN)1-x(ZnO)x(x = 0.25) solid solution; the reflectivity of the film can be reduced to 2% by combining the secondary chemical etching with the secondary electrochemical etching.
In this embodiment, the promoter nano-material particles having the surface plasmon resonance effect at the end surface far away from the light receiving surface are selected from nano-gold particles, prepared by immersion photoreduction and deposited on the iron oxide film, and have a particle size of 80 nm.
In the present embodiment, the substrate material double-sided connected transparent conductive glass is selected from indium tin oxide transparent conductive film glass.
The stacked spectral light-splitting solar photocatalytic reaction system can be used for water decomposition or degradation of various pollutants (including degradation of organic matters in sewage, degradation of volatile gases in indoor air, degradation of toxic heavy metal ions and the like).
The photocatalytic materials (gallium nitride-zinc oxide solid solution, cadmium sulfide, iron oxide, and nanogold promoter) used in this example all have very strong light absorption in the corresponding band of the solar spectrum, and exhibit very excellent photocatalytic performance in the respective responsive spectral ranges. In the embodiment, a stacked light splitting system is adopted, three serially connected photocatalytic film systems respectively generate photoproduction electrons and photoproduction holes, and the photoproduction electrons and the photoproduction holes can be transmitted along opposite directions, and finally, a reduction reaction and an oxidation reaction respectively occur at one end of a gallium nitride-zinc oxide solid solution and one end of iron oxide. Meanwhile, a porous-pyramid micro-nano structure with a light trapping effect is adopted at the light receiving end, so that the reflectivity of the system is remarkably reduced, and nano gold particles with a surface plasma resonance effect are adopted at the backlight end for supporting, so that near infrared light is further absorbed. Therefore, the embodiment simultaneously realizes the full spectrum response of the solar spectrum and the remarkable enhancement of the quantum conversion efficiency, and greatly improves the solar energy utilization rate.
Example 2
The invention relates to a laminated spectral light-splitting solar photocatalytic reaction system, wherein N =4, wherein a first layer of photocatalytic film material is a wide-band-gap photocatalytic film material responding to deep ultraviolet light; the second layer of photocatalytic film material is a wide-band-gap photocatalytic film material responding to ultraviolet light; the third layer of photocatalytic film material is a wide-band-gap photocatalytic film material responding to short-wave visible light; the fourth layer of photocatalytic film material is a narrow-band-gap photocatalytic film material responding to long visible light; a transition layer is arranged between two adjacent photocatalytic film materials for connection, and cocatalyst nano material particles with surface plasma resonance effect are deposited on the third layer and can respond to near infrared light; the end face close to the light receiving face is provided with an antireflection film with a porous-pyramid composite structure and a textured light trapping effect, and the material composition of the antireflection film is the same as that of the first layer of photocatalytic film material (as shown in figure 4); the band gap values of the four layers of semiconductor photocatalytic materials are gradually reduced to form a gradient band gap composite material system, and the conduction band edge position (namely, the conduction band bottom) and the valence band edge position (namely, the valence band top) of the four layers of semiconductor photocatalytic materials gradually decrease from the first layer of photocatalytic film material to the fourth layer of photocatalytic film material (as shown in fig. 4).
The first layer of semiconductor photocatalytic film material is a wide-band-gap photocatalytic film material responding to deep ultraviolet light, and tantalum oxide epsilon-Ta is selected in the embodiment2O5(corresponding to a basic band gap value of-3.9 eV); the second semiconductor photocatalytic film material is a wide-band-gap photocatalytic film material responding to ultraviolet light, and titanium oxide TiO is selected in the embodiment2(corresponding to a basic band gap value of-3.2 eV); the third layer of semiconductor photocatalytic film material is a photocatalytic film material responding to short visible light, and tantalum oxynitride TaON (corresponding to a basic band gap value of-2.5 eV) is selected in the embodiment; the fourth layer of semiconductor photocatalytic film material is a narrow-band-gap photocatalytic film material responding to long visible light, and tantalum nitride Ta is selected in the embodiment3N5(corresponding to a basic band gap value of-1.9 eV).
The position of the conduction band bottom and valence band top of the semiconductor material is from the first layer of semiconductor photocatalytic film material (i.e. tantalum oxide epsilon-Ta)2O5: -0.5V/3.4V), a second layer of semiconductor photocatalytic film material (i.e. titanium oxide TiO2: 0.4V/2.8V), a third layer of semiconductor photocatalytic thin film material (i.e., tantalum oxynitride TaON: 0.3V/2.2V) to the fourth layer of semiconductor photocatalytic film material (i.e., Ta tantalum nitride (Ta)3N5: -0.2V/1.7V).
