Patent Owner’s Response (IPR2015-01124)
`
`UNITED STATES PATENT AND TRADEMARK OFFICE
`
`
`
`
`
`
`
`
`BEFORE THE PATENT TRIAL AND APPEAL BOARD
`
`
`
`
`
`
`
`
`UMICORE AG & CO. KG,
`
`Petitioner,
`
`v.
`
`BASF CORPORATION
`
`Patent Owner.
`
`
`
`IPR2015-01124
`
`U.S. Patent 8,404,203
`
`
`
`PATENT OWNER’S RESPONSE TO PETITION
`FOR INTER PARTES REVIEW OF U.S. PATENT NO. 8,404,203
`
`
`
`
`
`
`
`
`
`
`
`
`
`
`
`
`
`

`
`
`
`
`
`Patent Owner’s Response (IPR2015-01124)
`
`Table of Contents
`
`I.
`II.
`
`INTRODUCTION ........................................................................................... 1
`THE 203 PATENT .......................................................................................... 6
`A. Overview of Zeolites ............................................................................. 6
`B.
`The Claimed Invention .......................................................................... 9
`C.
`Claim Construction ............................................................................. 12
`1.
`“[C]atalyst” (claim 1) ................................................................ 12
`2.
`“[Z]eolite having the CHA crystal structure” (claim 1) ........... 12
`3.
`“A process for the reduction of oxides of nitrogen
`contained in a gas stream” (claim 1) ......................................... 12
`III. SCOPE AND CONTENT OF THE PRIOR ART ......................................... 13
`A.
`The Known Problem with Metal-Exchanged Zeolites ........................ 14
`B.
`Zeolite Frameworks for the SCR of NOx ........................................... 16
`C.
`Summary of Prior Art in the IPR Grounds.......................................... 18
`1.
`U.S. 4,046,888 to Maeshima (Exhibit 1102) ............................ 18
`2.
`Dedecek (Exhibit 1107) ............................................................ 20
`3.
`U.S. 4,503,023 to Breck (Exhibit 1103) ................................... 21
`4.
`U.S. 2006/0039843 to Patchett (Exhibit 1105) ......................... 23
`IV. THE CHALLENGED CLAIMS ARE NOT OBVIOUS IN VIEW OF
`MAESHIMA, DEDECEK, BRECK AND PATCHETT 843 ....................... 24
`A. Maeshima in view of Breck (Ground 1: Claims 1, 14, 15, 19,
`20, 26, 27) ............................................................................................ 26
`B. Dedecek in view of Breck (Ground 3: Claims 1, 14, 15, 19, 20,
`26, 27) .................................................................................................. 28
`C. Maeshima and Breck in view of Patchett 843 (Ground 2:
`Claims 2–13, 16, 23–25, 28–31) ......................................................... 30
`D. Dedecek and Breck in view of Patchett 843 (Ground 4: Claims
`2–13, 16, 23–25, 28–31) ...................................................................... 34
`V. OBJECTIVE INDICIA STRONGLY SUPPORT A FINDING OF
`NONOBVIOUSNESS ................................................................................... 36
`A.
`Skepticism of Experts .......................................................................... 38
`
`i
`
`

`
`
`
`
`
`Patent Owner’s Response (IPR2015-01124)
`
`B. Unexpected Results ............................................................................. 40
`C.
`Commercial Success............................................................................ 43
`VI. PETITIONER’S CLAIMS OF PREDICTABILITY ARE WITHOUT
`MERIT ........................................................................................................... 45
`D.
`Criticality of the Claimed Ranges ....................................................... 47
`E.
`Predictability of Increasing Cu/Al Ratio ............................................. 50
`F.
`Predictability of Increasing SAR ........................................................ 52
`VII. CONCLUSION .............................................................................................. 54
`
`
`
`
`
`
`ii
`
`

