Umicore AG & Co. KG
`Exhibit 1009
`Page 1 of 303
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`Umicore AG & Co. KG
`Exhibit 1009
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`Umicore AG & Co. KG
`Exhibit 1009
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`Umicore AG & Co. KG
`Exhibit 1009
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`Umicore AG & Co. KG
`Exhibit 1009
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`Umicore AG & Co. KG
`Exhibit 1009
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`Umicore AG & Co. KG
`Exhibit 1009
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`Umicore AG & Co. KG
`Exhibit 1009
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`Umicore AG & Co. KG
`Exhibit 1009
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`Umicore AG & Co. KG
`Exhibit 1009
`Page 10 of 303
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`Umicore AG & Co. KG
`Exhibit 1009
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`Umicore AG & Co. KG
`Exhibit 1009
`Page 12 of 303
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`Umicore AG & Co. KG
`Exhibit 1009
`Page 13 of 303
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`Umicore AG & Co. KG
`Exhibit 1009
`Page 14 of 303
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`Umicore AG & Co. KG
`Exhibit 1009
`Page 15 of 303
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`Umicore AG & Co. KG
`Exhibit 1009
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`Umicore AG & Co. KG
`Exhibit 1009
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`Umicore AG & Co. KG
`Exhibit 1009
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`

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`Application/Control Number: 12/480,360
`Art Unit: 1793
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`Page 3
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`Applicant should note that documents not in the English language have been
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`considered only to the extent of statements of relevance, explanations provided in the
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`corresponding search reports provided and provided translations.
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`Claim Rejections - 35 USC § 112
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`The following is a quotation of the first paragraph of 35 U .S.C. 112:
`
`The specification shall contain a written description of the invention, and of the manner and process of
`making and using it, in such full, clear, concise, and exact terms as to enable any person skilled in the
`art to which it pertains, or with which it is most nearly connected, to make and use the same and shall
`set forth the best mode contemplated by the inventor of carrying out his invention.
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`Claims 33-43 are rejected under 35 U.S.C. 112, first paragraph, as failing to
`
`comply with the written description requirement. The claim(s) contains subject matter
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`which was not described in the specification in such a way as to reasonably convey to
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`one skilled in the relevant art that the inventor(s), at the time the application was filed,
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`had possession of the claimed invention. This is a new matter rejection.
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`Claims 33- 43 recite reduction of oxides of nitrogen in the presence of "a
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`catalyst comprising a zeolite having the CHA crystal structure promoted with sufficient
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`copper to prevent thermal degradation .... ".
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`This recitation is not supported by the originally filed specification. A thorough
`
`reading of the specification indicates that a CuCHA zeolite such as that set forth in claim
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`20 which is further promoted with an amount of free copper results in the prevention of
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`hydrothermal degradation. Paragraph 12 recites such a catalyst. The examples
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`compare such catalyst to the exchanged CuCHA zeolite that does not contain "free"
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`copper. Paragraph [0041] recites that the SCR catalyst is formed from a Cu exchanged
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`zeoltie having free copper in addition to ion-exchanged copper.
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`Umicore AG & Co. KG
`Exhibit 1009
`Page 19 of 303
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`

