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. EP21216315.0 and PCT/EP2022/086309, filed on December 16, 2021 and December 16, 2022, respectively.
Receipt is acknowledged of certified copies of papers required by 37 CFR 1.55.
Claim Rejections - 35 USC § 112
The following is a quotation of 35 U.S.C. 112(b):
(b) CONCLUSION.—The specification shall conclude with one or more claims particularly pointing out and distinctly claiming the subject matter which the inventor or a joint inventor regards as the invention.
The following is a quotation of 35 U.S.C. 112 (pre-AIA ), second paragraph:
The specification shall conclude with one or more claims particularly pointing out and distinctly claiming the subject matter which the applicant regards as his invention.
Claims 2, 7, and 10 are rejected under 35 U.S.C. 112(b) or 35 U.S.C. 112 (pre-AIA ), second paragraph, as being indefinite for failing to particularly point out and distinctly claim the subject matter which the inventor or a joint inventor (or for applications subject to pre-AIA 35 U.S.C. 112, the applicant), regards as the invention.
Claim 2 (lines 3-5) references “the nanoparticles” as being of the type A13A25O12:Ln but in claim 1, on which claim 2 depends, the nanoparticles are “of the type A2-xO3:Ln”. It is unclear whether two different types of nanoparticles are made or if the nanoparticles are simultaneously of both types, which by chemical formulas, does not appear possible considering that no further precursors are provided in first and/or second mixtures. Since, the claim references “the nanoparticle” originating from independent claim 1, it can be inferred that the nanoparticle is intended to simultaneously satisfy both types and would be produced from the same limitations in claim 1. From A2-xO3:Ln, A13A25O12:Ln likely comes from providing at least two salts of A that define A1 and A2 and satisfies A2-xO3:Ln when multiplied by 4, i.e., A(2-x)yO3y:Ln whereby y = 4 such that both “types” or formulas are satisfied. Thus, claim 2 is indefinite.
Claim 7 (line 2) references “the nanoparticles” as being of the type A13A25O12:Ln but in claim 1, on which claim 7 depends, the nanoparticles are “of the type A2-xO3:Ln”. It is unclear whether two different types of nanoparticles are made or if the nanoparticles are simultaneously of both types, which by chemical formulas, does not appear possible considering that no further precursors are provided in first and/or second mixtures. Since, the claim references “the nanoparticle” originating from independent claim 1, it can be inferred that the nanoparticle is intended to simultaneously satisfy both types and would be produced from the same limitations in claim 1. From A2-xO3:Ln, A13A25O12:Ln likely comes from providing at least two salts of A that define A1 and A2 and satisfies A2-xO3:Ln when multiplied by 4, i.e., A(2-x)yO3y:Ln whereby y = 4 such that both “types” or formulas are satisfied. Thus, claim 7 is indefinite.
Claim 10 recites a mixture comprising a protective matrix in the heating step. In light of the instant specification (pg 10 lines 10-20), the protective matrix “may be a salt”. It is unclear the scope and bounds of such protective matrices or how a salt serves the function to impart protection or to serve as a protective matrix. It is also unclear if only a salt can serve such a function in the claimed invention and/or where the scope of protection for such a protective matrix lies. Thus, claim 10 is indefinite.
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 16-19 are rejected under 35 U.S.C. 103 as being unpatentable over Krames et al (WO2020053429A2).
Claim 16, and subsequently dependent claims 17-19, contain product by process limitations. Product by process-based claims or limitations do not necessitate arrival to the specific process as claimed if the process does not materially affect the product to a different manner. "[E]ven though product-by-process claims are limited by and defined by the process, determination of patentability is based on the product itself. The patentability of a product does not depend on its method of production. If the product in the product-by-process claim is the same as or obvious from a product of the prior art, the claim is unpatentable even though the prior product was made by a different process." In re Thorpe, 777 F.2d 695, 698, 227 USPQ 964, 966 (Fed. Cir. 1985) (citations omitted). Furthermore, "[b]ecause validity is determined based on the requirements of patentability, a patent is invalid if a product made by the process recited in a product-by-process claim is anticipated by or obvious from prior art products, even if those prior art products are made by different processes." Amgen Inc. v. F. Hoffmann-La Roche Ltd., 580 F.3d 1340, 1370 n. 14, 92 USPQ2d 1289, 1312, n. 14 (Fed. Cir. 2009).
