TWI568005B - A solar cell module manufacturing method, a solar cell module manufacturing method, a solar cell module - Google Patents
A solar cell module manufacturing method, a solar cell module manufacturing method, a solar cell module Download PDFInfo
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- TWI568005B TWI568005B TW102120663A TW102120663A TWI568005B TW I568005 B TWI568005 B TW I568005B TW 102120663 A TW102120663 A TW 102120663A TW 102120663 A TW102120663 A TW 102120663A TW I568005 B TWI568005 B TW I568005B
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Classifications
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
- H01L31/00—Semiconductor devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation and specially adapted either for the conversion of the energy of such radiation into electrical energy or for the control of electrical energy by such radiation; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof
- H01L31/04—Semiconductor devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation and specially adapted either for the conversion of the energy of such radiation into electrical energy or for the control of electrical energy by such radiation; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof adapted as photovoltaic [PV] conversion devices
- H01L31/042—PV modules or arrays of single PV cells
- H01L31/05—Electrical interconnection means between PV cells inside the PV module, e.g. series connection of PV cells
- H01L31/0504—Electrical interconnection means between PV cells inside the PV module, e.g. series connection of PV cells specially adapted for series or parallel connection of solar cells in a module
- H01L31/0512—Electrical interconnection means between PV cells inside the PV module, e.g. series connection of PV cells specially adapted for series or parallel connection of solar cells in a module made of a particular material or composition of materials
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
- H01L31/00—Semiconductor devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation and specially adapted either for the conversion of the energy of such radiation into electrical energy or for the control of electrical energy by such radiation; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof
- H01L31/04—Semiconductor devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation and specially adapted either for the conversion of the energy of such radiation into electrical energy or for the control of electrical energy by such radiation; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof adapted as photovoltaic [PV] conversion devices
- H01L31/042—PV modules or arrays of single PV cells
- H01L31/05—Electrical interconnection means between PV cells inside the PV module, e.g. series connection of PV cells
- H01L31/0504—Electrical interconnection means between PV cells inside the PV module, e.g. series connection of PV cells specially adapted for series or parallel connection of solar cells in a module
- H01L31/0516—Electrical interconnection means between PV cells inside the PV module, e.g. series connection of PV cells specially adapted for series or parallel connection of solar cells in a module specially adapted for interconnection of back-contact solar cells
-
- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E10/00—Energy generation through renewable energy sources
- Y02E10/50—Photovoltaic [PV] energy
Description
本發明係關於一種太陽電池模組之製造方法、太陽電池用導電性接著劑、太陽電池模組，尤其係關於一種將形成於太陽電池之電極、與連接太陽電池間之標記線導電連接之太陽電池用導電性接著劑之改良。本申請案係基於2012年6月13日於日本提出申請之日本專利申請編號特願2012-134307而主張優先權者，藉由參照該申請案而引用於本申請案中。 The present invention relates to a method for manufacturing a solar cell module, a conductive adhesive for a solar cell, and a solar cell module, and more particularly to a solar cell that is electrically connected to an electrode formed on a solar cell and connected to a solar cell. Improvement of the conductive adhesive for batteries. The present application claims priority based on Japanese Patent Application No. 2012-134307, filed on Jan.
習知，使用有將於受光面設置p型電極與n型電極中之一者，於與受光面為相反側之背面設置p型電極與n型電極中之另一者之太陽電池複數個連接而成之太陽電池模組。此種太陽電池模組50係如圖8所示般，將設置於太陽電池51A之受光面之正面電極52、與設置於鄰接之太陽電池51B之背面的背面電極53藉由成為內部連接線之標記線54每幾處進行焊接，藉此構成太陽電池串。 It is known to use a solar cell in which one of a p-type electrode and an n-type electrode is provided on the light-receiving surface, and the other of the p-type electrode and the n-type electrode is provided on the back side opposite to the light-receiving surface. A solar cell module. As shown in FIG. 8, the solar cell module 50 is formed by the front surface electrode 52 provided on the light receiving surface of the solar cell 51A and the back surface electrode 53 provided on the back surface of the adjacent solar cell 51B. The marking line 54 is welded every few places, thereby constituting a string of solar cells.
又，有p型電極與n型電極均設置於太陽電池單元之背面之所謂背接觸型之太陽電池模組。背接觸型太陽電池模組係p型電極與n型電極均設置於太陽電池單元之背面，於連接複數個太陽電池單元時，由成為內部連接線之標記線將背面彼此連接。因此，背接觸型太陽電池模組無須於成為受光面之太陽電池單元正面設置電極或標記線，可謀求受光效率之提高，並且外觀亦變得良好。又，背接觸型太陽電池模組與於太陽電池 單元之正背面設置電極之類型不同，無須遍及一太陽電池單元之正面與另一太陽電池單元之背面地引繞標記線，製造步驟亦變得容易。 Further, a so-called back contact type solar cell module in which both the p-type electrode and the n-type electrode are provided on the back surface of the solar cell unit is provided. In the back contact type solar cell module, the p-type electrode and the n-type electrode are both disposed on the back surface of the solar cell unit, and when a plurality of solar cell units are connected, the back surfaces are connected to each other by a mark line which becomes an internal connection line. Therefore, the back contact type solar cell module does not need to provide an electrode or a marking line on the front surface of the solar cell unit that is a light receiving surface, and can improve the light receiving efficiency and the appearance is also good. Moreover, the back contact type solar cell module and the solar cell The type of electrodes disposed on the front and back sides of the unit is different, and it is not necessary to guide the marking lines over the front surface of one solar battery unit and the back surface of another solar battery unit, and the manufacturing steps are also easy.
圖9中表示習知之背接觸型太陽電池模組60中之太陽電池之連接構成。太陽電池61中，p型電極62及n型電極63於背面交替地並設，沿一側緣部形成與p型電極62之各一端連續之p型電極集電部64，沿另一側緣部形成有與n型電極63之各一端連續之n型電極集電部65。 FIG. 9 shows the connection configuration of the solar cells in the conventional back contact type solar cell module 60. In the solar cell 61, the p-type electrode 62 and the n-type electrode 63 are alternately arranged on the back surface, and a p-type electrode collecting portion 64 continuous with each end of the p-type electrode 62 is formed along one edge portion along the other side edge. An n-type electrode collecting portion 65 continuous with each end of the n-type electrode 63 is formed in the portion.
p型電極集電部64及n型電極集電部65於相對向之位置設置多處與標記線66之連接點67。而且，各太陽電池61係以p型電極集電部64與n型電極集電部65鄰接之方式配置，由細線狀之標記線66將各連接點67彼此焊接。 The p-type electrode collecting portion 64 and the n-type electrode collecting portion 65 are provided at a plurality of places where they are connected to the marking line 66 at a position opposite to each other. Further, each of the solar cells 61 is disposed such that the p-type electrode collecting portion 64 is adjacent to the n-type electrode collecting portion 65, and the respective connecting points 67 are welded to each other by the thin line-shaped marking line 66.
[專利文獻1]日本特開2005-191479號公報 [Patent Document 1] Japanese Patent Laid-Open Publication No. 2005-191479
但是，於將該等正背面設置有電極之太陽電池連接之太陽電池模組50或背接觸型之太陽電池模組60中，當藉由焊接進行標記線54、66之連接之情形時，由於要以約260℃之高溫進行連接處理，故有可能導致太陽電池51、61翹曲。 However, in the case of the solar cell module 50 or the back contact type solar cell module 60 in which the solar cells are connected to the front and back sides of the electrodes, when the bonding lines 54 and 66 are connected by soldering, The connection treatment is performed at a high temperature of about 260 ° C, which may cause the solar cells 51, 61 to warp.
又，為了提高太陽電池模組之輸出而必須降低標記線54、66產生之電阻值，因此必須增大標記線54、66之截面積。但是，若增大標記線之截面積，則標記線本身之剛性變高，有可能因伴隨熱膨脹之於與標記線54、66之焊接點之間產生的內部應力，而使標記線54、66之連接可靠性降低。進而，由於在焊接中使用助熔劑(flux)，故亦有可能因助熔劑之殘渣，而導致太陽電池51、61之密封樹脂之剝落或接著性變差。 Moreover, in order to increase the output of the solar cell module, it is necessary to reduce the resistance value generated by the marking lines 54, 66. Therefore, it is necessary to increase the cross-sectional area of the marking lines 54, 66. However, if the cross-sectional area of the marking line is increased, the rigidity of the marking line itself becomes high, and the marking lines 54 and 66 may be caused by internal stress generated between the welding points with the marking lines 54 and 66 accompanying thermal expansion. The connection reliability is reduced. Further, since a flux is used in the soldering, there is a possibility that the sealing resin of the solar cells 51, 61 is peeled off or the adhesion is deteriorated due to the residue of the flux.