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`Application/Control Number: 12/480,360
`Art Unit: 1793
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`Page 4
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`In view of the foregoing, it is considered that the applicant did not have
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`possession of the claimed process taking place in the presence of a material that is only
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`a CHA zeolite promoter with sufficient copper to prevent thermal degradation.
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`Claim Rejections- 35 USC§ 103
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`The following is a quotation of 35 U.S.C. 1 03(a) which forms the basis for all
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`obviousness rejections set forth in this Office action:
`
`(a) A patent may not be obtained though the invention is not identically disclosed or described as set
`forth in section 102 of this title, if the differences between the subject matter sought to be patented and
`the prior art are such that the subject matter as a whole would have been obvious at the time the
`invention was made to a person having ordinary skill in the art to which said subject matter pertains.
`Patentability shall not be negatived by the manner in which the invention was made.
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`The factual inquiries set forth in Graham v. John Deere Co., 383 U.S. 1, 148
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`USPQ 459 (1966), that are applied for establishing a background for determining
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`obviousness under 35 U.S.C. 103(a) are summarized as follows:
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`1.
`2.
`3.
`4.
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`Determining the scope and contents of the prior art.
`Ascertaining the differences between the prior art and the claims at issue.
`Resolving the level of ordinary skill in the pertinent art.
`Considering objective evidence present in the application indicating
`obviousness or nonobviousness.
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`This application currently names joint inventors. In considering patentability of
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`the claims under 35 U.S.C. 1 03(a), the examiner presumes that the subject matter of
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`the various claims was commonly owned at the time any inventions covered therein
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`were made absent any evidence to the contrary. Applicant is advised of the obligation
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`under 37 CFR 1 .56 to point out the inventor and invention dates of each claim that was
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`not commonly owned at the time a later invention was made in order for the examiner to
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`consider the applicability of 35 U.S.C. 1 03(c) and potential 35 U.S.C. 1 02(e), (f) or (g)
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`prior art under 35 U.S.C. 1 03(a).
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`Umicore AG & Co. KG
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`Umicore AG & Co. KG
`Exhibit 1009
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`Umicore AG & Co. KG
`Exhibit 1009
`Page 22 of 303
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`Umicore AG & Co. KG
`Exhibit 1009
`Page 23 of 303
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`Umicore AG & Co. KG
`Exhibit 1009
`Page 24 of 303
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`Umicore AG & Co. KG
`Exhibit 1009
`Page 25 of 303
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`Umicore AG & Co. KG
`Exhibit 1009
`Page 26 of 303
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`Umicore AG & Co. KG
`Exhibit 1009
`Page 27 of 303
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`Umicore AG & Co. KG
`Exhibit 1009
`Page 28 of 303
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`Umicore AG & Co. KG
`Exhibit 1009
`Page 29 of 303
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`Umicore AG & Co. KG
`Exhibit 1009
`Page 30 of 303
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`Umicore AG & Co. KG
`Exhibit 1009
`Page 31 of 303
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`Umicore AG & Co. KG
`Exhibit 1009
`Page 32 of 303
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`Umicore AG & Co. KG
`Exhibit 1009
`Page 33 of 303
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`Umicore AG & Co. KG
`Exhibit 1009
`Page 34 of 303
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`Umicore AG & Co. KG
`Exhibit 1009
`Page 35 of 303
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`Umicore AG & Co. KG
`Exhibit 1009
`Page 36 of 303
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`Umicore AG & Co. KG
`Exhibit 1009
`Page 37 of 303
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`Umicore AG & Co. KG
`Exhibit 1009
`Page 38 of 303
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`Umicore AG & Co. KG
`Exhibit 1009
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`Umicore AG & Co. KG
`Exhibit 1009
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`Umicore AG & Co. KG
`Exhibit 1009
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`Umicore AG & Co. KG
`Exhibit 1009
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`Umicore AG & Co. KG
`Exhibit 1009
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`Umicore AG & Co. KG
`Exhibit 1009
`Page 44 of 303
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`Umicore AG & Co. KG
`Exhibit 1009
`Page 45 of 303
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`Umicore AG & Co. KG
`Exhibit 1009
`Page 46 of 303
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`

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`AMENDMENT AND RESPONSE UNDER 37 C.F.R. § 1.114
`Serial Number: 12/480.360
`Filing Date: June 8. 2009
`Title: Copper CHA Zeolite Catalysts
`
`Docket No.: EH5328A
`
`CHA crystal structure and non-exchanged copper to prevent thermal degradation. The
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`application amply supports claims 47 and 48, as an amount of non-exchanged copper is not
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`essential to practice of the invention, but merely provides "enhanced" by non-exchanged copper.
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`See Patchett Declaration, <JI 8.
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`Secondary Considerations
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`While it is maintained that based on the above remarks, the Final Office Action has failed
`
`to establish a prima facie case of obviousness, it is respectfully submitted the secondary
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`considerations further weigh in favor patentability of the claims in the instant application.
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`In
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`Graham, the Supreme Court stated that "secondary considerations as commercial success, long
`
`felt but unsolved needs, failure of others, etc., might be utilized to give light to the circumstances
`
`surrounding the origin of the subject matter sought to be patented. As indicia of obviousness or
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`nonobviousness, these inquiries may have relevancy." See Graham, 383 U.S. at 17-18. Thus,
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`objective evidence of secondary considerations must be considered in making an obviousness
`
`decision. See Stratoflex, Inc. v. Aeroquip Corp., 713 F.2d 1530, 1538-39 (Fed. Cir. 1983). Any
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`initial obviousness determination is reconsidered anew in view of the proffered evidence of
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`nonobviousness. See In re Rinehart, 531 F.2d 1048, 1052 (CCPA 1976); In re Eli Lilly & Co.,
`
`902 F.2d 943, 945 (Fed. Cir. 1990).
`
`The attached Roth Declaration shows that pnor to the present invention, there was
`
`skepticism by experts that Cu-zeolites could be used to remediate NOx in diesel engines. In
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`2005, Dr. Roth, in his capacity as research group leader for NOx control catalysts at Engelhard
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`Corporation (the predecessor in interest to the assignee of the instant application) attempted to
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`secure a Department of Energy (DOE) funding for a proposal to study Cu-zeolites for SCR o
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`24
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`Umicore AG & Co. KG
`Exhibit 1009
`Page 47 of 303
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`

