DETAILED ACTION
Notice of Pre-AIA or AIA Status
The present application, filed on or after March 16, 2013, is being examined under the first inventor to file provisions of the AIA .
Priority
Acknowledgment is made of applicant’s claim for foreign priority under 35 U.S.C. 119 (a)-(d). The certified copy has been filed in parent Application No. JP2022-133298 and No. JP2023-118270, filed on August 24, 2022 and July 20, 2023, respectively.
Receipt is acknowledged of certified copies of papers required by 37 CFR 1.55.
Specification
The disclosure is objected to because of the following informalities: minor typo in 5th sentence of paragraph [0037], "the light dimeter" instead of "diameter".
Appropriate correction is required.
Claim Rejections - 35 USC § 102
The following is a quotation of the appropriate paragraphs of 35 U.S.C. 102 that form the basis for the rejections under this section made in this Office action:
A person shall be entitled to a patent unless –
(a)(1) the claimed invention was patented, described in a printed publication, or in public use, on sale, or otherwise available to the public before the effective filing date of the claimed invention.
(a)(2) the claimed invention was described in a patent issued under section 151, or in an application for patent published or deemed published under section 122(b), in which the patent or application, as the case may be, names another inventor and was effectively filed before the effective filing date of the claimed invention.
Claims 1-2 and 7-8 are rejected under 35 U.S.C. 102(a)(1)(a)(2) as being anticipated by Takaku et al (US Pat No. 10,727,378).
Regarding claim 1, Takaku in Figs. 3 and 4 depict fluorescent phases (bright) of a sintered body which contains crystal agglomerated particles containing a rare earth aluminate fluorescent material crystal phase of formula A3B5O12:Ce where “Each of the element A and the element B is at least one element selected from the following element groups: A: Sc, Y, and lanthanoids (except for Ce), and B: Al and Ga”. The dark portions correspond to Al2O3 (aluminum oxide) phase which are disposed around fluorescent crystal particles. Therefore, Takaku teaches the claimed “A sintered body comprising: crystal agglomerated particles containing a rare earth aluminate fluorescent material crystal phase; and an aluminum oxide phase, wherein the aluminum oxide phase is disposed around the crystal agglomerated particle”.
Regarding claim 2, Takaku teaches the limitations of claim 1. Figs. 3 and 4 depict multiple fluorescent phases of a sintered body in cross-sectional view as well as dark regions (Al2O3) phases which are disposed between two or more of the fluorescent crystal particle phases. Therefore, Takaku anticipates the claimed “The sintered body according to claim 1, wherein the sintered body includes two or more of the crystal agglomerated particles in a cross-sectional view, and the aluminum oxide phase is disposed between the two or more of the crystal agglomerated particles”.
Regarding claim 7, Takaku teaches the limitations of claim 1 and further discloses the sintered body contains a rare earth aluminate fluorescent material crystal phase of formula A3B5O12:Ce where “Each of the element A and the element B is at least one element selected from the following element groups: A: Sc, Y, and lanthanoids (except for Ce), and B: Al and Ga” (Col 6 lines 10-20). Additionally, examples 1-4 teach synthesis of sintered body compositions where A is Y, Y with Gd, or Lu. Therefore, Takaku anticipates the claimed “The sintered body according to claim 1, wherein the rare earth aluminate fluorescent material crystal phase comprises at least one element selected from the group consisting of Y, La, Lu, Gd, and Tb”.