Krames teaches a first and second luminescent materials/nanoparticles for use in a composition in electron transfer (FRET) applications (paragraphs [0040-45]). Krames states the luminescent materials comprise a host lattice which may be doped with ions, including lanthanides (paragraph [0044]). The host lattice is an oxide, garnet, phosphate, vanadate, or combination of these such as Y2O3 among others. In provided examples (see Figs. 2-12), Krames provides LaPO4:Eu3+/LaPO4:Tb3+ and YAG:Ce nanoparticles. It would have been prima facie obvious to one of ordinary skill in the art, as of the effective filing date, to substitute the LaPO4 or the YAG nanoparticles for Y2O3 with the same doping lanthanides as a known alternative host lattice suitable for FRET luminescent compositions and arrive at the invention as claimed. Thus, Krames teaches the claimed “Nanoparticles of the type A2-xO3:Lnx, wherein A is one or more of yttrium, scandium, aluminium, gallium, or a lanthanide; Ln is at least one lanthanide; and 0<x<2, which have been obtained by:- providing a first mixture comprising at least a salt of A, a salt of Ln, and a solvent, - providing a second mixture comprising a precipitating agent and a solvent,- contacting said first mixture with said second mixture in a microjet reactor process to obtain a third mixture comprising nanoparticles, and - subjecting said nanoparticles to a heating step.”.
Regarding claim 17, Krames teaches the nanoparticles of claim 16. In examples, Krames uses Tb, Eu, and Ce. Further in paragraphs [0040-44], Krames teaches the nanoparticles comprise a host lattice which are doped with (optically) active ions. Thus, Krames teaches the claimed “The nanoparticles of claim 16, wherein:- the Ln comprises an ion chosen from the group of Tb3+, Eu3+ and Ce3+, and/or - the nanoparticles comprise active ions disposed in a host lattice”.
Regarding claim 18, Krames teaches the nanoparticles of claim 16. Krames teaches a mixing of two luminescent materials (nanoparticles) into an improved luminescent composition (paragraphs [0001, 0009, 0015]). Thus, Krames teaches a luminescent composition comprising the nanoparticles. Therefore, Krames teaches the claimed “A luminescent composition comprising the nanoparticles of claim 16.”.
Regarding claim 19, Krames teaches the luminescent composition of claim 18. As described above, Krames provides a first and second luminescent material into the luminescent composition. In paragraph [0015], Krames teaches providing a “composition comprising a first luminescent material and a second luminescent material, wherein said first luminescent material and said second luminescent material are selected such that said second luminescent material has an emission spectrum which overlaps at least partly with one or more of excitation bands of said first luminescent material; and wherein said first luminescent material and said second luminescent material are so arranged to each other to allow non-radiative energy transfer from said second luminescent material to said first luminescent material; and annealing said composition”. Krames teaches providing luminescent materials that can be of Y2O3:Ln where Ln is Eu, Tb, Ce as described in the rejections above. Although Krames does not provide examples using such luminescent materials of Y2O3 type, it would have been prima facie obvious to one of ordinary skill in the art, as of the effective filing date, to substitute the LaPO4 or the YAG nanoparticles for Y2O3 with the same doping lanthanides as a known alternative host lattice suitable for FRET luminescent compositions and arrive at the invention as claimed. Thus Krames teaches the claimed “The luminescent composition of claim 18, wherein the luminescent composition comprises a first luminescent material and a second luminescent material, wherein said first luminescent material and said second luminescent material are selected such that said second luminescent material has an emission spectrum that overlaps at least partly with one or more of excitation bands of the first luminescent material, and wherein said first luminescent material and/or said second luminescent material comprises nanoparticles of the type A2-xO3:Lnx, wherein A is one or more of yttrium, scandium, aluminium, gallium, or a lanthanide; Ln is at least one lanthanide; and 0<x<2, which have been obtained by:- providing a first mixture comprising at least a salt of A, a salt of Ln, and a solvent,- providing a second mixture comprising a precipitating agent and a solvent,- contacting said first mixture with said second mixture in a microjet reactor process to obtain a third mixture comprising nanoparticles, and- subjecting said nanoparticles to a heating step”.