又，標記線54、66之連接中亦有不使用焊料，而使用於成為接著劑之絕緣性之熱硬化性樹脂組成物中含有導電性粒子之導電性接著漿料之方法。於使用導電性接著漿料之連接中，經由導電性接著漿料於太陽電池51、61之電極上配置標記線54、66，藉由自標記線54、66之上進行熱加壓，而使導電性粒子由太陽電池51、61之電極與標記線54、66夾持，由此謀求電性導通及機械性連接。但是，於使用導電性接著漿料之連接中，為了抑制連接電阻之上升而必須增多導電性粒子之含量。因此，藉由增多導電性粒子之含量而熱硬化性樹脂相對減少，標記線54、66之接著強度有可能降低。 Further, in the connection of the marking lines 54 and 66, there is a method in which a conductive paste of conductive particles is used in an insulating thermosetting resin composition which is an adhesive, without using solder. In the connection using the conductive paste, the mark lines 54 and 66 are placed on the electrodes of the solar cells 51 and 61 via the conductive paste, and the heat is applied from the mark lines 54 and 66. The conductive particles are sandwiched between the electrodes of the solar cells 51 and 61 and the marking lines 54 and 66, thereby achieving electrical conduction and mechanical connection. However, in the connection using the conductive paste, it is necessary to increase the content of the conductive particles in order to suppress an increase in the connection resistance. Therefore, the thermosetting resin is relatively reduced by increasing the content of the conductive particles, and the bonding strength of the marking lines 54 and 66 may be lowered.
進而，於近年來之太陽電池中，為了降低因熱加壓產生之負荷，於連接標記線54、66之導電性接著劑中亦要求速硬化性。因此，使用藉由反應速度較快之自由基聚合而固化之導電性接著劑。但是，若反應速度較快，則在由標記線54、66與太陽電池51、61之電極夾持導電性粒子之前黏合劑樹脂便硬化，亦有可能損害電性連接可靠性。又，若欲藉由增多導電性粒子之含量來維持連接可靠性，則黏合劑樹脂相對減少，標記線54、66之接著強度有可能降低。 Further, in recent solar cells, in order to reduce the load due to thermal pressurization, rapid hardenability is also required in the conductive adhesive for connecting the marking lines 54 and 66. Therefore, a conductive adhesive which is cured by radical polymerization having a high reaction rate is used. However, if the reaction rate is fast, the binder resin is hardened before the conductive particles are sandwiched between the marking wires 54, 66 and the electrodes of the solar cells 51, 61, and the electrical connection reliability may be impaired. Further, if the connection reliability is to be maintained by increasing the content of the conductive particles, the binder resin is relatively decreased, and the bonding strength of the marking lines 54 and 66 may be lowered.
因此，本發明之目的在於提供一種即便於使用導電性接著劑進行連接之情形時，亦不會損害導通可靠性或接著強度之太陽電池模組之製造方法、太陽電池用導電性接著劑、太陽電池模組。 Accordingly, it is an object of the present invention to provide a solar cell module manufacturing method, a solar cell conductive adhesive, and a solar cell which do not impair the conduction reliability or the bonding strength even when a conductive adhesive is used for connection. Battery module.
為解決上述課題，本發明之太陽電池模組之製造方法係製造將形成於複數個太陽電池之電極彼此經由連接用導體連接而成之太陽電池模組之方法，且使導電性接著劑介存於上述太陽電池之電極與上述連接用導體之間，具有將上述電極與上述連接用導體加熱按壓而使上述導電性接著劑硬化，從而將上述電極與上述連接用導體連接之步驟，上述導電性接 著劑係於熱硬化性樹脂中含有焊料粉及銀粉，上述焊料粉於上述加熱按壓處理下與上述銀粉反應，生成高熔點焊料合金，其顯示高於上述焊料粉之熔融溫度之熔點。 In order to solve the above problems, the method for manufacturing a solar cell module of the present invention is to manufacture a solar cell module in which electrodes of a plurality of solar cells are connected to each other via a connection conductor, and to deposit a conductive adhesive. Between the electrode of the solar cell and the connecting conductor, the electrode and the connecting conductor are heated and pressed to cure the conductive adhesive, and the electrode is connected to the connecting conductor. Connect The coating agent contains a solder powder and a silver powder in the thermosetting resin, and the solder powder reacts with the silver powder under the heat pressing treatment to form a high melting point solder alloy which exhibits a melting point higher than a melting temperature of the solder powder.
又，本發明之太陽電池用導電性接著劑係將形成於構成太陽電池模組之太陽電池之電極、與連接形成於複數個上述太陽電池之上述電極彼此之連接用導體加以連接者，且於熱硬化性樹脂含有焊料粉及銀粉，上述焊料粉為Sn-Bi，Sn-Bi：銀粉之質量比為2：1~1：2。 Further, the conductive adhesive for a solar cell of the present invention is formed by connecting an electrode formed on a solar cell constituting the solar cell module to a connection conductor connecting the electrodes formed in the plurality of solar cells, and The thermosetting resin contains solder powder and silver powder, and the solder powder is Sn-Bi, and the mass ratio of Sn-Bi:silver powder is 2:1 to 1:2.
又，本發明之太陽電池模組係將形成於複數個太陽電池之電極彼此經由連接用導體連接而成者，且形成於上述太陽電池之電極與上述連接用導體係利用導電性接著劑而連接，上述導電性接著劑係於熱硬化性樹脂中含有焊料粉及銀粉，上述焊料粉於上述加熱按壓處理下與上述銀粉反應，生成高熔點焊料合金，其顯示高於上述焊料粉之熔融溫度之熔點。 Further, in the solar battery module of the present invention, the electrodes formed in the plurality of solar cells are connected to each other via a connection conductor, and the electrode formed in the solar cell and the connection guide system are connected by a conductive adhesive. The conductive adhesive contains solder powder and silver powder in the thermosetting resin, and the solder powder reacts with the silver powder under the heat pressing treatment to form a high melting point solder alloy, which is higher than the melting temperature of the solder powder. Melting point.
根據本發明，於熱硬化性樹脂中含有焊料粉及銀粉，上述焊料粉於上述加熱按壓處理下與上述銀粉反應，生成高熔點焊料合金，其顯示高於上述焊料粉之熔融溫度之熔點。因此，於使導電性接著劑熱硬化時，在達到熱硬化處理溫度之前焊料粉便熔融，藉此可由熱硬化性樹脂中相對少量之已熔融之焊料粉形成經由銀粉連續之網狀結構(金屬之連續相)，發揮較高之導通可靠性，並且可使熱硬化性樹脂之含量相對增大，使太陽電池之電極與連接用導體之接著強度提高。 According to the invention, the solder powder and the silver powder are contained in the thermosetting resin, and the solder powder reacts with the silver powder under the heat pressing treatment to form a high melting point solder alloy which exhibits a melting point higher than a melting temperature of the solder powder. Therefore, when the conductive adhesive is thermally hardened, the solder powder is melted before reaching the heat hardening treatment temperature, whereby a continuous network of the silver powder can be formed from a relatively small amount of the molten solder powder in the thermosetting resin (metal The continuous phase) exhibits high conduction reliability and relatively increases the content of the thermosetting resin, thereby improving the bonding strength between the electrode of the solar cell and the connecting conductor.
1‧‧‧太陽電池模組 1‧‧‧Solar battery module
2‧‧‧太陽電池 2‧‧‧Solar battery
3‧‧‧連接用導體 3‧‧‧Connecting conductor
4‧‧‧太陽電池串 4‧‧‧Solar battery string
5‧‧‧矩陣 5‧‧‧Matrix
6‧‧‧片材 6‧‧‧Sheet
7‧‧‧表面護罩 7‧‧‧Surface shield
11‧‧‧p型電極 11‧‧‧p-type electrode
12‧‧‧n型電極 12‧‧‧n type electrode
13‧‧‧p型電極集電部 13‧‧‧p type electrode collector
14‧‧‧n型電極集電部 14‧‧‧n type electrode collector
16‧‧‧絕緣基板 16‧‧‧Insert substrate
17‧‧‧配線 17‧‧‧Wiring
17a‧‧‧端子 17a‧‧‧ Terminal
18‧‧‧絕緣層 18‧‧‧Insulation
20‧‧‧導電性接著漿料 20‧‧‧ Conductivity followed by slurry
21‧‧‧導電性接著膜 21‧‧‧ Conductive adhesive film
23‧‧‧熱硬化性樹脂 23‧‧‧ thermosetting resin
24‧‧‧轉盤 24‧‧‧ Turntable
30‧‧‧太陽電池模組 30‧‧‧Solar battery module
31‧‧‧太陽電池 31‧‧‧Solar battery
32‧‧‧標記線 32‧‧‧ mark line
33‧‧‧正面電極 33‧‧‧Front electrode
34‧‧‧背面電極 34‧‧‧Back electrode
圖1係表示太陽電池模組之分解立體圖。 Fig. 1 is an exploded perspective view showing a solar battery module.
圖2係表示太陽電池單元之受光面側之立體圖。 Fig. 2 is a perspective view showing the light receiving surface side of the solar battery unit.
圖3係表示太陽電池單元之剖面圖。 Fig. 3 is a cross-sectional view showing a solar battery unit.
圖4係表示太陽電池單元之製造步驟之剖面圖。 Fig. 4 is a cross-sectional view showing a manufacturing step of the solar battery unit.
圖5係表示導電性接著膜之剖面圖。 Fig. 5 is a cross-sectional view showing a conductive adhesive film.
圖6係表示太陽電池模組之剖面圖。 Fig. 6 is a cross-sectional view showing a solar battery module.
圖7係用以說明實施例之立體圖。 Figure 7 is a perspective view for explaining an embodiment.
圖8係表示習知之太陽電池模組之剖面圖。 Figure 8 is a cross-sectional view showing a conventional solar cell module.