Regarding claim 8, Takaku teaches the limitations of claim 1 (see also rejection under claim 7). Furthermore in examples 1-4 (particularly ex 4 sample 28), Takaku discloses Ce present at mol% of 0.05, 0.1, 0.3, 0.5, 0.7, 1, and 2 (corresponds to stoichiometric ratios of 0.0005, 0.001, 0.003, 0.005, 0.007, 0.01, and 0.02 satisfying claimed n). Example 4 sample 28 would correspond to formula of structure (Lu0.997Ce0.003)3(Al1-mGam)5O12. Under example 4, Takaku discloses that proportions of raw materials were varied so that specific sintered bodies were synthesized which can tailor porosity, translucent phase sizes, and area ratios (Table 1). Therefore, Takaku teaches the claimed “The sintered body according to claim 1, wherein the rare earth aluminate fluorescent material crystal phase has a composition represented by the following formula (I): (R11-nCen)3(Al1-mM1m)5kO12 (I) wherein R1 represents at least one element selected from the group consisting of Y, La, Lu, Gd, and Tb; M1 represents at least one element selected from the group consisting of Ga and Sc; and m, n, and k respectively satisfy 0 ≤ m ≤ 0.02, 0.001 ≤ n ≤ 0.017, and 0.95 ≤ k ≤ 1.10”.
Claims 9 and 10 are rejected under 35 U.S.C. 102(a)(1)(a)(2) as being anticipated by Irie (US PGPub 20130256599).
Regarding claim 9,
Irie teaches in paragraphs [0057] and [0058] providing a first mixture that is wet mixed and then dried using a spray drier (preparation 1), thus meeting claimed “A method for producing a sintered body comprising: (a) providing a first mixture obtained by wet mixing raw materials and then drying;”.
In paragraph [0060], Irie further teaches dry mixing the first mixture with aluminum oxide, thus meeting claimed limitation “(b) dry mixing the first mixture and aluminum oxide particles to obtain a second mixture;”.
In paragraph [0060] Irie also discloses molding the second mixture following dry mixing, thus meeting claimed limitation “(c) molding the second mixture obtained in (b) to obtain a molded body;”
Irie finally describes degreasing and subsequently firing the molded body to prepare a ceramic composite. Degreasing and firing the molded body or powders results in creation of a phosphor sintered body. To one of ordinary skill in the art, the process of degreasing and firing is synonymous with calcining, thus meeting the claimed limitation “and (d) calcining the molded body obtained in (c)”. Therefore, Irie exemplifies the claimed “A method for producing a sintered body comprising: (a) providing a first mixture obtained by wet mixing raw materials and then drying; (b) dry mixing the first mixture and aluminum oxide particles to obtain a second mixture; (c) molding the second mixture obtained in (b) to obtain a molded body; and (d) calcining the molded body obtained in (c)”.
Regarding claim 10, Irie teaches the limitations of claim 9. Furthermore, Irie teaches use of Y2O3, CeO2, and Al2O3 powders for the first wet mixture in paragraph [0057]. Additionally, in paragraph [0062], Irie teaches synthesis with optional use Ga2O3 or Sc2O3 mixed in prescribed ratio of preparation 1 (the Y, Ce, and Al powder). Therefore, Irie teaches the claimed limitation “The method for producing a sintered body according to claim 9, wherein the first mixture comprises first oxide particles containing at least one element R1 selected from the group consisting of Y, La, Lu, Gd, and Tb, second oxide particles containing Ce, third oxide particles containing Al, optionally fourth oxide particles containing at least one element M1 selected from the group consisting of Ga and Sc, and optionally rare earth aluminate fluorescent material particles”.
Claim Rejections - 35 USC § 103
The following is a quotation of 35 U.S.C. 103 which forms the basis for all obviousness rejections set forth in this Office action:
A patent for a claimed invention may not be obtained, notwithstanding that the claimed invention is not identically disclosed as set forth in section 102, if the differences between the claimed invention and the prior art are such that the claimed invention as a whole would have been obvious before the effective filing date of the claimed invention to a person having ordinary skill in the art to which the claimed invention pertains. Patentability shall not be negated by the manner in which the invention was made.
Claims 3-6 are rejected under 35 U.S.C. 103 as being unpatentable over Takaku et al in view of Irie (US Pat No. 10,216,076).