Claims 16-19 are rejected under 35 U.S.C. 103 as being unpatentable over Krames et al (WO2020053429A2) as applied to claim 16 above, and further in view of Puppe et al (US PGPub 20100019201).
As described in the rejection of claim 16 above, claims 16-19 contain product by process limitations. Product by process-based claims or limitations do not necessitate arrival to the specific process as claimed if the process does not materially affect the product to a different manner. "[E]ven though product-by-process claims are limited by and defined by the process, determination of patentability is based on the product itself. The patentability of a product does not depend on its method of production. If the product in the product-by-process claim is the same as or obvious from a product of the prior art, the claim is unpatentable even though the prior product was made by a different process." In re Thorpe, 777 F.2d 695, 698, 227 USPQ 964, 966 (Fed. Cir. 1985) (citations omitted). Furthermore, "[b]ecause validity is determined based on the requirements of patentability, a patent is invalid if a product made by the process recited in a product-by-process claim is anticipated by or obvious from prior art products, even if those prior art products are made by different processes." Amgen Inc. v. F. Hoffmann-La Roche Ltd., 580 F.3d 1340, 1370 n. 14, 92 USPQ2d 1289, 1312, n. 14 (Fed. Cir. 2009). Regardless, Krames teaches nanoparticles of the type A2-xO3:Lnx (such as Y2O3:Ln) but does not teach a method for preparing such nanoparticles nor limits how they should be prepared prior to implementation into a luminescent composition. Puppe does teach a method for preparing yttrium containing (examples 1-2), yttrium and europium containing (example 3), dysprosium-containing (a lanthanide, examples 4-5), and cerium-containing (a lanthanide, example 6) nanoparticles which follows the microjet reactor process as claimed. Puppe teaches such a method enables wet-chemical production of nanosize to microsize particles of compounds of the rare earth metals and other transition metals and also for the production of colloid-chemically stable sols of these particles without low yield, low period of operation, and unsatisfactory colloidal stability (paragraphs [0025-27, 0029]). Example 3 provides the most relevant process as an acetate of yttrium and an acetate of europium (salts of A and Ln as claimed) are provided in aqueous solutions as a first starting material. A second starting material provided is an aqueous solution of triethanolamine (a precipitating agent as disclosed in paragraph [0054]). These aqueous solutions contain a solvent as described in paragraphs [0033-36]. The two starting materials are pumped together through the reactor (see Fig. 1) where the two mixtures are contacted with one another, forming a third mixture, and obtaining colloidally stable and slightly turbid sol containing europium-doped yttrium nanoparticles (Y2O3:Eu). Although Puppe does not specifically use a microjet reactor in their process, Puppe teaches that such reactors can be implemented as a suitable microreactor (paragraph [0074]) which includes MicroJetReactor. It would have been prima facie obvious to one of ordinary skill in the art, as of the effective filing date, to substitute the microreactor utilized by Puppe for a microjet reactor as a known alternative microreactor capable of producing nanoparticles and arrive at the limitation as claimed. Finally, the nanoparticles (after contacting mixtures) are calcined at 800°C (thus subjected to heating step, paragraph [0127]). It would have been prima facie obvious to one of ordinary skill in the art, as of the effective filing date, to prepare the nanoparticles described by Krames, using the method informed by Puppe, as a known method of preparing such nanoparticles with higher yield, higher periods of operation, and satisfactory colloidal stability and arrive at the invention as claimed. Therefore, Krames and Puppe teach the claimed “Nanoparticles of the type A2-xO3:Lnx, wherein A is one or more of yttrium, scandium, aluminium, gallium, or a lanthanide; Ln is at least one lanthanide; and 0<x<2, which have been obtained by:- providing a first mixture comprising at least a salt of A, a salt of Ln, and a solvent, - providing a second mixture comprising a precipitating agent and a solvent,- contacting said first mixture with said second mixture in a microjet reactor process to obtain a third mixture comprising nanoparticles, and - subjecting said nanoparticles to a heating step.”.