`
`
`
`
`
`Exhibit 1101
`
`Exhibit 1102
`
`Exhibit 1103
`
`Exhibit 1104
`
`Exhibit 1105
`
`Exhibit 1106
`
`Exhibit 1107
`
`Exhibit 1108
`
`Exhibit 1110
`
`Exhibit 1111
`
`Exhibit 1112
`
`Exhibit 1113
`
`Exhibit 1114
`
`Exhibit 1115
`
`
`
`Patent Owner’s Response (IPR2015-01124)
`
`Petitioner’s Table of Exhibits
`
`U.S. 7,601,662
`
`U.S. 4,046,888 to Maeshima
`
`U.S. 4,503,023 to Breck
`
`U.S. 6,709,644 to Zones
`
`U.S. Pat. App. Pub. 2006/0039843 to Patchett
`
`U.S. Pat. App. Pub. 2005/0031514 to Patchett
`
`Dedecek et al., “Siting of the Cu+ Ions in Dehydrated Ion
`Exchanged Synthetic and Natural Chabasites: a Cu+
`Photoluminescence Study,” Microporous and Mesoporous
`Materials, Vol. 32, pp. 63-74 (1999).
`
`Expert Declaration of Dr. Lercher
`
`U.S. 4,961,917 to Byrne
`
`U.S. 5,516,497 to Speronello
`
`Ishihara et al., “Copper Ion-Exchanged SAPO-34 as a
`Thermostable Catalyst for Selective Reduction of NO with
`C3H6,”169 Journal of Catalysis 93-102 (1997)
`
`U.S. 4,297,328 to Ritscher
`
`Chung, S.Y. et al., “Effect of Si/Al Ratio of Mordenite and
`ZSM-5 Type Zeolite Catalysts on Hydrothermal Stability for
`NO Reduction by Hydrocarbons,” Studies in Surface Science
`and Catalysis, vol. 130, pp. 1511-1516 at 1513 (2000)
`
`Declaration of Dr. Frank-Walter Schutze
`
`
`
`
`
`iii
`
`

`
`
`
`
`
`Exhibit 2001
`
`Exhibit 2002
`
`Exhibit 2003
`
`Exhibit 2004
`
`Exhibit 2005
`
`Exhibit 2006
`
`Exhibit 2007
`
`Exhibit 2008
`
`Exhibit 2009
`
`Exhibit 2010
`
`Exhibit 2011
`
`Exhibit 2012
`
`Patent Owner’s Response (IPR2015-01124)
`
`Patent Owner’s Table of Exhibits
`
`Declaration of Stanley Roth in the Inter Partes
`Reexamination of U.S. Patent No. 7,601,662
`
`Cavataio, G., et. al., “Enhanced Durability of a Cu/Zeolite
`Based SCR Catalyst.” SAE Int. J. Fuels. Lubr., Vol. 1, Issue
`1 (2008).
`
`Declaration of Ahmad Moini in the Inter Partes
`Reexamination of U.S. Patent No. 7,601,662
`
`Second Declaration of Pramod Ravindran in the Inter Partes
`Reexamination of U.S. Patent No. 7,601,662
`
`Third Party Comments After Patent Owner’s Response After
`ACP in the Inter Partes Reexamination of U.S. Patent No.
`7,601,662
`
`USPTO Right of Appeal Notice for Reexamination of U.S.
`Patent No. 7,601,662
`
`Request for Inter Partes Reexamination in the proceedings of
`U.S. Patent No. 7,601,662
`
`Order Granting/Denying Request for Inter Partes
`Reexamination of U.S. Patent No. 7,601,662
`
`Declaration of Stacey I. Zones in the Inter Partes
`Reexamination of U.S. Patent No. 7,601,662
`
`Declaration of Gary L. Haller in the Inter Partes
`Reexamination of U.S. Patent No. 7,601,662
`
`Second Declaration of Ahmad Moini in the Inter Partes
`Reexamination of U.S. Patent No. 7,601,662
`
`Centi, G., et. al., “Nature of Active Species in Copper-Based
`Catalysts and their Chemistry of Transformation of Nitrogen
`Oxides,” Applied Catalysis A: General, Vol. 132, Issue 2
`(1995)
`
`
`iv
`
`