圖9係表示習知之太陽電池模組之俯視圖。 Fig. 9 is a plan view showing a conventional solar battery module.
以下，一面參照圖式，一面對應用本發明之太陽電池模組之製造方法、太陽電池用導電性接著劑、太陽電池模組詳細地進行說明。再者，當然，本發明並不僅限定於以下實施形態，可於不脫離本發明之主旨之範圍內進行各種變更。又，圖式為模式性者，有各尺寸之比率等與現實者不同之情形。具體之尺寸等應參考以下之說明進行判斷。又，當然，圖式相互間亦包含相互之尺寸之關係或比率不同之部分。 Hereinafter, a method of manufacturing a solar cell module to which the present invention is applied, a conductive adhesive for a solar cell, and a solar cell module will be described in detail with reference to the drawings. It is a matter of course that the present invention is not limited to the embodiments described below, and various modifications can be made without departing from the spirit and scope of the invention. Further, the pattern is a pattern, and there is a case where the ratio of each size is different from the actual one. The specific dimensions and the like should be judged by referring to the following instructions. Moreover, of course, the drawings also include portions in which the relationship or ratio of the dimensions is different from each other.
[太陽電池模組] [Solar battery module]
關於應用本發明之太陽電池模組1，以p型電極與n型電極均設置於太陽電池之背面之所謂背接觸型之太陽電池模組為例進行說明。 In the solar battery module 1 to which the present invention is applied, a so-called back contact type solar battery module in which both a p-type electrode and an n-type electrode are provided on the back surface of the solar battery will be described as an example.
[太陽電池] [solar battery]
如圖1所示，太陽電池模組1具備矩陣5，該矩陣5具有複數個太陽電池單元2藉由成為內部連接線之連接用導體3而串列連接之太陽電池串4，且將該太陽電池串4複數個排列而成。而且，太陽電池模組1係藉由將該矩陣5與密封接著劑之片材6及設置於受光面側之表面護罩7一併總括地層疊而密封，最後，藉由在周圍安裝鋁等之金屬框架9而形成。 As shown in FIG. 1 , the solar cell module 1 includes a matrix 5 having a plurality of solar battery cells 2 connected in series by a connecting conductor 3 serving as an internal connecting wire, and the solar cell string 4 is connected in series. The battery string 4 is arranged in plural numbers. In addition, the solar cell module 1 is integrally sealed by laminating the matrix 5 together with the sheet 6 for sealing the adhesive and the surface shield 7 provided on the light-receiving surface side, and finally, aluminum or the like is attached thereto. The metal frame 9 is formed.
作為密封接著劑，例如可使用乙烯-乙烯醇樹脂(EVA)等透光性密封材。又，作為表面護罩7，例如可使用玻璃或透光性塑膠等透光 性之材料。 As the sealing adhesive, for example, a light-transmitting sealing material such as ethylene-vinyl alcohol resin (EVA) can be used. Further, as the surface shield 7, for example, light such as glass or translucent plastic can be used. Material of sex.
[太陽電池] [solar battery]
太陽電池2可使用單晶型矽型、多晶矽型、非晶矽型等之矽光電轉換元件、或薄膜型、化合物型、色素增感型等之光電轉換元件等作為光電轉換元件。其中，太陽電池2可較佳地使用發電效率優異之單晶型矽型之光電轉換元件。 As the solar cell 2, a photoelectric conversion element such as a single crystal type germanium type, a polycrystalline germanium type, or an amorphous germanium type, or a photoelectric conversion element such as a thin film type, a compound type or a dye-sensitized type can be used as the photoelectric conversion element. Among them, the solar cell 2 can preferably use a photoelectric conversion element of a single crystal type which is excellent in power generation efficiency.
[pn電極] [pn electrode]
如圖2及圖3所示，太陽電池2於成為受光面之正面2a未形成電極，於與受光面為相反側之背面2b形成有極性不同之p型電極11及n型電極12。 As shown in FIG. 2 and FIG. 3, the solar cell 2 has no electrodes formed on the front surface 2a of the light-receiving surface, and the p-type electrode 11 and the n-type electrode 12 having different polarities are formed on the back surface 2b opposite to the light-receiving surface.
太陽電池2中，線狀之p型電極11及n型電極12於背面2b交替地並設，且沿一側緣部設置與複數個p型電極11之各一端連接之p型電極集電部13，沿另一側緣部設置有與複數個n型電極12之各一端連接之n型電極集電部14。p型電極集電部13及n型電極集電部14沿太陽電池2之相對向之一側緣部及另一側緣部設置，且具有特定之寬度。藉此，太陽電池2係將p型電極11及p型電極集電部13、n型電極12及n型電極集電部14分別形成為梳狀，且分別相互錯開地進入至梳痕之間。 In the solar cell 2, the linear p-type electrode 11 and the n-type electrode 12 are alternately arranged on the back surface 2b, and a p-type electrode collecting portion connected to each end of the plurality of p-type electrodes 11 is provided along one edge portion. 13. An n-type electrode collecting portion 14 connected to each end of the plurality of n-type electrodes 12 is provided along the other side edge portion. The p-type electrode collecting portion 13 and the n-type electrode collecting portion 14 are provided along one side edge portion and the other side edge portion of the solar cell 2, and have a specific width. Thereby, the solar cell 2 has the p-type electrode 11 and the p-type electrode collecting portion 13, the n-type electrode 12, and the n-type electrode collecting portion 14 formed in a comb shape, respectively, and are respectively shifted into the comb marks. .
該等p型電極11、n型電極12、p型電極集電部13及n型電極集電部14例如係藉由在太陽電池2之背面2b將Ag漿料等導電性漿料以特定圖案塗佈、焙燒而形成。 The p-type electrode 11, the n-type electrode 12, the p-type electrode collecting portion 13, and the n-type electrode collecting portion 14 are formed of a specific pattern such as an Ag paste or the like on the back surface 2b of the solar cell 2, for example. It is formed by coating and baking.
而且，太陽電池2係藉由下述之連接用導體3而將p型電極集電部13與鄰接之太陽電池2之n型電極集電部14電性連接，藉此構成串列連接之太陽電池串4。連接用導體3與p型電極集電部13及n型電極集電部14之連接係藉由下述之導電性接著漿料20而進行。 Further, in the solar battery 2, the p-type electrode collecting portion 13 and the n-type electrode collecting portion 14 of the adjacent solar battery 2 are electrically connected by the connecting conductor 3 described below, thereby constituting the tandem-connected sun. Battery string 4. The connection between the connection conductor 3 and the p-type electrode collecting portion 13 and the n-type electrode collecting portion 14 is performed by the following conductive paste 20 described below.
[連接用導體] [Connecting conductor]
接著，對連接太陽電池2彼此之連接用導體3進行說明。如圖3所示，連接用導體3係於絕緣基板16上形成配線17，且具有例如用以將複數個太陽電池2串列連接之端子17a。作為絕緣基板16，可使用PET(聚對苯二甲酸乙二酯)、PEN(聚萘二甲酸乙二酯)、聚醯亞胺等高分子樹脂基板、使絕緣樹脂含浸於玻璃纖維而成之複合材料等。又，作為配線17、端子17a，可使用銅、鋁、鐵-鎳合金等。 Next, the conductor 3 for connecting the solar cells 2 to each other will be described. As shown in FIG. 3, the connection conductor 3 is formed on the insulating substrate 16 to form a wiring 17, and has, for example, a terminal 17a for connecting a plurality of solar cells 2 in series. As the insulating substrate 16, a polymer resin substrate such as PET (polyethylene terephthalate), PEN (polyethylene naphthalate) or polyimine can be used, and the insulating resin can be impregnated into the glass fiber. Composite materials, etc. Further, as the wiring 17 and the terminal 17a, copper, aluminum, an iron-nickel alloy or the like can be used.
再者，連接用導體3之配線17上係由絕緣層18被覆。絕緣層18由絕緣材料所構成，防止因自例如EVA片材釋出之乙酸氣體所致之腐蝕。作為絕緣材料，例如可列舉環氧樹脂、丙烯酸系樹脂、胺酯樹脂等，既可單獨使用該等樹脂，亦可併用2種以上。又，該等樹脂中亦可含有矽土、雲母、氧化鋁、硫酸鋇等無機粉末。 Further, the wiring 17 of the connection conductor 3 is covered with an insulating layer 18. The insulating layer 18 is composed of an insulating material to prevent corrosion due to acetic acid gas released from, for example, an EVA sheet. Examples of the insulating material include an epoxy resin, an acrylic resin, and an amine ester resin. These resins may be used alone or in combination of two or more. Further, these resins may contain inorganic powders such as alumina, mica, alumina, and barium sulfate.
連接用導體3係將端子17a經由下述之導電性接著漿料20等導電性接著劑分別配置於設置於一太陽電池2A之背面2b之p型電極集電部13、及設置於與該一太陽電池2A鄰接之另一太陽電池2B之背面2b之n型電極集電部14。繼而，連接用導體3藉由利用加熱按壓頭或減壓貼合機進行熱加壓，而使導電性接著漿料20硬化。藉此，複數個太陽電池2相互連接。 In the connection conductor 3, the terminal 17a is placed on the p-type electrode collecting portion 13 provided on the back surface 2b of the solar cell 2A via a conductive adhesive such as the following conductive paste 20, and is provided in the same. The solar cell 2A is adjacent to the n-type electrode collecting portion 14 of the back surface 2b of the other solar cell 2B. Then, the connecting conductor 3 is thermally pressurized by a heating press head or a pressure-reducing bonding machine to cure the conductive subsequent paste 20. Thereby, a plurality of solar cells 2 are connected to each other.
