TWI478373B - A centrifugal separation apparatus, a method for manufacturing a solid particle by centrifugal separation, and a solid particle for a light emitting diode device - Google Patents

A centrifugal separation apparatus, a method for manufacturing a solid particle by centrifugal separation, and a solid particle for a light emitting diode device Download PDF

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TWI478373B
TWI478373B TW098113800A TW98113800A TWI478373B TW I478373 B TWI478373 B TW I478373B TW 098113800 A TW098113800 A TW 098113800A TW 98113800 A TW98113800 A TW 98113800A TW I478373 B TWI478373 B TW I478373B
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solid particle
solid particles
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TW201039461A (en
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Hung Tu Lu
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Kunshan Nano New Material Technology Co Ltd
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離心分離裝置、離心分離固體粒子之製造方法及用於發光二極體裝置之固體粒子 Centrifugal separation device, method for producing centrifugally separated solid particles, and solid particles for light emitting diode device

本發明是有關於一種離心分離裝置、離心分離固體粒子之製造方法及用於發光二極體裝置之固體粒子,特別是有關於一種藉由控制液體與器壁之相對流速以達到分離固體粒子之裝置及其方法。 The present invention relates to a centrifugal separation device, a method for producing centrifugally separated solid particles, and a solid particle for a light-emitting diode device, and more particularly to a method for controlling separation of solid particles by controlling a relative flow velocity of a liquid and a wall. Apparatus and method therefor.

典型白光發光二極體(LED)係以藍光晶粒與黃色螢光粉以適當比例混合而得到白光,其中亦可依不同比例配出如第1圖所示之色座標圖中藍到黃之各種色彩。目前,LED所摻混之螢光粉之粒徑分佈均相當不一,例如一真實LED截面圖如第2圖所示,其中螢光粉粒徑大小不一,且較大尺度螢光粉有沉澱至晶粒表面的現象,過去曾有報導比較螢光粉粒徑對其發光效益有明顯影響,粒徑之不統一可能影響在LED中之螢光效果導致色彩及亮度的分散。此外,在LED製程中,點膠用針筒內之螢光粉在矽膠內的沉澱速率也受其粒徑的影響,導致前後點出的螢光膠中之螢光粉比例不一致,造成色彩及亮度的嚴重分散,如第3圖所示。 A typical white light-emitting diode (LED) is obtained by mixing blue light crystals and yellow phosphor powder in an appropriate ratio to obtain white light, wherein blue to yellow color can also be assigned in different color ratios as shown in FIG. Various colors. At present, the particle size distribution of the phosphor powder blended by the LED is quite different. For example, a true LED cross-sectional view is shown in FIG. 2, wherein the phosphor powder has different particle sizes, and the large-scale phosphor powder has Precipitation to the surface of the grain, it has been reported in the past that the particle size of the phosphor powder has a significant effect on the luminous efficiency. The inconsistency of the particle size may affect the dispersion of color and brightness caused by the fluorescent effect in the LED. In addition, in the LED process, the precipitation rate of the phosphor powder in the dispensing syringe is also affected by the particle size of the silicone powder, resulting in inconsistent proportion of the phosphor powder in the fluorescent glue which is pointed out before and after, resulting in color and The brightness is severely dispersed, as shown in Figure 3.

離心分離用於分離液體中的固體粒子是一個非常高效率的技術,其原理如下: Centrifugal separation is a very efficient technique for separating solid particles from liquids. The principle is as follows:

顆粒與流體在離心力場中作相對運動時,受到三個力的作用:離心力Fc、浮力Fb、曳引力Fd。對於一定的顆粒和流體,離心力Fc、浮力Fb一定,但曳引力Fd卻隨著顆粒運動速度而變化,最後顆粒與液體間之相對速度將平 衡於一終端速度ut,此時顆粒所受的諸力之和為零 When the particles and the fluid move relative to each other in the centrifugal force field, they are subjected to three forces: centrifugal force F c , buoyancy F b , and traction force F d . For certain particles and fluids, the centrifugal force F c and the buoyancy F b are certain, but the traction force F d changes with the particle movement speed. Finally, the relative velocity between the particles and the liquid will be balanced to a terminal velocity u t . The sum of the forces received is zero

離心力Fc與浮力Fb方向始終相反,對球狀微粒而言若其直徑及密度分別為φ及ρp,而液體的密度為ρL The centrifugal force F c and the buoyancy F b direction are always opposite. For the spherical particles, if the diameter and density are φ and ρ p , respectively, and the density of the liquid is ρ L

其中r為旋轉半徑,ω為角速度,並且 Where r is the radius of rotation and ω is the angular velocity, and

Re為雷諾係數,最後可得終端速度ut Re is the Reynolds coefficient, and finally the terminal speed u t is

根據上式離心機中粒子沉澱之終端速度正比於粒徑的平方,大體上來說粒徑較大的粒子會先行沉澱至器壁。但是沉澱所需的時間除了與終端速度有關外亦與粒子至器壁的距離有關,即使是很小的粒子只要離器壁不遠亦可能在極短時間內沉澱,更何況離心機內液體旋轉達到平衡狀態所需的時間亦難以掌控。因此,僅以沉澱時間的先後來清楚分離不同粒徑的顆粒是幾乎不可能的。 According to the terminal velocity of the particle precipitation in the above-mentioned centrifuge, the particle size is larger than the square of the particle diameter, and generally, the particle having a larger particle size is precipitated first to the wall. However, the time required for precipitation is related to the distance from the particle to the wall, in addition to the speed of the terminal. Even small particles can precipitate in a very short time as long as they are not far from the wall, not to mention the liquid rotation in the centrifuge. The time required to reach equilibrium is also difficult to control. Therefore, it is almost impossible to clearly separate particles of different particle diameters only in the order of precipitation time.

