Patent Application: US-94533586-A

Abstract:
a temperature compensating capacitor of monolithic or multilayered configuration comprising a dielectric ceramic body and at least two electrodes buried therein . the ceramic body is composed of a major ingredient expressed by the formula , o } k o 2 , where m is at least either of magnesium and zinc , and where x , y , k and z are numerals in the ranges of zero to 0 . 995 inclusive , 0 . 005 to 0 . 100 inclusive , 1 . 00 to 1 . 04 inclusive , and 0 . 005 to 0 . 100 inclusive , respectively . to this major ingredient is added a minor proportion of a mixture of boric oxide , silicon dioxide , and one or more metal oxides selected from among barium oxide , magnesium oxide , zinc oxide , strontium oxide and calcium oxide . for the fabrication of capacitors the mixture of the above major ingredient and additives in finely divided form are formed into moldings of desired shape and size , each with at least two electrodes buried therein . the moldings and electrodes are cosintered in a reductive or neutral atmosphere and then are reheated at a lower temperature in an oxidative atmosphere . the cosintering temperature can be so low that nickel or like base metal can be employed as the electrode material .

Description:
we have illustrated in fig1 one of many monolithic ceramic capacitors of identical construction fabricated in the subsequent examples of our invention by way of a preferable embodiment thereof . generally designated 10 , the representative capacitor is shown to have an interlamination of three dielectric ceramic layers 12 and two film electrodes 14 . the three ceramic layers 12 constitute in combination a solid dielectric body 15 having the low temperature sintered ceramic compositions in accordance with our invention . the two film electrodes 14 , which can be of a low cost base metal such as , typically , nickel , extend from the opposite sides of the dielectric body 15 toward , and terminate short of , the other sides of the dielectric body and so have an overlapping , parallel spaced relation to each other . a pair of conductive terminations 16 contact the respective film electrodes 14 . each termination 16 is shown to comprise a baked on zinc layer 18 , a plated on copper layer 20 , and a plated on solder layer 22 . typically , and as fabricated in the subsequent examples of our invention , the intermediate one of the three dielectric layers 12 has a thickness of 0 . 02 millimeter . the area of that part of each film electrode 14 which overlaps the other film electrode is 25 square millimeters ( 5 × 5 millimeters ). we fabricated 88 different sets of test capacitors , each constructed as in fig1 some having their dielectric bodies formulated in accordance with the ceramic compositions of our invention and others not , and measured their electrical properties . table 1 lists the compositions of the dielectric bodies of all the test capacitors fabricated . we have defined the major ingredient of the ceramic compositions in accordance with our invention as {( sr 1 - x - y ca x m y ) o } k ( ti 1 - z zr z ) o 2 . accordingly , in table 1 , we have given various combinations of the atomic numbers k , x , y and z in the formula to indicate the specific major ingredients employed in the various tests . since m can be either or both of mg and zn , we have given the relative proportions of the two metals wherever both of them are employed . the ceramic compositions of our invention further include mixtures , in various proportions , of additives b 2 o 3 , sio 2 and a metal oxide or oxides ( mo ). table 1 specifies the amounts , in parts by weight , of the additive mixtures with respect to 100 parts by weight of the major ingredient , as well as the relative proportions , in mole percent , of the additives b 2 o 3 , sio 2 and mo . further , since mo can be any one or more of bao , mgo , zno , sro and cao , table 1 gives the relative proportions , in mole percent , of these metal oxides , wherever one or more of them are employed . table 1__________________________________________________________________________ceramic compositions additivesmajor ingredient ( 100 wt . parts ) composition motest - y amount ( mole %) ( mole %) no . - k - x mg zn total - z ( wt . part ) b . sub . 2 o . sub . 3 sio . sub . 2 mo bao mgo zno sro cao__________________________________________________________________________ 1 1 . 0 0 . 