CN111500265A - Double-layer core-shell structure nanoparticle with adjustable surface temperature - Google Patents
Double-layer core-shell structure nanoparticle with adjustable surface temperature Download PDFInfo
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- CN111500265A CN111500265A CN202010107951.4A CN202010107951A CN111500265A CN 111500265 A CN111500265 A CN 111500265A CN 202010107951 A CN202010107951 A CN 202010107951A CN 111500265 A CN111500265 A CN 111500265A
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Abstract
The invention relates to a double-layer core-shell structure nanoparticle with adjustable surface temperature, which comprises a nanosphere and a nanoshell, wherein the nanoshell covers the outside of the nanosphere, the nanosphere is made of a non-absorptive material, and the nanoshell is made of a metal material.
Description
Technical Field
The invention relates to a double-layer core-shell structure nanoparticle with adjustable surface temperature, belonging to the fields of micro-nano manufacturing, photo-thermal treatment and laser heating.
Background
The metal nano-particle radiation absorbs heat, namely, the radiation electromagnetic wave (such as light) and the metal nano-particle induce local surface plasmon resonance (L SPR) in interaction, so that the absorption effect of the nano-particle is greatly enhanced, and the absorbed heat can be concentrated in the metal nano-particle, the nano-particle absorbing a large amount of heat can be used as a heat source to transfer heat to a surrounding medium to cause local temperature increase, and has the advantages of high conversion efficiency, flexible control, high localization and the like.
The premise of heat generation of nanoparticles is that nanoparticles have radiation absorption characteristics, and at present, the achievement of absorption enhancement of nanoparticles is more, but the structure with the best radiation absorption effect is not necessarily the strongest in heat generation capacity. The heat generation rule of the core-shell structure nano-particles still has a plurality of problems to be solved, which to a certain extent hinders the application of the heat generation absorption characteristic of the nano-particles in the practical field. Especially, the realization of higher particle surface temperature becomes an important direction for the structure optimization of the current core-shell nano particles.
According to the research of practical application, the metal material and the inner layer and the outer layer of the non-absorptive dielectric medium are coated to form the spherical and square composite nano particles, the core-shell nano particles can modulate the L SPR position and the space temperature distribution by changing the radius ratio, the shape and the sequence of the inner layer and the outer layer of the core-shell nano particles, the dependence relationship between the core-shell nano particles and various structural parameters is complex, and the theoretical guidance of a system is still lacked in how to select the proper structural parameters in practical application.
Disclosure of Invention
The invention aims to provide a double-layer core-shell structure nanoparticle with adjustable surface temperature.
The technical scheme for realizing the purpose of the invention is as follows:
the invention provides a core-shell structure nanoparticle capable of regulating and controlling steady-state temperature, which comprises the following components: the nano-scale comprises a nano-scale body and a nano-shell, wherein the nano-shell covers the outside of the nano-scale body; the nanospheres are made of a non-absorbent material and the shell of the nanospheres is made of a metal material.
Further, the spherical shell is Au, and the nanosphere is SiO2。
Wherein, SiO2The radius of (2) is 30nm, and the shell thickness of Au is 5-12 nm.
SiO2Has a radius of 30nm and a shell thickness of Au of 8 nm.
Further, the spherical shell is Fe3O4, and the nanosphere is SiO2。
Wherein, SiO2Has a radius of 30nm and a shell thickness of 5-12nm of Fe3O 4.
SiO2Has a radius of 30nm and a shell thickness of 12nm of Fe3O 4.
Compared with the prior art, the invention has the following remarkable advantages:
1. the nano heat source utilizing the heat generation phenomenon of nano particle radiation absorption has the characteristics of nano-scale local heating and extremely small thermal inertia, and the temperature of the heat source can be controlled by a non-contact control mode of illumination, which is an advantage that a common heat source does not have;
2. the invention considers the limitation of single material particles in practical application, adopts the combination of the absorptive medium and the non-absorptive medium to form the core-shell structure nano particles, calculates the steady-state temperature of the core-shell nano particles with different structural parameters, and can design the core-shell structure which is most suitable in different applications according to the rule between the structural parameters and the steady-state temperature.
Drawings
FIG. 1 is a schematic of a core double shell nanoparticle.
FIG. 2 shows SiO with different Au shell thicknesses2@ Au spherical composite nanoparticle absorption factor spectrogram.
FIG. 3 is a graph of 30nmSiO when excited at 700nm2@8nmAu three-dimensional cross-sectional view of electric field distribution and thermal power density near the spherical composite nanoparticle.
FIG. 4 shows (a) 30nmSiO when excited at 670nm2The steady state temperature profile of @10nmAu spherical composite nanoparticles; (b) the maximum temperature Tmax of the particles, the surface temperature Ts and the thickness of the Au shell are shown in a graph. SiO22The core radius is 30 nm.