有鑑於上述習知技藝之問題,根據本發明之其中一目的就是在提供一種離 心分離裝置,其係巧妙的應用曳引力將較小粒徑的固體粒子曳引至空間中不同位置與較大粒徑的固體粒子分離開。其原理如下: In view of the above-mentioned problems of the prior art, one of the objects according to the present invention is to provide an The heart separation device, which is ingeniously applied to drag the solid particles of smaller particle size, is separated from the solid particles of larger particle size at different positions in the space. The principle is as follows:

粒子與器壁或粒子與粒子間之最大靜磨擦力Fr正比於離心力Fc和浮力Fb之差 The maximum static friction force F r between the particle and the wall or particle is proportional to the difference between the centrifugal force F c and the buoyancy F b

若液體與器壁有一相對速度v,則液體對粒子之曳引力Fd正比於粒子粒徑φ和相對速度v之乘積 If the liquid has a relative velocity v with the wall, the traction force F d of the liquid to the particle is proportional to the product of the particle size φ and the relative velocity v.

因此,曳引力與最大靜磨擦力和粒徑有不同的指數關係,只要適當控制液體與器壁之相對流速即可調整曳引力與最大靜磨擦力之平衡點。其中所受曳引力低於平衡點之粒徑較小粒子,即其所受曳引力大於最大靜磨擦力之粒子,無法留滯在器壁會被液體曳引帶往其他位置,只有曳引力高於平衡點之粒徑較大粒子,即其所受曳引力小於最大靜磨擦力之粒子可以留滯在器壁,進而可以分離出不同粒徑之粒子。 Therefore, the traction force has a different exponential relationship with the maximum static friction force and the particle diameter, and the balance point between the traction force and the maximum static friction force can be adjusted by appropriately controlling the relative flow velocity of the liquid and the wall. The particles with smaller particle diameters below the equilibrium point, that is, the particles whose traction force is greater than the maximum static friction force, cannot be left behind in the wall and will be carried by liquid to other places, only the traction force is high. The larger particle size at the equilibrium point, that is, the particles whose traction force is less than the maximum static friction force can be retained on the wall, and the particles of different particle sizes can be separated.

根據本發明之另一目的,提出一種離心分離裝置,以改善液固相離心機對於不同粒徑或密度固體粒子之篩選能力。此離心分離裝置包括一容置單元、一驅動單元和一控制單元。其中,容置單元用以置放含有固體粒子之液體,驅動單元係用以驅動容置單元運轉,使容置單元之器壁和液體產生相對流速,以及控制單元則用於控制驅動單元驅動該容置單元的速度,進而控制液體和器壁的相對流速,使液體對固體粒子之曳引力,和固體粒子與器壁間或固體粒子與固體粒子間之最大靜摩擦力達一預設之平衡點,使得粒徑較小之固體粒子因其所受曳引力大於最大靜磨擦力,無法留滯在器壁 而被液流帶往其他位置,因此可以明確的將液體中的固體粒子依粒徑大小區隔開來,藉以取得具預設粒徑範圍之固體粒子。 According to another object of the present invention, a centrifugal separation apparatus is proposed to improve the ability of a liquid-solid phase centrifuge to screen solid particles of different particle sizes or densities. The centrifugal separation device comprises a receiving unit, a driving unit and a control unit. The accommodating unit is configured to place a liquid containing solid particles, the driving unit is configured to drive the accommodating unit to operate, the relative flow rate of the wall of the accommodating unit and the liquid is generated, and the control unit is configured to control the driving unit to drive the The speed of the unit is controlled to control the relative flow rate of the liquid and the wall, so that the traction of the liquid against the solid particles and the maximum static friction between the solid particles and the walls or between the solid particles and the solid particles reach a predetermined equilibrium point. Therefore, the solid particles with smaller particle size cannot be retained in the wall because the traction force is greater than the maximum static friction force. The liquid stream is carried to other locations, so that the solid particles in the liquid can be clearly separated according to the particle size, thereby obtaining solid particles having a predetermined particle size range.

根據本發明之再一目的,提出一種離心分離固體粒子之製造方法。其步驟包括:將含有固體粒子之液體置放於一容置單元內。藉由驅動單元驅動容置單元運轉,使容置單元之器壁與液體產生相對流速。利用控制單元控制容置單元之速度進而控制其相對流速,以調整液體對固體粒子之曳引力,和固體粒子與器壁間或固體粒子與固體粒子間之最大靜摩擦力之平衡點,以及取得預設具粒徑範圍之固體粒子。此外,可藉由重覆上述步驟並逐漸減小相對流速,而分離出不同粒徑之固體粒子。 According to still another object of the present invention, a method of producing a centrifugally separated solid particle is proposed. The method comprises the steps of: placing a liquid containing solid particles in a receiving unit. The driving unit drives the accommodating unit to operate, so that the wall of the accommodating unit generates a relative flow velocity with the liquid. The control unit controls the speed of the accommodating unit and controls its relative flow rate to adjust the traction force of the liquid on the solid particles, and the balance point between the solid particles and the wall or the maximum static friction between the solid particles and the solid particles, and obtain the pre-preparation Set solid particles in the particle size range. Further, solid particles of different particle sizes can be separated by repeating the above steps and gradually reducing the relative flow rate.

此外,根據本發明之離心分離裝置及離心分離固體粒子之製造方法,其液體與器壁之相對流速,可以以任何方式產生,如機械推進、非平衡軸轉動、振動等。所使用之液體可以為水溶液或有機溶劑,且所選用之固體粒子係為不溶於水材料。且可分離得之固體粒子之粒徑範圍可以為微米等級,甚至是奈米等級。 Further, according to the centrifugal separation apparatus and the method for producing centrifugally separated solid particles of the present invention, the relative flow velocity of the liquid and the wall can be produced in any manner, such as mechanical propulsion, unbalanced shaft rotation, vibration, and the like. The liquid used may be an aqueous solution or an organic solvent, and the selected solid particles are insoluble in water. The detachable solid particles may have a particle size ranging from micron to nanometer.