[導電性接著劑] [conductive adhesive]
接著，對連接太陽電池2之p型電極集電部13、n型電極集電部14、與連接用導體3之導電性接著劑進行說明。導電性接著劑可使用於例如成為接著劑之熱硬化性樹脂組成物中含有焊料粉及銀粉之導電性接著漿料20。 Next, the p-type electrode collecting portion 13, the n-type electrode collecting portion 14, and the conductive adhesive for connecting the connecting conductor 3, which are connected to the solar battery 2, will be described. The conductive adhesive agent can be used as a conductive paste 20 containing solder powder and silver powder in a thermosetting resin composition which is, for example, an adhesive.
作為構成熱硬化性樹脂之硬化成分，可使用藉由與硬化劑進行熱硬化處理而具有接著作用之環氧樹脂、酚樹脂、胺酯樹脂等，其中，為了助熔劑成分之不活性化，較佳為使用環氧樹脂。作為此種環氧樹脂， 可例示雙酚A型環氧樹脂、雙酚F型環氧樹脂、酚醛清漆型環氧樹脂等環氧丙醚型環氧樹脂。此外，可應用脂環式環氧樹脂或含雜環之環氧樹脂等通常已知者。 As the curing component constituting the thermosetting resin, an epoxy resin, a phenol resin, an amine ester resin or the like which is used for thermal curing treatment with a curing agent can be used, and in order to inactivate the flux component, Good use of epoxy resin. As such an epoxy resin, A glycidyl ether type epoxy resin such as a bisphenol A type epoxy resin, a bisphenol F type epoxy resin, or a novolak type epoxy resin can be exemplified. Further, an alicyclic epoxy resin or a heterocyclic-containing epoxy resin or the like is generally known.
再者，於反應速度相對較快之脂環式環氧樹脂之情形時，伴隨其之使用而熱硬化性樹脂之硬化速度加快，故較佳為更迅速地進行藉由已熔融之焊料粉之網狀結構(金屬之連續相)形成。於此情形時，只要使用更低熔點之焊料粉即可。 Further, in the case of an alicyclic epoxy resin having a relatively fast reaction rate, the curing rate of the thermosetting resin is accelerated with the use thereof, so that it is preferably carried out more rapidly by the molten solder powder. A network structure (continuous phase of metal) is formed. In this case, it is only necessary to use a solder powder having a lower melting point.
又，作為硬化劑，使用與硬化成分對應之硬化劑。於硬化成分為環氧樹脂之情形時，於熱硬化時不會產生氣體、與環氧樹脂混合時可實現較長之適用期、且可實現所獲得之硬化物之電性特性、化學特性及機械特性間之良好之平衡之方面而言，較佳為使用酸酐作為硬化劑。 Further, as the curing agent, a curing agent corresponding to the curing component is used. When the hardening component is an epoxy resin, no gas is generated during thermal curing, and a long pot life can be achieved when mixed with the epoxy resin, and the electrical properties and chemical properties of the obtained cured product can be achieved. In terms of a good balance between mechanical properties, it is preferred to use an acid anhydride as a hardener.
又，若使用具有助熔劑活性者作為硬化劑，則於熱硬化時，可使相對於銀粉之已熔融之焊料之潤濕性提高，可由導電性接著劑之熱硬化物中相對少量之已熔融之焊料粉形成經由銀粉連續之網狀結構(金屬之連續相)。因此，可發揮較高之導通可靠性，且可使熱硬化性樹脂之含量相對增大，使太陽電池之電極與連接用導體之接著強度提高。 Further, when a developer having a flux activity is used as a curing agent, the wettability of the molten solder with respect to the silver powder can be improved at the time of thermal curing, and a relatively small amount of molten material can be melted by the thermal curing agent of the conductive adhesive. The solder powder forms a continuous network structure (continuous phase of metal) via silver powder. Therefore, it is possible to exhibit high conduction reliability, and the content of the thermosetting resin can be relatively increased, and the bonding strength between the electrode of the solar cell and the connecting conductor can be improved.
作為使硬化劑表現助熔劑活性之方法，可列舉藉由公知之方法於硬化劑導入羧基、磺醯基、磷酸基等質子酸基。其中，自與環氧樹脂之反應性之方面而言，較佳為應用羧基。 As a method of expressing the activity of the flux by the curing agent, a protonic acid group such as a carboxyl group, a sulfonyl group or a phosphate group may be introduced into the curing agent by a known method. Among them, a carboxyl group is preferably used from the viewpoint of reactivity with an epoxy resin.
因此，作為硬化成分為環氧樹脂之情形時之較佳之硬化劑，可列舉存在游離之羧基之三羧酸之單酸酐，較佳可列舉環己烷-1,2,4-三羧酸-1,2-酸酐。 Therefore, as a curing agent which is preferably a case where the curing component is an epoxy resin, a monocarboxylic acid anhydride of a tricarboxylic acid having a free carboxyl group may be mentioned, and preferably cyclohexane-1,2,4-tricarboxylic acid- 1,2-anhydride.
熱硬化性樹脂中之硬化成分與硬化劑之含有比例根據硬化成分或硬化劑之種類而不同，但於硬化成分為環氧樹脂，且硬化劑為三羧酸之單酸酐之情形時，即便環氧樹脂之含量相對過多或過少均成為硬化不 充分，故以莫耳當量基準之當量比([環氧樹脂]/[硬化劑])計較佳為1：0.5~1：1.5、更佳為1：0.8~1：1.2。 The content ratio of the hardening component to the curing agent in the thermosetting resin varies depending on the type of the curing component or the curing agent. However, when the curing component is an epoxy resin and the curing agent is a monocarboxylic acid monocarboxylic acid anhydride, even the ring is used. If the content of oxygen resin is relatively too much or too little, it will become hardened. Although it is sufficient, the equivalent ratio ([epoxy resin] / [hardener]) based on the molar equivalent is preferably from 1:0.5 to 1:1.5, more preferably from 1:0.8 to 1:1.2.
於熱硬化性樹脂，除上述硬化成分及硬化劑以外，可於不損害發明之效果之範圍內添加調配於公知之熱硬化性接著劑之各種添加劑、例如顏料、紫外線吸收劑、硬化促進劑、矽烷偶合劑。 In the thermosetting resin, in addition to the hardening component and the curing agent, various additives such as a pigment, an ultraviolet absorber, a curing accelerator, and the like, which are blended in a known thermosetting adhesive, may be added to the extent that the effects of the invention are not impaired. Decane coupling agent.
熱硬化性樹脂可藉由將硬化成分或硬化劑、及其他添加劑利用通常方法均勻地混合而進行調整。 The thermosetting resin can be adjusted by uniformly mixing a hardening component, a curing agent, and other additives by a usual method.
於上述熱硬化性樹脂含有焊料粉及銀粉。銀粉之電阻較小但熔點較高，藉由熱硬化性樹脂之通常之熱硬化處理時之加熱不會熔融，故為了僅使用銀粉作為導電性粒子來實現效率較佳之導電性，而必須使未熔融之銀粉彼此接觸。為此，於熱硬化性樹脂調配大量銀粉，但若調配大量銀粉，則熱硬化性樹脂之含量相對減少而可能導致接著力降低。因此，於本發明中，作為調配於熱硬化性樹脂之金屬填料之總量之一部分，使用顯示熱硬化溫度附近之熔融溫度之焊料粉，由已熔融之焊料粉於銀粉間進行網狀結構化(金屬之連續相化)。 The thermosetting resin contains solder powder and silver powder. The silver powder has a small electric resistance but a high melting point, and the heating during the usual heat hardening treatment of the thermosetting resin does not melt. Therefore, in order to achieve high-efficiency conductivity by using only silver powder as the conductive particles, it is necessary to The molten silver powder is in contact with each other. For this reason, a large amount of silver powder is blended in the thermosetting resin, but if a large amount of silver powder is blended, the content of the thermosetting resin is relatively reduced, which may cause a decrease in the adhesion force. Therefore, in the present invention, as one of the total amount of the metal filler blended in the thermosetting resin, the solder powder which exhibits the melting temperature in the vicinity of the thermosetting temperature is used, and the molten solder powder is mesh-structured between the silver powders. (Continuous phase of metal).
作為用於此種目的之焊料粉，具體而言，使用顯示熔融溫度低於熱硬化性樹脂之熱硬化處理溫度，且於熱硬化性樹脂之熱硬化處理條件下與銀粉反應，生成高熔點焊料合金，其顯示高於該焊料粉之熔融溫度之熔點。藉此可使熱硬化性樹脂之硬化物之耐熱性提高。 As the solder powder used for such a purpose, specifically, a hot-melt treatment temperature which exhibits a melting temperature lower than that of the thermosetting resin and a reaction with silver powder under the thermosetting treatment conditions of the thermosetting resin are used to form a high melting point solder. An alloy that exhibits a melting point above the melting temperature of the solder powder. Thereby, the heat resistance of the cured product of the thermosetting resin can be improved.
