throbber
Umicore AG & Co. KG
`Exhibit 1009
`Page 1 of 389
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`Umicore AG & Co. KG
`Exhibit 1009
`Page 2 of 389
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`Exhibit 1009
`Page 3 of 389
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`Umicore AG & Co. KG
`Exhibit 1009
`Page 4 of 389
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`Umicore AG & Co. KG
`Exhibit 1009
`Page 5 of 389
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`Exhibit 1009
`Page 6 of 389
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`Umicore AG & Co. KG
`Exhibit 1009
`Page 7 of 389
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`Umicore AG & Co. KG
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`Page 8 of 389
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`Page 9 of 389
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`Umicore AG & Co. KG
`Exhibit 1009
`Page 10 of 389
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`Umicore AG & Co. KG
`Exhibit 1009
`Page 11 of 389
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`Umicore AG & Co. KG
`Exhibit 1009
`Page 12 of 389
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`Exhibit 1009
`Page 13 of 389
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`Umicore AG & Co. KG
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`Page 14 of 389
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`Umicore AG & Co. KG
`Exhibit 1009
`Page 15 of 389
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`Umicore AG & Co. KG
`Exhibit 1009
`Page 16 of 389
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`Umicore AG & Co. KG
`Exhibit 1009
`Page 17 of 389
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`Umicore AG & Co. KG
`Exhibit 1009
`Page 18 of 389
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`Umicore AG & Co. KG
`Exhibit 1009
`Page 19 of 389
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`Umicore AG & Co. KG
`Exhibit 1009
`Page 20 of 389
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`Umicore AG & Co. KG
`Exhibit 1009
`Page 21 of 389
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`

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`Patent Owner's Response Under 37 CPR 1.941
`Reexamination Control No. 95/001,453
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`applicable to each of the rejections discussed in Section VI. E. 1-9 below and to new claims 39-55.
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`In addition, in Section IX., evidence is presented pertaining to secondary considerations, which is
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`applicable to each of the rejections discussed in Section VI. E. below and to new claims 39-55.
`1. Rejection of Claim 1 Over Yuen
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`The Office Action alleges that U.S. Patent Application Publication No.2006/0115403 (Yuen)
`
`teaches a process for the reduction of oxides of nitrogen contained in a gas stream comprising
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`contacting a molecular sieve having a CHA crystal structure and having a mole ratio of greater than
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`50 to 1500 of (1) an oxide selected from silicon oxide, germanium oxide or mixtures thereof to (2)
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`an oxide selected from aluminum oxide, iron oxide, titanium oxide, gallium oxide or mixtures
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`thereof. The Office Action further alleges that the molecular sieve described in Yuen can contain a
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`metal or metal ions within or on it which are capable of catalyzing the reduction of nitrogen oxides.
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`The Office Action cites to Example 3 in Yuen as providing a molecular sieve CHA having a silica to
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`alumina ratio of 166. The Office Action admits that CHAin Example 3 differs from the subject
`
`matter of claim 1 in that Example 3 does not contain copper. The Office relies on Yuen's
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`incorporation by reference in <JI 0034 of Ritscher as basis "that the catalyst of Yuen can be used in a
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`process including the reduction of oxides of nitrogen wherein an effective amount of catalytic copper
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`metal or copper ions is included within or on the zeolite." The basis of this rejection is respectfully
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`traversed.
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`a) Scope and Content of the Prior Art
`
`1.
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`No Reasons Given As to Why Yuen Example 3 is Of Interest
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`With regard to Yuen, absent consideration of varying weight percentages of oxide (1) and
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`oxide (2), there are three possibilities for oxide (1) and fourteen possibilities for oxide (2). In
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`addition, Yuen lists eleven different metals or metal ions and combinations thereof that can be
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`contained within or on the zeolite. Taking into account the different combinations of these eleven
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`metals together with the various combinations of oxide (1) and oxide (2), there are nearly three
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`thousand possible materials, taking into account only binary metal combinations, having the CHA
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`crystal structure described that may be capable of catalyzing the reduction of oxides of nitrogen.
