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A Conductive Paste Containing Lead-Free Glass Frit

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A Conductive Paste Containing Lead-Free Glass Frit (19) TZZ¥Z¥ _T (11) EP 3 032 546 A1 (12) EUROPEAN PATENT APPLICATION (43) Date of publication: (51) Int Cl.: 15.06.2016 Bulletin 2016/24 H01B 1/22 (2006.01) H01L 31/0224 (2006.01) (21) Application number: 15192068.3 (22) Date of filing: 29.10.2015 (84) Designated Contracting States: (72) Inventors: AL AT BE BG CH CY CZ DE DK EE ES FI FR GB • YEH, Chih-Hsien GR HR HU IE IS IT LI LT LU LV MC MK MT NL NO Hsinchu (TW) PL PT RO RS SE SI SK SM TR • SHIH, Po-Yang Designated Extension States: Hsinchu (TW) BA ME • HSIN, Pi-Yu Designated Validation States: Hsinchu (TW) MA (74) Representative: Viering, Jentschura & Partner (30) Priority: 08.12.2014 TW 103142666 mbB Patent- und Rechtsanwälte (71) Applicant: Giga Solar Materials Corp. Kennedydamm 55 / Roßstrasse Hsinchu (TW) 40476 Düsseldorf (DE) (54) A CONDUCTIVE PASTE CONTAINING LEAD-FREE GLASS FRIT (57) The present invention discloses a conductive rium-bismuth-lithium-oxide. The conductive paste of the paste comprising a conductive metal or a derivative present invention can be used in the preparation of an thereof, and a lead-free glass frit dispersed in an organic electrode of a solar cell with excellent energy conversion vehicle, wherein said lead-free glass frit comprises tellu- efficiency. EP 3 032 546 A1 Printed by Jouve, 75001 PARIS (FR) EP 3 032 546 A1 Description BACKGROUND OF THE INVENTION 5 Field of the Invention [0001] The present invention relates to a conductive paste comprising a conductive metal, a lead-free glass frit and an organic vehicle, and articles having said conductive paste applied thereto. 10 Description of related art [0002] Conventional solar cells or photovoltaic cells comprise a semiconductor substrate, a diffusion layer, an antire- flective coating, a back electrode and a front electrode. The antireflective coating is used to promote the light absorption, thereby increasing the cell’s efficiency; and typically comprises silicon (e.g., silicon nitride or silicon dioxide). However, 15 said anti-reflective coatings would increase electrical resistance between the semiconductor substrate and the front electrode, and result in insulation, which impair the flow of excited state electrons. [0003] In view of the above, when forming the front electrode, generally a conductive paste prepared by mixing a conductive metal or the derivative thereof (such as silver particles), glass (such as lead oxide-containing glass) and an organic vehicle, etc. is employed because the glass has low melting point, low melt viscosity and stability against 20 uncontrollable de-vitrification. The conductive paste can be printed as grid lines or other patterns on the semiconductor substrate by screen printing, stencil printing or the like, followed by fire-through. During firing, the conductive paste penetrates through the antireflective coating and forms electrical contact between the semiconductor substrate and the grid line or other patterns through metal contact. The front electrode is thus produced. [0004] To achieve proper fire-through, glasses having good solubility for the antireflective coating are preferably used 25 as the glass frit in conductive pastes. In conventional conductive pastes for forming front electrodes, glass frits often comprise lead oxide-containing glass because the glass eases the adjustment of softening point and provides relatively good adhesiveness for substrates, allows for relatively good fire-through and results in superior solar cell characteristics. [0005] However, increased environmental awareness in recent years has led to a desire for a switchover to lead-free materials for automotive, electronics and solar cell industries, etc. On the other hand, after firing, the ability to penetrate 30 the antireflective coating and form a good bond to the substrate as well as the excellent conversion efficiency of solar cells should take the factors including the composition of the conductive paste and the quality of the electrical contact made between the fired-through conductive paste and the semiconductor substrate into consideration. [0006] Accordingly, there is a need to provide a conductive paste comprising lead-free glass frit which can be fired at a lower temperature and has the properties of the abovementioned conventional lead-containing materials. 35 BRIEF SUMMARY OF THE INVENTION [0007] Present invention is to provide a conductive paste containing lead-free glass frit capable of being fired at a lower temperature and to provide a lead-free article comprising said conductive paste and having good substrate adhe- 40 siveness and excellent conversion efficiency after fire-through, thereby achieving the object of providing environmentally friendly materials for conductive pastes. [0008] To achieve the above object, one aspect of the present invention is to provide a conductive paste comprising: (a) about 85% to about 99.5% by weight of a conductive metal or the derivatives thereof, based on the weight of solids; 45 (b) about 0.5% to about 15% by weight of a lead-free glass frit containing tellurium-bismuth-lithium-oxide, based on the weight of solids; and (c) an organic vehicle; wherein the weight of solids is the total weight of the conductive metal (a) and the lead-free glass frit (b). 