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`AMENDMENT AND RESPONSE UNDER 37 C.F.R. § 1.114
`Serial Number: 12/480.360
`Filing Date: June 8. 2009
`Title: Copper CHA Zeolite Catalysts
`
`Docket No.: EH5328A
`
`NOx. However, the experts at the DOE concluded that Cu-exchanged zeolites lack the
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`hydrothermal stability needed to be commercially viable for SCR of NOx with ammonia for
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`diesel engines. Roth Declaration, <JI 6. In fact, Dr. Roth was told that several reviewers and the
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`DOE grant manager felt Cu zeolites were far too unstable to be commercially feasible. Roth
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`Declaration, <JI 7. The DOE further stated that "several other investigators who are presumable
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`experts in the area" were equally skeptical about the prospects of using Cu zeolites for SCR of
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`NOx in diesel engines. Roth Declaration, <JI 8. Such expressions of skepticism and disbelief by
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`experts is strong evidence of non-obviousness. See Environmental Designs, Ltd. v. Union Oil
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`Co-., 713 F. 2d 693, 698 (Fed. Cir. 1983), cert. denied, 464 U.S. 1043 (1984) ("Expressions of
`
`disbelief by experts constitute strong evidence of nonobviousness. United States v. Adams, 383
`
`U.S. 39, 52, 15 L. Ed. 2d 572, 86 S. Ct. 708 (1966).").
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`The Roth Declaration also provides evidence of long-felt need. As explained in the Roth
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`Declaration, the very recent literature, recognizing the excellent results provided by the instant
`
`invention have called the problem of NOx reduction in lean burn engines such as diesel engines
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`"daunting." Roth Declaration, <JI 10. At the time of the invention, impending Tier 2 Bin 5
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`standards were requiring higher NOx conversion, which the authors at Ford Motor Company
`
`recognized as "especially challenging" for temperatures in the range of 200° to 350° C. While
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`there were Cu/zeolite catalysts that delivered fresh performance, their performance degraded
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`over time as a result of high temperature deactivation. Roth Declaration, <JI 11. The present
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`invention satisfied a long-standing need, and the Ford Motor Company researchers indicated that
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`the material used in the process of the present invention was a "remarkable" Cu/zeolite that
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`showed high NOx conversion in the low temperature range. Roth Declaration, <JI 11. The instant
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`25
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`Umicore AG & Co. KG
`Exhibit 1009
`Page 48 of 303
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`Umicore AG & Co. KG
`Exhibit 1009
`Page 49 of 303
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`Umicore AG & Co. KG
`Exhibit 1009
`Page 50 of 303
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`Umicore AG & Co. KG
`Exhibit 1009
`Page 51 of 303
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`Umicore AG & Co. KG
`Exhibit 1009
`Page 52 of 303
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`Umicore AG & Co. KG
`Exhibit 1009
`Page 53 of 303
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`Umicore AG & Co. KG
`Exhibit 1009
`Page 54 of 303
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`Umicore AG & Co. KG
`Exhibit 1009
`Page 55 of 303
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`Umicore AG & Co. KG
`Exhibit 1009
`Page 56 of 303
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`Umicore AG & Co. KG
`Exhibit 1009
`Page 57 of 303
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`Umicore AG & Co. KG
`Exhibit 1009
`Page 58 of 303
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`Umicore AG & Co. KG
`Exhibit 1009
`Page 59 of 303
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`Umicore AG & Co. KG
`Exhibit 1009
`Page 60 of 303
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`Umicore AG & Co. KG
`Exhibit 1009
`Page 61 of 303
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`Umicore AG & Co. KG
`Exhibit 1009
`Page 62 of 303
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`Umicore AG & Co. KG
`Exhibit 1009
`Page 63 of 303
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`Umicore AG & Co. KG
`Exhibit 1009
`Page 64 of 303
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`Umicore AG & Co. KG
`Exhibit 1009
`Page 65 of 303
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`Umicore AG & Co. KG
`Exhibit 1009
`Page 66 of 303
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`Umicore AG & Co. KG
`Exhibit 1009
`Page 67 of 303
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`Umicore AG & Co. KG
`Exhibit 1009
`Page 68 of 303
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`Umicore AG & Co. KG
`Exhibit 1009
`Page 69 of 303
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`Umicore AG & Co. KG
`Exhibit 1009
`Page 70 of 303
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`Umicore AG & Co. KG
`Exhibit 1009
`Page 71 of 303
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`Umicore AG & Co. KG
`Exhibit 1009
`Page 72 of 303
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`