Regarding claim 17, Krames and Puppe teach the nanoparticles of claim 16. In examples, Krames uses Tb, Eu, and Ce. Further in paragraphs [0040-44], Krames teaches the nanoparticles comprise a host lattice which are doped with (optically) active ions. Puppe similarly teaches overlapping identities of host lattice and doping active ions. Thus, Krames and Puppe teaches the claimed “The nanoparticles of claim 16, wherein:- the Ln comprises an ion chosen from the group of Tb3+, Eu3+ and Ce3+, and/or - the nanoparticles comprise active ions disposed in a host lattice”.
Regarding claim 18, Krames and Puppe teach the nanoparticles of claim 16. Krames teaches a mixing of two luminescent materials (nanoparticles) into an improved luminescent composition (paragraphs [0001, 0009, 0015]). Thus, Krames teaches a luminescent composition comprising the nanoparticles. Therefore, Krames and Puppe teach the claimed “A luminescent composition comprising the nanoparticles of claim 16.”.
Regarding claim 19, Krames and Puppe teach the luminescent composition of claim 18. As described above, Krames provides a first and second luminescent material into the luminescent composition. In paragraph [0015], Krames teaches providing a “composition comprising a first luminescent material and a second luminescent material, wherein said first luminescent material and said second luminescent material are selected such that said second luminescent material has an emission spectrum which overlaps at least partly with one or more of excitation bands of said first luminescent material; and wherein said first luminescent material and said second luminescent material are so arranged to each other to allow non-radiative energy transfer from said second luminescent material to said first luminescent material; and annealing said composition”. Krames teaches providing luminescent materials that can be of Y2O3:Ln where Ln is Eu, Tb, Ce as described in the rejections above. Although Krames does not provide examples using such luminescent materials of Y2O3 type, it would have been prima facie obvious to one of ordinary skill in the art, as of the effective filing date, to substitute the LaPO4 or the YAG nanoparticles for Y2O3 with the same doping lanthanides as a known alternative host lattice suitable for FRET luminescent compositions and arrive at the invention as claimed. Thus Krames and Puppe teach the claimed “The luminescent composition of claim 18, wherein the luminescent composition comprises a first luminescent material and a second luminescent material, wherein said first luminescent material and said second luminescent material are selected such that said second luminescent material has an emission spectrum that overlaps at least partly with one or more of excitation bands of the first luminescent material, and wherein said first luminescent material and/or said second luminescent material comprises nanoparticles of the type A2-xO3:Lnx, wherein A is one or more of yttrium, scandium, aluminium, gallium, or a lanthanide; Ln is at least one lanthanide; and 0<x<2, which have been obtained by:- providing a first mixture comprising at least a salt of A, a salt of Ln, and a solvent,- providing a second mixture comprising a precipitating agent and a solvent,- contacting said first mixture with said second mixture in a microjet reactor process to obtain a third mixture comprising nanoparticles, and- subjecting said nanoparticles to a heating step”.
Claims 1-6, 8-10, and 16-17 are rejected under 35 U.S.C. 103 as being unpatentable over Puppe et al (US PGPub 20100019201).
Regarding claim 1, Puppe teaches a method for preparing yttrium containing (examples 1-2), yttrium and europium containing (example 3), dysprosium-containing (a lanthanide, examples 4-5), and cerium-containing (a lanthanide, example 6) nanoparticles which follow the microjet reactor process as claimed. Puppe teaches such a method enables wet-chemical production of nanosize to microsize particles of compounds of the rare earth metals and other transition metals and also for the production of colloid-chemically stable sols of these particles without low yield, low period of operation, and unsatisfactory colloidal stability (paragraphs [0025-27, 0029]). Example 3 provides the most relevant process as an acetate of yttrium and an acetate of europium (salts of A and Ln as claimed) are provided in aqueous solutions as a first starting material. A second starting material provided is an aqueous solution of triethanolamine (a precipitating agent as disclosed in paragraphs [0054-56]). These aqueous solutions contain a solvent as described in paragraphs [0033-36]. The two starting materials are pumped together through the reactor (see Fig. 1) where the two mixtures are contacted with one another, forming a third mixture, and obtaining colloidally stable and slightly turbid sol containing europium-doped yttrium nanoparticles (Y2O3:Eu). Although Puppe does not specifically use a microjet reactor in their process, Puppe teaches that such reactors can be implemented in place of a microreactor (paragraphs [0073-74]). Puppe discloses a MicroJetReactor as an example jet reactor which would be considered a “microjet reactor”. It would have been prima facie obvious to one of ordinary skill in the art, as of the effective filing date, to substitute the mixer utilized by Puppe for the MicroJetReactor as a known alternative mixing unit capable of producing nanoparticles and arrive at the limitation as claimed. Finally, the nanoparticles (after contacting mixtures) are calcined at 800°C (thus subjected to heating step, paragraph [0127]). Thus, Puppe teaches the claimed “A method of making luminescent nanoparticles of the type A2-xO3:Lnx, wherein A is one or more of yttrium, scandium, aluminium, gallium, or a lanthanide; Ln is at least one lanthanide; and 0<x<2, said method comprising:- providing a first mixture comprising at least a salt of A, a salt of Ln, and a solvent,- providing a second mixture comprising a precipitating agent and a solvent,- contacting said first mixture with said second mixture in a microjet reactor process to obtain a third mixture comprising nanoparticles, and- subjecting said nanoparticles to a heating step”.