作為此種焊料粉，可較佳地列舉Sn-Bi系焊料粉、Sn-In系焊料粉、Sn-Zn系焊料粉，其中，自低溫熔融性之觀點而言，可更佳地列舉Sn-Bi系焊料粉、Sn-In系焊料粉。作為Sn-Bi系焊料粉之具體例，可列舉Sn-58Bi共晶系焊料粉(熔點139℃)，作為Sn-In系焊料粉之具體例，可列舉Sn-52In系焊料粉(熔點117℃)，作為Sn-Zn系焊料粉之具體例，可列舉Sn-9Zn系焊料粉(熔點199℃)。 As such a solder powder, Sn-Bi solder powder, Sn-In solder powder, and Sn-Zn solder powder are preferable, and from the viewpoint of low-temperature meltability, Sn- is more preferably listed. Bi-based solder powder and Sn-In solder powder. Specific examples of the Sn-Bi solder powder are Sn-58Bi eutectic solder powder (melting point: 139 ° C). Specific examples of the Sn-In solder powder include Sn-52In solder powder (melting point: 117 ° C) Specific examples of the Sn-Zn-based solder powder include Sn-9Zn-based solder powder (melting point: 199 ° C).
作為銀粉及焊料粉之粒子形狀，可列舉球狀、扁平狀、粒狀、針狀等形狀。 Examples of the particle shape of the silver powder and the solder powder include a spherical shape, a flat shape, a granular shape, and a needle shape.
銀粉與焊料粉之質量比係若前者過多，則有網狀結構(金屬之連續相)變少之傾向，若前者過少，則有高熔點焊料之生成量變少之傾向，故以質量比計較佳為1：2~2：1，更佳為1：1.5~1.5：1。 If the mass ratio of the silver powder to the solder powder is too large, the network structure (continuous phase of the metal) tends to be small. If the former is too small, the amount of the high melting point solder tends to decrease, so that it is preferable to use a mass ratio. It is 1:2~2:1, more preferably 1:1.5~1.5:1.
導電性接著漿料20係藉由將以上說明之金屬填料與熱硬化性樹脂利用通常方法均勻地混合而調整者，亦可視需要添加有機溶劑。此處，金屬填料之熱硬化性樹脂中之含量(由以下式(1)定義之質量基準之金屬填料填充率)若過低，則有難以形成網狀結構(金屬之連續相)之傾向，若過高則有熱硬化性樹脂之接著力降低之傾向，故較佳為75~95%，更佳為80~90%。 The conductive adhesive slurry 20 is adjusted by uniformly mixing the metal filler and the thermosetting resin described above by a usual method, and an organic solvent may be added as needed. When the content of the metal-filled thermosetting resin (the metal filler filling rate based on the mass ratio defined by the following formula (1)) is too low, it tends to be difficult to form a network structure (continuous phase of metal). If it is too high, the adhesive strength of the thermosetting resin tends to decrease, so it is preferably from 75 to 95%, more preferably from 80 to 90%.
金屬填料填充率(%)={金屬填料/(金屬填料+硬化成分+硬化劑)}×100 (1) Metal filler filling rate (%) = {metal filler / (metal filler + hardening component + hardener)} × 100 (1)
[製造步驟] [manufacturing steps]
接著，參照圖4對太陽電池模組1之製造步驟進行說明。本發明之一實施形態之太陽電池模組1之製造方法係配置形成有與形成於太陽電池2之背面2b之電極集電部13、14導通連接之端子17a之絕緣基板16，且於該端子17a上塗佈導電性接著漿料20。繼而，於絕緣基板16上載置密封接著材之片材6a，於其上積層太陽電池2。 Next, a manufacturing procedure of the solar battery module 1 will be described with reference to Fig. 4 . In the method of manufacturing the solar cell module 1 according to the embodiment of the present invention, the insulating substrate 16 having the terminals 17a electrically connected to the electrode collecting portions 13 and 14 formed on the back surface 2b of the solar cell 2 is disposed, and the terminal is formed at the terminal. The conductive paste 20 is applied to 17a. Then, a sheet 6a of a sealing adhesive is placed on the insulating substrate 16, and the solar cell 2 is laminated thereon.
此時，太陽電池2進行形成於背面2b之p型電極集電部13及n型電極集電部14、與連接用導體3之端子17a之位置對準。藉此，連接用導體3係跨及2個太陽電池2間鄰接之p型電極集電部13及n型電極集電部14而配置。 At this time, the solar cell 2 is aligned with the p-type electrode collecting portion 13 and the n-type electrode collecting portion 14 formed on the back surface 2b and the terminal 17a of the connecting conductor 3. Thereby, the connection conductor 3 is disposed across the p-type electrode collecting portion 13 and the n-type electrode collecting portion 14 which are adjacent to each other between the two solar cells 2.
再者，塗佈於p型電極集電部13上之導電性接著漿料20不會觸碰到附近之n型電極12，又，塗佈於n型電極集電部14上之導電性接 著漿料20不會觸碰到附近之p型電極11。同樣地，配置於p型電極集電部13上之連接用導體3之一端子17a不會觸碰到附近之n型電極12，又，配置於n型電極集電部14上之連接用導體3之另一端子17a不會觸碰到附近之p型電極11。 Further, the conductive paste 20 applied to the p-type electrode collecting portion 13 does not touch the n-type electrode 12 in the vicinity, and is electrically connected to the n-type electrode collecting portion 14. The slurry 20 does not touch the nearby p-type electrode 11. Similarly, the terminal 17a of the connection conductor 3 disposed on the p-type electrode collecting portion 13 does not touch the n-type electrode 12 in the vicinity, and the connecting conductor disposed on the n-type electrode collecting portion 14 The other terminal 17a of 3 does not touch the nearby p-type electrode 11.
繼而，於太陽電池2之受光面上載置密封接著材之片材6b，於其上載置表面護罩7。然後，將該積層體自表面護罩7之上面以層疊裝置(減壓貼合機)使其層疊壓接一面藉由加熱器進行加熱。藉此，該積層體中，密封材片材6a、6b流動，太陽電池2之電極集電部13、14與端子17a經由導電性接著漿料20電性、機械地連接，並且藉由密封材片材6a、6b之硬化而被層疊密封。 Then, a sheet 6b of a sealing material is placed on the light receiving surface of the solar cell 2, and a surface shield 7 is placed thereon. Then, the laminated body is heated by a heater by laminating and pressing the upper surface of the surface shield 7 by a laminating apparatus (pressure reducing bonding machine). Thereby, in the laminated body, the sealing material sheets 6a and 6b flow, and the electrode collecting portions 13 and 14 of the solar cell 2 and the terminal 17a are electrically and mechanically connected via the conductive bonding paste 20, and are sealed by the sealing material. The sheets 6a and 6b are hardened and laminated and sealed.
藉由該熱加壓步驟，導電性接著漿料20藉由減壓貼合機以特定之溫度(例如150~180℃)、特定之壓力(例如0.5~2.0MPa)進行特定時間熱加壓。此時，導電性接著漿料20中，在達到熱硬化處理溫度之前焊料粉便熔融，藉此由熱硬化性樹脂中相對少量之已熔融之焊料粉形成經由銀粉連續之網狀結構(金屬之連續相)。又，導電性接著漿料20中，熱硬化性樹脂自連接用導體3與p型電極集電部13及n型電極集電部14之間流出並且夾持銀粉或上述網狀結構(金屬之連續相)，於該狀態下熱硬化性樹脂硬化。藉此，經由導電性接著漿料20，連接用導體3與p型電極集電部13及n型電極集電部14導通連接，相鄰接之太陽電池2串列連接。最後，在周圍安裝鋁等之金屬框架9，從而完成太陽電池模組1。 By the heat pressurization step, the conductive paste 20 is thermally pressurized at a specific temperature (for example, 150 to 180 ° C) and a specific pressure (for example, 0.5 to 2.0 MPa) by a pressure-reducing laminator for a specific period of time. At this time, in the conductive paste 20, the solder powder is melted before reaching the heat curing temperature, whereby a relatively small amount of molten solder powder in the thermosetting resin forms a continuous network structure via silver powder (metal Continuous phase). Further, in the conductive subsequent paste 20, the thermosetting resin flows out from the connection conductor 3, the p-type electrode collecting portion 13 and the n-type electrode collecting portion 14, and sandwiches the silver powder or the above-mentioned mesh structure (metal In the continuous phase, the thermosetting resin is cured in this state. Thereby, the connection conductor 3 is electrically connected to the p-type electrode collecting portion 13 and the n-type electrode collecting portion 14 via the conductive bonding paste 20, and the adjacent solar cells 2 are connected in series. Finally, a metal frame 9 of aluminum or the like is attached around to complete the solar cell module 1.