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`AMENDMENT I RESPONSE UNDER 37 CFR § 1.111
`Serial Number: 12/480,360
`Filing Date: Jun 8, 2009
`Title: Processes For Reducing Nitrogen Oxides Using Copper CHA Zeolite Catalysts
`
`Docket:EH5328A
`
`32. (Original) The exhaust process of claim 31, wherein said diesel oxidation catalyst and
`
`catalyzed soot filter are upstream from said catalyst comprising a zeolite having the CHA crystal
`
`structure.
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`33. (Currently Amended) A SCR process for the reduction of oxides of nitrogen contained in an
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`exhaust gas stream from an internal combustion engine wherein said SCR process comprises
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`contacting the gas stream with a nitrogenous reductant and a catalyst deposited on a substrate,
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`the catalyst comprising a zeolite having the CHA crystal structure having a silica to alumina
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`mole ratio less than about 50 and promoted with sufficient copper to provide a copper to
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`aluminum atomic ratio of about 0.25 to about 0.50 including non eJcchanged copper to prevent
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`thermal, the catalyst resistant to significant degradation of ths zeolite fresh NOx conversion
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`performance of the catalyst when exposed to temperatures of at least about 600°C and high water
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`vapor environments of about 10% or more for at least about 6 hours.
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`34. (Cancelled)
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`35. (Cancelled)
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`36. (Currently Amended) The process of claim 33, wherein the zeolite contains ion eJcchanged
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`copper and an amount of non eJcchanged copper sufficient to and the catalyst maintain§. about
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`90% of fresh NOx conversion of the catalyst in an exhaust gas stream containing nitrogen oxides
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`Page 4 of23
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`Umicore AG & Co. KG
`Exhibit 1009
`Page 73 of 303
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`Umicore AG & Co. KG
`Exhibit 1009
`Page 74 of 303
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`Umicore AG & Co. KG
`Exhibit 1009
`Page 75 of 303
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`Umicore AG & Co. KG
`Exhibit 1009
`Page 76 of 303
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`Umicore AG & Co. KG
`Exhibit 1009
`Page 77 of 303
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`Umicore AG & Co. KG
`Exhibit 1009
`Page 78 of 303
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`Umicore AG & Co. KG
`Exhibit 1009
`Page 79 of 303
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`Umicore AG & Co. KG
`Exhibit 1009
`Page 80 of 303
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`

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`Umicore AG & Co. KG
`Exhibit 1009
`Page 81 of 303
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`