`
`Patent Owner’s Response (IPR2015-01124)
`
`Second Declaration of Stanley Roth in the Inter Partes
`Reexamination of U.S. Patent No. 7,601,662
`
`Kwak, J., et. al., “Excellent Activity and Selectivity of Cu-
`SSZ-13 in the Selective Catalytic Reduction of NOx with
`NH3,” Journal of Catalysis (2010)
`Dedecek, J., et. al., “Effect of Framework Charge Density on
`Catalytic Activity of Copper Loaded Molecular Sieves on
`Chabazite Structure in Nitrogen (II) Oxide Decomposition,”
`Collect. Czech. Chem. Commun., Vol. 65 (2000)
`
`Biography of Gary Coad (not used)
`
`Blakeman, P., “The role of pore size on thermal stability of
`zeolite supported Cu SCR catalysts,” Catalysis Today (2014)
`
`Expert Declaration of Dr. Michael Tsapatsis (February 12,
`2016)
`
`Declaration of Dr. Ahmad Moini (February 12, 2016)
`
`Gao, F., et. al., “Effects of Si/Al ratio on Cu/SSZ-13 NH3-
`SCR catalysts: Implications for the active species and the
`roles of Bronsted acidity,” Journal of Catalysis (2015)
`
`Tolonen, K., “The effect of NO2 on the activity of fresh and
`aged zeolite catalysts in the NH3-SCR reaction,” Catalysis
`Today (2005)
`
`Brandenberger, S., “The State of the Art in Selective
`Catalytic Reduction of NOx by Ammonia Using Metal-
`Exchanged Zeolite Catalysts,” Catalysis Reviews (2008)
`
`Sjovall, H., “Selective catalytic reduction NOx with NH3
`over Cu-ZSM-5—The effect of changing the gas
`composition,” Applied Catalysis B (2006)
`
`Park, J., “Hydrothermal stability of CuZSM5 catalyst in
`reducing NO by NH3 for the urea selective catalytic
`reduction process,” Journal of Catalysis (2006)
`
` v
`
`
`
`
`
`
`Exhibit 2013
`
`Exhibit 2014
`
`Exhibit 2015
`
`Exhibit 2016
`
`Exhibit 2017
`
`Exhibit 2018
`
`Exhibit 2019
`
`Exhibit 2020
`
`Exhibit 2021
`
`Exhibit 2022
`
`Exhibit 2023
`
`Exhibit 2024
`
`

`
`Patent Owner’s Response (IPR2015-01124)
`
`Andersson, L., “Selective Catalytic Reduction of NOx Over
`Acid-Leached Mordenite Catalysts,” Catalysis Today (1989)
`
`Gabrielsson, P., “Urea-SCR in automotive applications,”
`Topics in Catalysis, Vol. 28, Nos. 1-4 (April 2004)
`
`Deposition of Dr. Johannes Lercher (January 18, 2016)
`(mini-transcript)
`
`Request to Dismiss Appeal by Johnson Matthey Inc., filed in
`Reexamination Control No. 95/001,453 (dated February 27,
`2013)
`
`Wichertlova, B., “Differences in the structure of copper
`active sites for decomposition and selective reduction of
`nitric oxide with hydrocarbons and ammonia,” Catalysis
`Today (1996)
`
`Komatsu, T., “Kinetic Studies of Reduction of Nitric Oxide
`with Ammonia and Cu2+-Exchanged Zeolites,” Journal of
`Catalysis (1994)
`
`Sullivan, J., “Conditions in which Cu-ZSM-5 outperforms
`supported vanadia catalysts in SCR of NOx by NH3,”
`Applied Catalysis (1995).
`
`Krocher, O., “Investigation of the selective catalytic
`reduction of NO by NH3 on Fe-ZSM5 monolith catalysts,”
`Applied Catalysis (2006)
`Baerlocher, “Atlas of Zeolite Framework Types,” 6th Ed.
`(2007) (excerpts)
`
`Declaration of Olivia Schmidt (February 12, 2016)
`
`U.S. 4,544,538 to Zones
`
`
`vi
`
`
`
`
`Exhibit 2025
`
`Exhibit 2026
`
`Exhibit 2027
`
`Exhibit 2028
`
`Exhibit 2029
`
`Exhibit 2030
`
`Exhibit 2031
`
`Exhibit 2032
`
`Exhibit 2033
`
`Exhibit 2034
`
`Exhibit 2035
`
`
`
`

`
`
`
`
`I.
`
`INTRODUCTION
`
`Patent Owner’s Response (IPR2015-01124)
`
`The 203 Patent claims a process for the reduction of oxides of nitrogen
`
`contained in a gas stream in the presence of oxygen comprising contacting the gas
`
`stream with a copper-exchanged CHA1 zeolite (“CuCHA”) having a silica-to-
`
`alumina ratio (“SAR”) between 15 and 100 and copper to aluminum ratio (“Cu/Al
`
`ratio”) between 0.25 and 0.5. The process also includes adding a reductant to the
`
`gas stream such as ammonia (NH3). Prior to the 203 invention it was well known
`
`that the usefulness of metal-exchanged zeolite catalysts was limited due to low
`
`hydrothermal stability—meaning the catalytic activity degrades significantly after
`
`aging in high temperature aqueous environments. The inventors of the 203 Patent
`
`undertook extensive experimentation to solve this problem. The excellent
`
`properties of the claimed CuCHA catalyst, including activity over a wide
`
`temperature range and enhanced hydrothermal stability, are undisputed and were
`
`also unexpected. Patent Owner submits that upon review of the full record, it will
`
`be clear that Petitioner has ignored the state of the art, which shows that the
`
`technology at issue is complex and unpredictable, and has improperly cherry
`
`picked selected portions of select prior art using the patent claims as a roadmap. In
`
`1 Zeolites are classified by frameworks (i.e., structure). There are 231 currently
`
`identified zeolite frameworks, one of which is the CHA framework. Exhibit 2018
`
`(hereinafter “Tsapatsis Decl.”) at ¶ 57.
`
`1
`
`