Regarding claim 3, Takaku teaches the limitations of claim 1 but does not disclose largest diameter size (ergo the “maximum length” according to applicants) among the Al2O3 phases. Irie does disclose average crystal particle sizes for Al2O3 phases. In Table 1, Irie describes different sintered body compositions which include rare earth aluminate fluorescent crystal (phosphor) phase and an Al2O3 (scatterer) phase (outside of Comp. Ex. 1). The table lists various average crystal particle sizes for the Al2O3 phase which are all > 1.0 μm. Therefore, the maximum length of these oxide phases are all > 1.0 μm. Irie also discloses in Col 3 lines 28-36 that by increasing particle size of phosphor phase to be larger than that of scatterer phase, scattering of excitation light can be increased. Further, by having uniform crystal particle phase of scatterer prevents light scattering loss and suggests a preferable particle size of the scatterer between 1.0 and 1.5 μm. Therefore, one of ordinary skill in the art could tailor the composition of their sintered body according to teachings of Irie to have a uniform Al2O3 phase where particles are uniformly larger than 1.0 μm to prevent scattering loss. Together, the teachings of Takaku and Irie meet the claimed “The sintered body according to claim 1, wherein the aluminum oxide phase has a maximum length that is 1.0 μm or more on a surface or a cross section of the sintered body”.
Regarding claim 4, Takaku teaches the limitations of claim 1 but reports area ratios of translucent to fluorescent phases. Takaku discloses in Col 3 lines 40-59 effects of varying mean grain size between translucent and fluorescent phases, thus effects of changing area%. In table 1, Irie discloses compositions where the vol% of Al2O3 exists at 1, 5, and 10%. Additionally, Irie discloses compositions that have thicknesses of 50, 300, 500, and 1000 μm. Assuming homogeneity in composition, a cross-section of Irie’s samples taken by SEM would hold the area% constant. However, given that the Al2O3 particle size is roughly 20% or 50% of the average fluorescent particle size, a cross section of homogenous distribution between particles could at most hold the area% constant to vol% (5% for Exs. 4-5 and 7-12) and would likely cut the vol% to a percentage consistent to particle size difference. So, for particle sizes 50% the size of fluorescent particles, the area% likely cuts down to 50% the vol% (from 5 down to 2.5%). One of ordinary skill in the art could tailor their area% using the teachings of Takaku and Irie to produce a sintered body with more uniform light scattering or luminescence. Therefore, the teachings of Takaku and Irie together meet the claimed “The sintered body according to claim 1, wherein the aluminum oxide phase on a surface or a cross section of the sintered body is in a range of 2.5 area% or more and 10.0 area% or less relative to 100 area% of the surface or the cross section”.
Regarding claim 5, Takaku teaches the limitations of claim 1 but does not disclose crystal agglomerated particles (fluorescent rare earth aluminate phase) of sizes > 10.0 μm or less than 150.0 μm. Irie discloses in Table 1, Ex 6, an average particle size for phosphor phase of 15 μm. Irie teaches that by having larger crystal particles (preferably 15 μm or less), sufficient light emission efficiency and more excellent mechanical strength can be obtained (Col 3 lines 14-20). Therefore, it would have been obvious for one of ordinary skill in the art to use crystal agglomerated particles of larger size to improve light transmission and mechanical strength of the composite. Together, Takaku and Irie teach the claimed “The sintered body according to claim 1, wherein the crystal agglomerated particles have a maximum length in a range of 10.0 μm or more and 150.0 μm or less on a surface or a cross section of the sintered body”.
Regarding claim 6, Takaku teaches the limitations of claim 1 but does not report vol% of Al2O3 phase within the claimed range. In Table 1, Irie lists sintered body compositions where the Al2O3 phase exists at vol% of 5 and 10. In Col. 2 lines 45-63, Irie describes benefits having phosphor and scatterer vol% within claimed range. When scatterer phase exceeds 10vol%, the content of phosphor phase is relatively low, leading to cases where satisfactory light emission efficiency cannot be obtained. When scatterer phase is below 1vol%, excitation light is easily propagated in the phosphor phase to increase the size of a light emitting spot, thus decreasing the quantity of light that can be condensed. Therefore, it would have been obvious to one of ordinary skill in the art to increase the scatter vol% phase of Takaku to a range reported by Irie in order to maximize light emission efficiency while condensing the light (better resolution) to an allowable range. Together, Irie and Takaku teach the claimed “The sintered body according to claim 1, wherein the aluminum oxide phase has a volume ratio in a range of 2.5% by volume or more and 10.0% by volume or less relative to 100% by volume of a total of the crystal agglomerated particles and the aluminum oxide phase”.