根據本發明之又一目的,提出一種發光二極體裝置,其包括如本發明之離心分離固體粒子之製造方法所製造之固體粒子。此發光二極體裝置係包括一基座、一設置於基座上之發光二極體晶片、一包括固體粒子和矽膠且覆蓋於發光二極體晶片上之光致發光體、以及一電流調整裝置。其中固體粒子可為螢光粉,例如釔鋁石榴石(vttrium aluminum garnet,YAG)。此外,螢光粉更可為由母體材料與添加物所組成,這些材料大多為二至六族的離子化合物,常用之母體材料係由二族的鈣、鍶、鋇、鋅或鎘、汞搭配六族的硫、硒製備而成,添加物則多為錳、銅、銀或鑭系元素銪、釤、鋱等過渡金屬。 According to still another object of the present invention, there is provided a light-emitting diode device comprising solid particles produced by the method for producing centrifugally separated solid particles of the present invention. The light emitting diode device comprises a base, a light emitting diode chip disposed on the base, a photoluminescence body comprising solid particles and silicone and covering the light emitting diode chip, and a current adjustment Device. The solid particles may be a fluorescent powder such as vttrium aluminum garnet (YAG). In addition, the phosphor powder may be composed of a matrix material and an additive. Most of these materials are two to six ionic compounds. The commonly used parent materials are composed of two groups of calcium, barium, strontium, zinc or cadmium and mercury. Six kinds of sulfur and selenium are prepared, and the additives are mostly transition metals such as manganese, copper, silver or lanthanides such as lanthanum, cerium and lanthanum.

根據本發明之再又一目的,提出一種用於發光二極體裝置之固體粒子,其 製造方法包括:(a)設置含有固體粒子之液體於容置單元內;(b)驅動容置單元運轉,使容置單元之器壁與液體產生一相對流速;(c)控制容置單元之速度,進而控制相對流速,以調整液體對固體粒子之曳引力,和固體粒子與器壁間或固體粒子與固體粒子間之最大靜摩擦力之平衡點;以及(d)待一段時間後,取得具一預設粒徑範圍之固體粒子。其中,該固體粒子可為螢光粉,例如釔鋁石榴石(yttrium aluminum garnet,YAG)。因此,此具預設粒徑範圍之固體粒子即可添加於發光二極體中,以增加發光二極體效能。 According to still another object of the present invention, a solid particle for a light emitting diode device is proposed. The manufacturing method comprises: (a) setting a liquid containing solid particles in the accommodating unit; (b) driving the accommodating unit to operate, causing a wall of the accommodating unit to generate a relative flow rate with the liquid; (c) controlling the accommodating unit; Speed, and thus relative flow rate, to adjust the traction of the liquid to the solid particles, and the balance between the solid particles and the wall or the maximum static friction between the solid particles and the solid particles; and (d) after a period of time, obtain A solid particle of a predetermined particle size range. Wherein, the solid particles may be a fluorescent powder such as yttrium aluminum garnet (YAG). Therefore, the solid particles having the predetermined particle size range can be added to the light-emitting diode to increase the efficiency of the light-emitting diode.

承上所述,依本發明之離心分離裝置及離心分離固體粒子之製造方法,其可具有一或多個下述優點: According to the above, the centrifugal separation device and the method for producing the centrifugally separated solid particles of the present invention may have one or more of the following advantages:

1.可應用於發光二極體(LED)之螢光粉粒徑的篩選,以解決LED因粒徑大小不一造成色彩及亮度分散的問題。 1. It can be applied to the screening of the phosphor particle size of the light-emitting diode (LED) to solve the problem that the color and brightness of the LED are dispersed due to the different particle size.

2.可應用於任何不溶於水的固體材料之分離,例如樹脂、塑膠、金屬、石墨、乙酸乙酯、三聚氰胺、聚乙烯、聚苯乙烯、聚酯、聚氯化乙烯、聚醯胺、聚丙烯、耐綸、聚偏氟乙烯、聚胺甲酸乙酯、丙烯酸樹脂、聚矽氧烷、結晶性纖維素、澱粉、矽石、氧化鋁、滑石、高嶺土、氧化鈦、氧化鋅、石英、磷酸鈣、螢光粉等材料。 2. Can be applied to the separation of any solid material that is insoluble in water, such as resin, plastic, metal, graphite, ethyl acetate, melamine, polyethylene, polystyrene, polyester, polyvinyl chloride, polyamine, poly Propylene, nylon, polyvinylidene fluoride, polyurethane, acrylic resin, polyoxyalkylene, crystalline cellulose, starch, vermiculite, alumina, talc, kaolin, titanium oxide, zinc oxide, quartz, phosphoric acid Calcium, fluorescent powder and other materials.

3.可分離得之固體粒子之粒徑範圍可以小到1-10nm,甚至是1-3nm。 3. The particle size range of the separable solid particles can be as small as 1-10 nm or even 1-3 nm.

