IN THE UNITED STATES PATENT AND TRADEMARK OFFICE
`
`BEFORE THE PATENT TRIAL AND APPEAL BOARD
`
`
`
`U.S. Patent No. 7,601,662
`
`U.S. Patent No. 8,404,203
`
`Filed:
`
`Feb. 27, 2008
`
`Filed:
`
`Jun. 8, 2009
`
`Issued:
`
`Oct. 13, 2009
`
`Issued:
`
`Mar. 26, 2013
`
`Inventors: Ivor Bull, et al.
`
`Inventors: Ivor Bull, et al.
`
`Title: Copper CHA Zeolite Catalysts
`
`Title: Processes for Reducing Nitrogen
`Oxides Using Copper CHA Zeolite
`Catalysts
`
`
`
`
`
`
`
`DECLARATION OF DR. MICHAEL TSAPATSIS
`
`I, Michael Tsapatis, make this declaration in connection with the Inter
`
`Partes Reviews of U.S. Patent Nos. 7,601,662 (“the 662 Patent”) (IPR2015-01121,
`
`-1125) and 8,404,203 (“the 203 Patent”) (IPR2015-01123, -1124). All statements
`
`herein made of my own knowledge are true, and all statements herein made based
`
`on information and belief are believed to be true. I am over age 21 and otherwise
`
`competent to make this declaration. Although I am being compensated for my
`
`time in preparing this declaration, the positions articulated herein are my own, and
`
`I have no stake in the outcome of this proceeding or any related litigation or
`
`administrative proceedings.
`
`Exhibit 2018.001
`
`

`
`I.
`
`Background and Qualifications
`Appendix A to this declaration is my curriculum vitae. As shown in
`
`1.
`
`my curriculum vitae, I have devoted my career to various fields of zeolite catalysts
`
`and adjacent fields of research. From 2008 to 2013, I served as an Editor for
`
`Microporous and Mesoporous Materials, which is the official journal of the
`
`International Zeolite Association. In 2013, I was elected as a council member of
`
`the International Zeolite Association.
`
`2.
`
`I am a Professor at the University of Minnesota Twin Cities and am
`
`the Amundson Chair in Chemical Engineering and Materials Science at the
`
`University of Minnesota Twin Cities. At the University of Minnesota Twin Cities,
`
`I lead the Tsapatsis Research Group, which is housed in the department of
`
`Chemical Engineering & Materials Science. The research of the Tsapatsis
`
`Research Group is focused on innovative research on, among other things, highly
`
`selective membranes and catalysts with properties tailored for specific purposes.
`
`In the course of this research, we have substantial interactions with those in the
`
`relevant industries. I have worked on zeolite synthesis, structure determination
`
`and applications in separations and catalysis for 25 years. I have supervised more
`
`than 30 Ph.D. theses and 20 post-doctoral studies, and graduates from my group
`
`are employed in the chemical, petrochemical and microelectronics industries while
`
`18 former students and postdoctoral fellows hold academic positions.
`
` 2
`
`
`
`Exhibit 2018.002
`
`

`
`3.
`
`I received a diploma in Chemical Engineering from the University of
`
`Patras in Greece. Following this, I received my MS in Chemical Engineering from
`
`the California Institute of Technology in 1991 and my Ph.D. in Chemical
`
`Engineering from the California Institute of Technology in 1994. In 1994, I
`
`continued my post-doctoral research and training in Chemical Engineering at the
`
`California Institute of Technology. From 1994 to 1999, I was an Assistant
`
`Professor at the University of Massachusetts in Amherst. Thereafter, I was
`
`awarded early tenure and became an Associate Professor at the University of
`
`Massachusetts from 1999 to 2003. From 2003 to present, I have been a Professor
`
`at the University of Minnesota Twin Cities and have held the Amundson chair
`
`since 2008.
`
`4.
`
`I have published approximately 220 papers and have been invited to
`
`present approximately 140 lectures including for ExxonMobil (UMass Amherst),
`
`Lindsay (Texas A&M), Merck Sharp and Dohme (UPR), Van Ness (RPI), Robert
`
`W. Vaughan (Caltech), DB Robinson (Alberta), SV Sotirchos (Foundation for
`
`Research and Technology, Greece) and GCA Schuit Lectures (Delaware).
`
`5.
`
`I am the inventor/co-inventor of 10 issued patents and 7 patent
`
`applications. I am the recipient of the Alpha Chi Sigma Award for Chemical
`
`Engineering Research from the American Institute of Chemical Engineers
`
`(AIChE), the Breck Award from the International Zeolite Association (co-awarded
`
` 3
`
`
`
`Exhibit 2018.003
`
`