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`See, Haller Decl. <JI 11; Olson Decl. <JI 8. Yuen discusses that the materials described can be used for
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`the "reduction of oxides of nitrogen in a gas stream" in an internal combustion engine, and this
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`statement includes a variety of reactions, including adsorption, dissociation and/or oxidizing NO by
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`22
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`Umicore AG & Co. KG
`Exhibit 1009
`Page 22 of 389
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`

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`Patent Owner's Response Under 37 CPR 1.941
`Reexamination Control No. 95/001,453
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`oxygen, adsorption and/or dissociation of N02, reducing NO by the selective catalytic reduction
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`(SCR) of NO with ammonia in the presence of oxygen, reducing NO by the selective catalytic
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`reduction of NO with hydrocarbons with and without oxygen present, and reduction of NO with
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`other reducing molecules present in exhaust gas such as hydrogen, methane, or CO. The mechanism
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`and the reaction conditions of each of these reactions can vary widely, and to say that a particular
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`material such as a specific Cu zeolite, such as ZSM-5, is useful for reduction of oxides of nitrogen
`
`does not mean that the specific zeolite will be effective for each of these reaction types. See, Haller
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`Decl. <JI 8. Yuen does not specifically teach or describe the selective catalytic reduction of nitrogen
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`oxides (NOx) in the presence of a reductant such as ammonia and does not provide any examples or
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`guidance as to what parameters are important in providing an improved catalytic material having
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`hydrothermal stability. See, Olson Decl. <JI 9; Haller Dec. <JI 12.
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`From the thousands of materials and 16 working Examples described in Yuen, the Office
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`Action appears to randomly select Example 3 as a starting point to provide a zeolite having CHA
`
`crystal structure and a silica to alumina ratio greater than 15. No explanation is given for this
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`selection of Example 3 in the Office Action. See, Olson Decl. <JI 10. There is nothing pointing to or
`
`suggesting that Example 3 has any particularly good properties, especially for NOx reduction. As
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`emphasized in KSR, "it can be important to identify a reason that would have prompted a person of
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`ordinary skill in the relevant field to combine the elements in the way the claimed new invention
`
`does." 550 U.S at 401. However, no such reasoning is provided. See Esai, 533 F.3d at 1359 ("KSR
`
`assumes a starting reference point or points in the art, prior to the time of invention, from which a
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`skilled artisan might identify a problem and pursue potential solutions.") In re Yamououchi Pharm.
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`Co. v. Danbury Pharmacal, Inc., 231 F.3d 1339, 1345 (Fed. Cir. 2000) ("At the outset, Danbury did
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`not show the required motivation for selecting example 44 as a lead compound.")
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`11.
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`Yuen Incorporates by Reference a Three-Way Catalytic Process
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`The Office Action is also deficient in a lack of reasoning as to why the skilled artisan would
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`even modify the material in Example 3 of Yuen as suggested in the Office Action. The Office
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`Action apparently relies on an incorporation of reference of Ritscher, which pertains to a three-way
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`catalytic process using a mixture of alumina, a zeolite and copper metal. The Office Action states
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`that the rejection is over Yuen and not Yuen in view of Ritscher because of the incorporation by
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`reference. Regardless of how the rejection is considered, either as Yuen alone, as Yuen
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`Umicore AG & Co. KG
`Exhibit 1009
`Page 23 of 389
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`

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`Patent Owner's Response Under 37 CPR 1.941
`Reexamination Control No. 95/001,453
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`incorporating Ritscher by reference, or as Yuen in view of Ritscher, the rejection fails to establish a
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`prima facie case of obviousness.
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`At paragraph 0034, Yuen states "[o]ne example of such a process for the catalytic reduction
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`of oxides of nitrogen in the presence of a zeolite is disclosed in U.S. Pat. No. 4,297,328, issued Oct.