Regarding claim 2, Puppe teaches the method of claim 1. Puppe teaches in example 3 use of europium as a dopant lanthanide. Puppe also broadly teaches in paragraph [0047] that rare earth metals provided can be any lanthanides. Thus, Puppe teaches the claimed “The method of claim 1, wherein Ln is chosen from the group consisting of europium, terbium, or cerium, and/or wherein the nanoparticles are of the type A13A25O12:Ln, wherein A1 is one or more selected from the group of yttrium, lutetium, and gadolinium; A2 is one or more selected from the group of aluminium, gallium, and scandium; and Ln is at least one lanthanide”.
Regarding claim 3, Puppe teaches the method of claim 1. In paragraph [0051], Puppe teaches suitable solvents which include amides and amines which are understood to be bases. Puppe teaches interchangeably that the starting mixtures can contain any of the disclosed suitable solvents from paragraph [0051], although such solvents utilized in examples are not necessarily provided. It would have been prima facie obvious to one of ordinary skill in the art, as of the effective filing date, to choose from any of the bases as a known suitable solvent for use in preparing nanoparticles in the reactor process of Puppe and arrive at the invention as claimed. Thus, Puppe teaches the claimed “The method of claim 1, wherein said first mixture comprises an acid or base”.
Regarding claim 4, Puppe teaches the method of claim 1. Puppe teaches in example 3 providing triethanolamine as a weakly basic precipitating agent (thus a base) as disclosed in paragraphs [0054-56] in starting material 2 (second mixture equivalent). Puppe teaches that using weakly basic compounds results in minimal formation of metal salt nuclei in starting mixtures (paragraph [0054]). Weakly basic solutions would be understood to have a pH of more than 7 since 7 indicates a neutral pH. Thus, Puppe teaches the claimed “The method of claim 1, wherein the second mixture has a pH of more than 7, and/or wherein said precipitating agent is a base”.
Regarding claim 5, Puppe teaches the method of claim 1. Puppe does not disclose the utilized temperature of the contacting step for example 3. The contacting step occurs in members 1 and 2 of Fig. 1 or the mixer/residence zone respectively. Puppe teaches that the first and second materials are mixed with one another to produce a homogenous mixture (third mixture) in paragraph [0037] whereby the temperature is subsequently increased for precipitation (paragraph [0038]) at 80°C or above (paragraph [0040]). Thus, the temperature of Puppe starts below 80°C for mixing as temperatures at or above that level results in precipitation which is not desired for the mixing step. Puppe teaches that the residence zone temperature is from 0-100°C (or 0-50°, or 0-30°C in paragraph [0081]). Therefore, the temperature would be reasonable to be held at room temperature (20-25°C, thus below 50°C) since no heating step is provided at this point. Additionally, the pressure is not specified for the contacting step but Puppe teaches in precipitation that the atmospheric pressure is above 1 atm (above ~ 1.01 bar). Thus, Puppe suggests a temperature below 80°C and/or a pressure above 1.01 bar which are both within the claimed ranges. Overlapping ranges have been held to present a prima facie case of obviousness over the prior art. It would have been prima facie obvious to one of ordinary skill in the art, as of the effective filing date, to select from the overlapping portion of the ranges for temperatures and/or pressures in the mixing step as such parameters represent variables that can induce precipitation and thus staying outside the ranges for precipitation steps would lead one of ordinary skill to arrive at the limitations as claimed in the mixing/contacting step to minimize precipitation before necessary and arrive at the invention as claimed. Therefore, Puppe teaches the claimed “The method of claim 1, wherein the contacting step is performed at a temperature of 50°C or lower and/or at a pressure of 5 bar or lower.”