Claims 9-10 and 14-15 are rejected under 35 U.S.C. 103 as being unpatentable over Irie (US PGPub 20130256599) in view of Hirai et al (US PGPub 20210403382).
Regarding claim 9,
Irie teaches in paragraphs [0057] and [0058] providing a first mixture that is wet mixed and then dried using a spray drier (preparation 1), thus meeting claimed “A method for producing a sintered body comprising: (a) providing a first mixture obtained by wet mixing raw materials and then drying;”.
In paragraph [0060], Irie further teaches dry mixing the first mixture with aluminum oxide, thus meeting claimed limitation “(b) dry mixing the first mixture and aluminum oxide particles to obtain a second mixture;”.
In paragraph [0060] Irie also discloses molding the second mixture following dry mixing, thus meeting claimed limitation “(c) molding the second mixture obtained in (b) to obtain a molded body;”
Irie finally describes firing the molded body under vacuum atmosphere but does not specifically disclose calcining. Hirai et al also teaches a sintered body composition does not dry mix their first mixture and Al2O3. Hirai does disclose in paragraph [0040] that “these particles can be mixed in wet or dry manner”. Following molding, Hirai calcines the molded body in example 1 (paragraph [0109]), thus meeting the claimed “and (d) calcining the molded body obtained in (c)”.
Therefore, it would have been obvious to one of ordinary skill in the art at the effective date of filing to substitute the calcining step of Hirai to the method of Irie with predictable results. It is well known in the art that calcining the mixture removes impurities and induces thermal decomposition. Together, Irie and Hirai teach the claimed limitations of claim 9 “A method for producing a sintered body comprising: (a) providing a first mixture obtained by wet mixing raw materials and then drying; (b) dry mixing the first mixture and aluminum oxide particles to obtain a second mixture; (c) molding the second mixture obtained in (b) to obtain a molded body; and (d) calcining the molded body obtained in (c)”.
Regarding claim 10, Irie and Hirai together teach the limitations of claim 9. Furthermore, Irie teaches use of Y2O3, CeO2, and Al2O3 powders for the first wet mixture in paragraph [0057]. Additionally, in paragraph [0062], Irie teaches synthesis with optional use of Ga2O3 or Sc2O3 mixed in prescribed ratio of preparation 1 (the Y, Ce, and Al oxide powders). Hirai also teaches wet mixing of rare earth aluminates with Y2O3 and Al2O3. As explained in paragraph [0056], Hirai describes that mixing a second rare earth aluminate along with the separate aluminum oxide powder allows for synthesis of a ceramic composition containing three unique crystal phases. The first crystal phase containing the first rare earth aluminate fluorescent material integrated with the second rare earth aluminate fluorescent material can convert wavelengths of light emitted from excitation source, allowing the ceramic complex to emit light with high luminance. The interface between the second and third crystal phases scatters light, thus increasing the light absorption efficiency of the first crystal phase and the wavelength efficiently converted. Therefore, it would have been prima facie obvious to one of ordinary skill in the art, as of the effective filing date, to optionally mix second rare earth aluminates to produce a ceramic complex of three crystal phases that converts wavelengths of light and emits light with high luminance. Together, the teachings of Irie and Hirai match the claimed limitation “The method for producing a sintered body according to claim 9, wherein the first mixture comprises first oxide particles containing at least one element R1 selected from the group consisting of Y, La, Lu, Gd, and Tb, second oxide particles containing Ce, third oxide particles containing Al, optionally fourth oxide particles containing at least one element M1 selected from the group consisting of Ga and Sc, and optionally rare earth aluminate fluorescent material particles”.