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`27, 1981 to Ritscher et al. which is incorporated by reference herein." Yuen appears to incorporate
`
`by reference the process of Ritscher, which is a three-way catalytic process for reducing
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`hydrocarbons, carbon monoxide and oxides of nitrogen in gasoline fueled engines. See, Zenon
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`Envtl., Inc. v. United States Filter Corp., 506 F.3d 1370, 1378-1379 (Fed. Cir. 2007). ("Based on our
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`review of the record, we disagree with the court's conclusion that the intervening patents
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`incorporated by reference, with sufficient particularity to one reasonably skilled in the art, the gas
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`distribution system disclosed in the '373 patent."). Yuen does not appear to be particularly
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`concerned or interested in copper as a metal of interest, as Yuen describes eleven possible metals
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`and metal ions to be contained on the zeolite. See, Haller Decl. <JI 13; Olson Decl. <JI 12.
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`b)
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`Differences Between the Art and the Claimed Invention
`
`1.
`
`Yuen/Ritscher Does Not Teach Cu/ Al Ratio of Claim 1
`
`Putting aside the issue of incorporation by reference, Yuen/Ritscher does not teach the Cu/ Al
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`ratio in claim 1. A close review of the Example in Ritscher reveals that the catalyst is a mixture of
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`80% zeolite and 20% alumina containing 7.3 weight percent copper. From the information provided
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`in Ritscher, it is impossible to determine the actual copper content on the zeolite because the copper
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`is added to mixture of zeolite and alumina. See, Haller Decl. <JI 16. Accordingly, with no way to
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`know the Cu/ Al ratio in Ritscher, the Office Action fails to provide a zeolite having the CHA crystal
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`structure, a silica to alumina ratio greater than 15 and a Cu/Al ratio greater than 0.25.
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`11.
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`No Reasons are Provided to Modify Yuen's Example 3
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`Even if the amount of copper in Ritscher provided a Cu/ Al ratio of 0.25 or greater, which is
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`denied, no reasons are given or evident as to why the skilled artisan would make such modification
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`of Yuen's Example 3. See Esai, 533 F.3d at 1359 ("KSR presupposes that the record up to the time
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`of invention would give some reasons, available within the knowledge of one of skill in the art, to
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`make particular modifications to achieve the claimed compound.") It is questionable why one of
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`ordinary skill in the art would consider the copper content of Ritscher's mixture of 20% alumina and
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`80% ZSM-5 zeolite as relevant to the materials in Yuen. Each of the zeolites disclosed in Yuen has
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`Exhibit 1009
`Page 24 of 389
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`

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`Patent Owner's Response Under 37 CPR 1.941
`Reexamination Control No. 95/001,453
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`a different structure from CHA, and as discussed below, the structure of the zeolite of the example,
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`ZSM-5, is distinctly different from the structure of CHA. See, Olson Decl. <JI<JI 28-29. There are no
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`common composite building units between ZSM-5 and CHA structured zeolites, the pore sizes of
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`ZSM-5 and CHA zeolites are different, and ZSM-5 materials belong to a unique family of zeolites
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`called the pentasil zolites, which refer to the five member ring building unit. See, Olson Decl. <JI 30.
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`One skilled in the art would not use the information in Ritscher pertaining to different zeolite
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`structure types to modify the zeolites in Yuen having the CHA crystal structure because of these
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`differences and the unpredictability in the art. See, Olson Decl. <JI 30. There would be no expectation
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`of success in doing so. See, Haller Decl. <JI 15.
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`111.
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`Yuen/Ritscher Teaches Away
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`A person of ordinary skill in the art would not modify the zeolite in Yuen according to the
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`teachings of Ritscher for another reason-the samples in Ritscher exhibited terrible NOx conversion
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`under lean conditions. The invention of claim 1 of the '662 patent is a catalyst that exhibits
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`especially good low temperature NOx conversion and maintenance of NOx conversion upon
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`hydrothermal aging. As Dr. Haller observes, the catalyst in Ritscher is a three-way catalyst, which is
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`not designed for use in a lean operating environment. See, Haller Decl. <JI 17. It is well known that
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`three-way catalysts, which are effective for the abatement of hydrocarbons, carbon monoxide and
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`NOx in traditional gasoline powered engines, are not effective in lean burn engines such as diesel
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`engines. See, Haller Decl. <JI 8. The catalytic results of the material in Ritscher makes this clear-for
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`each of the samples tested, upon aging (4 hours in 10% H20) and under lean conditions, (Table Vat
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`column 7 of Ristscher) there was no NOx conversion. Such results would lead a person of ordinary
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`skill in the art not to modify Yuen in accordance with Ritscher, because Yuen was seeking a catalyst
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`for reducing nitrogen oxides in excess oxygen (lean conditions). See, Haller Decl. <JI 17. In
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`accordance with KSR, when the prior art teaches away from combining elements from the prior art,
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`an invention is more likely to be nonobvious. 550 U.S. at 416.