37 0 . 01 0 . 01 0 . 02 0 . 03 2 . 0 15 25 60 20 20 20 20 20 2 &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; 30 -- 70 &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; 3 &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; 90 -- 10 &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; 4 &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; 90 10 -- &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; 5 &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; 25 75 -- &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; 6 &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; 15 &# 34 ; 10 &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; 7 &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; 20 65 15 &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; 8 &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; 10 &# 34 ; 25 &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; 9 &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; 50 40 &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; 10 &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; 5 40 55 &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; 11 &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; 10 25 65 &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; 12 &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; 15 10 75 &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; 13 &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; 95 -- 5 &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; 14 &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; 45 25 30 100 -- -- -- -- 15 &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; -- 100 -- -- -- 16 &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; -- -- 100 -- -- 17 &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; -- -- -- 100 -- 18 &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; -- -- -- -- 10019 &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; 20 20 20 20 2020 &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; 35 50 15 -- 30 30 20 2021 &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; 25 35 40 30 -- 30 20 2022 &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; 35 15 50 20 30 -- 30 &# 34 ; 23 &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; 60 10 30 &# 34 ; 20 30 -- 3024 &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; 50 30 20 &# 34 ; &# 34 ; &# 34 ; 30 -- 25 &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; 75 15 10 10 10 40 20 2026 &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; 60 40 -- -- -- -- -- -- 27 &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; 55 -- 45 10 40 10 20 2028 1 . 02 0 &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; 35 40 25 20 20 20 &# 34 ; &# 34 ; 29 &# 34 ; 0 . 2 &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; 30 &# 34 ; 0 . 38 &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; 31 &# 34 ; 0 . 55 &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; 32 &# 34 ; 0 . 8 &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; 33 &# 34 ; 0 . 98 &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; 34 1 . 01 0 0 . 005 0 0 . 005 0 . 05 &# 34 ; 30 60 10 &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; 35 &# 34 ; &# 34 ; 0 . 01 &# 34 ; 0 . 01 &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; 36 &# 34 ; &# 34 ; 0 . 03 &# 34 ; 0 . 03 &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; 37 &# 34 ; &# 34 ; 0 . 05 &# 34 ; 0 . 05 &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; 38 &# 34 ; &# 34 ; 0 . 10 &# 34 ; 0 . 10 &# 34 ; &# 34 ; 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; 0 . 98 0 . 02 &# 34 ; 0 . 02 &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; 48 &# 34 ; 0 . 97 0 . 03 &# 34 ; 0 . 03 &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; 49 &# 34 ; 0 . 95 0 . 05 &# 34 ; 0 . 05 &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; 50 &# 34 ; 0 . 90 0 . 10 &# 34 ; 0 . 10 &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; 51 &# 34 ; 0 . 88 0 . 12 &# 34 ; 0 . 12 &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; 52 &# 34 ; 0 . 37 0 &# 34 ; 0 &# 34 ; &# 34 ; 65 20 15 &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; 53 &# 34 ; &# 34 ; 0 . 005 0 . 005 0 . 01 &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; 54 &# 34 ; &# 34 ; 0 . 01 0 . 01 0 . 02 &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; 55 &# 34 ; &# 34 ; &# 34 ; 0 . 