Regarding claim 14, Irie and Hirai teach the method of claim 9. Irie does not disclose the volume amount of Al2O3 used in dry mixture, but they disclose in paragraph [0061] that by changing amounts of the different powders, the ceramic composites have a changed volume ratio of aluminum oxide particles. In paragraph [0056], Hirai discloses a ceramic complex comprising first crystal phase (rare earth aluminate) of 5-45% volume, second crystal phase (second earth aluminate) of 0.5-50% volume, and third crystal phase (Al2O3 akin to aluminum oxide of claim 9(b)) of remaining volume %. Hirai does not directly teach an Al2O3 phase comprising 2.5-10.0% by volume in examples but leaves the realm of possibility open as described. Furthermore, Hirai teaches that as first and second crystal phases increase by volume (Al2O3 phase decreases by volume), the relative luminance also increases or improves. Therefore, it would have been obvious to one of ordinary skill in the art to take the teachings of Hirai to implement volume ratio of Al2O3 in the combined methods of Irie and Hirai to produce a sintered body of desired luminance. Together, Irie and Hirai meet the claimed “The method for producing a sintered body according to claim 9, wherein in (b), an amount of the aluminum oxide particles are in a range of 2.5% by volume or more and 10.0% by volume or less relative to 100% by volume of a total amount of the first mixture and the aluminum oxide particles”.
Regarding claim 15, Irie and Hirai teach the method of claim 9. Furthermore, Hirai discloses a calcining temperature of 1,650°C for the molded body in example 1 (paragraph [0109]). In paragraph [0044], Hirai suggests an acceptable temperature range for calcining of 1,550-1,800°C. Hirai explains that the reaction between the aluminum oxide particles and the oxide particles can be promoted without dissolving the first rare earth aluminate fluorescent material to produce a ceramic complex containing a first crystal phase with a large crystal diameter containing the first rare earth aluminate fluorescent material integrated with the second rare earth aluminate, a second crystal phase composed of the second rare earth aluminate, and a third crystal phase composed of the aluminum oxide. It would have been obvious to select a calcining temperature within that range which falls within the claimed limitation in order to produce a ceramic complex containing those integrated crystal phases without dissolution of fluorescent materials. Therefore, Irie and Hirai together meet the claimed “The method for producing a sintered body according to claim 9, wherein the molded body is calcined at a calcining temperature in a range of 1,300°C or higher and 1,800°C or lower”.
Claims 11-13 are rejected under 35 U.S.C. 103 as being unpatentable over Irie (US PGPub 20130256599) in view of Hirai et al as applied to claims 9-10 above, and further in view of Taketomi et al (USPGPub 20220041509).
Regarding claim 11, Irie and Hirai teach the method of claim 9 but neither disclose BET specific surface areas for their Al2O3 particles. Irie uses Al2O3 powder of 0.3 µm (average particle size) for the wet mix of claim 9a and dry mix claim 9b, but the average particle size of the mixtures are 20 µm (first mixture) and 50 µm (second mixture). Hirai discloses use of Al2O3 particles that should have FSSS average particle diameter D3 between 0.1-1.5 µm for easier growth during calcination (paragraph [0038]) and uses a D3 size of 0.6 µm in example 1. Taketomi et al discloses a wet or dry mix of rare earth aluminate phosphor particles (YAG and LAG) with Al2O3 particles which have BET specific surface area of 5 m2/g (see Tables 1 and 2). Taketomi also discloses in paragraphs [0052] and [0056] that the aluminum oxide should ideally have specific surface area of 5 m2/g to form crystalline phases within range of desired absolute maximum length. Additionally, Taketomi discloses that oxide particles having “large specific surface area” are oxide particles having “a small particle size”. Therefore, it would have been obvious to one of ordinary skill in the art to substitute the Al2O3 particles used by Taketomi in the combined method of Irie and Hirai to synthesize sintered body composites having crystalline phases of desired maximum length. Together, Irie, Hirai and Taketomi meet the claimed “The method for producing a sintered body according to claim 9, wherein the aluminum oxide particles to be dry-mixed with the first mixture have a BET specific surface area in a range of 1.0 m2/g or more and 10.0 m2/g or less”.