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`c)
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`Conclusion-Claim 1 is Not Obvious Over Yuen
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`In view of the above, it is clear that the skilled artisan seeking to make an improved catalyst
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`that has good low temperature NOx conversion and that maintains good NOx conversion upon
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`hydrothermal aging for use as an SCR catalyst used under lean conditions would not arrive at the
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`invention of claim 1 from Yuen. Yuen provides no guidance as to what elements are important to
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`Umicore AG & Co. KG
`Exhibit 1009
`Page 25 of 389
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`

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`Patent Owner's Response Under 37 CPR 1.941
`Reexamination Control No. 95/001,453
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`provide a catalyst having high NOx conversion, let alone high NOx conversion at low temperatures.
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`There are thousands of possibilities in Yuen. See Esai, 533 F.3d at 1359 ("the Supreme Court's
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`analysis in KSR presumes that the record before the time of invention would supply some reasons for
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`narrowing the prior art universe to a "finite number of identified, predictable solutions.") In addition,
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`Yuen fails to teach or suggest all of the elements of claim 1 because the Cu/ Al ratio is ambiguous in
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`Ritscher. Moreover, a person of ordinary skill in the art would not combine the teachings in Yuen
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`with information in Ritscher pertaining copper on or within ZSM-5 zeolites because the materials are
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`different and the art is unpredictable, especially when different zeolites with different structure types
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`are considered. See id, (" To the extent an art is unpredictable, as the chemical arts often are, KSR's
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`focus on these "identified predictable solutions" may present a difficult hurdle because potential
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`solutions are less likely to be genuinely predictable.") Finally, Yuen/Ritscher teaches away from the
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`invention defined by claim 1, because the Examples in Ritscher exhibit zero NOx conversion upon
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`hydrothermal aging and under lean conditions. Withdrawal of the rejection is respectfully requested.
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`2. Rejection of Claims 1-11 Over Zones in view of Ishihara, as evidenced by the Centi
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`Declaration
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`In the Office Action, claims 1-11 are rejected as allegedly being obvious over Zones in view
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`of Ishihara as evidenced by the Centi Declaration. These rejections are respectfully traversed.
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`a) Scope and Content of the Prior Art
`
`1.
`
`Zones
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`Like the selection of Yuen in the rejection of claim 1 discussed above, the Office Action
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`selects Zones among numerous other references that disclose the utility of various zeolites that can
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`be used for the abatement of oxides of nitrogen. The Centi Declaration is relied upon in the rejection
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`over Zones in view of Ishihara. However, the Centi Declaration hardly makes a compelling case for
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`the selection of the materials in Zones among the many other zeolites that were available in the art as
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`a starting point for the improved reduction of nitrogen oxides. The Centi Declaration merely states:
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`"a person of ordinary skill that was aware of both the Zones '644 patent and Ishihara would have had
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`a reasonable expectation that loading the chabazite zeolite described in Zones '644 patent using the
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`ion-exchange method described in Ishihara would have resulted in a copper chabazite zeolite that
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`would be effective at the conversion of NO to nitrogen."
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`Umicore AG & Co. KG
`Exhibit 1009
`Page 26 of 389
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`

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`Patent Owner's Response Under 37 CPR 1.941
`Reexamination Control No. 95/001,453
`
`a.
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`Scope and Content of Zones
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`Reduction of Nitrogen Oxides
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`The statement quoted immediately above from Dr. Centi's declaration that modified materials
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`of Zones "would have resulted in a copper chabazite zeolite that would be effective at the conversion
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`of NO to nitrogen" could be made for a wide variety of the almost 200 framework types of zeolites if
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`copper or some other promoter metal was exchanged into the zeolite. See, Haller Decl. <JI 18, 20. As
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`noted by Dr. Haller in his Declaration, the more important question is why would a person of skill in
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`the art select one of the many zeolites available at the time of the '662 patent filing, and then choose
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`the selected silica to alumina ratio and then further choose the amount of copper among the various
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`other metal ions (iron, cobalt, nickel, cerium, etc.) that promote the reduction of oxides of nitrogen?
