US2009239122A1PendingUtilityA1

Glass and glass-ceramic sealant compositions

50
Assignee: BROW RICHARD KPriority: Oct 15, 2004Filed: Jun 4, 2008Published: Sep 24, 2009
Est. expiryOct 15, 2024(expired)· nominal 20-yr term from priority
Inventors:Richard K. BrowSigno Tadeu Dos ReisGlendon M. Benson
C04B 37/005C03C 3/062H01M 8/2425C03C 8/24C03C 10/0054C04B 2237/10Y10T29/4911C04B 37/025C03C 3/066H01M 2008/1293C04B 2237/348C03C 3/068C04B 2237/405C03C 10/0036C03C 10/0009H01M 8/0271H01M 8/0282Y02E60/50
50
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Claims

Abstract

A glass ceramic material sealed fuel cell device, including a first fuel cell portion and a sealant layer bonded to the first cell portion. The sealant layer includes at least three metal oxides RO-M 2 O 3 —SiO 2 combined together. R is selected from the group consisting of zinc, strontium, calcium, magnesium and combinations thereof. M is selected from the group consisting of aluminum, boron, lanthanum, iron and combinations thereof. RO is present in an amount of between about 45 mol % and about 55 mol %. M 2 O 3 is present in an amount of between about 5 mol % and about 10 mol %. SiO 2 is present in an amount of about 40 mol %. RO includes RnO present in an amount of at least about 5 mol %.

Claims

exact text as granted — not AI-modified
1 . A glass ceramic material sealed device, comprising in combination:
 a first substrate; and   a sealant layer bonded to the first substrate;   wherein the sealant layer includes at least three metal oxides RO-M 2 O 3 —SiO 2  combined together;   wherein R is selected from the group consisting of zinc, strontium, calcium, magnesium and combinations thereof;   wherein M is selected from the group consisting of aluminum, boron, lanthanum, iron and combinations thereof;   wherein the RO is present in an amount of between about 45 mol % and about 55 mol %;   wherein the M 2 O 3  is present in an amount of between about 5 mol % and about 10 mol %;   wherein said SiO 2  is present in an amount of about 40 mol %; and   wherein the RO includes ZnO present in an amount of at least about 5 mol %.   
     
     
         2 . The device of  claim 1  wherein the M 2 O 3  includes Al 2 O 3  present in an amount of between about 2 mol % and about 5 mol %. 
     
     
         3 . The device of  claim 1  wherein the sealant layer includes at least 25 mol % ZnO. 
     
     
         4 . The device of  claim 1  wherein the sealant layer includes at least 20 mol % MgO. 
     
     
         5 . The device of  claim 1  wherein the first substrate is a substantially yttria-stabilized zirconia electrolyte. 
     
     
         6 . The device of  claim 1  wherein the first substrate is a solid oxide fuel cell component. 
     
     
         7 . The device of  claim 1  wherein the first substrate and the sealant layer have substantially similar coefficients of thermal expansion. 
     
     
         8 . The device of  claim 1  wherein the sealant layer is substantially amorphous. 
     
     
         9 . The device of  claim 1  wherein the sealant layer is substantially crystalline. 
     
     
         10 . The device of  claim 1  further comprising a second substrate bonded to the sealant layer. 
     
     
         11 . A glass ceramic material sealed device, comprising in combination:
 a substrate; and   a sealant layer bonded to the substrate;   wherein the sealant layer has a composition of X[(RO).(M 2 O 3 ).(SiO 2 )]Y(QO 2 );   wherein 0.95≦X≦1.0;   wherein 0≦Y≦0.05;   wherein Q is selected from the group consisting of titanium, zirconium and combinations thereof;   wherein R is selected from the group consisting of strontium, calcium, magnesium, zinc and combinations thereof;   wherein M is selected from the group consisting of aluminum, boron, lanthanum, iron and combinations thereof;   wherein the RO is present in an amount of about 50 mol %;   wherein the M 2 O 3  is present in an amount of about 5 mol %;   wherein said SiO 2  is present in an amount of about 45 mol %; and   wherein R contains at least about 5 mol % zinc.   
     
     
         12 . The device of  claim 11  wherein Al 2 O 3  is present in amounts less than about 3 mol %. 
     