FIG. 5 shows different Fe3O4Of shell thicknessSiO2@Fe3O4A spherical composite nanoparticle absorption factor spectrogram; SiO22The core radius is 30 nm.
FIG. 6 is a graph of 30nmSiO when excited at 230nm2@12nmFe3O4Three-dimensional cross-sectional views of electric field distribution and thermal power density near spherical composite nanoparticles.
FIG. 7 is (a) 30nmSiO when excited at 230nm2@12nmFe3O4A steady state temperature profile of the spherical composite nanoparticle;
(b) maximum temperature Tmax of the particles, surface temperature Ts and Fe3O4Graph of shell thickness, SiO2The core radius is 30 nm.
Detailed Description
The invention will be further explained with reference to the drawings
Single metal double-layer composite nano particle formed by compounding Au and SiO2
1. The peak absorption intensity of L SPR is blue shifted along with the increase of the thickness of the shell when the absorbing material Au is used as the shell, the peak absorption intensity is increased and then decreased, and the maximum absorption peak value is realized at 30nmSiO2@8nmAu, the maximum steady-state temperature rise of 85K is realized at 30nmSiO2@10nmAu under the irradiation of L SPR peak monochromatic light, in addition, when the transparent medium SiO2 is used as the shell, the position of the L SPR peak is not shifted along with the increase of the thickness of the shell, the peak absorption intensity and the corresponding steady-state temperature are gradually reduced, and the steady-state temperature rise is nearly 80K at most.
2. The influence of the shape. When the shell is made of an absorbing material Au, the square particles have higher absorption peak values compared with spherical particles with equivalent volumes; the electric field and the thermal power generate a unique sharp corner concentration effect; but the steady state temperature rise is 24K lower than that of the spherical particles due to the larger heat dissipation surface of the square particles. In addition, when the transparent medium SiO2 is used as a shell, the absorption capacity of the square particles is similar to that of the spherical particles; also affected by the heat dissipating surface, the steady state temperature rise is lower than that of spherical particles. Spherical particles are advantageous over shaped particles for steady state temperature rise applications where heat is generated from the particles.
3. Comparing the influence of the sequence of the inner layer and the outer layer, the calculation results of the Au shell and the Au core structure show that under the same irradiation intensity and the same gold material volume (30nmSiO2@8nmAu and 30nmAu @5nmSiO2), the peak absorption, the maximum temperature of the stable particles and the surface temperature of the particles of the Au shell are higher, and in addition, when the absorbing medium is positioned on the shell layer, the peak displacement of L SPR is obvious, so that the peak regulation from visible light to infrared bands is convenient to realize, and the conclusion shows that the absorbing medium Au has better application values in the fields of photothermal diagnosis and treatment (the maximum temperature of the particles), nano fluid (the surface temperature of the particles), energy conversion (peak absorption), photothermal imaging (the maximum temperature of the particles and the surface temperature of the particles) and the like.
And secondly, compounding Fe3O4 and SiO2 to form the single-metal double-layer composite nano-particle.
1. Influence of shell thickness. When the shell is made of the absorbing material Fe3O4, the peak position is hardly changed along with the increase of the shell thickness of the Fe3O4, and the peak absorption is continuously increased; a steady state temperature rise of 23K was achieved at 30nmSiO2@12nmFe3O 4. In addition, when the transparent medium SiO2 is used as a shell, the peak absorption intensity and the corresponding steady-state temperature gradually decrease with the increase of the shell thickness, and the steady-state temperature rise is as high as 20K.
2. The influence of the shape. When the absorbing material Fe3O4 is used as a shell, the square particles have higher absorption peak values compared with the spherical particles with equivalent volume; the sharp corner concentration effect of the electric field and the thermal power is not obvious; and because of the bigger radiating surface of square granule, steady state temperature rise is very close with spherical granule. For Fe3O4 with lower absorption capacity, there is no obvious difference between the absorption and heat generation capacity of spherical particles and square particles.
3. The influence of the order of the inner and outer layers. Under the same irradiation intensity and the same volume of the Fe3O4 material, the peak absorption and the steady-state temperature of the Fe3O4 shell are both higher than those of the Fe3O4 core. It was confirmed that, in the case of the (inner core having a radius of 30 nm), the absorption capacity and the heat generating capacity were larger when the absorbing medium was used as the shell than when the absorbing medium was used as the core, and the irradiation intensity and the volume of the absorbing material were the same. Research also finds that the peak absorption and steady-state temperature of Fe3O4 are far lower than those of single-metal double-layer composite nanoparticles formed by compounding Au and SiO2 under the same condition no matter the Fe3O4 is positioned in a shell layer or a core; in addition, the wavelength position of the absorption peak of Fe3O4 is not obviously changed no matter the Fe3O4 is positioned in a shell layer or a core layer, and the Fe3O4 is positioned in an ultraviolet region near 250nm, which means that the absorption medium Fe3O4 has better stability of the wavelength of the absorption peak in the ultraviolet region, has better application prospect in the fields of photochemical catalysis and sensors, and the small and stable wavelength of the absorption peak plays an important role in adjusting the peak of the inner core of the three-layer composite nano-particle.