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`See, In re May, 574 F.2d 1082, 1093 (C.C.P.A. 1978) ("Thus, merely because those skilled in the art
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`would have expected the compound of claim 11 to have analgesic activity, does not mean, as the
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`board apparently suggests, that an irrebuttable presumption of obviousness has been established.
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`Those properties which would have been expected must be balanced against the unexpected
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`properties.")
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`Like Yuen discussed above, Zones merely teaches that a zeolite having the CHA structure
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`can be used for the reduction of oxides of nitrogen in excess oxygen. This description can include
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`several different reactions. See, Haller Decl. <JI 8; Olson Decl. <JI 16. As noted in Dr. Zones'
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`declaration, the Zones patent does not specifically disclose or suggest that the zeolite having the
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`CHA structure is useful for selective catalytic reduction of oxides of nitrogen in the presence of a
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`reductant, and the Zones patent does not disclose any data pertaining to NOx reduction or suggest
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`that the CHA material is particularly good for NOx reduction at low temperatures or has good
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`hydrothermal stability compared to other zeolites. See, Zones Decl. <JI 8; Olson Decl. <JI 16. There are
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`patents published before the filing date of the '662 patent to at least twenty other structure types of
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`zeolites naming Dr. Zones and other researchers at Chevron, all of which stated a utility for reducing
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`oxides of nitrogen. In fact, as Dr. Zones notes, many of these patents contain language that is
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`identical or very similar to the statement in the Zones patent, namely that the "zeolite may contain a
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`metal or metal ions (such as cobalt, copper or mixtures thereof) capable of catalyzing the reduction
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`of the oxides of nitrogen, and may be conducted in the presence of a stoichiometric excess of
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`oxygen." See, Zones Decl. <JI 9; Olson Decl. <JI 17. This appears to be a common practice when a new
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`Umicore AG & Co. KG
`Exhibit 1009
`Page 27 of 389
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`

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`Patent Owner's Response Under 37 CPR 1.941
`Reexamination Control No. 95/001,453
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`zeolite is discovered, as a variety of other potential uses besides reduction of nitrogen oxides are
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`disclosed. See, Olson Decl. <JI 15; Haller Decl. <JI 19; Zones Decl. <JI 7-9.
`
`As Dr. Centi has noted, from the time period of 1999 to 2009, a search of journals and review
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`articles for the terms "zeolite and nitrogen oxides" located 1270 publications containing both terms,
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`and that despite the large variety of zeolites studied including identification of active sites and
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`reaction mechanisms in zeolites, as of 2010, the complexity of the problem has resulted in the
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`limited transferability of these studies to the development of improved catalysts. See, Olson
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`Decl. <JI 7, citing Centi et al., Environmental Catalysis Over Zeolites, in Zeolites and Catalysis, Vol.
`
`1, (2010). While it is observed that the time period of 1999 to 2009 extends past the filing date of
`
`the '662 patent, this information is provided as evidence that many zeolites promoted with a metal
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`will exhibit some NOx reduction activity and that there were well over 1000 studies conducted in a
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`10 year period on NOx reduction and zeolites. However, even as of 2010, it was concluded that
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`because of the complexity in the science of zeolites and nitrogen oxides reduction, the development
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`of improved catalysts has been a difficult proposition. See, id.
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`In summary, not much can be concluded from the Zones patent with regard to its usefulness
`
`as a catalyst that exhibits especially good NOx reduction, particularly at low temperatures, and as a
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`catalyst that maintains good NOx conversion after exposure to hydrothermal conditions. Indeed, in
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`his Declaration, Dr. Zones states that the Zones patent provides no information to indicate that the
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`chabazite materials described in the Zones patent were especially good for reduction of oxides of
`
`nitrogen at low temperatures and had good hydrothermal stability. See, Zones Decl. <JI 12. No
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`reasons seemed to exist at the time of the filing date of the '662 patent to select the materials in
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`Zones as a starting point from the universe of other zeolites that were stated to be useful for NOx
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`reduction. See Esai, 533 F.3d at 1359 ("the Supreme Court's analysis in KSR presumes that the
`
`record before the time of invention would supply some reasons for narrowing the prior art universe
`
`to a "finite number of identified, predictable solutions.")