     
         13 - 18 . (canceled) 
     
     
         19 . A method of joining at least two solid ceramic parts, comprising the steps of:
 (a) providing a blend of RO, M 2 O 3 , and SiO 2  that substantially matches a coefficient of thermal expansion of the at least two solid ceramic parts, wherein R is selected from the group consisting of strontium, calcium, magnesium and zinc and combinations thereof, and M is selected from the group consisting of aluminum, boron, lanthanum, iron and combinations thereof;   (b) placing the blend at an interface of said at least two ceramic parts as a pre-assembly;   (c) heating the pre-assembly to a temperature sufficient to cause the blend to flow into said interface as an assembly; and   (d) cooling the assembly and solidifying said blend thereby joining the at least two ceramic parts;   wherein ZnO is present in an amount of at least about 5 mol %;   wherein the RO is present in an amount from about 40 mol % to about 60 mol %;   wherein the M 2 O 3  is present in an amount from about 2 mol % to about 10 mol %; and   wherein the SiO 2  is present in an amount from about 35 mol % to about 45 mol %.   
     
     
         20 . The method of  claim 19  wherein the joining is sealing. 
     
     
         21 . The method of  claim 19  wherein the coefficient of thermal expansion is from about 80(10 −7 ) per degree Celsius to about 120(10 −7  per degree Celsius as measured from 25 degrees Celsius to 700 degrees Celsius. 
     
     
         22 . The method of  claim 19 , further comprising at least one additional metal oxide. 
     
     
         23 . The method of  claim 22  wherein the at least one additional metal oxide is selected from the group consisting of TiO 2 , ZrO 2  and combinations thereof. 
     
     
         24 . The method of  claim 19 , wherein the at least two ceramic parts are parts of a solid oxide fuel cell. 
     
     
         25 . The method of  claim 19 , wherein one of the respective at least two ceramic parts is a yttria-stabilized zirconia electrolyte. 
     
     
         26 . The method of  claim 19  further comprising the step of:
 (e) at least partially crystallizing the interfacial layer.   
     
     
         27 . The method of  claim 26  wherein during step (e) at least one alkaline earth-zinc pyrosilicate crystalline phase forms 
     
     
         28 . A method of joining a ceramic piece to a second piece, comprising the steps of:
 (a) providing a glass powder having a composition of RO, M 2 O 3 , and SiO 2  that substantially matches a coefficient of thermal expansion of the at least two solid ceramic parts, wherein R is selected from the group consisting of strontium, calcium, magnesium and zinc and combinations thereof, and M is selected from the group consisting of aluminum, boron, lanthanum, iron and combinations thereof; wherein the RO is present in an amount from about 40 mol % to about 60 mol %; wherein ZnO is present in an amount of at least about 5 mol %; wherein the M 2 O 3  is present in an amount from about 2 mol % to about 10 mol %; and wherein the SiO 2  is present in an amount from about 35 mol % to about 45 mol %;   (b) placing the glass powder at an interface of the ceramic piece and the second piece as a pre-assembly;   (c) heating the pre-assembly to a temperature sufficient to cause the glass powder to soften and flow into said interface to form an interfacial layer; and   (d) cooling and solidifying the interfacial layer thereby joining the ceramic piece and the second piece.   
     
     
         29 . The method of  claim 28  further comprising the step of:
 (e) at least partially crystallizing the interfacial layer.   
     
     
         30 . The method of  claim 28 , further comprising at least one additional metal oxide. 
     
     
         31 . The method of  claim 30  wherein said at least one additional metal oxide is selected from the group consisting of TiO 2 , ZrO 2  and combinations thereof. 
     
     
         32 . The method of  claim 30 , wherein one of the respective ceramic and second pieces is part of a solid oxide fuel cell. 
     
     
         33 . A glass composition, comprising:
 about 45 mol % to about 55 mol % RO;   about 5 mol % to about 10 mol % M 2 O 3 ; and   about 40 mol % to about 45 mol % SiO 2 ;   
       wherein R is selected from the group consisting of strontium, calcium, magnesium and zinc and combinations thereof,
 wherein M is selected from the group consisting of aluminum, boron, lanthanum, iron and combinations thereof; and 
 wherein ZnO is present in an amount of at least about 5 mol %. 
 