50 DETAILED DESCRIPTION OF THE INVENTION [0009] In one preferred embodiment of the present invention, the conductive metal of the derivatives thereof includes silver powder. [0010] In one preferred embodiment of the present invention, tellurium oxide, bismuth oxide, and lithium oxide are 55 present in an amount of about 60 wt.% to about 90 wt.%, about 0.1 wt.% to about 20 wt.% and about 0.1 wt.% to about 20 wt.% in the lead-free glass frit, respectively. [0011] In one embodiment of the present invention, the organic vehicle is a solution comprising a polymer and a solvent. [0012] In a further preferred embodiment of the present invention, the lead-free glass frit comprises one or more 2 EP 3 032 546 A1 elements selected from the group consisting of phosphorus (P), barium (Ba), sodium (Na), magnesium (Mg), zinc (Zn), calcium (Ca), strontium (Sr), tungsten (W), aluminum (Al), potassium (K), zirconium (Zr), vanadium (V), selenium (Se), iron (Fe), indium (In), manganese (Mn), tin (Sn), nickel (Ni), antimony (Sb), silver (Ag), silicon (Si), erbium (Er), germanium (Ge), titanium (Ti), gallium (Ga), cerium (Ce), niobium (Nb), samarium (Sm) and lanthanum (La) or the oxide thereof in 5 an amount of about 0.1 % to about 10 % by weight of the lead-free glass frit. In another embodiment of the present invention, the organic vehicle comprises one or more functional additives, such as viscosity modifiers, dispersing agents, thixotropic agents, wetting agents, etc. [0013] Another aspect of the present invention is to provide an article comprising a semiconductor substrate and an abovementioned conductive paste applied on the semiconductor substrate. In one embodiment of the present invention, 10 the article is a semiconductor device. In another embodiment of the present invention, the semiconductor device is a solar cell. [0014] The foregoing has outlined the technical features and the technical effects of the present invention. It should be appreciated by a person of ordinary skill in the art that the specific embodiments disclosed may be easily combined, modified, replaced and/or conversed for other articles, processes or usages within the spirit of the present invention. 15 Such equivalent scope does not depart from the protection scope of the present invention as set forth in the appended claims. [0015] Without intending to limit the present invention, illustrative embodiments are described below to allow for full understanding of the present invention. The present invention may also be put into practiced by embodiments in other forms. 20 [0016] The conductive paste of the present invention comprising a lead-free glass frit can be applied in various indus- tries, preferably in a semiconductor industry, more preferably in a solar cell industry. The abovementioned conductive paste comprises: (a) a conductive metal or the derivative thereof, (b) a lead-free glass frit containing tellurium-bismuth- lithium-oxide and (c) an organic vehicle; wherein the inorganic components including the conductive metal (a) and the lead-free glass frit (b) are uniformly dispersed in the organic vehicle (c). 25 [0017] In the present invention, the organic vehicle is not a part of solid components. Hence, the weight of solids refers to the total weight of the solid components including the conductive metal (a) and the lead-free glass frit (b), etc. [0018] The conductive metal of the present invention is not subject to any special limitation as long as it does not have an adverse effect on the technical effect of the present invention. The conductive metal can be one single element selected from the group consisting of silver, aluminum and copper; and also can be alloys or mixtures of metals, such 30 as gold, platinum, palladium, nickel and the like. From the viewpoint of conductivity, pure silver is preferable. [0019] In the case of using silver as the conductive metal, it can be in the form of silver metal, silver derivatives and/or the mixture thereof. Examples of silver derivatives include silver oxide (Ag 2O), silver salts (such as silver chloride (AgCl), silver nitrate (AgNO3), silver acetate (AgOOCCH3), silver trifluoroacetate (AgOOCCF3) or silver phosphate (Ag3PO4), silver-coated composites having a silver layer coated on the surface or silver-based alloys or the like. 35 [0020] The conductive metal can be in the form of powder (for example, spherical shape, flakes, irregular form and/or the mixture thereof) or colloidal suspension or the like. The average particle size of the conductive metal is not subject to any particular limitation, while 0.1 to 10 microns is preferable. Mixtures of conductive metals having different average particle sizes, particle size distributions or shapes, etc.
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