[效果] [effect]
根據太陽電池模組1之製造方法，於熱硬化性樹脂所含有之焊料粉顯示熔融溫度低於熱硬化性樹脂之熱硬化處理溫度，且於熱硬化性樹脂之熱硬化處理條件下與銀粉反應，生成高熔點焊料合金，其顯示高於該焊料粉之熔融溫度之熔點。藉此，可於熱硬化性樹脂硬化之前，於硬化溫度以下 由熱硬化性樹脂中相對少量之已熔融之焊料粉形成經由銀粉連續之高熔點焊料合金之網狀結構(金屬之連續相)，使連接用導體3之端子17a與太陽電池2之各電極集電部13、14之間導通，其後使熱硬化性樹脂熱硬化。因此，太陽電池模組1可發揮高導通可靠性，並且使熱硬化性樹脂之含量相對增大，使太陽電池之電極與連接用導體之接著強度提高。 According to the manufacturing method of the solar cell module 1, the solder powder contained in the thermosetting resin exhibits a melting temperature lower than the thermosetting treatment temperature of the thermosetting resin, and reacts with the silver powder under the thermosetting treatment conditions of the thermosetting resin. A high melting point solder alloy is formed which exhibits a melting point higher than the melting temperature of the solder powder. Thereby, it can be below the hardening temperature before the thermosetting resin is cured. A network structure (continuous phase of metal) of a high-melting-point solder alloy continuous through a silver powder is formed from a relatively small amount of molten solder powder in the thermosetting resin, and the electrode 17 of the connection conductor 3 and the electrode of the solar cell 2 are set. The electric portions 13 and 14 are electrically connected to each other, and thereafter the thermosetting resin is thermally cured. Therefore, the solar cell module 1 can exhibit high conduction reliability and relatively increase the content of the thermosetting resin, thereby improving the bonding strength between the electrode of the solar cell and the connecting conductor.
又，導電性接著漿料20中由於銀粉具有高之熱導性，故熱硬化性樹脂整體具備較高之熱導性。因此，導電性接著漿料20於熱加壓步驟中具有速硬化性，加熱時間成為短時間而抑制對太陽電池2之熱衝擊，又，可縮短工站時間(tact time)。進而，於使用導電性接著漿料20製造而成之太陽電池模組1中，已熔融之焊料粉於熱硬化處理下與銀粉反應，生成高熔點焊料合金，其顯示高於該焊料粉之熔融溫度之熔點，故導電性接著劑層之耐熱性提昇，可使機械性之連接可靠性提高。 Further, in the conductive paste 20, since the silver powder has high thermal conductivity, the thermosetting resin as a whole has high thermal conductivity. Therefore, the conductive adhesive slurry 20 has rapid hardenability in the hot pressurization step, the heating time is short, and the thermal shock to the solar cell 2 is suppressed, and the tact time can be shortened. Further, in the solar cell module 1 manufactured by using the conductive paste 20, the molten solder powder is reacted with the silver powder under the heat hardening treatment to form a high melting point solder alloy, which is higher than the melting of the solder powder. Since the melting point of the temperature is increased, the heat resistance of the conductive adhesive layer is improved, and the mechanical connection reliability can be improved.
[導電性接著膜] [Electrically conductive film]
再者，導電性接著劑除導電性接著漿料20以外，亦可製成如圖5所示般，藉由使熱硬化性樹脂含有膜形成樹脂而形成為膜狀之導電性接著膜21。膜形成樹脂相當於平均分子量為10000以上之高分子量樹脂，自膜形成性之觀點而言，較佳為10000~80000左右之平均分子量。作為膜形成樹脂，可使用環氧樹脂、改質環氧樹脂、胺酯樹脂、苯氧基樹脂等各種樹脂，其中，自膜形成狀態、連接可靠性等觀點而言，可較佳地使用苯氧基樹脂。 In addition to the conductive paste 20, the conductive adhesive may be formed into a film-shaped conductive adhesive film 21 by including a thermosetting resin containing a film-forming resin as shown in FIG. The film-forming resin corresponds to a high molecular weight resin having an average molecular weight of 10,000 or more, and is preferably an average molecular weight of about 10,000 to 80,000 from the viewpoint of film formability. As the film-forming resin, various resins such as an epoxy resin, a modified epoxy resin, an amine ester resin, and a phenoxy resin can be used. Among them, benzene can be preferably used from the viewpoints of film formation state, connection reliability, and the like. Oxy resin.
導電性接著膜21係藉由如下操作而形成，即，將混合上述金屬填料與熱硬化性樹脂並且適當地添加有機溶劑之樹脂組成物塗佈於基底膜22上，藉由使溶劑揮發而積層熱硬化性樹脂層23。作為基底膜22，無特別限制，可使用PET(Poly Ethylene Terephthalate，聚對苯二甲酸乙二酯)、OPP(Oriented Polypropylene，定向聚丙烯)、PMP(Poly-4-methlpentene-1，聚-4-甲基戊烯-1)、PTFE(Polytetrafluoroethylene，聚四氟乙烯)等。作為溶劑， 可使用甲苯、乙酸乙酯等、或其等之混合溶劑。 The conductive adhesive film 21 is formed by applying a resin composition in which the metal filler and the thermosetting resin are mixed and an organic solvent is appropriately added to the base film 22, and laminating the solvent by volatilizing the solvent. Thermosetting resin layer 23. The base film 22 is not particularly limited, and PET (Poly Ethylene Terephthalate, polyethylene terephthalate), OPP (Oriented Polypropylene), PMP (Poly-4-methlpentene-1, poly-4) can be used. -methylpentene-1), PTFE (polytetrafluoroethylene) or the like. As a solvent, A mixed solvent of toluene, ethyl acetate, or the like, or the like can be used.
又，導電性接著膜21形成為膠帶狀且被捲繞於轉盤24而保管，於實際使用時，自轉盤24拉出，並切割為與形成於連接用導體3之端子17a大致同等之特定長度。其後，導電性接著膜21係將熱硬化性樹脂層23暫貼於端子17a上，於剝離基底膜22後，配置太陽電池2之p型電極集電部13及n型電極集電部14。太陽電池2中，鄰接之p型電極集電部13及n型電極集電部14係跨及形成於連接用導體3之端子17a間而配置，藉此形成複數個太陽電池2藉由連接用導體3連接而成之太陽電池串4。其後，藉由與上述步驟相同之步驟形成太陽電池模組1。 Further, the conductive adhesive film 21 is formed in a tape shape and is wound around the turntable 24 for storage. When actually used, the conductive adhesive film 21 is pulled out from the turntable 24 and cut into a specific length substantially equal to the terminal 17a formed on the connecting conductor 3. . Thereafter, the conductive adhesive film 21 temporarily bonds the thermosetting resin layer 23 to the terminal 17a, and after the base film 22 is peeled off, the p-type electrode collecting portion 13 and the n-type electrode collecting portion 14 of the solar cell 2 are disposed. . In the solar battery 2, the adjacent p-type electrode collecting portion 13 and the n-type electrode collecting portion 14 are disposed across the terminal 17a formed between the connecting conductors 3, thereby forming a plurality of solar cells 2 by connection. A solar cell string 4 in which conductors 3 are connected. Thereafter, the solar cell module 1 is formed by the same steps as those described above.
再者，導電性接著膜22並不限定於形成為長條狀之轉盤形狀，亦可為對應於端子17a之短條形狀。 Further, the conductive adhesive film 22 is not limited to the shape of a turntable formed in a long shape, and may be a short strip shape corresponding to the terminal 17a.
[正背面連接型之情形] [The case of the front side connection type]
又，上述中以所謂之背接觸型之太陽電池模組1為例進行了說明，但本發明亦可適用於如圖6所示般，將於受光面31a設置有由p型電極與n型電極中之一者所構成之正面電極33，於與受光面31a相反側之背面31b設置有由p型電極與n型電極中之另一者所構成之背面電極34之太陽電池31經由成為連接用導體之標記線32複數個連接而成之太陽電池模組1。 Further, although the solar battery module 1 of the back contact type has been described as an example, the present invention can also be applied to a light-receiving surface 31a provided with a p-type electrode and an n-type as shown in FIG. The front surface electrode 33 formed of one of the electrodes is connected to the solar cell 31 provided with the back surface electrode 34 composed of the other of the p-type electrode and the n-type electrode on the back surface 31b opposite to the light-receiving surface 31a. The solar cell module 1 is connected by a plurality of conductor marking lines 32.
標記線32例如係藉由使用厚度為50~300μm之帶狀銅箔，且視需要實施鍍金、鍍銀、鍍錫、鍍焊料等而形成。又，標記線32係經由導電性接著劑將一端側配置於一太陽電池31之正面電極33上，將另一端側配置於與一太陽電池31鄰接之另一太陽電池之背面電極34上。 The marking line 32 is formed, for example, by using a strip-shaped copper foil having a thickness of 50 to 300 μm, and if necessary, performing gold plating, silver plating, tin plating, solder plating, or the like. Further, the marking line 32 is disposed on the front surface 33 of one solar cell 31 via a conductive adhesive, and the other end side is disposed on the back surface electrode 34 of another solar cell adjacent to one solar cell 31.
於此情形時，作為使形成於太陽電池31之正面電極33及背面電極34與標記線32導通連接之導電性接著劑，亦使用上述導電性接著漿料20、或導電性接著膜21。導電性接著漿料20或導電性接著膜21被供給至形成於太陽電池31之受光面31a及背面31b之正面電極33及背面電極34 與標記線32之間，且自標記線32上藉由未圖示之加熱按壓頭以特定溫度、特定壓力進行特定時間加熱按壓而使其熱硬化。 In this case, the conductive adhesive paste 20 or the conductive adhesive film 21 is also used as the conductive adhesive that electrically connects the front surface electrode 33 and the back surface electrode 34 formed on the solar cell 31 to the mark line 32. The conductive paste 20 or the conductive adhesive film 21 is supplied to the front surface electrode 33 and the back surface electrode 34 formed on the light receiving surface 31a and the back surface 31b of the solar cell 31. Between the marking line 32 and the marking line 32, the heating pressing head (not shown) is heated and pressed at a specific temperature and a specific pressure for a specific time to be thermally cured.