`
`
`
`
`re Fritch, 972 F.2d 1260, 1266 (Fed. Cir. 1992) (“It is impermissible to use the
`
`Patent Owner’s Response (IPR2015-01124)
`
`claimed invention as an instruction manual or ‘template’ to piece together the
`
`teachings of the prior art so that the claimed invention is rendered obvious.”); Novo
`
`Nordisk A/S v. Caraco Pharm. Labs., Ltd., 719 F.3d 1346, 1365 (Fed. Cir. 2013)
`
`(“In the search for scientific truth ‘[o]ne cannot ... pick and choose among isolated
`
`disclosures in the prior art to deprecate the claimed invention;…it is necessary to
`
`consider prior art that supports unobviousness of the claimed invention, as well as
`
`that which weighs against it.”) (internal citations omitted).
`
`Grounds 1 and 3 of the Petition assert the combination of Maeshima (U.S.,
`
`4,046,888) (Exhibit 1102) or Dedecek (Exhibit 1107) in view of Breck (U.S.
`
`4,503,023) (Exhibit 1103). First, Petitioner’s contention that there would be a
`
`reasonable expectation of success in combining these references is based on the
`
`conclusion, which is also copied in the Institution Decision (Paper No.9, at p. 10,
`
`21), that increasing SAR as taught by Breck “does not have a significant
`
`detrimental effect on the ability to ion-exchange zeolites, or the utility of the
`
`zeolites in the catalytic process in which lower silica precursors have been
`
`employed.” Petition at 47. This conclusion disregards the chemistry of the de-
`
`alumination technique disclosed in Breck, and is contradicted by the expert opinion
`
`of Dr. Tsapatsis, as well as the deposition testimony of Petitioner’s own expert.
`
`Both experts agree that the de-alumination process disclosed in Breck for
`
`
`
`2
`
`

`
`
`
`
`increasing SAR negatively impacts the ability to ion-exchange zeolites, and while
`
`Patent Owner’s Response (IPR2015-01124)
`
`it may improve stability, comes at the cost of catalytic activity. Accordingly, there
`
`is a detrimental effect of increasing SAR, and Petitioner simply ignored this effect
`
`when asserting that the 203 claims are obvious based on Maeshima or Dedecek in
`
`view of Breck.
`
`Second, the Petitioner’s combination of Maeshima or Dedecek with Breck
`
`simply presumes that a person of ordinary skill in the art would select a CuCHA
`
`zeolite for improvement with respect to the NH3 SCR of NOx. Maeshima
`
`discloses nine zeolites, and points a person of ordinary skill in the art to large pore
`
`size2 zeolites. As admitted by Petitioner’s expert, there is no example of a CuCHA
`
`catalyst in Maeshima. Breck discloses ten zeolites, notes that the de-alumination
`
`process is inefficient for the CHA framework as compared to other zeolites, and
`
`does not include any teachings regarding the NH3 SCR of NOx. Dedecek discloses
`
`CuCHA compositions but, as conceded by Petitioner’s expert, it also includes no
`
`teachings regarding the NH3 SCR of NOx.
`
`While Maeshima, Dedecek and Breck are silent about the properties of a
`
`CuCHA zeolite for the SCR of NOx, another prior art patent, U.S. 4,961,917
`
`(“Byrne”) (Exhibit 1110), which issued in 1990 and is cited by Petitioner,
`
`
`2 CHA zeolites have a small pore size (~3.8 Angstroms). Tsapatsis Decl. at ¶ 59.
`
`
`
`3
`
`