1‧‧‧發光二極體裝置 1‧‧‧Lighting diode device

10‧‧‧金屬反射杯 10‧‧‧Metal reflector cup

20‧‧‧底部 20‧‧‧ bottom

30‧‧‧發光二極體晶片 30‧‧‧Light Emitter Wafer

40‧‧‧藍光 40‧‧‧Blue

50‧‧‧光致發光螢光體 50‧‧‧Photoluminescent phosphor

51‧‧‧容置單元 51‧‧‧ accommodating unit

52‧‧‧驅動單元 52‧‧‧Drive unit

53‧‧‧控制單元 53‧‧‧Control unit

60‧‧‧黃光 60‧‧‧ Huang Guang

70‧‧‧電流調整裝置 70‧‧‧ Current adjustment device

S61-S64‧‧‧流程步驟 S61-S64‧‧‧ Process steps

第1圖 係為典型之色座標圖;第2圖 係為一真實發光二極體之截面圖;第3圖 係為具不同螢光粉粒徑之點膠用針筒之示意圖及其粒徑對發光二極 體色彩的影響之關係曲線圖;第4圖 係為本發明之曳引力與最大靜摩擦力和粒徑之關係曲線圖;第5圖 係為本發明之離心分離裝置之示意圖;第6圖 係為本發明之離心分離固體粒子之製造方法之流程圖;第7A圖 係為螢光粉藉由本發明之離心分離固體粒子之製造方法分離前之粒徑分佈曲線圖;第7B圖 係為螢光粉藉由本發明之離心分離固體粒子之製造方法分離後之粒徑分佈曲線圖;第8圖 係為本發明之具螢光粉之發光二極體裝置之一實施例之示意圖;第9圖 係為本發明之螢光粉粒徑對色彩影響之一實施例之曲線圖;第10圖 係為本發明之不同螢光粉粒徑之色座標(x)與亮度之關係曲線圖;第11圖 係為第10圖之色座標(x)為0.32所得之其亮度與粒徑關係曲線圖;第12A圖 係為粒徑的分散程度對色座標(x)的分散影響之關係曲線圖;以及第12B圖 係為粒徑的分散程度對亮度的分散影響之關係曲線圖。 Figure 1 is a typical color coordinate map; Figure 2 is a cross-sectional view of a real light-emitting diode; Figure 3 is a schematic view of a dispensing syringe with different phosphor powder sizes and its particle size Pair of light-emitting diodes Figure 4 is a graph showing the relationship between the traction force of the present invention and the maximum static friction force and particle diameter; Figure 5 is a schematic view of the centrifugal separation device of the present invention; A flow chart of a method for producing a centrifugally separated solid particle of the present invention; FIG. 7A is a particle size distribution curve of the fluorescent powder before separation by the method for producing a centrifugally separated solid particle of the present invention; and FIG. 7B is a fluorescent powder. The particle size distribution curve after separation by the method for producing centrifugally separated solid particles of the present invention; FIG. 8 is a schematic view showing an embodiment of the light-emitting diode device with fluorescent powder of the present invention; The graph of one embodiment of the effect of the particle size of the phosphor powder on the color of the present invention; FIG. 10 is a graph showing the relationship between the color coordinates (x) and the brightness of the different phosphor powder sizes of the present invention; The relationship between the brightness and the particle diameter of the color coordinate (x) of Fig. 10 is 0.32; the 12A is the relationship between the dispersion degree of the particle size and the dispersion effect of the color coordinate (x); and the 12B The figure is the degree of dispersion of the particle size versus brightness Dispersing the graph of influence.

請參閱第4圖,其係為本發明之曳引力與最大靜摩擦力和粒徑之關係曲線圖。圖中,高流速液體對粒子產生之曳引力與低流速液體對粒子產生之曳引力分別與粒子之粒徑成正比,而最大靜摩擦力係與粒徑立方成正比。此外,對於粒徑較小之粒子,液體對其產生之曳引力係大於最大靜摩擦力,而粒徑較大之粒子,液體對其產生之曳引力係小於最大靜摩擦力。 Please refer to Fig. 4, which is a graph showing the relationship between the traction force and the maximum static friction and particle diameter of the present invention. In the figure, the traction force generated by the high flow rate liquid on the particles and the traction force generated by the low flow rate liquid on the particles are proportional to the particle size of the particles, and the maximum static friction force is proportional to the particle size cube. In addition, for particles with a small particle size, the traction force generated by the liquid is greater than the maximum static friction force, and the particles having a larger particle diameter, the traction force generated by the liquid is less than the maximum static friction force.

請參閱第5圖,其係為本發明之離心分離裝置之示意圖。圖中,離心分離之裝置包括一容置單元51,其係用於置放含有固體粒子之液體;一驅動單元52,其係用以驅動容置單元51運轉,使液體和容置單元51之器壁產生相對 流速;以及一控制單元53,係用以控制驅動單元52驅動容置單元51的速度,進而控制液體與器壁之相對流速,以調整液體對固體粒子之曳引力,和固體粒子與器壁間或固體粒子與固體粒子間之最大靜摩擦力之平衡點,藉以分離出不同粒徑範圍之固體粒子。 Please refer to Fig. 5, which is a schematic view of the centrifugal separation device of the present invention. In the figure, the centrifugal separation device comprises a accommodating unit 51 for arranging a liquid containing solid particles, and a driving unit 52 for driving the accommodating unit 51 to operate, so that the liquid and the accommodating unit 51 Wall is relatively a flow rate; and a control unit 53 for controlling the speed at which the driving unit 52 drives the accommodating unit 51, thereby controlling the relative flow rate of the liquid and the wall to adjust the traction force of the liquid against the solid particles, and between the solid particles and the wall Or the equilibrium point of the maximum static friction between the solid particles and the solid particles, thereby separating solid particles of different particle size ranges.