`
`Metals and Copper Content
`
`Zones is silent on an amount of copper to be used on the chabazite zeolite. Dr. Zones
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`confirms this fact in his Declaration. While the Zones patent mentions that a zeolite having the CHA
`
`crystal structure may contain a metal or metal ions (such as cobalt, copper or mixtures thereof)
`
`capable of catalyzing the reduction of oxides of nitrogen, and may be conducted in the presence of
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`Umicore AG & Co. KG
`Exhibit 1009
`Page 28 of 389
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`

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`Patent Owner's Response Under 37 CPR 1.941
`Reexamination Control No. 95/001,453
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`stoichiometric excess of oxygen at column 1, lines 61-65, there is no further discussion of an amount
`
`of copper, cobalt or combinations thereof that could be used for the reduction of oxides of nitrogen.
`
`See, Zones Decl. <JI 11; Haller Decl. <JI 20. The Request and the Office Action erroneously rely on a
`
`later passage in the Zones patent pertaining to a different catalytic reaction to provide a purported
`
`range of 0.05% to 5% by weight of copper. Dr. Zones himself notes that this range is a discussion in
`
`reference to an amount of ammonium or metal cation for a catalyst for the reduction of lower
`
`alcohols. See, Zones Decl. <JI 11; Haller Decl. <JI 20. As Dr. Zones further explains, this passage
`
`pertaining to 0.05 to 5% by weight can include metals from Groups I to VIII of the periodic table,
`
`which includes all metals in the Periodic Table. This passage makes reference to group lA metals
`
`specifically, but Group lA metals do not include copper. Furthermore, this passage should have no
`
`bearing on the passage in the '662 patent at col. 1, lines 61-65 pertaining to reduction of oxides of
`
`nitrogen, and there is no teaching in the '662 patent of the amount of copper, cobalt or mixtures
`
`thereof that can be used for a catalyst for the reduction of oxides of nitrogen. See, Zones Decl. <JI 11.
`
`In summary, there is absolutely no teaching of an amount of copper to be used in the
`
`chabazite material described in the Zones patent.
`
`b.
`
`Scope and Content of Ishihara
`
`Ishihara is a study comparing the hydrothermal stability of Cu-SAP034, a
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`silicoaluminophosphate and selective catalytic reduction (SCR) of NOx using a hydrocarbon
`
`reductant, propene. Ishihara states that the CU -SAP034 is hydrothermally stable.
`
`b)
`
`Differences Between Art and Claimed Invention
`
`1.
`
`Differences from Claims 1-11 Generally
`
`a.
`
`Zones Does Not Disclose SCR or Copper Amount
`
`As noted above, the Zones patent says nothing about catalysts for the SCR of NOx in the
`
`presence of ammonia. Zones also does not disclose an amount of copper, cobalt or mixtures thereof
`
`to provide an effective catalyst for generally reducing oxides of nitrogen.
`
`b.
`
`Ishihara's SAP0-34 is Not Similar to CHA Zeolite Having Silica to
`
`Alumina Ratio Greater Than 15
`
`The relevance of Ishihara to the claimed invention, a zeolite having the CHA crystal structure
`
`and a silica to alumina ratio greater than 15, is questionable. As explained by Dr. Haller, SAP0-34
`
`is a silicoaluminophophate having a vastly different reaction chemistry from an aluminosilicate
`
`29
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`Umicore AG & Co. KG
`Exhibit 1009
`Page 29 of 389
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`

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`Patent Owner's Response Under 37 CPR 1.941
`Reexamination Control No. 95/001,453
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`chabazite, as evidenced by the Lok article providing the results for n-butane cracking cited in Dr.