`
`
`
`
`explicitly teaches that small pore size zeolites, such as copper-exchanged naturally
`
`Patent Owner’s Response (IPR2015-01124)
`
`occurring chabazite (which has the CHA structure), should not be used for the SCR
`
`of NOx because of susceptibility to sulfate poisoning. Byrne is the only prior art
`
`cited by Petitioner that actually discusses the properties of a CHA zeolite for the
`
`NH3 SCR of NOx and it teaches away from using a CHA zeolite. Accordingly, the
`
`prior art cited in the Petition does not show that the pertinent properties of the
`
`CHA zeolite would have led a person of ordinary skill to select that framework for
`
`further improvement. See Otsuka Pharmaceutical Co., Ltd. v. Sandoz, Inc., 678
`
`F.3d 1280, 1292 (Fed. Cir. 2012) (“With respect to claims of obviousness in
`
`patents involving chemical compounds, in determining whether a chemist would
`
`have selected a prior art compound as a lead, the analysis is guided by evidence of
`
`the compound’s pertinent properties. Such properties may include positive
`
`attributes such as activity and potency, adverse effects such as toxicity, and other
`
`relevant characteristics in evidence. Absent a reason or motivation based on such
`
`prior art evidence, mere structural similarity between a prior art compound and the
`
`claimed compound does not inform the lead compound selection. Were it
`
`otherwise, the analysis would impermissibly rely upon ex post reasoning.”).
`
`Third, the additional combination of Maeshima and Breck or Dedecek and
`
`Breck with Patchett 843 (Exhibit 1105) in Grounds 2 and 4 for the dependent
`
`claims fares no better. Petitioner argues that one of ordinary skill in the art would
`
`
`
`4
`
`

`
`
`
`
`have had a reasonable expectation of success inserting a CuCHA zeolite into the
`
`Patent Owner’s Response (IPR2015-01124)
`
`exhaust treatment system disclosed in Patchett 843. However, Petitioner fails to
`
`reconcile this argument with the fact that Patchett 843 teaches that the system
`
`should use a large pore size zeolite—i.e., a pore diameter of at least 7 Angstroms.
`
`CHA zeolites are small pore size zeolites having a pore diameter half that size
`
`(~3.8 Angstroms). Moreover, Patchett 843 incorporates Byrne (Exhibit 1110) and
`
`Speronello (Exhibit 1111) for their disclosure of “suitable SCR catalyst
`
`compositions.” Speronello requires the use of medium and large pore size zeolites,
`
`while Byrne requires the use of large pore size zeolites and also teaches away from
`
`using small pore size zeolites, such as a CHA zeolite, because of susceptibility to
`
`sulfate poisoning.
`
`Finally, Petitioner’s theory of obviousness is in direct conflict with the fact
`
`that there was a known and longstanding problem that limited the usefulness of
`
`metal-exchanged zeolites for the selective catalytic reduction of nitrogen oxides in
`
`the presence of ammonia (“NH3 SCR of NOx”). Metal-exchanged zeolites
`
`suffered from low hydrothermal stability—meaning the catalytic activity degrades
`
`significantly after aging in high temperature water environments. There is an
`
`abundance of literature between 1995 and 2008 (but not found anywhere in the
`
`Petition or Petitioner’s expert declaration) describing the problem with metal-
`
`exchanged zeolites, but no solution. It is undisputed that the claimed CuCHA
`
`
`
`5
`
`

`
`
`
`
`catalyst is a solution to this problem. This invention has since led to significant
`
`Patent Owner’s Response (IPR2015-01124)
`
`commercial success. Petitioner, now wanting to reap the benefits of Patent
`
`Owner’s labors, makes the contrived argument that the claimed invention was
`
`nothing more than “routine optimization.” However, Petitioner’s argument that
`
`this solution was “routine” based on prior art from the 1970s and 1980s simply
`
`cannot be reconciled with the fact that, between 1995 and 2008, numerous
`
`researchers acknowledged the existence of a critical problem with metal-
`
`exchanged zeolites for the SCR of NOx, but no solution.
`
`The hindsight reasoning that is employed throughout the Petition should be
`
`rejected. Oracle Corp., et al., v. Crossroads Systems, Inc., IPR2014-01207, Paper
`
`78 at 37 (Jan. 29, 2016) (“This type of reasoning—where relevant parts of the
`
`reference are disregarded for the proposed combination without sufficient
`
`explanation of why a person of ordinary skill would do so—is precisely the type of
`
`hindsight reasoning that must be rejected.”). For the reasons stated more fully
`
`herein, Patent Owner respectfully requests that the Board confirm the patentability
`
`of all challenged claims of the 203 Patent.
`
`II. THE 203 PATENT
`A. Overview of Zeolites
`
`Zeolites are crystalline framework materials that contain pores of a
`
`molecular size. Tsapatsis Decl. at ¶ 56. The technical definition of a zeolite has
`
`
`
`6
`
`