Regarding claim 6, Puppe teaches the method of claim 1. Furthermore, Puppe provides in example 3 preparation of Y2O3:Eu which fits the type Y2O3:Ln as claimed. Additionally, Puppe teaches broadly that Yttrium, scandium, and lanthanum can be used as well as any other lanthanides and transition metals. Thus, Puppe teaches the claimed “The method of claim 1, wherein the nanoparticles are of the type Y2O3:Ln, Sc2O3:Ln, Lu2O3:Ln, and/or Gd2O3:Ln”.
Regarding claim 8, Puppe teaches the method of claim 1. Furthermore, in Fig. 1, Puppe shows separate feeding of the starting materials into the mixing zone or microjet reactor. Thus Puppe teaches the claimed “The method of claim 1, wherein the microjet reactor has a nozzle size of between 200 and 300 µm, and/or wherein the first mixture and the second mixture are separately fed into the microjet reactor”.
Regarding claim 9, Puppe teaches the method of claim 1. In paragraph [0043], Puppe teaches that the prepared nanoparticles should have D50 that is between 1 and 100nm in at least one spatial dimension. Additionally, Puppe teaches heating/calcining such nanoparticles at 800°C (thus 200°C or more). Therefore, Puppe teaches the claimed “The method of claim 1, wherein said heating comprises:- heating particles having a D50 value of ≥ 1nm, and a D50 value of ≤ 100 nm, - heating the nanoparticles at a temperature of 200 °C or more”.
Regarding claim 10, Puppe teaches the method of claim 1. In paragraph [0061], Puppe teaches that soluble substances such as low molecular weight additives, salts, surfactants, polymers, dispersants, and complexing agents can be added to starting solutions. The addition of such substances enables targeted coagulation of the nano-particles to be induced so as to simplify solid-liquid separation and enable reversible coagulation such that agglomerated particles can be redispersed (paragraph [0062]). Further, the colloid-chemical stability of the particles in the sols can be optimized by addition of such additives (paragraph [0068]). Improving such stability and redispersion are protective functions of these substances in solution, thus acting as a protective matrix in solution. Although Puppe reports adding such agents to the starting solution, the soluble substances are understood to be present throughout the reaction as the additives impart stability to the obtained nanoparticles. It would have been prima facie obvious to one of ordinary skill in the art, as of the effective filing date, to include a soluble substances such as salts into the mixture with obtained nanoparticles as such substances enable reversible coagulation and improve colloid-chemical stability of the nanoparticles in sols to arrive at the invention as claimed. Thus, Puppe teaches the claimed “The method of claim 1, wherein said heating comprises heating a mixture comprising the nanoparticles and a protective matrix”.