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`AMENDMENT I RESPONSE UNDER 37 CFR § 1.111
`Serial Number: 12/480,360
`Filing Date: Jun 8, 2009
`Title: Processes For Reducing Nitrogen Oxides Using Copper CHA Zeolite Catalysts
`
`Docket:EH5328A
`
`H\
`'Il1r~ '64-4 [Kitent does not q.:oe.c ifkally disclose or suggest that. the zeolite having the CHA
`cryst<.)l stn1c.t.u.re. is use.ful for selec:rive ..:.:atalyt.k re<.h.lction of oxides of nitrogen in the. pres-en;.~~ of
`a reductant~ such as anunonia. 'Ibere is no dioc:ussic>11, suggestion or example in the '644 patent
`indicating that a zeolite. having the CH.A crystal stniC.ture cc>11taining copper e.xb.ibitt> improved
`seh~(:tive. catalytic n·oduction of oxides of nitrogen at. temp,?.m.ttu·e.s beknv 350" C compared to
`other z.ooHte.s, or that a zeolite. having the CHi\ crys.tal structure. and containing c.oppt'r maintains.
`exce Uent conversion of oxides of nitrogen after hydrothennal aging at te.Jnperatures in e.xcess of
`6..-"iO"' C and 10%, H:::'O. I understand that many Zt.X1lite.s aJ.nta:ining c.opJpe.r and oth€::r me.t.a.ls have.
`had limited applicatioo as §elective catalytic reduction z~atalysts in diesel engines t.~.:.~ause. of
`problems rek:1.ted tn nt':ti.ntetlatit.e. fJ.f good nitrogen oxide conversion upon hydn:Jthennal exposure
`at terr1pe.rantre.s in exce.;::s of 6.:50" C
`
`As was discussed at length in the interview, all zeolites that are promoted with a promoter metal
`
`such as copper, cobalt, nickel, ceria, etc. are expect to have some activity in the reduction of
`
`oxides of nitrogen. But the question of obviousness of the presently claimed invention is not
`
`whether the claimed process would have exhibited some activity, but whether the claimed
`
`process would have excellent activity at temperatures below 350° C that is maintained after
`
`hydrothermal aging. Failure to consider the excellent attributes of the copper promoted CHA
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`materials of the present invention including excellent low temperature conversion after
`
`hydrothermal aging, resistance to poisoning from hydrocarbons and low generation (make) of
`
`N20, a greenhouse gas, fails to consider the invention as a whole.
`
`It has long been the law that ascertaining the differences between the prior art and the
`
`claims at issue requires interpreting the claim language, and considering both the invention and
`
`the prior art references as a whole. "In delineating the invention as a whole, we look not only to
`
`the subject matter which is literally recited in the claim in question ... but also to those properties
`
`of the subject matter which are inherent in the subject matter and are disclosed in the
`
`specification ... Just as we look to a chemical and its properties when we examine the
`
`obviousness of a composition of matter claim, it is this invention as a whole, and not some part
`
`of it, which must be obvious under 35 U.S.C. 103." In re Antonie, 559 F.2d 618, 620, 195 USPQ
`
`6,8 (CCPA 1977) (emphasis in original).
`
`Page 13 of23
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`Umicore AG & Co. KG
`Exhibit 1009
`Page 82 of 303
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`Umicore AG & Co. KG
`Exhibit 1009
`Page 83 of 303
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`Umicore AG & Co. KG
`Exhibit 1009
`Page 84 of 303
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`Umicore AG & Co. KG
`Exhibit 1009
`Page 85 of 303
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`Umicore AG & Co. KG
`Exhibit 1009
`Page 86 of 303
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`Umicore AG & Co. KG
`Exhibit 1009
`Page 87 of 303
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`Umicore AG & Co. KG
`Exhibit 1009
`Page 88 of 303
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`Umicore AG & Co. KG
`Exhibit 1009
`Page 89 of 303
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`Umicore AG & Co. KG
`Exhibit 1009
`Page 90 of 303
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`Umicore AG & Co. KG
`Exhibit 1009
`Page 91 of 303
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`Umicore AG & Co. KG
`Exhibit 1009
`Page 92 of 303
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`Umicore AG & Co. KG
`Exhibit 1009
`Page 93 of 303
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`Umicore AG & Co. KG
`Exhibit 1009
`Page 94 of 303
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`Umicore AG & Co. KG
`Exhibit 1009
`Page 95 of 303
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`Umicore AG & Co. KG
`Exhibit 1009
`Page 96 of 303
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`Umicore AG & Co. KG
`Exhibit 1009
`Page 97 of 303
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`Umicore AG & Co. KG
`Exhibit 1009
`Page 98 of 303
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`Umicore AG & Co. KG
`Exhibit 1009
`Page 99 of 303
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`Umicore AG & Co. KG
`Exhibit 1009
`Page 100 of 303
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`

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`IN THE UNITED STATES PATENT AND TRADEMARK OFFICE
`
`Exarniner: DIA.MOND, ALAND
`
`Group Art Unit: 3991
`
`Confirmation No: 2755
`
`)
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`)
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`)
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`)
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`)
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`)
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`In Inter Partes Reexamination of:
`
`BULLET AL
`
`Reexamination Control No. 95/001,453
`
`Patent No. 7,601,662
`
`Issued: October 13, 2009
`
`For: COPPER CB:A
`ZEOLITE CATALYSTS
`
`Mail Stol' Inter ]Joartes Reexam
`Central Reexrunination Unit
`Commissioner for Patents
`P.O. Box 1450
`Alexandria, VA 22313-1450
`
`DECLARATION OF STANLEY ROTH, ]>ItO. UNDER 37 C.F.R. § 1.132
`
`I, Stan Roth, do declare and say as follows:
`
`1. I am currently the research group leader for diesel oxidation catalysts ru1d soot filters for
`
`BASF Corporation, located in Iselin, New Jersey. In 2005, I held the position of research group
`
`leader for NOx control catalysts for Engelhard Corporation, which was subsequently acquired by
`
`BASF Corporation.
`
`2. I received a doctorate degree in Inorganic Chemistry in 1982 from University of Illinois.
`
`I have been involved in the research and development of catalysts since 1986, and since 1995 I
`
`have worked in the areas of research and development of catalysts for automotive emissions, in
`
`pruiicular diesel engines.
`
`3. I am fruniliar with United States Patent No. 7,601,662 ("the '662 patent"), which is
`
`directed to a catalyst comprising a zeolite having the CHA crystal structure, a silica to alumina
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`Umicore AG & Co. KG
`Exhibit 1009
`Page 101 of 303
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`