02 0 . 03 &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; 56 &# 34 ; &# 34 ; 0 . 02 0 . 03 0 . 05 &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; 57 &# 34 ; &# 34 ; 0 . 05 &# 34 ; 0 . 10 &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; 58 &# 34 ; &# 34 ; 0 . 06 0 . 06 0 . 12 &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; 59 1 . 0 &# 34 ; 0 . 01 0 . 01 0 . 02 0 &# 34 ; 75 0 25 &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; 60 &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; 0 . 002 &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; 61 &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; 0 . 005 &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; 62 &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; 0 . 01 &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; 63 &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; 0 . 05 &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; 64 &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; 0 . 10 &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; 65 &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; 0 . 12 &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; 66 1 . 01 &# 34 ; &# 34 ; 0 0 . 01 0 . 05 0 55 20 &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; 67 &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; 0 . 2 &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; 68 &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; 1 &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; 69 &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; 3 &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; 70 &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; 5 &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; 71 &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; 10 &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; 72 &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; 12 &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; 73 0 . 99 0 &# 34 ; 0 . 01 0 . 02 0 . 03 2 . 0 30 10 60 &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; 74 1 . 0 &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; 75 1 . 005 &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; 76 1 . 01 &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; 77 1 . 02 &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; 78 1 . 03 &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; 79 1 . 04 &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; 80 1 . 05 &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; 81 0 . 99 0 . 37 &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; 35 25 40 &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; 82 1 . 0 &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; 83 1 . 005 &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; 84 1 . 01 &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; 85 1 . 02 &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; 86 1 . 03 &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; 87 1 . 04 &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; 88 1 . 05 &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; &# 34 ; __________________________________________________________________________ according to table 1 , the major ingredient of the dielectric bodies of the capacitors of test no . 1 was {( sr 0 . 61 ca 0 . 37 mg 0 . 01 zn 0 . 01 ) o } 1 . 0 ( ti 0 . 97 zr 0 . 03 ) o 2 . one hundred parts of the this major ingredient was admixed with 2 . 0 parts by weight of a mixture of 15 mole percent b 2 o 3 , 25 mole percent sio 2 and 60 mole percent mo . mo was a mixture of 20 mole percent bao , 20 mole percent mgo , 20 mole percent zno , 20 mole percent sro and 20 mole percent cao . for the fabrication of the capacitors of test no . 1 we started with the preparation of the major ingredient of their dielectric bodies . we prepared the following start materials : these start materials had all purities of not less than 99 . 0 percent . the above specified weights of the start materials do not include those of the impurities contained . we charged the start materials into a pot mill together with alumina balls and 2 . 