`
`Centi's Declaration submitted by the Requestor. See, Haller Decl. <JI 21. Additionally, the way in
`
`which cations are substituted into a silicoaluminophosphate is completely different than the way in
`
`which cations are substituted in an aluminosilicate zeolite having a silica to alumina ratio greater
`
`than 15. See, Haller Decl. <JI 21; Olson Decl. <JI 21. Moreover, the catalytic activity of the materials
`
`defined by the claims of the '662 patent and the materials in Ishihara are different because the
`
`properties of these two different types of materials depend not on their framework type alone, but
`
`also on the chemistry of each unique material. See, Olson Decl. <JI 21.
`
`Thus, it is doubtful that the Ishihara reference has any relevance to the catalytic properties of
`
`a zeolite having the CHA crystal structure and a silica to alumina ratio greater than 15. The Office
`
`Action inappropriately draws conclusions from the Ishihara patent that are broader than warranted.
`
`As Dr. Haller notes, the Office Action's statement "that a person of ordinary skill "at the time of the
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`priority filing of the Bull '662 patent looking to make a copper exchanged chabazite zeolite for the
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`reduction of oxides of nitrogen with the chabazite of Zones '644 patent would have been motivated
`
`to use the ion exchange technique described in Ishihara to add copper to the chabazite of Zones '644
`
`because Ishihara used and preferred SAP0-34, which is a very well known silico-aluminophosphate
`
`molecular sieve having a structure of the chabazite type." is equivalent to saying that MgO, SnAs,
`
`UC, LiH, and TiN are all chemically like NaCl because they all have the same rock salt (NaCl)
`
`crystallographic structure. See, Haller Decl. <JI 22.
`
`c.
`
`The Reaction Chemistry And Conditions in Ishihara
`
`Besides the differences noted above, Ishihara uses propene, a hydrocarbon, as a reductant in
`
`the SCR reaction. One of ordinary skill in the art would not be able to draw any conclusions
`
`regarding the usefulness of a material as a catalyst for an ammonia SCR reaction based on its
`
`catalytic activity using a hydrocarbon reductant because different reducing agents preferentially
`
`adsorb on different sites in different forms and lead to different mechanisms of action. See, Haller
`
`Decl. <JI 9. On this point, Dr. Haller concludes that "[i]t is for this reason that NO reduction by
`
`hydrocarbons and NO reduction by ammonia on Cu zeolites do not generally have parallel behavior
`
`and why using the results of hydrocarbon reduction of NO is not a good guide to NO reduction by
`
`ammonia on the same Cu zeolite, let alone for two different Cu zeolite catalysts when the structure
`
`type and/or composition of the zeolites are different." See, Haller Decl. <JI 9.
`
`30
`
`Umicore AG & Co. KG
`Exhibit 1009
`Page 30 of 389
`
`

`
`Patent Owner's Response Under 37 CPR 1.941
`Reexamination Control No. 95/001,453
`
`In addition to the different reductant, the space velocities used in the Ishihara paper are
`
`extremely low and about an order of 10 times lower than the space velocities used in automotive
`
`exhaust. This is an important consideration when interpreting the results discussed further below,
`
`because one of skill in the art would expect catalytic testing results to be better under low space
`
`velocity. See, Haller Decl. <JI 24; Olson Decl. <JI 23.
`
`d.
`
`Zones in View of Ishihara Does Not Provide the Cu/ Al Ratio in
`
`Claims 1-11
`
`Claims 1-11 require a Cu/ Al ratio of at least 0.25. While the Centi Declaration purports to
`
`state that the amount of copper in Ishihara would provide the same Cu/ Al ratio as in claims 1-11, this
`
`ignores the fundamental differences between the material of the claimed invention and
`
`silicoaluminophosphates. The Office Action provides an oversimplified analysis by merely
`
`transferring the weight percentages used on the silicoaluminophosphate materials in Ishihira to the
`
`aluminosilicate zeolites having a silica to alumina ratio greater than 15 in Zones. The invention
`
`defined in claims 1-11 states a Cu/ Al ratio. If the person of ordinary skill in the art considered
`
`Ishihara's study of interest, which is denied, Dr. Haller concludes that the Cu/ Al ratios of the
`
`materials in Ishihara have Cu/Al ratios in the range of 0.04 to 0.13, which are far outside the ranges
`
`in claims 1-11. See, Haller Decl. <JI 23.