In the present embodiment, the design and control of the transition layer mainly consider the matching of lattice constants and the band positionsThe matching can be regulated and controlled through the composition of the solid solution. The difference of the positions of the bottom of the guide belt of the four selected photocatalytic materials is very small, and photogenerated electrons can smoothly pass through the epsilon-Ta without further regulation and control2O5Through TiO of conduction band2And conduction band of TaON, eventually to Ta3N5The conduction band of (a). However, the position difference of the top of the valence band is large, and the photogenerated holes can be smoothly transmitted by regulation and control. Meanwhile, the crystal structures of the three photocatalytic materials have similarity and all use octahedrons as basic units. Thus, the transition layer can be designed using solid solution. In this embodiment, the transition layer between the first and second semiconductor photocatalytic thin film materials is Ti1-xTaxO2(x = 0.35) solid solution (lattice constant close to TiO)2A crystal constant of (a); the belt edge position: -0.45V/3.15V); TiO is selected as a transition layer between the second layer and the third layer of semiconductor photocatalytic film materials2(1-x)N2x(x = 0.25) solid solution (lattice constant close to TiO)2A crystal constant of (a); the belt edge position: -0.35V/2.60V); ta is selected as a transition layer between the third layer and the fourth layer of semiconductor photocatalytic film materials3N5(1-x)O5x(x = 0.25) solid solution (lattice constant close to that of TaON; band edge position: -0.25V/1.95V).
In this embodiment, the end surface near one end of the light receiving surface is an antireflection film with a porous-pyramid composite structure (the surface of the film has a pyramid composite structure arranged closely, and the surface has a porous structure), and the material composition is tantalum oxide epsilon-Ta2O5(ii) a The reflectivity of the film can be reduced to 2% by combining the secondary chemical etching with the secondary electrochemical etching.
In this embodiment, the promoter nano-material particles having the surface plasmon resonance effect at the end surface far away from the light receiving surface are selected from nano-silver particles, prepared by immersion photoreduction and deposited on the iron oxide film, and the particle size of the promoter nano-material particles is 100 nm.
In the present embodiment, the substrate material double-sided connected transparent conductive glass is selected from indium tin oxide transparent conductive film glass.
The stacked spectral light-splitting solar photocatalytic reaction system can be used for water decomposition or degradation of various pollutants (including degradation of organic matters in sewage, degradation of volatile gases in indoor air, degradation of toxic heavy metal ions and the like).
The photocatalytic materials (tantalum oxide, titanium oxide, tantalum oxynitride, tantalum nitride, and nano-silver promoters) used in this embodiment all have very strong light absorption in the corresponding bands of the solar spectrum, and exhibit very excellent photocatalytic performance in the respective responsive spectral ranges. In the embodiment, a stacked light splitting system is adopted, four serially connected photocatalytic film systems respectively generate photoproduction electrons and photoproduction holes, and the photoproduction electrons and the photoproduction holes can be transmitted along opposite directions, and finally, a reduction reaction is generated at one end of tantalum oxide and an oxidation reaction is generated at one end of tantalum nitride respectively. Meanwhile, a porous-pyramid micro-nano structure with a light trapping effect is adopted at the light receiving end, so that the reflectivity of the system is remarkably reduced, and nano silver particles with a surface plasma resonance effect are adopted at the backlight end for supporting, so that near infrared light is further absorbed. Therefore, the embodiment simultaneously realizes the full spectrum response of the solar spectrum and the remarkable enhancement of the quantum conversion efficiency, and greatly improves the solar energy utilization rate.
Claims (3)
1. The utility model provides a stromatolite formula spectrum beam split solar energy photocatalysis reaction system which characterized in that: the material is obtained by depositing sequentially arranged N layers of photocatalytic film materials with gradually decreasing optical band gap values and continuously changing band edge positions on a substrate material layer by layer, wherein N is more than or equal to 3; a transition layer is arranged between two adjacent photocatalytic film materials for connection, a cocatalyst with a surface plasma resonance effect is deposited on the Nth layer, an antireflection film with a porous-pyramid composite structure and a textured light trapping effect is arranged on the end face close to the light receiving face, and the material composition of the antireflection film is the same as that of the first layer of photocatalytic film material;
the cocatalyst is nano Ag particles, nano Au particles, nano Pt particles and Cu2S nanoparticles, Cu2One of Se nanoparticles;
the transition layer is obtained by solid solution of photocatalytic materials at two sides, and the mismatch degree of the lattice constant of the transition layer material and the photocatalytic materials at two ends is less than 10%.
2. The stacked spectral solar photocatalytic reaction system according to claim 1, characterized in that: when N =3, the first layer of photocatalytic film material is a wide-band-gap photocatalytic film material responding to ultraviolet light; the second layer of photocatalytic film material is a photocatalytic material responding to short-wave visible light; the third layer of photocatalytic film material is a narrow-band-gap photocatalytic film material responding to long-wave visible light; a transition layer is arranged between two adjacent photocatalytic film materials for connection, and a cocatalyst with surface plasma resonance effect is deposited on the third layer and can respond to near infrared light; the end face close to the light receiving face is provided with an antireflection film with a porous-pyramid composite structure and a suede light trapping effect, and the material composition of the antireflection film is the same as that of the first layer of photocatalytic film material.
3. The stacked spectral solar photocatalytic reaction system according to claim 1 or 2, characterized in that: the substrate material is transparent conductive glass with two communicated surfaces.
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