請參閱第6圖,其係為本發明之離心分離固體粒子之製造方法之流程圖。其步驟包括:步驟61,置放含有固體粒子之液體於一容置單元內。步驟62,驅動容置單元運轉,使容置單元之器壁與液體產生一相對流速。步驟63,控制容置單元之速度,進而控制其相對流速,以調整液體對固體粒子之曳引力,和固體粒子與器壁間或固體粒子與固體粒子間之最大靜摩擦力達一預設平衡點,使得曳引力大於最大靜摩擦力而無法留滯在器壁之粒徑較小之固體粒子被曳引至空間中不同位置,而與粒徑較大而曳引力小於最大靜摩擦力之固體粒子分離開,以及步驟64,取得預設粒徑範圍之固體粒子。可藉由重複上述步驟,可分離具不同粒徑範圍之固體粒子。其中,取得預設粒徑範圍之固體粒子之方式則可視粒徑大小而定,例如若所欲取得係為粒徑較大之固體粒子,即保留留滯於器壁之固體粒子,而將液體中之粒徑較小固體粒子移除;反之,若所欲取得係為粒徑較小之固體粒子,則保留液體中之固體粒子,而將留滯於器壁之粒徑較大固體粒子移除。 Please refer to Fig. 6, which is a flow chart of the method for producing the centrifugally separated solid particles of the present invention. The step includes the following steps: placing the liquid containing the solid particles in a receiving unit. In step 62, the accommodating unit is operated to generate a relative flow rate of the wall of the accommodating unit with the liquid. Step 63, controlling the speed of the accommodating unit, and controlling the relative flow rate thereof, to adjust the traction force of the liquid on the solid particles, and the maximum static friction between the solid particles and the wall or between the solid particles and the solid particles reaches a preset equilibrium point. The solid particles whose traction force is greater than the maximum static friction force and cannot be retained on the wall of the vessel are drawn to different positions in the space, and are separated from the solid particles having a larger particle diameter and a traction force smaller than the maximum static friction force. And step 64, obtaining solid particles of a predetermined particle size range. The solid particles having different particle size ranges can be separated by repeating the above steps. The method of obtaining the solid particles in the predetermined particle size range may be determined according to the particle size. For example, if the solid particles having a larger particle diameter are desired, the solid particles remaining in the wall are retained, and the liquid is retained. In the case of a solid particle having a smaller particle size, if it is desired to obtain a solid particle having a smaller particle size, the solid particles in the liquid are retained, and the solid particles having a larger particle size remaining on the wall are moved. except.

請參閱第7A和7B圖,其係分別為螢光粉藉由本發明之離心分離固體粒子之製造方法分離前和分離後之粒徑分佈曲線圖。所使用之螢光粉係為發黃色螢光之釔鋁石榴石(yttrium aluminum garnet,YAG)。如第7A圖示,典型之螢光粉粒徑分佈範圍非常廣,其分佈範圍約為0.1-40μm。然而,藉由本發明之離心分離方法,可控制分離出不同之預設粒徑範圍,如第7B圖中所示,可分離取得各種不同粒徑範圍之YAG螢光粉。 Please refer to FIGS. 7A and 7B, which are respectively a particle size distribution curve of the phosphor powder before and after separation by the method for producing the centrifugally separated solid particles of the present invention. The phosphor powder used was yellow yttrium aluminum garnet (YAG). As shown in Figure 7A, a typical phosphor particle size distribution is very broad and has a distribution ranging from about 0.1 to about 40 microns. However, by the centrifugal separation method of the present invention, it is possible to control the separation of different predetermined particle size ranges, and as shown in Fig. 7B, YAG phosphor powders of various particle size ranges can be separated.

請參閱第8圖,其係為本發明之具螢光粉之發光二極體裝置之一實施例之示 意圖。此發光二極體裝置1包括一金屬反射杯10、一發光二極體晶片30、一光致發光螢光體50及一電流調整裝置70。其中,金屬反射杯10係包括一底部20。發光二極體晶片30係發藍光40,且設置於金屬反射杯10的底部20上。光致發光螢光體50之組成係包括根據本發明之離心分離固體粒子之製造方法所製造得粒徑均一之發黃光60之螢光粉和矽膠,且此光致發光螢光體50係覆蓋於發光二極體晶片30上,進而與藍光40混合而發出白光,以及電流調整裝置70係用以調整發光二極體裝置1的電流量。另外,發藍光40之發光二極體晶片30可為氮化鎵、氮化銦鎵或其混合物之材料所製得,而發黃光60之螢光粉可為含有三價鈰(Ce3+)之釔鋁石榴石。 Please refer to FIG. 8 , which is a schematic diagram of an embodiment of a phosphor-emitting diode device of the present invention. The LED device 1 includes a metal reflector cup 10, a light emitting diode chip 30, a photoluminescence phosphor 50, and a current adjustment device 70. The metal reflector cup 10 includes a bottom portion 20. The LED wafer 30 emits blue light 40 and is disposed on the bottom 20 of the metal reflector cup 10. The composition of the photoluminescence phosphor 50 includes a phosphor powder and a tantalum gel having a uniform particle size of yellow light 60 produced according to the method for producing a centrifugally separated solid particle of the present invention, and the photoluminescence phosphor 50 is The light-emitting diode chip 30 is covered, and then mixed with the blue light 40 to emit white light, and the current adjusting device 70 is used to adjust the amount of current of the light-emitting diode device 1. In addition, the blue light emitting diode 30 of the blue light 40 may be made of a material of gallium nitride, indium gallium nitride or a mixture thereof, and the fluorescent powder of the yellow light 60 may contain trivalent germanium (Ce 3+). ) 钇 aluminum garnet.

請參閱第9圖,其係為本發明之螢光粉粒徑對色彩影響之一實施例之曲線圖。圖中,係為藉由本發明之離心分離固體粒子之製造方法所製造得之螢光粉導入白光發光二極體封裝後,在相同螢光粉濃度下,不同粒徑對色彩的影響,其顯示螢光粉粒徑確實影響螢光效益。 Please refer to Fig. 9, which is a graph showing an embodiment of the effect of the particle size of the phosphor powder on the color of the present invention. In the figure, the effect of different particle sizes on color at the same phosphor powder concentration after the phosphor powder produced by the method for producing centrifugally separated solid particles of the present invention is introduced into a white light emitting diode package is displayed. Fluorescent powder particle size does affect the fluorescence benefits.