`
`
`
`
`traditionally only referred to porous aluminosilicate materials. However, over the
`
`Patent Owner’s Response (IPR2015-01124)
`
`past twenty years the traditional definition has loosened in the art and now refers to
`
`porous molecular sieves, which includes non-aluminosilicate materials such as
`
`silico-aluminophosphates. Id.
`
`The International Zeolite Association currently recognizes 231 different
`
`zeolite framework (i.e., structure) types. Id. at ¶ 57. The 203 Patent claims a
`
`zeolite catalyst having the CHA framework. Each zeolite framework has its own
`
`structural characteristics, such as the pore size, pore shape, and pore connectivity.
`
`See id. at ¶ 58. As shown in the figures below, the structure of a zeolite differs
`
`dramatically between zeolite frameworks:
`
`CHA
`
`
`FAU
`
`
`
`
`
`
`There are four basic pore size classifications for zeolites: small, medium, large, and
`
`extra-large. For example, the CHA framework is a small pore size zeolite, having
`
`a pore diameter of approximately 3.8 Angstroms, while the FAU framework is a
`
`
`
`7
`
`

`
`
`
`
`large pore size zeolite, having a pore diameter of approximately 7.4 Angstroms.
`
`Patent Owner’s Response (IPR2015-01124)
`
`Id. at ¶ 59.
`
`
`
`The crystal structures of aluminosilicate zeolites are built of AlO4 and SiO4
`
`tetrahedra that are linked by the sharing of oxygen atoms. Id. at ¶ 60. The
`
`tetrahedron containing the aluminum atom is charge balanced by association with a
`
`cation, which is most commonly Na+ or K+. Id. It is well known that metals can
`
`be introduced into the zeolite by replacing some of the cations in the zeolite with
`
`metal cations, such as copper (Cu2+), iron (Fe3+), or any other suitable alternative
`
`metal ion. Id. There are a near-limitless number of zeolite compositions that can
`
`be made through combination of different framework types and metal-exchange
`
`ions. Id.
`
`
`
`The behavior of a zeolite for a particular process, such as the NH3 SCR of
`
`NOx, is complex. Id. at ¶ 61. The fact that one zeolite framework behaves in a
`
`certain way for a particular reaction does not mean that other frameworks will
`
`perform in the same manner. This is because the behavior of a zeolite for a
`
`particular process depends on a variety of factors, including framework type,
`
`Bronsted acidity, SAR, the type, concentration, and siting of metal exchange ions,
`
`and of course, the nature and conditions of the process itself. Id. The complex
`
`nature of zeolite catalysis is exemplified by a publication in the Journal of
`
`
`
`8
`
`

`
`
`
`
`Catalysis3 in 2015 by authors from the Institute for Integrated Catalysis. This
`
`Patent Owner’s Response (IPR2015-01124)
`
`paper examined the claimed CuCHA catalyst and explains that “[t]he mechanism
`
`for ammonia selective catalytic reduction (NH3-SCR) over Cu ion exchanged
`
`zeolite catalysts is still widely debated.” Exhibit 2020.001.4 Thus, despite the fact
`
`that the invention occurred nearly a decade earlier, researchers in the field are still
`
`trying explain why the claimed CuCHA catalyst works as well as it does.
`
`Tsapatsis Decl. at ¶ 172. The paper further notes that:
`
`Overall, the interplay between Cu ion loading, Cu ion mobility and
`reaction temperature makes the entire NH3-SCR reaction network
`quite complicated. Indeed, SCR catalysis is further influenced by
`CHA zeolite Si/Al ratios, and the effects are at least twofold: Si/Al
`ratios affect Cu ion locations as briefly discussed above, as well as
`significantly altering Brønsted acidity and, therefore, NH3 storage of
`the catalysts.
`
`Exhibit 2020.002. In sum, the properties of a zeolite catalyst for the NH3-SCR of
`
`NOx are unpredictable.
`
`B.
`
`The Claimed Invention
`
`Before the invention of the 203 Patent, it was well-known in the art that
`
`metal-exchanged zeolite catalysts for the NH3 SCR of NOx exhibited poor
`
`
`3 Petitioner’s expert is the editor-in-chief of the Journal of Catalysis.
`
`4 All emphasis herein is added unless otherwise specified.
`
`
`
`9
`
`