Regarding claim 12, Irie and Hirai teach the method of claim 10 but use uniform particle sizes for the aluminum oxide particles between wet and dry mixes (do not disclose BET sizes). Irie uses Al2O3 powder of 0.3 µm (average particle size) for the wet mix of claim 9a and dry mix claim 9b, but the average particle size of the mixtures are 20 µm (first mixture) and 50 µm (second mixture), thus suggesting that particle sizes can differ between mixes and that particles of higher surface area (lower diameter) should be dry mixed with particles of lower surface area (larger diameter). In Tables 1 and 2, Taketomi shows the effect of mixing Al2O3 particles with LAG phosphor particles having lower specific surface area (BETs of 11.8 vs 8.8 m2/g, respectively) or with YAG phosphor particles having higher specific surface area (5.5 vs. 8.0 m2/g, respectively). The improvement in relative flux is stronger from using Al2O3 having a lower surface area than the YAG phosphor (examples 7-8, Table 2) compared to improvement noted in Al2O3 having higher surface are than LAG phosphor (examples 3-4, Table 1). Regardless of phosphor identity (YAG or LAG), Tables 1 and 2 of Taketomi suggest the importance of mixing previously formed rare earth aluminate materials (YAG or LAG) with another Al2O3 material. Furthermore, Taketomi discloses in paragraph [0052] an allowable range of BET sizes for aluminum oxide used in the first formed rare earth aluminate (50 m2/g or less) and in paragraph [0054] an allowable range for the formed rare earth aluminate between 6 and 15 m2/g. If the specific surface area of the rare earth aluminate used as a raw material with the second aluminum oxide used is too large, it is difficult to uniformly disperse the particles and may be difficult to form homogeneous rare earth aluminate phosphor crystal phases. Additionally, Taketomi discloses in paragraph [0056] that to form rare earth aluminate crystalline phases of desired maximum length, then “the rare earth aluminate phosphor particles and at least one type of particle selected from the various oxide particles, or the rare earth aluminate phosphor particles and all of the oxide particles have a specific surface area of 5 m2/g or greater according to the BET method”. Therefore, the combined teachings of Taketomi, Irie, and Hirai suggest that mixing particle phases of different sizes can tailor the sintered body composition in terms of luminance, density, and homogeneity of crystalline distribution. It would have been obvious to one of ordinary skill in the art to experimentally tailor sizing parameters of aluminum oxides (below 50m2/g in first mixture and between 5 to 15 m2/g in second mixture) according to disclosure of Taketomi paragraphs [0052] to [0056] to adjust luminosity of sintered body. Together, Irie, Hirai, and Taketomi meet the claimed “The method for producing a sintered body according to claim 10, wherein the aluminum oxide particles have a BET specific surface area smaller than a BET specific surface area of the third oxide particles containing Al.”.
Regarding claim 13, Irie and Hirai teach the method of claim 10. As described in the rejections for claims 11 and 12, Irie and Hirai do not specify their BET specific surface areas for Al2O3. Taketomi teaches wet mixing of Al2O3 particles having BET specific surface area of 11.8 m2/g (Table 1 examples 1-2 and paragraph [0091]) with CeO2 and Lu2O3 particles. Taketomi discloses in paragraphs [0052], [0054], and [0056] that by using Al2O3 particles of BET specific surface area between 6 to 15 m2/g, sintered bodies can be formed with uniform distribution and homogeneity of crystalline phases and rare earth aluminate crystalline phases of desired maximum length. Therefore, it would have been obvious to one of ordinary skill in the art to substitute the Al2O3 oxides of 11.8 m2/g BET specific surface art taught by Taketomi with the methods disclosed by Irie and Hirai to produce sintered bodies having uniform distribution and homogeneity of crystalline phases and rare earth aluminate crystalline phases of desired maximum length. Together, the teachings of Irie, Hirai and Taketomi meet the claimed “The method for producing a sintered body according to claim 10, wherein the third oxide particles containing Al have a BET specific surface area in a range of more than 10.0 m2/g and 15.0 m2/g or less.”.
Conclusion
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/NWFG/Examiner, Art Unit 1759
/MELVIN C. MAYES/Supervisory Patent Examiner, Art Unit 1759
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