於該熱加壓步驟中，導電性接著劑係可於熱硬化性樹脂硬化之前，由熱硬化性樹脂中相對少量之已熔融之焊料粉形成經由銀粉連續之網狀結構(金屬之連續相)，於由標記線32與太陽電池31之正面電極33及背面電極34夾持該網狀結構之後使熱硬化性樹脂熱硬化。因此，太陽電池模組1發揮較高之導通可靠性，並且可使熱硬化性樹脂之含量相對增大，使太陽電池31之電極33、34與成為連接用導體之標記線32之接著強度提高。 In the thermal pressurization step, the conductive adhesive can form a continuous network structure (continuous phase of metal) via silver powder from a relatively small amount of molten solder powder in the thermosetting resin before the thermosetting resin is cured. After the mesh structure is sandwiched between the marking line 32 and the front surface electrode 33 and the back surface electrode 34 of the solar cell 31, the thermosetting resin is thermally cured. Therefore, the solar cell module 1 exhibits high conduction reliability, and the content of the thermosetting resin is relatively increased, so that the bonding strength between the electrodes 33 and 34 of the solar cell 31 and the marking line 32 serving as the connecting conductor is improved. .
再者，於此情形時，導電性接著膜21亦可代替基底膜22，或者於與基底膜22相反側設置標記線32。 Further, in this case, the conductive adhesive film 21 may be provided instead of the base film 22, or the marking line 32 may be provided on the opposite side to the base film 22.
[實施例] [Examples]
接著，對本發明之實施例進行說明。本實施例中，作為實施例及比較例，使用代替於熱硬化性樹脂所含有之金屬填料之複數個導電性接著漿料，形成連接形成於玻璃基板上之Ag電極與形成於軟性基板(FPC)之連接端子之連接構造體樣品，測定Ag電極-連接端子間之導通電阻。 Next, an embodiment of the present invention will be described. In the present embodiment, as an example and a comparative example, a plurality of conductive pastes instead of the metal filler contained in the thermosetting resin were used to form an Ag electrode formed on a glass substrate and formed on a flexible substrate (FPC). The connection structure of the connection terminal of the connection terminal measures the on-resistance between the Ag electrode and the connection terminal.
如圖7所示，於玻璃基板40，遍及整個表面地形成Ag固體電極41，於該Ag電極41上，將實施例及比較例之導電性接著漿料42印刷為厚度200μm、直徑5mm之圓形。於其上，重疊預先將連接部分挖空成直徑10mm之圓形之EVA片材。FPC43係藉由形成與導電性接著劑之形狀為相同形狀之連接端子44，將該連接端子44自EVA片材之開口部對準重疊於相面對之導電性接著漿料42，並以減壓貼合機進行壓接而製作連接構造體樣品。 As shown in FIG. 7, an Ag solid electrode 41 was formed over the entire surface of the glass substrate 40, and the conductive paste 42 of the examples and the comparative examples was printed on the Ag electrode 41 to have a thickness of 200 μm and a diameter of 5 mm. shape. On top of this, the overlapping portion was previously hollowed out into a circular EVA sheet having a diameter of 10 mm. The FPC 43 is formed by forming the connection terminal 44 having the same shape as that of the conductive adhesive, and the connection terminal 44 is overlapped from the opening portion of the EVA sheet to overlap the facing conductive paste 42 and is reduced. The pressure bonding machine was crimped to produce a connection structure sample.
熱壓接之條件為160℃(導電性接著漿料之溫度)、0.1MPa、20分鐘。又，連接構造體樣品之Ag電極-連接端子間之導通電阻係使用數 位萬用表，於連接初期與TCT(Temperature Cycle Test(溫度循環試驗)：-40℃、30min125℃、30min；200個循環)後進行測定。而且，將相對於連接初期之電阻值之電阻值之上升率未達15%之情形設為○，將15%以上且未達30%設為△，將30%以上之情形設為×。 The conditions of the thermocompression bonding were 160 ° C (conductivity followed by the temperature of the slurry), 0.1 MPa, and 20 minutes. Further, the on-resistance between the Ag electrode and the connection terminal of the connection structure sample was performed using a digital multimeter, and the TCT (Temperature Cycle Test): -40 ° C, 30 min at the initial stage of connection. The measurement was carried out after 125 ° C, 30 min; 200 cycles). In addition, the case where the rate of increase of the resistance value with respect to the resistance value at the initial stage of connection is less than 15% is ○, and 15% or more and less than 30% are set to Δ, and 30% or more is set to ×.
構成導電性接著漿料之熱硬化性樹脂係藉由混合雙酚F型環氧樹脂(三菱化學股份有限公司製造：JER806)100質量份作為硬化成分、及環己烷-1,2,4-三羧酸-1,2-酸酐(三菱氣體化學股份有限公司製造：H-TMAn/H-TMAn-S)80質量份作為硬化劑而獲得。 The thermosetting resin constituting the conductive paste is 100 parts by mass of a bisphenol F type epoxy resin (manufactured by Mitsubishi Chemical Corporation: JER806) as a hardening component, and cyclohexane-1,2,4- 80 parts by mass of tricarboxylic acid-1,2-anhydride (manufactured by Mitsubishi Gas Chemical Co., Ltd.: H-TMAn/H-TMAn-S) was obtained as a curing agent.
於實施例1中，相對於上述熱硬化性樹脂100質量份，混合平均粒徑20μm之Sn-58Bi焊料粉(三井金屬礦業股份有限公司製造：Sn-Bi焊料粉)470質量份、及銀粉(福田金屬箔粉工業股份有限公司製造：AgC-224)230質量份(Sn-Bi：銀粉≒2：1)作為金屬填料。 In Example 1, 470 parts by mass of Sn-58Bi solder powder (manufactured by Mitsui Mining Co., Ltd.: Sn-Bi solder powder) having an average particle diameter of 20 μm and silver powder were mixed with respect to 100 parts by mass of the above thermosetting resin. Futian Metal Foil Powder Industry Co., Ltd. manufactured: AgC-224) 230 parts by mass (Sn-Bi: silver powder ≒ 2:1) as a metal filler.
於實施例2中，相對於上述熱硬化性樹脂100質量份，混合平均粒徑20μm之Sn-58Bi焊料粉(三井金屬礦業股份有限公司製造：Sn-Bi焊料粉)420質量份、及銀粉(福田金屬箔粉工業股份有限公司製造：AgC-224)280質量份(Sn-Bi：銀粉=1.5：1)作為金屬填料。 In Example 2, 420 parts by mass of Sn-58Bi solder powder (manufactured by Mitsui Mining & Mining Co., Ltd.: Sn-Bi solder powder) having an average particle diameter of 20 μm and silver powder were mixed with respect to 100 parts by mass of the above thermosetting resin. Manufactured by Fukuda Metal Foil Powder Co., Ltd.: AgC-224) 280 parts by mass (Sn-Bi: silver powder = 1.5:1) as a metal filler.
於實施例3中，相對於上述熱硬化性樹脂100質量份，混合平均粒徑20μm之Sn-58Bi焊料粉(三井金屬礦業股份有限公司製造：Sn-Bi焊料粉)350質量份、及銀粉(福田金屬箔粉工業股份有限公司製造：AgC-224)350質量份(Sn-Bi：銀粉=1：1)作為金屬填料。 In Example 3, 350 parts by mass of Sn-58Bi solder powder (manufactured by Mitsui Mining Co., Ltd.: Sn-Bi solder powder) having an average particle diameter of 20 μm and silver powder were mixed with respect to 100 parts by mass of the above thermosetting resin. Fukuda Metal Foil Powder Industry Co., Ltd. manufactured: AgC-224) 350 parts by mass (Sn-Bi: silver powder = 1:1) as a metal filler.
於實施例4中，相對於上述熱硬化性樹脂100質量份，混合平均粒徑20μm之Sn-58Bi焊料粉(三井金屬礦業股份有限公司製造：Sn-Bi焊料粉)450質量份、及銀粉(福田金屬箔粉工業股份有限公司製造：AgC-224)450質量份(Sn-Bi：銀粉=1：1)作為金屬填料。 In Example 4, 450 parts by mass of Sn-58Bi solder powder (manufactured by Mitsui Mining Co., Ltd.: Sn-Bi solder powder) having an average particle diameter of 20 μm and silver powder were mixed with respect to 100 parts by mass of the above thermosetting resin. Futian Metal Foil Powder Industry Co., Ltd. manufactured: AgC-224) 450 parts by mass (Sn-Bi: silver powder = 1:1) as a metal filler.