In practical applications, the maximum temperature that the nanoparticles and the surrounding medium can reach under continuous illumination is an important parameter index. According to the previous calculation of the absorption scattering characteristics of the nano particles with different core/shell thickness ratios, the wavelength which enables the absorption factor of the nano particles to reach the maximum value under each structure is selected as the wavelength of incident light, and the stable surface temperature (Ts) which can be reached by the core-shell nano particles with various structures is calculated and used as the support data of the core-shell nano particles with adjustable and controllable stable temperature.
Two kinds of composite nano particles (Au and SiO) with different core-shell ratios, shapes and inner-outer layer sequences are calculated by a numerical simulation method2Complex, Fe3O4And SiO2Composite) resonance absorption spectrum and steady-state temperature distribution, and combined absorption spectrum, electric field distribution, thermal power density distribution, particle and medium steady-state temperature distribution analysis research on radiation absorption and heat generation characteristics of composite nanoparticles under different structural parameters, and combined with different application fields, research on structural optimization of single-metal double-layer composite nanoparticles, and realize regulation and control of steady-state temperature of nanoparticles and surrounding media.
The influence of different structural parameters (shell thickness, shape, inner and outer layer sequence) on the absorption capacity of the core-shell nanoparticles and the steady-state surface temperature is as follows, and is used for designing and meeting the requirements on the steady-state temperature under different applications. For core-shell nanoparticles of two different materials, the influence of the structural parameters on them is different.
Based on the phenomenon and properties of radiation absorption heat generation of metal nanoparticles, the thermal properties of the nanoparticles are researched on the basis of the research on the local surface plasmon resonance (L SPR) characteristics of the metal nanoparticles.
The invention provides a core-shell structure nanoparticle capable of regulating and controlling steady-state temperature, which comprises a nanosphere and a nanoshell, wherein the nanoshell covers the outside of the nanosphere, the nanosphere is made of a non-absorptive material, and the nanoshell is made of a metal material.
With SiO2@ Au core-shell, SiO2@Fe3O4The core-shell nanoparticles were studied and calculated, and the physical model is shown in FIG. 1, SiO2Radius of 30nm, Au, Fe3O4The shell thickness is d, and the size change of the whole particle is controlled by changing the shell thickness d (5/8/10/12 nm).
Consider the radiation absorption and heat generation conditions in the 400-and 900nm bands, where radiation absorption is characterized by an absorption factor, an electric field distribution, and a thermal power density, and heat generation is characterized by a temperature distribution.
SiO22@ Au core-shell nanoparticles: 30nmSiO2@8nmAu achieves the maximum absorption peak; 30nmSiO2@10nmAu maximum steady state temperature rise 85K.
SiO according to different shell thicknesses2The absorption factor spectrogram (physical model is shown in figure 1(a), and numerical simulation result is shown in figure 2) of the @ Au core-shell composite nanoparticle, and the absorption resonance of the nanoparticle is greatly dependent on the core-shell ratio and shows highly flexible adjustability. For SiO with radius of 30nm2And with the increase of the thickness of the gold shell, the resonance absorption peak always moves towards the short wave direction, namely blue shift, the absorption capacity of the absorption peak is firstly increased and then decreased, and the peak value absorption capacity is maximum when the thickness d of the gold shell is equal to 8 nm. The absorption peak can be changed within the wavelength range of hundreds of nanometers by changing the shell thickness, and the thinner the shell layer is, the larger the blue shift is, and the wavelength change range passes through the visible light to the infrared region.
FIG. 2 SiO for different Au shell thicknesses2@ Au spherical composite nanoparticle absorption factor spectrogram. SiO22The radius of the core is 30nm
Drawing the condition that the thickness of the gold shell is 8nm and the wavelength is 700nm when the absorption peak is maximumThe electric field distribution and the thermal power density of the particles are shown in a three-dimensional cross section, as shown in figure 3, when the electric field distribution at L SPR is observed, SiO is found2The phenomenon that the peak value of the @ Au absorption peak is firstly enlarged and then reduced along with the increase of the thickness of the gold shell is related to the special resonance surface, namely the radiation absorption characteristic of the gold shell nano particles is formed by the gold shell, water (outer layer) and SiO2The two surfaces in contact (inner layer) together determine the ("double surface effect"). When the thickness of the gold shell is 8nm, the effect of the two aspects influencing the combined action is strongest, and the ratio of the surface resonance absorption intensity to the projection section of the incident light of the particle is the largest, namely the radiation absorption capacity is strongest at the moment.