     
     
         34 . The composition of  claim 33  further comprising:
 about 25 mol % SrO;   about 25 mol % ZnO   about 10 mol % Al 2 O 3 ; and   about 40 mol % SiO 2 .   
     
     
         35 . The composition of  claim 33  further comprising:
 about 27.5 mol % SrO;   about 27.5 mol % ZnO   about 5 mol % Al 2 O 3 ; and   about 40 mol % SiO 2 .   
     
     
         36 . The composition of  claim 33  further comprising:
 about 25 mol % SrO;   about 25 mol % ZnO   about 5 mol % Al 2 O 3 ;   about 5 mol % Fe 2 O 3 ; and   about 40 mol % SiO 2 .   
     
     
         37 . The composition of  claim 33  further comprising:
 about 26 mol % SrO;   about 26 mol % ZnO   about 2 mol % Al 2 O 3 ;   about 2 mol % B 2 O 3 ; and   about 44 mol % SiO 2 .   
     
     
         38 . The composition of  claim 33  further comprising:
 about 26 mol % SrO;   about 13 mol % CaO;   about 13 mol % ZnO;   about 2 mol % Al 2 O 3 ;   about 2 mol % B 2 O 3 ;   about 42 mol % SiO 2 ; and   about 2 mol % TiO 2      
     
     
         39 . The composition of  claim 33  further comprising:
 about 18.5 mol % SrO;   about 19.2 mol % CaO;   about 13.2 mol % ZnO;   about 1.9 mol % B 2 O 3 ;   about 2.9 mol % La 2 O 3 ;   about 42.2 mol % SiO 2 ; and   about 2 mol % TiO 2      
     
     
         40 . A glass ceramic material sealed fuel cell device, comprising in combination:
 a first fuel cell portion; and   a sealant layer bonded to the first cell portion;   wherein the sealant layer includes at least three metal oxides RO-M 2 O 3 —SiO 2  combined together;   wherein R is selected from the group consisting of zinc, strontium, calcium, magnesium and combinations thereof;   wherein M is selected from the group consisting of aluminum, boron, lanthanum, iron and combinations thereof;   wherein the RO is present in an amount of between about 45 mol % and about 55 mol %;   wherein the M 2 O 3  is present in an amount of between about 5 mol % and about 10 mol %;   wherein said SiO 2  is present in an amount of about 40 mol %; and   wherein the RO includes RnO present in an amount of at least about 5 mol %.   
     
     
         41 . The device of  claim 33  wherein the M 2 O 3  includes Al 2 O 3  present in an amount of between about 2 mol % and about 5 mol %. 
     
     
         42 . The device of  claim 33  wherein the sealant layer includes at least 25 mol % ZnO. 
     
     
         43 . The device of  claim 33  wherein the sealant layer includes at least 20 mol % MgO. 
     
     
         44 . The device of  claim 33  wherein the first fuel cell portion is a substantially yttria-stabilized zirconia electrolyte. 
     
     
         45 . The device of  claim 33  wherein the first fuel cell portion is a solid oxide fuel cell component. 
     
     
         46 . The device of  claim 33  wherein the first fuel cell portion and the sealant layer have substantially similar coefficients of thermal expansion. 
     
     
         47 . The device of  claim 33  wherein the sealant layer is substantially amorphous. 
     
     
         48 . The device of  claim 33  wherein the sealant layer is substantially crystalline. 
     
     
         49 . The device of  claim 1  further comprising a second substrate bonded to the sealant layer. 
     
     
         50 . A glass ceramic material sealed fuel cell device, comprising in combination:
 a solid oxide fuel cell component; and   a sealant layer bonded to the substrate;   wherein the sealant layer has a composition of X[(RO).(M 2 O 3 ).(SiO 2 )]Y(QO 2 );   wherein 0.95≦X≦1.0;   wherein 0≦Y≦0.05;   wherein Q is selected from the group consisting of titanium, zirconium and combinations thereof;   wherein R is selected from the group consisting of strontium, calcium, magnesium, zinc and combinations thereof;   wherein M is selected from the group consisting of aluminum, boron, lanthanum, iron and combinations thereof;   wherein the RO is present in an amount of about 50 mol %;   wherein the M 2 O 3  is present in an amount of about 5 mol %;   wherein said SiO 2  is present in an amount of about 45 mol %; and wherein R contains at least about 5 mol % zinc.   
     