5 liters of water and mixed them together for 15 hours . then the mixture was introduced into a stainless steel vat and therein dried by air heated to 150 ° c . for four hours . then the dried mixture was crushed into relatively coarse particles , which were subsequently fired in air within a tunnel furnace at 1200 ° c . for two hours . there was thus obtained the major ingredient of the above specified composition in finely divided form . b 2 o 3 : 11 . 18 grams ( 15 mole percent ) to these substances we added 300 cubic centimeters of alcohol , and the resulting slurry was stirred for 10 hours in a polyethylene pot with alumina balls . then the mixture was air fired at 1000 ° c . for two hours . then , charged into an alumina pot together with 300 cubic centimeters of water , the fired mixture was pulverized with alumina balls over a period of 15 hours . then the pulverized mixture was dried at 150 ° c . for four hours . there was thus obtained in finely divided form the desired additive mixture of 15 mole percent b 2 o 3 , 25 mole percent sio 2 and 60 mole percent mo , with the mo consisting of 12 mole percent bao , 12 mole percent mgo , 12 mole percent zno , 12 mole percent sro , and 12 mole percent cao . twenty grams ( two weight percent ) of this additive mixture was added to 1000 grams of the above prepared major ingredient . further , to this mixture , we added 15 percent by weight of an organic binder and 50 percent by weight of water with respect to the total weight of the major ingredient and additives . the organic binder was an aqueous solution of acrylic ester polymer , glycerine , and condensed phosphate . the mixture of all these was ball milled into a slurry . then this slurry was defoamed in vacuum . then the defoamed slurry was charged into a reverse roll coater thereby to be shaped into a thin , continuous strip on an elongate supporting strip of polyester film . then the strip was dried by heating to 100 ° c . on the supporting film . the green ceramic strip thus obtained , approximately 25 microns thick , was subsequently punched into &# 34 ; squares &# 34 ; sized 10 by 10 centimeters . these green ceramic squares are to become the ceramic layers 12 , fig1 in the completed test capacitors 10 . for the fabrication of the base metal film electrodes 14 on the ceramic layers 12 , we prepared 10 grams of nickel in finely divided form , with an average particle size of 1 . 5 microns , and a solution of 0 . 9 gram of ethyl cellulose in 9 . 1 grams of butyl &# 34 ; carbitol &# 34 ; ( trademark for diethylene glycol monobutyl ether ). both were intimately interminged by being agitated for 10 hours , thereby providing an electroconductive paste . then this paste was &# 34 ; printed &# 34 ; on one surface of each green ceramic square , which had been prepared as above described , through a screen having 50 perforations of rectangular shape , each sized seven by 14 millimeters . after drying the printed paste , two green squares were stacked , with their printings directed upwardly , and with the printings on the two squares offset from each other to an extent approximately half the pitch of their patterns in the longitudinal direction . the thus stacked two printed squares were placed between two separate stacks of four unprinted squres each with a thickness of 60 microns . the resulting stack of printed and unprinted squares were pressed in their thickness direction under a pressure of approximately 40 tons at 50 ° c ., thereby firmly bonding the stacked squares to one another . then the bonded squares were cut in a latticed pattern into 50 laminate chips of identical construction . we employed a furnace capable of atmosphere control for cofiring the above prepared green dielectric bodies and , buried therein , the conductive layers which were to become the film electrodes 14 in the completed capacitors 10 . the chips were first air heated in this furnace to 600 ° c . at a rate of 100 ° c . per hour , thereby driving off the organic binder that had been used for providing the slurry of the powdered major ingredient and additives . then the furnace atmosphere was changed from air to a reductive ( nonoxidative ) atmosphere consisting of two percent by volume of molecular hydrogen and 98 percent by volume of molecular nitrogen . in this reductive atmosphere the furnace temperature was raised from 600 ° c . to 1130 ° c . at a rate of 100 ° c . per hour . the maximum temperature of 1130 ° c ., at which the ceramic bodies formulated in accordance with our invention were to be sintered to maturity , was maintained for three hours . then the furnace temperature