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`LY!ter Partes Reexamination No. 95/001,453
`Declaration of Stanley Roth, Ph.D.
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`ratio of about 15 and an atomic ratio of copper to aluminum exceeding about 0.25, with specific
`
`claims directed to silica to alumina ratios in the range of 15 to 40 and copper to aluminum ratios
`
`in the range of about 0.25 to 0.50. Such catalysts are useful fbr the abaternent of nitrogen oxides
`
`in lean bum engines such as diesel engines, particularly by selective catalytic reduction in excess
`
`oxygen in the presence of a reductant such as anm1onia.
`
`I understand that the '662 patent
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`presently under reexamination in the United States Patent and Trademark Oflice, and that all of
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`the claims have been rejected as allegedly being obvious over various cited references.
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`4. In 2005, I contacted a university professor, whom Engelhard was working with to obtain
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`Department of Energy (DOE) funding for a proposal to study Cu-zeolites for selective catalytic
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`reduction (SCR) of nitrogen oxides (NOx). Exhibit A attached hereto is a copy of the e-mail
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`correspondence with the university prof(~ssor on the DOE proposal, with the names of the
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`professor, DOE review personnel and other personnel redacted. As shown on page 7 of Exhibit
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`B, the grant proposal was wait-listed because the DOE grant rnonitor concluded that "Cu-
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`exchanged zeolites lack the hydrothem1al stability needed to be commercially viable for SCR of
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`NOx vvith ammonia for diesel engines."
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`5. After receiving the infonnation that the grant proposal had been vvait-listed, I wrote back
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`to the professor asking if the proposal could be reconsidered. The professor explained that
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`"some reviewers, and my DOE grant :riiqnager simply think Cu-exchanged zeolites are far to [sic,
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`too] unstable to water to be commercially feasible, so they do not want to fund work in the area."
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`(Exhibit A, at page 5).
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`6. After vvriting to the professor a second time, the professor quoted the DOE contact as
`
`stating:
`
`"Clarifying the vvater-stability issue, without revealing proprietary
`knowledge, would be a good point to address in a new version. I have
`
`2
`
`Umicore AG & Co. KG
`Exhibit 1009
`Page 102 of 303
`
`

`
`Inter Partes Reexamination No. 95/001,453
`Declaration of Stanley Roth, Ph.D.
`
`heard the same negative comment about the prospects for Cu-zeolites from
`several other investigators who presumably are also experts in this area.
`Thus, it is imperative to argue/present evidence that dispels such belief.
`More that the practicality of the concept, such as prospects for large-scale
`commercialization, the BES reviewers will be seeking fur the rationale
`that will lead to new/corrected mechanistic understanding underlying such
`stability (or lack thereof)."
`
`(Exhibit A, page 3 ).
`
`7. The professor further quoted one of the reviewers as stating:
`
`"The structure-property-processing relationships that the PI's describe as
`the scientific goals are meritorious and worthy of support. The PI's
`weaken their position considerably, hovvever, by emphasizing the
`technology of SCR in diesel vehides \Vhen in fact propose to study de(cid:173)
`N Ox via ammonia over Cu-exchanged mordenite. Moreover, the PI's
`completely side step the issue of catalysts deactivation in the presence of
`water; I believe this to be the primary reason why metal-exchanged
`zeolites have limited application. It is interesting to note that not a single
`metal-zeolite for SCR was commercialized in the USA in the 1990'2 (see
`John Annor, App. Cat. A, V222, page 407(2001))."
`
`(Exhibit A .. , pages 3-4).
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`8. The statements made by the DOE contact and reviewers represented the view of many
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`researchers and those skilled in the art that Cu-zeolites could not be used as catalysts for the SCR
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`of NOx because of the inability to maintain NOx conversion upon exposure to hydrotherrnal
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`conditions-namely temperatures in excess of 650° C and H20 of 10%.
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`Even the recent
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`literature, recognizing the results achieved in the '662 patent have called the problem of NOx
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`reduction in lean bum engines as "daunting". (Exhibit B, f]rst page).
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`9. The challenge before the invention of the '662 patent was to provide a zeolite materia!
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`promoted with a metal or metal ion that exhibited high NOx conversion across a wide
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`temperature range, including temperatures in the range of 200° to 350° C and that maintained
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`high NOx conversion after hydrothennal aging of temperatures above 650° C, and in some cases
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`3
`
`Umicore AG & Co. KG
`Exhibit 1009
`Page 103 of 303
`
`