     
         51 . The device of  claim 42  wherein Al 2 O 3  is present in amounts less than about 3 mol %. 
     
     
         52 . The device of  claim 42  wherein the solid oxide fuel cell component is an yttria stabilized zirconia electrolyte substrate. 
     
     
         53 . A solid oxide fuel cell comprising:
 a first ceramic oxide electrolyte layer;   a second ceramic oxide electrolyte layer; and   a joint layer bonded disposed between and bonded to the first and second ceramic oxide electrolyte layers;   wherein the joint layer has a composition of X[(RO).(M 2 O 3 ).(SiO 2 )]Y(QO 2 );   wherein 0.95≦X≦1.0;   wherein 0≦Y≦0.05;   wherein Q is selected from the group consisting of titanium, zirconium and combinations thereof;   wherein R is selected from the group consisting of strontium, calcium, magnesium, zinc and combinations thereof;   wherein M is selected from the group consisting of aluminum, boron, lanthanum, iron and combinations thereof;   wherein the RO is present in an amount of about 50 mol %;   wherein the M 2 O 3  is present in an amount of about 5 mol %;   wherein the SiO 2  is present in an amount of about 45 mol %; and wherein R contains at least about 5 mol % zinc.   
     
     
         54 . The device of  claim 46  wherein the first and second ceramic oxide electrolyte layers and the joint layer have substantially similar coefficients of thermal expansion. 
     
     
         55 . The device of  claim 46  wherein the joint layer is substantially amorphous. 
     
     
         56 . The device of  claim 46  wherein the joint layer is substantially crystalline. 
     
     
         57 . A solid oxide fuel cell system, comprising:
 a first ceramic oxide electrolyte layer;   a second ceramic oxide electrolyte layer; and   a joint layer bonded disposed between and bonded to the first and second ceramic oxide electrolyte layers;   wherein the joint layer includes at least three metal oxides RO-M 2 O 3 —SiO 2  combined together;   wherein R is selected from the group consisting of zinc, strontium, calcium, magnesium and combinations thereof;   wherein M is selected from the group consisting of aluminum, boron, lanthanum, iron and combinations thereof;   wherein the RO is present in an amount of between about 45 mol % and about 55 mol %;   wherein the M 2 O 3  is present in an amount of between about 5 mol % and about 10 mol %;   wherein said SiO 2  is present in an amount of about 40 mol %; and   wherein the RO includes ZnO present in an amount of at least 5 mol %.   
     
     
         58 . The device of  claim 50  wherein the first and second ceramic oxide electrolyte layer and the joint layer have substantially similar coefficients of thermal expansion. 
     
     
         59 . The device of  claim 50  wherein the joint layer is substantially amorphous. 
     
     
         60 . The device of  claim 50  wherein the joint layer is substantially crystalline. 
     
     
         61 . A fuel cell device having a joint disposed between at least two solid oxide fuel cell parts comprising:
 a first solid oxide fuel cell electrolyte layer;   a second solid oxide fuel cell electrolyte layer; and   a joint layer bonded between the first and second solid oxide fuel cell electrolyte layers and further comprising:   at least three metal oxides RO, M 2 O 3 , and SiO 2  combined together;   wherein R is selected from the group consisting of strontium, calcium, magnesium and zinc and combinations thereof;   wherein M is selected from the group consisting of aluminum, boron, lanthanum, iron and combinations thereof;   wherein the joint substantially matches a coefficient of thermal expansion of at least two solid ceramic parts;   wherein the RO is present in an amount from about 40 mol % to about 60 mol %;   wherein the M 2 O 3  is present in an amount from about 2 mol % to about 10 mol %;   wherein said SiO 2  is present in an amount from about 35 mol % to about 45 mol %; and   wherein ZnO is present in an amount of at least about 5 mol %.   
     
     
         62 . The device of  claim 54  wherein the first and second ceramic oxide electrolyte layer and the joint layer have substantially similar coefficients of thermal expansion. 
     
     
         63 . The device of  claim 54  wherein the joint layer is substantially amorphous. 
     
     
         64 . The device of  claim 54  wherein the joint layer is substantially crystalline.

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