was lowered to 600 ° c . at a rate of 100 ° c . per hour . then , with the furnace atmosphere again changed to air ( oxidative atmosphere ), the temperature of 600 ° c . was maintained for 30 minutes for the oxidizing heat treatment of the sintered chips . then the furnace temperature was allowed to drop to room temperature . there were thus obtained the dielectric ceramic bodies 15 , fig1 cosintered with the film electrodes 14 buried therein . we proceeded to the production of the pair of conductive terminations 16 on both sides of each ceramic body 15 through which are exposed the film electrodes 14 . first , for the production of the inmost zinc layers 18 , a conductive paste composed of zinc , glass frit and vehicle was coated on both sides of each ceramic body 15 . the coatings on drying were air heated to 550 ° c . and maintained at that temperature for 15 minutes , thereby completing the zinc layers 18 each in direct contact with one of the two firm electrodes 14 . then the intermediate copper layers 20 were formed over the zinc layers 18 by electroless plating . then the outermost solder layers 22 were formed by electroplating a lead tin alloy over the copper layers 20 . we have thus completed the fabrication of monolithic , multilayered ceramic test capacitors , each constructed as in fig1 in accordance with the ceramic composition of test no . 1 of table 1 . the composition of the ceramic bodies 15 of the thus completed capacitors proved substantially akin to that before sintering . it is therefore reasoned that the sintered ceramic bodies 15 are of perovskite structures , with the additives ( 15 mole percent b 2 o 3 , 25 mole percent sio 2 , 12 mole percent bao , 12 mole percent mgo , 12 mole percent zno , 12 mole percent sro , and 12 mole percent cao ) uniformly dispersed among the crystal grains of the major ingredient . as for the other ceramic compositions of table 1 , designated tests nos . 2 through 88 , we made similar test capacitors through exactly the same procedure as that set forth in the foregoing in connection the test no . 1 composition , except for the temperature of sintering in the reductive atmosphere , which will be referred to presently . all the capacitors of test nos . 1 through 88 were then tested as to their specific dielectric constants , temperature coefficients , q factors , and resistivities . the following are the methods we employed for the measurement of these properties : the capacitance of each test capacitor was first measured at a temperature of 20 ° c ., a frequency of one megahertz , and an effective alternating current voltage of 0 . 5 volt . then the specific dielectric constant was computed from the measured value of capacitance , the area ( 25 square millimeters ) of each of the overlapping parts of the two film electrodes 14 , and the thickness ( 0 . 05 millimeter ) of that ceramic layer 12 which intervenes between the film electrodes . the capacitance c 85 at 85 ° c . and capacitance c 20 at 20 ° c . of each test capacitor were first measured . then the temperature coefficient tc of capacitance was computed by the equation ## equ1 ## the q factor was measured by a q meter at a frequency of one megahertz , a temperature of 20 ° c ., and an effective alternating current voltage of 0 . 5 volt . resistance between the pair of conductive terminations 16 of each test capacitor was measured after the application of a direct current voltage of 50 volts for one minute at a temperature of 20 ° c . then the resistivity was computed from the measured resistance value and the size of the test capacitors . table 2 gives the results of the measurements by the above described methods , as well as the maximum temperatures at which the test capacitors were sintered in the reductive atmosphere during their manufacture . it will be noted from this table that the specific dielectric constants of the test no . 1 capacitors , for instance , averaged 250 , their temperature coefficients of capacitances - 970 ppm per degree c ., their q factors 11 , 000 , and their resistivities 2 . 0 × 10 megohm - centimeters . the temperature coefficients of the capacitances of the test capacitors were practically constant in the normal range of their operating temperatures , making the capacitors well suited for use as temperature compensating capacitors . table 2______________________________________firing temperature & amp ; capacitor characteristics electrical properties temperaturefiring specific coefficient oftest temp . dielectric capacitance q resistivityno . (° c .) constant ( ppm /° c .) factor ( megohm - cm ) ______________________________________ 1 1130 250 - 970 11000 2 . 