Regarding claim 16, Puppe teaches the method of claim 1 to prepare such nanoparticles of the claimed type whereby the method is implicitly contained. Puppe teaches a method for preparing yttrium containing (examples 1-2), yttrium and europium containing (example 3), dysprosium-containing (a lanthanide, examples 4-5), and cerium-containing (a lanthanide, example 6) nanoparticles which follow the microjet reactor process as claimed. Puppe teaches such a method enables wet-chemical production of nanosize to microsize particles of compounds of the rare earth metals and other transition metals and also for the production of colloid-chemically stable sols of these particles without low yield, low period of operation, and unsatisfactory colloidal stability (paragraphs [0025-27, 0029]). Example 3 provides the most relevant process as an acetate of yttrium and an acetate of europium (salts of A and Ln as claimed) are provided in aqueous solutions as a first starting material. A second starting material provided is an aqueous solution of triethanolamine (a precipitating agent as disclosed in paragraphs [0054-56]). These aqueous solutions contain a solvent as described in paragraphs [0033-36]. The two starting materials are pumped together through the reactor (see Fig. 1) where the two mixtures are contacted with one another, forming a third mixture, and obtaining colloidally stable and slightly turbid sol containing europium-doped yttrium nanoparticles (Y2O3:Eu). Although Puppe does not specifically use a microjet reactor in their process, Puppe teaches that such reactors can be implemented in place of a microreactor (paragraphs [0073-74]). Puppe discloses a MicroJetReactor as an example jet reactor which would be considered a “microjet reactor”. It would have been prima facie obvious to one of ordinary skill in the art, as of the effective filing date, to substitute the mixer utilized by Puppe for the MicroJetReactor as a known alternative mixing unit capable of producing nanoparticles and arrive at the limitation as claimed. Finally, the nanoparticles (after contacting mixtures) are calcined at 800°C (thus subjected to heating step, paragraph [0127]). Thus, Puppe teaches the claimed “Nanoparticles of the type A2-xO3:Lnx, wherein A is one or more of yttrium, scandium, aluminium, gallium, or a lanthanide; Ln is at least one lanthanide; and 0<x<2, which have been obtained by:- providing a first mixture comprising at least a salt of A, a salt of Ln, and a solvent, - providing a second mixture comprising a precipitating agent and a solvent,- contacting said first mixture with said second mixture in a microjet reactor process to obtain a third mixture comprising nanoparticles, and - subjecting said nanoparticles to a heating step.”
Regarding claim 17, Puppe teaches the nanoparticles of claim 16. Furthermore, Puppe uses europium (Eu3+) as a dopant/lanthanide in example 3. Thus, Puppe teaches the claimed “The nanoparticles of claim 16, wherein:- the Ln comprises an ion chosen from the group of Tb3+, Eu3+ and Ce3+, and/or - the nanoparticles comprise active ions disposed in a host lattice”.
Claims 2 and 7 are rejected under 35 U.S.C. 103 as being unpatentable over Puppe et al as applied to claim 1 above, and further in view of Kudryashova et al (NPL: "Synthesis of Yttrium-Aluminum Garnet Using a Microreactor with Impinging Jets").
Regarding claim 2, Puppe teaches the method of claim 1 but does not specifically teach nanoparticles of type A13A25O12:Ln. Puppe provides Europium as Ln in example 3. Puppe broadly teaches other elements that can compose the nanoparticles which overlap with identities of A1 and A2 as claimed (paragraph [0047]) and possible inorganic nanoparticles that are aluminum oxides (paragraph [0071]). In an analogous microjet reactor process (microreactor with impinging jets), Kudryashova teaches preparation of yttrium-aluminum garnet (YAG, Y3Al5O12) nanoparticles with parallel steps to that of Puppe without provision of the doping ion/lanthanide. It would have been prima facie obvious to one of ordinary skill in the art, as of the effective filing date, to prepare the YAG nanoparticles of Kudryashova using the method of Puppe with addition of a dopant as dopants are known to improve luminescent properties and as a known alternative luminescent nanoparticle (YAG) having a stable crystal structure, increased radiation resistance, and resistance to oxidation as taught by Kudryashova and arrive at the invention as claimed. Thus, Puppe and Kudryashova teach the claimed “The method of claim 1, wherein Ln is chosen from the group consisting of europium, terbium, or cerium, and/or wherein the nanoparticles are of the type A13A25O12:Ln, wherein A1 is one or more selected from the group of yttrium, lutetium, and gadolinium; A2 is one or more selected from the group of aluminium, gallium, and scandium; and Ln is at least one lanthanide”.