`
`
`
`
`hydrothermal stability—that is they exhibited a significant decline in catalytic
`
`Patent Owner’s Response (IPR2015-01124)
`
`activity after exposure to high temperatures (e.g., above 500º C) and water vapor.
`
`See Exhibit-1101 at 1:35-38, 1:47-51. In an effort to solve this well-known
`
`problem, the inventors of the 203 Patent undertook an extensive examination of
`
`over 900 zeolites, including twelve different framework types, different silica-to-
`
`alumina ratios, different metal ions, and different metal ion concentrations.
`
`Exhibit-2003 at ¶¶ 4-5. Ultimately, the inventors of the 203 Patent discovered that
`
`a copper-exchanged aluminosilicate zeolite with the CHA structure type
`
`(“CuCHA”) exhibited excellent NOx conversion over a wide temperature range
`
`and excellent hydrothermal stability. Id. The 203 Patent claims precisely this
`
`invention.
`
`Claim 1 covers a process for the reduction of oxides of nitrogen contained in
`
`a gas stream where the process comprises contacting the gas stream with a catalyst
`
`comprising a copper-exchanged zeolite having the CHA structure (“CuCHA”) with
`
`a mole ratio of silica-to-alumina (SAR) between about 15 and about 100, and a
`
`copper to aluminum atomic ratio (Cu/Al) from 0.25 to 0.50.
`
`Dependent claim 14 requires adding a reductant to the gas stream.
`
`Dependent claims 15 and 16 require that the reductant comprises ammonia, an
`
`ammonia precursor, or urea. Dependent claims 17-22 include narrower ranges for
`
`the SAR (25-40, about 30) and Cu/Al ratio (0.30-0.50, about 0.40).
`
`
`
`10
`
`

`
`
`
`
`
`Patent Owner’s Response (IPR2015-01124)
`
`Dependent claims 23 and 24 require that the catalyst is disposed on either a
`
`honeycomb flow through substrate or wall flow filter substrate.
`
`Dependent claim 26 is a process including similar to claims 1 and 14, but
`
`including a broader range of SAR (15-150) and Cu/Al (0.25-1). Dependent claims
`
`27 and 28 require that the reductant comprises, ammonia, an ammonia precursor,
`
`or urea. Dependent claims 29 and 30 require that the catalyst is disposed on either
`
`a honeycomb flow through substrate or wall flow filter substrate.
`
`Dependent claim 2 requires that the gas stream is an exhaust gas stream from
`
`an internal combustion engine and the catalyst is disposed on a honeycomb flow
`
`through substrate. Dependent claim 3 requires that the gas stream comprises
`
`ammonia and at least a portion of the flow through substrate is coated with
`
`CuCHA to reduce oxides of nitrogen. Dependent claim 4 requires that the flow
`
`through substrate is coated with Pt and CuCHA to oxidize ammonia.
`
`Dependent claims 5-7 require the same limitations as 2-4, except for a
`
`honeycomb wall flow substrate.
`
`Dependent claims 8-13, 25 and 31 are directed to an exhaust gas treatment
`
`system including a catalyzed soot filter and a diesel oxidation catalyst.
`
`
`
`11
`
`

`
`
`
`
`
`Patent Owner’s Response (IPR2015-01124)
`
`C. Claim Construction
`
`1.
`
`“[C]atalyst” (claim 1)
`
`The term “catalyst” is not indefinite. Tsapatsis Decl. at ¶ 51. This term also
`
`does not require construction, as the plain words of the claim are clear as to what
`
`the catalyst comprises.
`
`2.
`
` “[Z]eolite having the CHA crystal structure” (claim 1)
`
`The 203 Patent defines the CHA structure as “defined by the International
`
`Zeolite Association.” Exhibit 1101 at 1:59-61. Chabazite is a naturally occurring
`
`zeolite that has the CHA framework, however, there are other zeolites that also
`
`have the CHA structure, such as SSZ-13, described in U.S. 4,544,538 (Exhibit
`
`2035), and SSZ-62, described in U.S. 6,709,644 (Exhibit 1104). Tsapatsis Decl. at
`
`¶ 52. Accordingly, “a zeolite having the CHA crystal structure” means a zeolite
`
`having the crystal structure as set forth in the IZA’s data sheet for the CHA
`
`framework. Id.
`
`3.
`
` “A process for the reduction of oxides of nitrogen contained in
`a gas stream” (claim 1)
`
`Petitioner claims this phrase “should be interpreted to require only what it
`
`states.” Petition at 5. Patent Owner agrees, and therefore, the phrase does not
`
`require construction. While the 662 Patent claims at issue do not refer to
`
`temperature or hydrothermal aging, the claims nonetheless cover a catalyst
`
`composition that exhibits certain enhanced properties. Tsapatsis Decl. at ¶¶ 53-55.
`
`
`
`12
`
`