0 × 10 . sup . 7 2 &# 34 ; 253 - 985 10800 1 . 8 × 10 . sup . 7 3 &# 34 ; 248 - 980 10500 1 . 7 × 10 . sup . 7 4 &# 34 ; 245 - 970 10400 1 . 8 × 10 . sup . 7 5 &# 34 ; 243 - 965 10500 2 . 0 × 10 . sup . 7 6 1300 not coherently bonded on firing . 7 &# 34 ; &# 34 ; 8 &# 34 ; &# 34 ; 9 &# 34 ; &# 34 ; 10 &# 34 ; &# 34 ; 11 &# 34 ; &# 34 ; 12 &# 34 ; &# 34 ; 13 &# 34 ; &# 34 ; 14 1130 254 - 985 11000 2 . 3 × 10 . sup . 715 1120 253 - 980 11200 2 . 2 × 10 . sup . 716 &# 34 ; 246 - 967 10700 1 . 9 × 10 . sup . 717 1130 251 - 970 11000 2 . 0 × 10 . sup . 718 1120 248 - 968 10800 2 . 1 × 10 . sup . 719 1130 250 - 970 11000 2 . 0 × 10 . sup . 720 &# 34 ; 247 - 968 10900 1 . 9 × 10 . sup . 721 &# 34 ; 251 - 971 11000 1 . 9 × 10 . sup . 722 &# 34 ; 253 - 977 11200 2 . 1 × 10 . sup . 723 &# 34 ; 250 - 972 11000 1 . 8 × 10 . sup . 724 &# 34 ; 251 - 965 11100 1 . 9 × 10 . sup . 725 &# 34 ; 247 - 962 10900 1 . 7 × 10 . sup . 726 &# 34 ; 250 - 970 11000 1 . 8 × 10 . sup . 727 &# 34 ; 251 - 973 11100 2 . 2 × 10 . sup . 728 1120 306 - 3130 11500 5 . 4 × 10 . sup . 729 &# 34 ; 300 - 2360 11100 4 . 1 × 10 . sup . 730 1130 240 - 976 10300 2 . 2 × 10 . sup . 731 &# 34 ; 223 - 1310 9100 3 . 7 × 10 . sup . 732 1120 174 - 1665 8200 7 . 6 × 10 . sup . 733 &# 34 ; 146 - 1837 7000 1 . 4 × 10 . sup . 834 1140 322 - 3400 11600 5 . 0 × 10 . sup . 735 1130 333 - 3415 11700 8 . 0 × 10 . sup . 736 1120 342 - 3512 12100 8 . 4 × 10 . sup . 737 1110 397 - 3560 12300 8 . 0 × 10 . sup . 738 1130 336 - 3690 11700 4 . 0 × 10 . sup . 739 1270 not coherently bonded on firing . 40 1130 250 - 910 10400 1 . 8 × 10 . sup . 741 1120 254 - 895 10900 2 . 3 × 10 . sup . 742 &# 34 ; 259 - 846 11500 2 . 8 × 10 . sup . 743 1110 318 - 739 10800 3 . 2 × 10 . sup . 744 1130 296 - 693 8600 1 . 8 × 10 . sup . 745 1280 not coherently bonded on firing . 46 1120 162 - 1992 8100 1 . 4 × 10 . sup . 847 &# 34 ; 168 - 2073 8150 1 . 5 × 10 . sup . 848 1110 169 - 2180 8200 &# 34 ; 49 1100 207 - 2230 8700 1 . 3 × 10 . sup . 850 1120 174 - 2490 8100 8 . 0 × 10 . sup . 751 1260 not coherently bonded on firing . 52 1160 248 - 976 9800 9 . 0 × 10 . sup . 653 1150 255 - 993 10400 2 . 0 × 10 . sup . 754 1140 262 - 1090 10600 2 . 5 × 10 . sup . 755 1130 269 - 1200 10900 3 . 6 × 10 . sup . 756 1120 326 - 1190 &# 34 ; 4 . 0 × 10 . sup . 757 1140 288 - 1160 9200 2 . 4 × 10 . sup . 758 1300 not coherently bonded on firing . 59 1160 210 - 900 5900 9 . 5 × 10 . sup . 660 &# 34 ; 212 - 900 6100 9 . 7 × 10 . sup . 661 1150 220 - 910 7200 1 . 2 × 10 . sup . 762 1140 223 - 910 7500 1 . 3 × 10 . sup . 763 1120 261 - 1100 10500 2 . 5 × 10 . sup . 764 1140 247 - 1130 9700 6 . 0 × 10 . sup . 765 1280 not coherently bonded on firing . 66 1250 &# 34 ; 67 1180 268 - 1120 9900 2 . 1 × 10 . sup . 768 1170 267 - 1100 10000 &# 34 ; 69 1130 264 - 1080 9800 &# 34 ; 70 1100 258 - 1070 8000 2 . 0 × 10 . sup . 771 1080 251 - 1050 4800 1 . 7 × 10 . sup . 772 1060 249 - 1045 1070 1 . 6 × 10 . sup . 773 1140 340 - 1600 1300 1 . 6 × 10 . sup . 374 &# 34 ; 310 - 3200 11300 5 . 2 × 10 . sup . 775 1130 &# 34 ; - 3170 11400 5 . 3 × 10 . sup . 776 &# 34 ; 312 - 3180 11500 5 . 5 × 10 . sup . 777 1120 313 - 3190 11400 5 . 7 × 10 . sup . 778 &# 34 ; 315 - 3210 &# 34 ; 6 . 0 × 10 . sup . 779 1130 318 - 3220 11200 6 . 5 × 10 . sup . 780 1280 not coherently bonded on firing . 81 1140 252 - 600 1010 2 . 0 × 10 . sup . 382 1150 237 - 950 10000 2 . 2 × 10 . sup . 783 1140 239 - 950 &# 34 ; 2 . 3 × 10 . sup . 784 1130 240 - 933 10100 2 . 5 × 10 . sup . 785 &# 34 ; 239 - 937 10000 3 . 0 × 10 . sup . 786 &# 34 ; 240 - 951 9900 &# 34 ; 87 1140 237 - 955 9800 2 . 9 × 10 . sup . 788 1300 not coherently bonded on firing . ______________________________________ it will be observed from table 2 that the dielectric bodies of tests nos . 