於實施例5中，相對於上述熱硬化性樹脂100質量份，混合 平均粒徑20μm之Sn-58Bi焊料粉(三井金屬礦業股份有限公司製造：Sn-Bi焊料粉)280質量份、及銀粉(福田金屬箔粉工業股份有限公司製造：AgC-224)420質量份(Sn-Bi：銀粉=1：1.5)作為金屬填料。 In Example 5, it was mixed with respect to 100 parts by mass of the above thermosetting resin. 280 parts by mass of Sn-58Bi solder powder (manufactured by Mitsui Mining Co., Ltd.: Sn-Bi solder powder) having an average particle diameter of 20 μm, and 420 parts by mass of silver powder (manufactured by Fukuda Metal Foil Powder Co., Ltd.: AgC-224) Sn-Bi: silver powder = 1:1.5) as a metal filler.
於實施例6中，相對於上述熱硬化性樹脂100質量份，混合平均粒徑20μm之Sn-58Bi焊料粉(三井金屬礦業股份有限公司製造：Sn-Bi焊料粉)230質量份、及銀粉(福田金屬箔粉工業股份有限公司製造：AgC-224)470質量份(Sn-Bi：銀粉≒1：2)作為金屬填料。 In Example 6, 230 parts by mass of Sn-58Bi solder powder (manufactured by Mitsui Mining Co., Ltd.: Sn-Bi solder powder) having an average particle diameter of 20 μm and silver powder were mixed with respect to 100 parts by mass of the above thermosetting resin. Manufactured by Fukuda Metal Foil Powder Co., Ltd.: AgC-224) 470 parts by mass (Sn-Bi: silver powder ≒ 1:2) as a metal filler.
於比較例1中，相對於上述熱硬化性樹脂100質量份，混合銀粉(福田金屬箔粉工業股份有限公司製造：AgC-224)700質量份(Sn-Bi：銀粉=0：1)作為金屬填料。 In Comparative Example 1, 700 parts by mass (Sn-Bi: Silver powder = 0: 1) of a silver powder (manufactured by Fukuda Metal Foil Powder Co., Ltd.: AgC-224) was mixed as a metal with respect to 100 parts by mass of the above thermosetting resin. filler.
於比較例2中，相對於上述熱硬化性樹脂100質量份，混合平均粒徑20μm之Sn-58Bi焊料粉(三井金屬礦業股份有限公司製造：Sn-Bi焊料粉)700質量份(Sn-Bi：銀粉=1：0)作為金屬填料。 In Comparative Example 2, 700 parts by mass of Sn-58Bi solder powder (manufactured by Mitsui Mining Co., Ltd.: Sn-Bi solder powder) having an average particle diameter of 20 μm was mixed with respect to 100 parts by mass of the above thermosetting resin (Sn-Bi). : Silver powder = 1:0) as a metal filler.
如表1所示，於在熱硬化性樹脂含有焊料粉與銀粉作為金屬填料之實施例1~6中，TCT後之電阻值之上升率未達30%。其原因在於，在熱硬化性樹脂硬化之前，由熱硬化性樹脂中已熔融之焊料粉形成經由銀粉而連續之網狀結構(金屬之連續相)，使玻璃基板40之Ag固體電極41與FPC43之連接端子44之間導通，於該狀態使熱硬化性樹脂熱硬化。藉此，可知於實施例1~6中，玻璃基板40之Ag固體電極41與FPC43之連接端 子44牢固地連接，於TCT後亦發揮良好之導通性。 As shown in Table 1, in Examples 1 to 6 in which the thermosetting resin contained solder powder and silver powder as a metal filler, the rate of increase in resistance after TCT was less than 30%. This is because the molten metal powder in the thermosetting resin is formed into a continuous network structure (continuous phase of metal) via the silver powder before the thermosetting resin is cured, so that the Ag solid electrode 41 of the glass substrate 40 and the FPC 43 are formed. The connection terminals 44 are electrically connected to each other, and in this state, the thermosetting resin is thermally cured. Thereby, it is understood that the connection ends of the Ag solid electrode 41 of the glass substrate 40 and the FPC 43 in the first to sixth embodiments. The sub-44 is firmly connected and also exhibits good continuity after TCT.
另一方面，於僅含有焊料粉或銀粉之一者作為金屬填料之比較例1及比較例2中，初期導通電阻較高，於TCT後，玻璃基板40之Ag固體電極41與FPC43之連接端子44之間成為開路而無法測定電阻值。 On the other hand, in Comparative Example 1 and Comparative Example 2 in which only one of the solder powder or the silver powder was used as the metal filler, the initial on-resistance was high, and after the TCT, the connection terminals of the Ag solid electrode 41 and the FPC 43 of the glass substrate 40 were used. The gap between 44 becomes an open circuit and the resistance value cannot be measured.
若將實施例1與其他實施例進行對比，則於實施例1中，Ag粉相對較少，故高熔點焊料合金之生成量為相對少量，於TCT後電阻值稍微上升。藉此，可知銀粉與焊料粉之質量比為1：2~2：1，更佳為1：1.5~1.5：1。 Comparing Example 1 with other examples, in Example 1, since the Ag powder was relatively small, the amount of formation of the high-melting-point solder alloy was relatively small, and the resistance value slightly increased after TCT. Therefore, it can be seen that the mass ratio of the silver powder to the solder powder is 1:2 to 2:1, more preferably 1:1.5 to 1.5:1.
1‧‧‧太陽電池模組 1‧‧‧Solar battery module
2‧‧‧太陽電池 2‧‧‧Solar battery
2b‧‧‧背面 2b‧‧‧back
3‧‧‧連接用導體 3‧‧‧Connecting conductor
6‧‧‧片材 6‧‧‧Sheet
7‧‧‧表面護罩 7‧‧‧Surface shield
13‧‧‧p型電極集電部 13‧‧‧p type electrode collector
14‧‧‧n型電極集電部 14‧‧‧n type electrode collector
16‧‧‧絕緣基板 16‧‧‧Insert substrate
17‧‧‧配線 17‧‧‧Wiring
17a‧‧‧端子 17a‧‧‧ Terminal
18‧‧‧絕緣層 18‧‧‧Insulation
20‧‧‧導電性接著漿料 20‧‧‧ Conductivity followed by slurry
Claims (7)
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| JP2012134307A JP6080247B2 (en) | 2012-06-13 | 2012-06-13 | Method for manufacturing solar cell module, conductive adhesive for solar cell, solar cell module |
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| TW201413993A TW201413993A (en) | 2014-04-01 |
| TWI568005B true TWI568005B (en) | 2017-01-21 |
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| CN109659402A (en) * | 2019-01-24 | 2019-04-19 | 常州时创能源科技有限公司 | The series winding technique of solar battery sheet |
| JP2023000704A (en) | 2021-06-18 | 2023-01-04 | パナソニックＩｐマネジメント株式会社 | Conductive paste and conductive film formed using the same |
Citations (4)
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|---|---|---|---|---|
| US5428249A (en) * | 1992-07-15 | 1995-06-27 | Canon Kabushiki Kaisha | Photovoltaic device with improved collector electrode |
| CN101630704A (en) * | 2008-07-18 | 2010-01-20 | 三星电子株式会社 | Solar cell and manufacturing method thereof |
| JP2011066071A (en) * | 2009-09-15 | 2011-03-31 | Sharp Corp | Solar cell module and manufacturing method thereof |
| TW201213494A (en) * | 2010-09-20 | 2012-04-01 | Henkel Ag & Amp Co Kgaa | Electrically conductive adhesives |
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| JP2716641B2 (en) * | 1992-12-28 | 1998-02-18 | キヤノン株式会社 | Current collecting electrode of photovoltaic element and method of manufacturing the same |
| JP2000309773A (en) * | 1998-11-30 | 2000-11-07 | Nippon Handa Kk | Conductive adhesive and bonding method using same |
| JP2003347564A (en) * | 2002-05-28 | 2003-12-05 | Kyocera Corp | Photoelectric converter |
| JP2007103473A (en) * | 2005-09-30 | 2007-04-19 | Sanyo Electric Co Ltd | Solar cell device and solar cell module |
| MY157233A (en) * | 2009-03-11 | 2016-05-13 | Shinetsu Chemical Co | Connection sheet for solar battery cell electrode, process for manufacturing solar cell module, and solar cell module |
| KR101143295B1 (en) * | 2009-05-26 | 2012-05-08 | 주식회사 엘지화학 | Method for Preparation of Front Electrode for Solar Cell of High Efficiency |
| CN102509747A (en) * | 2011-11-08 | 2012-06-20 | 江西赛维Ldk太阳能高科技有限公司 | Connecting method for solar cells and bus-bar with conductive adhesives |
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Patent Citations (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US5428249A (en) * | 1992-07-15 | 1995-06-27 | Canon Kabushiki Kaisha | Photovoltaic device with improved collector electrode |
| CN101630704A (en) * | 2008-07-18 | 2010-01-20 | 三星电子株式会社 | Solar cell and manufacturing method thereof |
| JP2011066071A (en) * | 2009-09-15 | 2011-03-31 | Sharp Corp | Solar cell module and manufacturing method thereof |
| TW201213494A (en) * | 2010-09-20 | 2012-04-01 | Henkel Ag & Amp Co Kgaa | Electrically conductive adhesives |
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| CN104350610A (en) | 2015-02-11 |
| TW201413993A (en) | 2014-04-01 |
| WO2013187329A1 (en) | 2013-12-19 |
| CN104350610B (en) | 2017-02-22 |
| KR20150030700A (en) | 2015-03-20 |
| JP6080247B2 (en) | 2017-02-15 |
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