`
`Inter Partes Reexamination No. 95/001,453
`Declaration of Stanley Roth, Ph.D.
`
`as high as 800° C or 900" C. The researchers at Ford summarized the problem in the research
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`paper attached as Exhibit C (first page):
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`Passenger and. light duty diesel vehicles will require up to 90% NOx
`conversion over the Federal Test Procedure (FTP) to meet future Tier 2
`Bin 5 standards. This accomplishment is especialiy challenging for low
`exhaust temperature applications that mostly operate in the 200°- 350° C
`temperature regime. Selective catalytic reduction (SCR) catalysts
`.formulated \vith Cu/zeolites have shown the potential to deliver this level
`of perfomumce fresh, but their perfom1a.nce can easily deteriorate over
`tirne as a result of high temperature thermal deactivation.
`
`10. In 2006, I am aware that Engelhard Corporation provided samples of a Cu-zeoiite having
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`the CHA crystal structure deposited on a substrate to Ford Motor Company for SCR testing, and
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`I understand that this is the material tested and described in Exhibit C, a research paper by Ford
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`Motor Company entitled "Enhanced Durability of a Cu/Zeolite Based SCR Catlayst.. As noted in
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`Exhibit C (first page), it was believed that Fe-zeolites exhibited superior hydrothermal durability
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`compared to Cu-zeolites. After testing the samples that were sent to Ford, the Ford researchers
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`concluded that the material of the '662 patent is "remarkable". (Exhibit C, last page).
`
`In past years, no reported Culzeolite SCR formulation was able to yield.
`stable low temperature NOx per.f()rnu.mce after exposure to hydrothennal
`conditions consisting of 1 hour at 950° C. Within the last year, a
`remarkable Cu./zeolite SCR formulation was identified with high NOx
`conversion in the 200° C - 350° C temperature range.
`
`11. The material claimed in the '662 patent has been sold for use as a SCR catalyst for the
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`removal of NOx in diesel engines in several different automotive manufacturer vehicle
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`platforms. The material of the '662 patent has met a long-standing and previously unfulfilled
`
`need - a metal zeolite that exhibits both excellent NOx conversion over a wide temperature
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`range, including the range of 200° to 350° C, and that maintains high conversion after exposure
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`to hydrothermal conditions. This has allowed auto~notive manufacturers to rneet increasingly
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`stringent NOx standards that went into effect in 2010.
`
`4
`
`Umicore AG & Co. KG
`Exhibit 1009
`Page 104 of 303
`
`

`
`Inter Partes Reexamination No. 95/001,453
`Declaration of Stanley Roth, Ph.D.
`
`12. The Research & Development Council ofNew Jersey has recob'11ized the inventors ofthe
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`'662 patent with the 2010 Thomas A.lva Edison Patent Award in the environmental category,
`
`which recognizes the outstanding work done by New Jersey scientists and inventors by honoring
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`the most exceptional efforts.
`
`I hereby declare that all statements made herein of my own knowledge are true and that all
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`statements made herein on infom1ation and belief are believed to be true; and further that these
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`statements were made with the knowledge that willful hllse statements and the like so made are
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`punishable by fine or imprisonment, or both, under Section 1 001 of Title 18 of the United States
`
`Code, and that such willful faise statements may jeopardize the validity of the above-identified
`
`patent.
`
`Dated: January 20, 2011
`
`By:
`
`Respectfully submitted,
`
`5
`
`Umicore AG & Co. KG
`Exhibit 1009
`Page 105 of 303
`
`

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`EXHIBITS TO DECLAR£'\TION OF STANLEY ROTH, PH.D. UNDER 37 C.F.R. § 1.132
`
`EXHIBIT A
`
`Umicore AG & Co. KG
`Exhibit 1009
`Page 106 of 303
`
`