請參閱第10圖,其係為本發明之不同螢光粉粒徑之色座標(x)與亮度之關係曲線圖。圖中係顯示相同濃度下,不同螢光粉粒徑之色座標(x)與亮度之關係,其中斜線係為相同螢光粉之色座標(x)與亮度之經驗關係。依此推論各螢光粉各別調整比例一致達到x=0.32的常用色座標,則其亮度與粒徑關係如第11圖所示。第11圖中顯示粒徑小於3.5μm的螢光粉對亮度有顯注負面影響。因此,若能將螢光粉中粒徑小於3.5μm的部份移除當能提高產品亮度,而本發明之離心分離固體粒子之製造方法即能達成此目標。 Please refer to Fig. 10, which is a graph showing the relationship between the color coordinates (x) of different phosphor powder sizes and the brightness of the present invention. The figure shows the relationship between the color coordinates (x) of different phosphor powder sizes and the brightness at the same concentration, wherein the diagonal line is the empirical relationship between the color coordinates (x) of the same phosphor and the brightness. Based on this, it is inferred that the respective color coordinates of each phosphor powder are uniformly adjusted to reach x=0.32, and the relationship between brightness and particle size is as shown in Fig. 11. In Fig. 11, it is shown that the phosphor powder having a particle diameter of less than 3.5 μm has a significant negative effect on the brightness. Therefore, if the portion of the phosphor powder having a particle diameter of less than 3.5 μm can be removed, the brightness of the product can be improved, and the method for producing the centrifugally separated solid particles of the present invention can achieve the object.

請參閱第12A和12B圖,其係分別為粒徑的分散程度對色座標(x)及亮度的分散影響之關係曲線圖。圖中,可以看出粒徑的分散程度對色座標(x)及亮度均有非常線性的影響,其中第12A圖中右下角較偏移直線之點有其特殊光學原因並非實驗誤差。因此藉由本發明之離心分離固體粒子之製造方法所 製得之螢光粉,可以明顯提高白光發光二極體產品的色座標及亮度的集中度。 Please refer to Figures 12A and 12B, which are graphs showing the relationship between the dispersion degree of particle size and the dispersion of color coordinates (x) and brightness, respectively. In the figure, it can be seen that the degree of dispersion of the particle size has a very linear effect on the color coordinates (x) and the brightness. Among them, the point in the lower right corner of Fig. 12A that is offset from the straight line has its special optical reason and is not an experimental error. Therefore, the method for producing a centrifugally separated solid particle of the present invention The obtained phosphor powder can significantly improve the color coordinates and brightness concentration of the white light emitting diode product.

以上所述僅為舉例性,而非為限制性者。任何未脫離本發明之精神與範疇,而對其進行之等效修改或變更,均應包含於後附之申請專利範圍中。 The above is intended to be illustrative only and not limiting. Any equivalent modifications or alterations to the spirit and scope of the invention are intended to be included in the scope of the appended claims.

51‧‧‧容置單元 51‧‧‧ accommodating unit

52‧‧‧驅動單元 52‧‧‧Drive unit

53‧‧‧控制單元 53‧‧‧Control unit

Claims (29)