`
`
`
`
`Accordingly, these properties are pertinent to the evaluation of obviousness of the
`
`Patent Owner’s Response (IPR2015-01124)
`
`claimed compound. In re Papesch, 315 F.2d 381, 391 (CCPA 1963) (“From the
`
`standpoint of patent law, a compound and all of its properties are inseparable; they
`
`are one and the same thing.”); see also Sanofi-Synthelabo v. Apotex, Inc., 550 F.3d
`
`1075, 1086 (Fed. Cir. 2008) (“For chemical compounds, the structure of the
`
`compound and its properties are inseparable considerations in the obviousness
`
`determination.”).
`
`III. SCOPE AND CONTENT OF THE PRIOR ART
`As is evident from the literature discussed in this section, the invention
`
`claimed in the 203 Patent was plainly not the result of “routine optimization” as
`
`Petitioner suggests. The state of the prior art at the time of the 203 invention
`
`clearly evidenced a known problem with metal-exchanged zeolite catalysts, as well
`
`as substantial efforts to resolve that problem without success. Furthermore, the use
`
`of the CHA structure for the SCR of NOx is a key aspect of the 203 invention, yet
`
`Petitioner and its expert simply presume that a person of ordinary skill in the art
`
`would have selected and modified a CHA zeolite for the NH3 SCR of NOx.
`
`However, contrary to Petitioner’s presumption, the prior art literature plainly
`
`disfavored CHA zeolites for the NH3 SCR of NOx.
`
`
`
`13
`
`

`
`
`
`
`
`Patent Owner’s Response (IPR2015-01124)
`
`The sub-sections below address the general state of the art and provide an
`
`overview of the specific prior art references relied on in the grounds asserted by
`
`Petitioner.
`
`
`A. The Known Problem with Metal-Exchanged Zeolites
`
`It is beyond dispute that there was a known problem with metal-exchanged
`
`zeolites, which is described in research papers at least as early as 1995 and
`
`continuing up to the time of the invention of the 203 Patent. See Tsapatsis Decl. at
`
`¶¶ 64-71.
`
`In 1995, Centi, et al., highlighted the hydrothermal stability problem of
`
`copper-exchanged zeolites in a paper published in Applied Catalysis A:
`
`[S]everal unresolved problems limit the outlook for successful use of
`zeolites in automotive converters: (i) hydrothermal stability, (ii)
`sensitivity to poisoning, (iii) possibility of manufacturing suitable
`shapes with sufficient mechanical resistance to thermal stress and
`vibrations, (iv) high light-off temperature and limited temperature
`window, (v) possible formation of harmful byproducts, and (vi)
`necessity of post-engine hydrocarbon additions to reach the optimum
`hydrocarbon/NO ratio required to meet current and future legislative
`regulations on NO emissions. A low hydrothermal stability, in
`particular, is the more critical weakness of copper-containing
`zeolites.
`
`
`
`14
`
`

`
`
`
`
`Exhibit 2012.005. In 2005, 2006, and 2008, additional papers, all by different
`
`Patent Owner’s Response (IPR2015-01124)
`
`researchers, repeated the problem with metal-exchanged zeolites, and offered no
`
`solution:
`
`The aim of this study was to obtain knowledge about the activity of
`zeolite-based catalysts in the NH3-SCR reaction with excess of
`oxygen. The limited hydrothermal stability of zeolites may restrict
`their use[.]
`
`Exhibit 2021.002 (Catalysis Today, 2005).
`
`CuZSM5 has been reported as one of the most promising catalysts for
`the SCR of NOx from light- and heavy- duty diesel engines with urea.
`However, the hydrothermal stability of the catalyst is another critical
`issue to be resolved for the commercial application of urea SCR
`technology to automotive engines. CuZSM5 after hydrothermal aging
`under simulated flue gas stream at temperature above 600° C with
`10% water reveals significant catalyst deactivation.
`
`Exhibit 2024.010 (Journal of Catalysis, 2006).
`
`One of the challenges for the practical application of SCR catalysts
`is their durability under hydrothermal conditions. Fe-ZSM-5
`catalysts, for instance, have been reported to be very stable even in the
`presence of H2O, but at temperatures above 500° C deactivation is
`always observed
`
`***
`One of the major requirements for the practical application of zeolites in
`the SCR process is their durability under hydrothermal conditions, which
`is not yet sufficient. There is no guarantee that a zeolite-based catalyst will
`
`
`
`15
`
`

`
`
`
`
`
`Patent Owner’s Response (IPR2015-01124)
`
`be found that meets all of the diverse requirements for future SCR systems
`on diesel vehicles. Research is now targeting catalysts that combine both
`high activity at low temperatures and hydrothermal stability at high
`temperatures.
`
`Exhibit 2022.016, .029 (Catalysis Reviews: Science and