`
`Thus, even if the skilled artisan ignored all of the above reasons as to why there is no basis to
`
`combine Ishihara and Zones, their combined teachings would not meet the invention defined in
`
`claims 1-11 because the Cu/ Al ratio would be well below the claimed ranges in claims 1-11.
`
`e.
`
`Zones In View of Ishihara Teaches Away
`
`Even if a person of ordinary skill in the art considered the teachings of Ishihara relevant to
`
`catalyst material of claims 1-11 of the '662 patent, after reviewing the catalytic results in Ishihara, a
`
`person of ordinary skill in the art would be discouraged from using a Cu-SAP034 material having
`
`the CHA crystal structure for SCR of NOx. This is because the low temperature activity of the Cu(cid:173)
`
`SAP034 material is low to negligible. As shown in Ishihara Figure 5a, after aging at 800° C in 3%
`
`H20 the Cu SAP0-34 shows a mere 5% NOx conversion at 200° C, which is extremely poor
`
`conversion. Similarly, the NOx conversion at 250° Cis merely 5% after aging at 800° C in 3% H20,
`
`and at 300° C, the conversion is approximately 8%. At 350° C, the NOx conversion after aging at
`
`800° C in 3% H20 is approximately 14%. Compared to the fresh samples shown in Figure 1 of
`
`31
`
`Umicore AG & Co. KG
`Exhibit 1009
`Page 31 of 389
`
`

`
`Patent Owner's Response Under 37 CPR 1.941
`Reexamination Control No. 95/001,453
`
`Ishihara, the decline in NOx conversion at 300° C was approximately 73%. See, Olson Decl. <JI 23.
`
`These low results must be taken into consideration of the operating conditions, namely a low space
`
`velocity and milder hydrothermal aging conditions that the Examples in the '662 patent, both of
`
`which would be expected to provide higher catalytic activity compared to the '662 patent where the
`
`space velocity was almost 10 times higher and the aging conditions were more severe. See, Olson
`
`Decl. <JI 23; Haller Decl. <JI 24.
`
`Thus, by proceeding with the faulty reasoning in the Office Action to combine Zones and
`
`Ishihara, one of ordinary skill in the art would be discouraged from using the materials in Ishihara
`
`having the chabazite crystal structure because the catalytic performance at low temperatures and
`
`maintenance of NOx conversion after aging were both very poor. This is not only recognized by Dr.
`
`Haller and Dr. Olson, but also in the open literature. See MH Kim et al., Water Tolerance of DeNOx
`
`SCR Catalysts Using Hydrocarbons: Findings, Improvements and Challenges, Korean J. Chern Eng.
`
`18 (5) 725-740, at page 736, attached as Exhibit E to Dr. Olson's Declaration. The same authors also
`
`noted the unpredictability in the art, stating that "no single cause can elucidate the catalyst
`
`deactivation by water for the reduction of NO by HCs.lt varies with the catalyst, the reductant
`
`and the operating condition employed for the reduction." See, id.
`
`11.
`
`Claims 2-11 Are Also Not Obvious over Zones in View of Ishihara
`
`For the reasons provided above, claims 2-11 are not obvious over Zones in view of Ishihara.
`
`Claim 2
`
`Claim 2 is directed to a catalyst with the mole ratio of silica to alumina from about 15 to
`
`about 256 and the atomic ratio of copper to aluminum is from about 0.25 to about 0.50. Zones in
`
`view of Ishihara fails to provide motivation to make a catalyst with these specific ratios of silica to
`
`alumina and copper to aluminum. As discussed above, the Cu/ Al ratios in Ishihara are well outside
`
`this range.
`
`Claim 3
`
`Claim 3 further specifies that the mole ratio of silica to alumina is from about 25 to about 40.
`
`Again, Zones in view of Ishihara fails give information directing a person skilled in the art to
`
`provide catalyst with these specific ratios of silica to alumina and copper to aluminum as in claim 2
`
`discussed above.
`
`32
`
`Umicore AG & Co. KG
`Exhibit 1009
`Page

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