According to SiO2The temperature distribution of the @ Au composite nano-particles when the particles reach a steady state under the irradiation of monochromatic light is calculated and drawn, and a change curve of the maximum internal temperature rise of the particles and the temperature rise of the outermost surface of the particles under different gold shell thicknesses is calculated and drawn as shown in FIG. 4. FIG. 4(a) selects a structure with the maximum steady state temperature rise when the four gold shell thicknesses correspond to the L SPR wave crests of the particles under the irradiation of the monochromatic light respectively, namely the gold shell thickness is 10nm, the steady state temperature distribution is drawn when the 670nm monochromatic light is irradiated, the maximum surface temperature is 385K.
II, SiO2@Fe3O4Core-shell nanoparticles: monotonically increasing, 30nmSiO2@12nmFe3O4 achieved the maximum absorption peak and steady state temperature rise of 23K.
SiO according to different shell thicknesses2@Fe3O4The absorption factor spectrum of the core-shell composite nanoparticle (the physical model is shown in fig. 1(b), and the numerical simulation result is shown in fig. 5), and the absorption resonance of the nanoparticle is not influenced by the core-shell ratio. And the resonance peak is in a small wave band, can be applied in the ultraviolet region and in the microwave application fields of catalysis, sensors and the like, and the small and stable resonance absorption wavelength can be used for designing the multi-layer composite nanoparticle plasmon resonance peak regulation.
Selecting Fe3O4The shell thickness is the resonance peak at wavelength position 230nm of 12nm, and the electric field distribution and thermal power density of the particles are plotted in a three-dimensional cross-sectional view, as shown in fig. 6.
According to SiO2@Fe3O4When the composite nanoparticles reach the maximum surface temperature under monochromatic light irradiation, i.e. Fe3O4FIG. 7(a) shows a temperature profile of a monochromatic light irradiation at 230nm with a thickness of 12 nm. Discovery of Fe3O4The maximum temperature rise that can be achieved with the absorbent medium is very limited, with a maximum temperature of 323K, equivalent to a temperature rise of 23K.
According to SiO2@ Au core-shell and SiO2@ Fe3O4 core-shell nano-particles, research and calculation are carried out to obtain the optimal structure of the SiO2@ Au core-shell nano-particles: 30nmSiO2@8nmAu, which can achieve a maximum absorption peak of 5.9; the maximum surface temperature rise is 84K, and the peak regulation of an infrared band can be realized. Can be applied to the fields of laser heating and the like. The invention obtains the conclusion that the absorption capacity of the SiO2@ Fe3O4 core-shell nano-particles is increased along with the increase of the shell thickness and the surface temperature is monotonously increased, and can realize the absorption peak stabilized in an ultraviolet band.
Compared with the difference of core-shell structure nanoparticles with different structure parameters in the aspect of radiation absorption heat generation property, the structure optimization design is explored by combining with a specific application background, and the feasibility is better. On one hand, the core-shell nano particles with several structural parameters considered by the invention can be realized in preparation and are easy to control; on the other hand, the method can be applied to the exploration of the dependency relationship between the temperature rise of various material particles and surrounding media and various parameters, so that the problem of how to select a suitable core-shell nanoparticle structure and material in application is solved.
Claims (7)
1. A core-shell structure nanoparticle capable of regulating and controlling steady-state temperature is characterized by comprising: the nano-scale comprises a nano-scale body and a nano-shell, wherein the nano-shell covers the outside of the nano-scale body; the nanospheres are made of a non-absorbent material and the shell of the nanospheres is made of a metal material.
2. The controllable stable temperature core-shell nanoparticle of claim 1, wherein the spherical shell is Au and the nanospheres are SiO2。
3. The controllable steady-state temperature core-shell structure nanoparticle of claim 2, wherein the SiO is SiO2Half ofThe diameter is 30nm, and the shell thickness of Au is 5-12 nm.
4. The controllable steady-state temperature core-shell structure nanoparticle of claim 3, wherein SiO is SiO2Has a radius of 30nm and a shell thickness of Au of 8 nm.
5. The controllable stable temperature core-shell structure nanoparticle as claimed in claim 1, wherein the spherical shell is Fe3O4, and the nanosphere is SiO2。
6. The controllable steady-state temperature core-shell structure nanoparticle of claim 5, wherein SiO is SiO2Has a radius of 30nm and a shell thickness of 5-12nm of Fe3O 4.
7. The controllable steady-state temperature core-shell structure nanoparticle of claim 6, wherein SiO is SiO2Has a radius of 30nm and a shell thickness of 12nm of Fe3O 4.
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Application publication date: 20200807 |