一種離心分離裝置,其由下列單元所構成:一容置單元,用以置放含有一固體粒子之一液體;一驅動單元,用以驅動該容置單元在離心時同步運轉,使該容置單元之一器壁和該液體產生一相對流速;以及一控制單元,用以控制該驅動單元驅動該容置單元之速度,進而控制該相對流速,以調整該液體對該固體粒子之一曳引力,和該固體粒子與該器壁間或該固體粒子與該固體粒子間之一最大靜摩擦力之平衡點,藉以取得具一預設粒徑範圍之該固體粒子;其中當該曳引力低於該平衡點時,所受之該曳引力大於該最大靜磨擦力的該固體粒子無法留滯在器壁,而被液體曳引帶往其他位置;當該曳引力高於該平衡點時,所受之該曳引力小於該最大靜磨擦力之粒子留滯在器壁,進而分離出取得具該預設粒徑範圍之該固體粒子。 A centrifugal separation device is composed of the following units: a receiving unit for arranging a liquid containing a solid particle; and a driving unit for driving the accommodating unit to operate synchronously during centrifugation to enable the accommodating unit a wall of the unit and the liquid generate a relative flow rate; and a control unit for controlling the speed at which the driving unit drives the accommodating unit, thereby controlling the relative flow rate to adjust the liquid to drag the solid particle And a balance point between the solid particle and the wall or a maximum static friction between the solid particle and the solid particle, thereby obtaining the solid particle having a predetermined particle size range; wherein when the traction force is lower than the At the equilibrium point, the solid particles that are subjected to the traction force greater than the maximum static friction force cannot remain in the wall, but are carried by the liquid to other locations; when the traction force is higher than the equilibrium point, The particles whose traction force is less than the maximum static friction force are retained on the wall, and the solid particles having the predetermined particle size range are separated. 如申請專利範圍第1項所述之離心分離裝置,其中該預設粒徑範圍係為微米等級或奈米等級。 The centrifugal separation device of claim 1, wherein the predetermined particle size range is a micron rating or a nanometer rating. 如申請專利範圍第1項所述之離心分離裝置,其中該預設粒徑範圍係為1-10nm。 The centrifugal separation device of claim 1, wherein the predetermined particle size range is 1-10 nm. 如申請專利範圍第3項所述之離心分離裝置,其中該預設粒徑範圍係更進一步為1-3nm。 The centrifugal separation device of claim 3, wherein the predetermined particle size range is further 1-3 nm. 如申請專利範圍第1項所述之離心分離裝置,其中該驅動單元係以包括機械推進、非平衡軸轉動或振動方法產生該相對流速。 The centrifugal separation device of claim 1, wherein the driving unit generates the relative flow rate by a method including mechanical propulsion, unbalanced shaft rotation or vibration. 如申請專利範圍第1項所述之離心分離裝置,其中該液體包括水溶液或有機溶劑。 The centrifugal separation device of claim 1, wherein the liquid comprises an aqueous solution or an organic solvent. 如申請專利範圍第1項所述之離心分離裝置,其中該固體粒子係以不溶於水之材料製成。 The centrifugal separation device of claim 1, wherein the solid particles are made of a material that is insoluble in water. 如申請專利範圍第7項所述之離心分離裝置,其中該不溶於水之材料包括樹脂、塑膠、金屬、石墨、乙酸乙酯、三聚氰胺、聚乙烯、聚苯乙烯、聚酯、聚氯化乙烯、聚醯胺、聚丙烯、耐綸、聚偏氟乙烯、聚胺甲酸乙酯、丙烯酸樹脂、聚矽氧烷、結晶性纖維素、澱粉、矽石、氧化鋁、滑石、高嶺土、氧化鈦、氧化鋅、石英、磷酸鈣或螢光粉。 The centrifugal separation device of claim 7, wherein the water-insoluble material comprises resin, plastic, metal, graphite, ethyl acetate, melamine, polyethylene, polystyrene, polyester, polyvinyl chloride. , polyamide, polypropylene, nylon, polyvinylidene fluoride, polyurethane, acrylic resin, polyoxyalkylene, crystalline cellulose, starch, vermiculite, alumina, talc, kaolin, titanium oxide, Zinc oxide, quartz, calcium phosphate or phosphor powder. 如申請專利範圍第8項所述之離心分離裝置,其中該螢光粉包括釔鋁石榴石。 The centrifugal separation device of claim 8, wherein the phosphor powder comprises yttrium aluminum garnet. 如申請專利範圍第9項所述之離心分離裝置,其中該螢光粉係進一步包括由二族的鈣、鍶、鋇、鋅、或鎘、汞搭配六族的硫、硒製備而成之母體材料,以及與錳、銅、銀、或鑭系元素之鈰、銪、釤、鋱過渡金屬之添加物所組成。 The centrifugal separation device according to claim 9, wherein the phosphor powder further comprises a matrix prepared from a group of calcium, strontium, barium, zinc, or cadmium, mercury, and sulfur of the six groups. Materials, and additives with transition metals such as lanthanum, cerium, lanthanum and lanthanum of manganese, copper, silver or lanthanides. 一種離心分離固體粒子之製造方法,其由下列步驟所構成:置放含有一固體粒子之一液體於一容置單元內;驅動該容置單元在離心時同步運轉,使該容置單元之一器壁與該液體產生一相對流速;控制該容置單元之速度,進而控制該相對流速,以調整該液體對該固體粒子之一曳引力,和該固體粒子與該器壁間或該固體粒子與該固體粒子間之一最大靜摩擦力之平衡點;以及取得具一預設粒徑範圍之該固體粒子;其中當該曳引力低於該平衡點時,所受之該曳引力大於該最大靜磨擦力的該固體粒子無法留滯在器壁,而被液體曳引帶往其他位置;當該曳引力高於該平衡點時,所受之該曳引力小於該最大靜磨擦力之粒子留滯在器壁,進而分離出取得具該預設粒徑範圍之該固體粒子。 A method for manufacturing a centrifugally separated solid particle, which comprises the steps of: placing a liquid containing a solid particle in a receiving unit; driving the receiving unit to operate synchronously during centrifugation to make the receiving unit The wall generates a relative flow rate with the liquid; controlling the speed of the accommodating unit to control the relative flow rate to adjust the traction force of the liquid to one of the solid particles, and the solid particle and the wall or the solid particle a balance point of maximum static friction with the solid particle; and obtaining the solid particle having a predetermined particle size range; wherein when the traction force is lower than the equilibrium point, the traction force is greater than the maximum static force The frictional solid particles cannot stay on the wall and are carried by the liquid to other locations; when the traction force is higher than the equilibrium point, the traction force is less than the maximum static friction particle retention At the wall, the solid particles having the predetermined particle size range are separated. 如申請專利範圍第11項所述之離心分離固體粒子之製造方法,其中該曳引力係正比於該固體粒子之粒徑和該相對流速之乘積。 The method for producing a centrifugally separated solid particle according to claim 11, wherein the traction force is proportional to a product of a particle diameter of the solid particle and the relative flow velocity. 如申請專利範圍第11項所述之離心分離固體粒子之製造方法,其中該最大靜摩擦力係正比於該固體粒子之粒徑立方。 The method for producing a centrifugally separated solid particle according to claim 11, wherein the maximum static friction force is proportional to a particle diameter cube of the solid particle. 如申請專利範圍第11項所述之離心分離固體粒子之製造方法,其中該預設粒徑範圍係為微米等級或奈米等級。 