6 - 13 , 39 , 45 , 51 , 58 , 65 , 66 , 80 , and 88 were not coherently bonded on firing at temperatures as high as 1250 ° to 1300 ° c . in the reductive atmosphere . the corresponding ceramic compositions of table 1 fall outside the scope of our invention . the dielectric bodies of all the other tests could be sintered to maturity at temperatures less than 1200 ° c . before proceeding further with the examination of the results of table 2 we will determine the acceptable criteria of the four electrical properties in question for the temperature compensating ceramic capacitors provided by our invention . these criteria are : temperature coefficient of capacitance : from - 3690 to - 693 ppm per degree c . a reconsideration of table 1 in light of the 25 above established criteria of favorable electrical characteristics will reveal that the capacitors of tests nos . 52 , 59 , 60 , 72 , 73 and 81 do not meet these criteria . accordingly , the corresponding ceramic compositions of table 1 also fall outside the scope of our invention . all the test capacitors but those of tests nos . 6 - 13 , 39 , 45 , 51 , 52 , 58 - 60 , 65 , 66 , 72 , 73 , 80 , 81 and 88 satisfy the criteria , so that their ceramic compositions are in accord with our invention . now , let us study the ceramic compositions of table 1 and the corresponding capacitor characteristics , as well as the sintering temperatures , of table 2 in more detail . the ceramic compositions of test no . 66 contained no additive specified by our invention . the dielectric bodies formulated accordingly were not coherently bonded on firing at a temperature as high as 1250 ° c . consider the ceramic compositions of test no . 67 for comparison . they contained 0 . 2 part by weight of the additives with respect to 100 parts by weight of the major ingredient . even though the firing temperature was as low as 1180 ° c ., the resulting test capacitors possess the desired electrical characteristics . we set , therefore , the lower limit of the possible proportions of the additive mixture at 0 . 2 part by weight with respect to 100 parts by weight of the major ingredient . the test no . 72 ceramic composition contained as much as 12 parts by weight of the additives with respect to 100 parts by weight of the major ingredient . the resulting capacitors have an average q factor of 1070 , far less than the above established criterion of 4800 . when the proportion of the additive mixture was reduced to 10 parts by weight , as in test no . 71 , the resulting capacitors have all the desired characteristics . therefore , the upper limit of the possible proportions of the additive mixture is set at 10 parts by weight with respect to 100 parts by weight of the major ingredient . as for the major ingredient , the value of x was variously determined from zero to 0 . 995 in tests nos . 28 - 33 and 46 . the characteristics of the resulting capacitors all came up to the above criteria . the value of x can thus be anywhere between these limits . the value of y was set at zero in test no . 52 , and the characteristics of the resulting capacitors were unsatisfactory . when the value of y was increased to 0 . 005 as in tests nos . 34 and 40 , the resulting capacitors had all the desired characteristics . we set , therefore , the lowermost value of y at 0 . 005 . the value of y was made as high as 0 . 12 in tests nos . 39 , 45 , 51 and 58 . the resulting dielectric bodies were not coherently bonded on firing at temperatures of 1260 ° c . and more . the capacitors of the desired characteristics could be obtained when the value of y was decreased to 0 . 10 as in tests nos . 38 , 44 , 50 and 57 . the upper limit of the possible values of y is therefore 0 . 10 . the value of k in the formula of the major ingredient was set at 0 . 99 in tests nos . 73 and 81 . the resistivities of the resulting capacitors averaged 1 . 6 × 10 3 and 2 . 0 × 10 3 , both much lower than the desired lower limit of 1 . 0 × 10 7 . the above criteria were all satisfied when the value of k was increased to 1 . 00 as in tests nos . 74 and 82 . the lowermost possible value of k is therefore 1 . 00 . on the other hand , when the value of k was made as much as 1 . 05 as in tests nos . 80 and 88 , the resulting dielectric bodies were not coherently bonded on firing at as high temperatures as 1280 ° and 1300 ° c . the desired electrical characteristics were obtained when the value of k was reduced to 1 . 04 as in tests nos . 79 and 87 . accordingly , the greatest possible value of k is 1 . 04 . the value of z in the formula of the major ingredient was set at 0 . 002 in test no . 60 . the characteristics of the resulting capacitors reflect no advantage accruing from the use of zro 2 in the major ingredient . when the value of z was increased to 0 . 005 as in test no . 