Regarding claim 7, Puppe teaches the method of claim 1 but does not specifically teach nanoparticles of type A13A25O12:Ln. Puppe provides a weakly basic precipitating agent in the second mixture (thus pH above 7) and that the sols obtained in the process (paragraph [0096]) are slightly alkaline and preferably have a pH of 7-12 or 7-10, both of which overlap with the claimed pH ranges of second and third mixtures. Overlapping ranges have been held to present a prima facie case of obviousness over the prior art. It would have been prima facie obvious to one of ordinary skill in the art, as of the effective filing date, to select from the overlapping portion of the range as known suitable pHs proper for enabling dissolution of ions during mixing (first and second mixtures) while enabling precipitation during the precipitation step of the third mixture to arrive at the invention as claimed. Puppe broadly teaches other elements that can compose the nanoparticles which overlap with identities of A1 and A2 as claimed (paragraph [0047]) and possible inorganic nanoparticles that are aluminum oxides (paragraph [0071]). In an analogous microjet reactor process (microreactor with impinging jets), Kudryashova teaches preparation of yttrium-aluminum garnet (YAG, Y3Al5O12) nanoparticles with parallel steps to that of Puppe without provision of the doping ion/lanthanide. It would have been prima facie obvious to one of ordinary skill in the art, as of the effective filing date, to prepare the YAG nanoparticles of Kudryashova using the method of Puppe with addition of a dopant as dopants are known to improve luminescent properties and as a known alternative luminescent nanoparticle (YAG) having a stable crystal structure, increased radiation resistance, and resistance to oxidation as taught by Kudryashova and arrive at the invention as claimed. Thus, Puppe and Kudryashova teach the claimed “The method of claim 1, wherein the nanoparticles are of the type A13A25O12:Ln, wherein Al is one or more selected from the group of yttrium, lutetium, and gadolinium; A2 is one or more selected from the group of aluminium, gallium, and scandium; and Ln is at least one lanthanide, and wherein:- the pH of the second mixture is between 7 and 9, and/or - the pH of the third mixture is between 6 and 9”.
Claim 8 is rejected under 35 U.S.C. 103 as being unpatentable over Puppe et al as applied to claims 1 and 8 above, and further in view of Pharmaceutical Technology Editors (cited NPL news article).
Puppe teaches the method of claim 1 and the secondary limitation of claim 8. Puppe does not specify a nozzle size for the microjet reactor. Puppe does teach use of a MicroJet reactor which can be used for their microreactor process. In the news article provided by Pharmaceutical Technology Editors, the MJR PharmJet uses nozzles with sizes between 50-1200µm, thus overlapping with the claimed range between 200-300µm. The news article teaches that particle size and particle size distribution are controlled with variation of production parameters such as nozzle size. “The combination of the nozzle size and flow rate determines the mixing velocity of the two phases, which affects the particle size”. It would have been prima facie obvious to one of ordinary skill in the art, as of the effective filing date, to modify the nozzle size in the microjet reactor of Puppe, as informed by Pharmaceutical Technology Editors, to have a sufficient nozzle size within the overlapping ranges, as such a value represents an optimization of a result-effective variable (i.e. nanoparticle size and size distribution) for use in preparing luminescent nanoparticles and arrive at the invention as claimed. Thus, Puppe and Pharmaceutical Technology Editors teach the claimed “The method of claim 1, wherein the microjet reactor has a nozzle size of between 200 and 300 µm, and/or wherein the first mixture and the second mixture are separately fed into the microjet reactor”.
Claim 10 is rejected under 35 U.S.C. 103 as being unpatentable over Puppe et al as applied to claim 1 above, and further in view of Matsumura et al (WO2012081411A1).
Puppe teaches the method of claim 1 but does not teach a protective matrix. Matsumura similarly teaches preparation of luminescent phosphors which include those of Y2O3:Eu type (thus analogous to Puppe). In Matsumura’s production of nanoparticles, the nanoparticles are condensed in the presence of a polymer dispersant salt that act as a protective colloid (thus protective matrix) in a solvent. Matsumura teaches that such a protective colloid can be used as long as it “acts as a protective colloid in a solvent” thus suggesting protection of the nanoparticles against environmental conditions. It would have been prima facie obvious to one of ordinary skill in the art, as of the effective filing date, to include a polymer dispersant and salt with nanoparticles in the heating step of Puppe to function as a protective colloid in a solvent, as informed by Matsumura, and protect the nanoparticles against degradation and arrive at the invention as claimed. Thus, Puppe and Matsumura teach the claimed “The method of claim 1, wherein said heating comprises heating a mixture comprising the nanoparticles and a protective matrix”.
Conclusion
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/NWFG/Examiner, Art Unit 1759
/MELVIN C. MAYES/Supervisory Patent Examiner, Art Unit 1759
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