The method for producing a centrifugally separated solid particle according to claim 11, wherein the predetermined particle size range is a micron rating or a nanometer rating. 如申請專利範圍第11項所述之離心分離固體粒子之製造方法,其中該預設粒徑範圍係為1-10nm。 The method for producing a centrifugally separated solid particle according to claim 11, wherein the predetermined particle diameter ranges from 1 to 10 nm. 如申請專利範圍第15項所述之離心分離固體粒子之製造方法,其中該預設粒徑範圍係更進一步為1-3nm。 The method for producing a centrifugally separated solid particle according to claim 15, wherein the predetermined particle size range is further 1-3 nm. 如申請專利範圍第11項所述之離心分離固體粒子之製造方法,其中該相對流速係以包括機械推進、非平衡軸轉動或振動方法所產生。 The method for producing a centrifugally separated solid particle according to claim 11, wherein the relative flow rate is produced by a method including mechanical propulsion, unbalanced shaft rotation or vibration. 如申請專利範圍第11項所述之離心分離固體粒子之製造方法,其中該液體包括水溶液或有機溶劑。 The method for producing a centrifugally separated solid particle according to claim 11, wherein the liquid comprises an aqueous solution or an organic solvent. 如申請專利範圍第11項所述之離心分離固體粒子之製造方法,其中該固體粒子係以不溶於水之材料製成。 The method for producing a centrifugally separated solid particle according to claim 11, wherein the solid particle is made of a material that is insoluble in water. 如申請專利範圍第19項所述之離心分離固體粒子之製造方法,其中該不溶於水之材料包括樹脂、塑膠、金屬、石墨、乙酸乙酯、三聚氰胺、聚乙烯、聚苯乙烯、聚酯、聚氯化乙烯、聚醯胺、聚丙烯、耐綸、聚偏氟乙烯、聚胺甲酸乙酯、丙烯酸樹脂、聚矽氧烷、結晶性纖維素、澱粉、矽石、氧化鋁、滑石、高嶺土、氧化鈦、氧化鋅、石英、磷酸鈣或螢光粉。 The method for producing a centrifugally separated solid particle according to claim 19, wherein the water-insoluble material comprises resin, plastic, metal, graphite, ethyl acetate, melamine, polyethylene, polystyrene, polyester, Polyvinyl chloride, polyamide, polypropylene, nylon, polyvinylidene fluoride, polyurethane, acrylic resin, polyoxyalkylene, crystalline cellulose, starch, vermiculite, alumina, talc, kaolin , titanium oxide, zinc oxide, quartz, calcium phosphate or phosphor powder. 如申請專利範圍第20項所述之離心分離固體粒子之製造方法,其中該螢光粉包括釔鋁石榴石。 The method for producing a centrifugally separated solid particle according to claim 20, wherein the phosphor powder comprises yttrium aluminum garnet. 如申請專利範圍第21項所述之離心分離固體粒子之製造方法,其中該螢 光粉係進一步包括由二族的鈣、鍶、鋇、鋅、或鎘、汞搭配六族的硫、硒製備而成之母體材料,以及與錳、銅、銀、或鑭系元素之鈰、銪、釤、鋱過渡金屬之添加物所組成。 The method for producing a centrifugally separated solid particle according to claim 21, wherein the firefly The light powder system further comprises a parent material prepared from a group of calcium, strontium, barium, zinc, or cadmium, mercury, and a group of sulfur, selenium, and a manganese, copper, silver, or lanthanide element. It is composed of additives of transition metals such as lanthanum, cerium and lanthanum. 一種用於發光二極體裝置之固體粒子,其由下列製備方法所構成:置放含有一固體粒子之一液體於一容置單元內;驅動該容置單元在離心時同步運轉,使該容置單元之一器壁與該液體產生一相對流速;控制該容置單元之速度,進而控制該相對流速,以調整該液體對該固體粒子之一曳引力,和該固體粒子與該器壁間或該固體粒子與該固體粒子間之一最大靜摩擦力之平衡點;以及取得具一預設粒徑範圍之該固體粒子;其中當該曳引力低於該平衡點時,所受之該曳引力大於該最大靜磨擦力的該固體粒子無法留滯在器壁,而被液體曳引帶往其他位置;當該曳引力高於該平衡點時,所受之該曳引力小於該最大靜磨擦力之粒子留滯在器壁,進而分離出取得具該預設粒徑範圍之該固體粒子。 A solid particle for a light-emitting diode device, which is composed of the following preparation method: placing a liquid containing a solid particle in a receiving unit; driving the receiving unit to operate synchronously during centrifugation to make the volume The wall of the unit generates a relative flow rate with the liquid; controlling the speed of the accommodating unit to control the relative flow rate to adjust the traction force of the liquid to one of the solid particles, and between the solid particles and the wall Or a balance point of the maximum static friction between the solid particles and the solid particles; and obtaining the solid particles having a predetermined particle size range; wherein the traction force is received when the traction force is lower than the equilibrium point The solid particles larger than the maximum static friction force cannot be retained on the wall, but are carried by the liquid to other positions; when the traction force is higher than the equilibrium point, the traction force is less than the maximum static friction force. The particles remain in the wall and are separated to obtain the solid particles having the predetermined particle size range. 如申請專利範圍第23項所述之用於發光二極體裝置之固體粒子,其該固體粒子係為螢光粉。 The solid particles for a light-emitting diode device according to claim 23, wherein the solid particles are fluorescent powder. 如申請專利範圍第24項所述之用於發光二極體裝置之固體粒子,其該螢光粉包括釔鋁石榴石。 The solid particle for a light-emitting diode device according to claim 24, wherein the phosphor powder comprises yttrium aluminum garnet. 如申請專利範圍第25項所述之用於發光二極體裝置之固體粒子,其該螢光粉係進一步包括由二族的鈣、鍶、鋇、鋅、或鎘、汞搭配六族的硫、硒製備而成之母體材料,以及與錳、銅、銀、或鑭系元素之鈰、銪、釤、鋱過渡金屬之添加物所組成。 The solid particle for a light-emitting diode device according to claim 25, wherein the phosphor powder further comprises sulfur of a group of two groups of calcium, barium, strontium, zinc, or cadmium or mercury. The parent material prepared from selenium and the additive of transition metal of lanthanum, cerium, lanthanum and cerium with manganese, copper, silver or lanthanide. 如申請專利範圍第23項所述之用於發光二極體裝置之固體粒子,其中該預設粒徑範圍係為微米等級或奈米等級。 The solid particle for a light-emitting diode device according to claim 23, wherein the predetermined particle size range is a micron rating or a nanometer rating. 如申請專利範圍第23項所述之用於發光二極體裝置之固體粒子,其中該預設粒徑範圍係為1-10nm。 The solid particles for a light-emitting diode device according to claim 23, wherein the predetermined particle size range is 1-10 nm. 如申請專利範圍第28項所述之用於發光二極體裝置之固體粒子,其中該預設粒徑範圍係更進一步為1-3nm。 The solid particles for a light-emitting diode device according to claim 28, wherein the predetermined particle size range is further 1-3 nm.
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TW200528538A (en) * 2004-01-29 2005-09-01 Univ Keio Metal oxide phosphor microparticle, and its producing process, method of separating thereof and dispersion liquid utilizing same; fluorescence conversion membrane and converter; fluorescent liquid and paste; phosphor and process for producing thereof

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