61 , all the desired characteristics could be obtained . the lowermost possible value of z is therefore 0 . 005 . on the other hand , when the value of z was made as much as 0 . 12 as in test no . 65 , the resulting dielectric bodies were not coherently bonded on firing at as high a temperature as 1280 . the desired characteristics were all realized when the value of z was reduced to 0 . 100 as in test no . 64 . the greatest possible value of z is therefore 0 . 100 . we have ascertained from the results of table 2 that the acceptable range of the relative proportions of b 2 o 3 , sio 2 and mo , the additives of the ceramic compositions in accordance with our invention , can be definitely stated in reference to the ternary diagram of fig2 . the point a in the ternary diagram indicates the test no . 1 additive composition of 15 mole percent b 2 o 3 , 25 mole percent sio 2 and 60 mole percent mo . the point b indicates the test no . 2 additive composition of 30 mole percent b 2 o 3 , zero mole percent sio 2 and 70 mole percent mo . the point c indicates the test no . 3 additive composition of 90 mole percent b 2 o 3 , zero mole percent sio 2 and 10 mole percent mo . the point d indicates the test no . 4 additive composition of 90 mole percent b 2 o 3 , 10 mole percent sio 2 and zero mole percent mo . the point e indicates the test no . 5 additive composition of 25 mole percent b 2 o 3 , 75 mole percent sio 2 and zero mole percent mo . the relative proportions of the additives b 2 o 3 , sio 2 and mo of the ceramic compositions in accordance with our invention are within the region bounded by the lines sequentially connecting the above stated points a , b , c , d and e in the ternary diagram of fig2 . tables 1 and 2 prove that the additive compositions within the above defined region makes possible the provision of capacitors of the desired electrical characteristics . the additive compositions of tests nos . 6 - 13 all fall outside that region , and the corresponding dielectric bodies were not coherently bonded on firing at a temperature of 1300 ° c . the above specified acceptable range of the relative proportions of the additives holds true regardless of whether only one of bao , mgo , zno , sro and cao is employed as mo , as in tests nos . 14 - 18 , or two or more or all of them are employed in suitable relative proportions as in other tests . although we have disclosed our invention in terms of specific examples thereof , we understand that our invention is not to be limited by the exact details of such disclosure but admits of a variety of modifications or alterations within the usual knowledge of the ceramists , chemists or electricians without departing from the scope of the invention . the following , then , is a brief list of such possible modifications or alterations : 1 . the low temperature sinterable ceramic compositions of our invention may include various additives not disclosed herein . an example is a mineralizer such as manganese dioxide . used in a proportion ( preferably from 0 . 05 to 0 . 10 percent by weight ) not adversely affecting the desired characteristics of the resulting capacitors , such a mineralizer will lead to the improvement of sinterability . 2 . the start materials of the ceramic compositions in accordance with our invention may be substances such as oxides or hydroxides other than those employed in the foregoing examples . 3 . the temperature of the oxidizing heat treatment need not necessarily be 600 ° c . but can be variously determined in a range ( from 500 ° to 1000 ° c . for the best results ) not exceeding the temperature of the preceding sintering in a nonoxidative atmosphere , the oxidizing temperature being dependent upon factors such as the particular base metal electrode material in use and the degree of oxidation required for the ceramic material . 4 . the temperature of cosintering in a nonoxidative atmosphere may also be changed in consideration of the particular electrode material in use . we recommend a range of 1050 ° to 1200 ° c . if the electrode material is nickel , as we have ascertained from experiment that little or no flocculation of the nickel particles takes place in that temperature range . 5 . the dielectric bodies and electrodes may be cosintered in a neutral , instead of reductive , atmospere . 6 . the ceramic compositions disclosed herein may be employed for capacitors other than those of the multilayered configuration .