`
`EXHIBITS TO DECLAR£'\TION OF STANLEY ROTH, PH.D. UNDER 37 C.F.R. § 1.132
`
`Stan Roth/RD/ENGELHARD
`
`09/28/2005 02:55PM
`
`To Jamesllllllllll!llllll!llllll!llllll!llllll!llllll!llllll!llllll-'i'.~i>!>
`cc
`
`Subject RE: proposal on Cu-zeolites for NOx SCRLtn)s.
`
`Jim,
`
`I have been out of the country for the past week. How did we leave this issue of your DOE proposal?
`
`From my perspective you can go ahead as planned in your memo below. Hopefully our discussion has
`been useful. You can modify your introduction to include the comparative zeolite requirements for HC(cid:173)
`SCR and NH3-SCR. Let me know if you require me to slightly modify my 2005 memo to state that
`"Preliminary experimental data shows thermal durability to 800"C"
`
`In the zeolite literature there are probably many examples of structures with hydrothermal durability to the
`700-SOO"C range. The big issue appears to be your DOE reviewers that have experience limited to the
`Cu-ZSM5 HC-SCR example, where catalytic performance quickly died after modest hydrothermal aging.
`
`I understand that you like Mordinite because it's symmetry makes calculations easier. And that many of
`your papers have concerned work on ZSM-5. Is part of the problem with your DOE proposal that you are
`stressing continual work on these zeolites?
`
`Moving forward, I would not really recommend either of these zeolites for the NH3-NOx application. Do
`we want to take our relationship to the next step, and have Engelhard supply you with samples for
`evaluation/modelling. This will of course require confidentiality/secrecy agreements, and in the past it has
`taken months to iron out all the legal implications. In cases were the University requires retention of
`patent rights, Engelhard has declined to participate in potentially useful programs. The alternative is to
`keep the relationship on an informal basis. That limits the relevance of your work to model catalyst
`systems, but also puts no limitations on publication of the results. Let me know you thoughts on this
`subject.
`
`Regards,
`Stan
`
`09/16/2005 05:05PM
`
`cc:
`Subject:
`
`RE: proposal on Cu-zeolites for NOx SCR
`
`Hi Stan,
`
`Thanks very much for the explanation.
`really clarified the issues for me.
`
`I knew part of it, but what you said
`
`I would like to go ahead and resubmit my proposal mostly as is but with more
`explanation of the stabilization issue, as that was the only major objection
`
`Umicore AG & Co. KG
`Exhibit 1009
`Page 107 of 303
`
`

`
`EXHIBITS TO DECLAR£'\TION OF STANLEY ROTH, PH.D. UNDER 37 C.F.R. § 1.132
`
`to our proposal, which otherwise was very favorably reviewed.
`
`So, my plan is to change our intro to include solrm~e~.~o~f~~~~~~~~~~·s data from
`of the I
`11111111111, and some data from (
`Institute.
`
`With your permission, I will also clarify some of the stability issues using
`the info only from your Sept 16 email, and none of your proprietary info.
`
`I would like to also ask if I could reuse the letter you had given me in
`January 2005, but with a current date?
`
`Hopefully that will be enough. The DOE really wants me to resubmit by mid(cid:173)
`September to meet their January review, so I am unfortunately being rushed in
`my revisions.
`
`Thanks again for your help!
`
`Best wishes,
`Jim
`
`James 111111111111111
`Professor
`Department of Chemical and Materials Engineering
`University
`
`(fax)
`
`-----Original Message-----
`From: Stan_Roth@engelhard. com
`[nk j_ J. t: o; .''i:.-':n ___ r-zo::.hi<:,:,nqe l ha;:·-·:1 < C()H:]
`Sent: Friday, September 16, 2005 12:38 PM
`To: James
`Stan_Roth@engelhard.com
`Cc:
`Subject: RE: proposal on Cu-zeolites for NOx SCR
`
`Jim,
`
`Thank you for these reviewer quotes.
`At last I finally understand where the objections to your proposals are
`comming from.
`
`5-10 years ago there was much effort worldwide on the reaction of HC+NOx,
`oven known as active lean NOx or HC-SCR. There are propably 500+
`literature references to this catalyst concept. There were two main types
`of catalyst used for this reaction:
`(1) Pt-ZSM5 which functioned from 180-250°C but had as it's main weakness
`that the reaction was not selective and produced predominately N20 rather
`than N2.
`(2) Cu-ZSM5 which was had an activity window from 300-500°C, did not
`produce N20, but had as it's main weaknees that the catalyst deactivated
`and could not survive extended hydrothermal treatment over 550°C. The
`mechanism of deactivation was clearly demonstrated to be loss of strong
`
`Umicore AG & Co. KG
`Exhibit 1009
`Page 108 of 303
`
`

`
`EXHIBITS TO DECLAR£'\TION OF STANLEY ROTH, PH.D. UNDER 37 C.F.R. § 1.132
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`acid sites in the zeolite