`
`in 2013 with Prof. Caro), the Charles M.A. Stine Award from the Materials
`
`Engineering & Sciences Division of AIChE, a David and Lucile Packard
`
`Foundation Fellowship, a National Science Foundation CAREER Award, a
`
`Camille Dreyfus Teacher-Scholar Award and of a North American Membrane
`
`Society Fellowship. I was elected fellow of the American Association for the
`
`Advancement of Science (2011) and a member of the National Academy of
`
`Engineering (2015) with Election Citation: For design and synthesis of zeolite-
`
`based materials for selective separation and reaction.
`
`A.
`6.
`
`Status as an Independent Expert Witness
`
`I have been retained in this matter by BASF Corporation to provide
`
`expert analysis and opinions regarding the 662 and 203 Patents. I am being
`
`compensated at the rate of $300 per hour for my work. My fee is not contingent on
`
`the outcome of this matter or on any of the positions I have taken, as discussed
`
`below. I have no financial interest in BASF Corporation.
`
`7.
`
`I have been advised that Umicore AG & Co. KG (hereinafter referred
`
`to as “Petitioner”) is challenging the validity of the 662 and 203 Patents. I have no
`
`financial interest in Petitioner.
`
`II. Materials Considered
`I have reviewed the 662 and 203 Patents and their respective
`8.
`
`prosecution histories. I have also reviewed the following documents:
`
` 4
`
`
`
`Exhibit 2018.004
`
`

`
`Petitioner’s Exhibits
`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 Declarations of Dr. Lercher submitted in IPR2015-
`01121, -01123, -01124, -01125
`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
`U.S. 4,544,538 to Zones
`
`Patent Owner’s 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
`
` 5
`
`
`
`Exhibit 1002
`Exhibit 1003
`Exhibit 1004
`Exhibit 1005
`Exhibit 1006
`Exhibit 1007
`
`Exhibit 1008
`
`Exhibit 1010
`Exhibit 1011
`Exhibit 1012
`
`Exhibit 1013
`Exhibit 1014
`
`Exhibit 1015
`Exhibit 1016
`
`
`Exhibit 2001
`
`Exhibit 2002
`
`Exhibit 2003
`
`Exhibit 2004
`
`Exhibit 2005
`
`Exhibit 2018.005
`
`

`
`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)
`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)
`Blakeman, P., “The role of pore size on thermal stability of
`zeolite supported Cu SCR catalysts,” Catalysis Today (2014)
`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)
`
` 6
`
`
`
`Exhibit 2006
`
`Exhibit 2007
`
`Exhibit 2008
`
`Exhibit 2009
`
`Exhibit 2010
`
`Exhibit 2011
`
`Exhibit 2012
`
`Exhibit 2013
`
`Exhibit 2014
`
`Exhibit 2015
`
`Exhibit 2017
`
`Exhibit 2019
`Exhibit 2020
`
`Exhibit 2021
`
`Exhibit 2022
`
`Exhibit 2018.006
`
`

`
`Exhibit 2023
`
`Exhibit 2024
`
`Exhibit 2025
`
`Exhibit 2026
`
`Exhibit 2027
`
`Exhibit 2029
`
`Exhibit 2030
`
`Exhibit 2031
`
`Exhibit 2032
`
`Exhibit 2033
`
`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)
`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)
`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)
`
`
`III. Understanding of the Law
`
`9.
`
`I have not been asked to offer an opinion on the law. However, as an
`
`expert assisting in determining validity, I understand that I am obliged to follow
`
`existing law. I have therefore been asked to apply the following legal principles to
`
`my analysis.
`
` 7
`
`
`
`Exhibit 2018.007
`
`

`
`10. A claim is invalid for obviousness if 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.
`
`11.
`
`In determining whether a claimed invention is obvious, one should
`
`consider the scope and content of the prior art, the level of ordinary skill in the
`
`relevant art, the differences between the claimed invention and the prior art, and
`
`whether the claimed invention would have been obvious to one of ordinary skill in
`
`the art in light of those differences.
`
`12.
`
`I understand that certain objective factors, sometimes known as
`
`“secondary considerations” must, if present, be taken into account in determining
`
`whether a claimed invention would have been obvious. These factors, which
`
`include the invention’s commercial success, satisfying a long felt but unsolved
`
`need, the failure of others, praise by others, and teaching away by others, may
`
`often be the most probative and cogent evidence of non-obviousness. I understand
`
`that one purpose of these secondary considerations is to guard as a check against
`
`hindsight bias, and avoid having a fact finder develop a hunch that the claimed
`
`invention was obvious, and then construct a selective version of the facts that
`
`confirms that hunch. Such evidence may often establish that an invention
`
`appearing to have been obvious in light of the prior art was not obvious.
`
` 8
`
`
`
`Exhibit 2018.008
`
`

`
`13. The person of ordinary skill in the art is a hypothetical person who is
`
`presumed to be aware of all of the pertinent art. The person of ordinary skill is not
`
`an automaton, and may be able to fit together the teachings of multiple prior art
`
`references employing ordinary creativity and the common sense that familiar items
`
`may have obvious uses beyond their primary purposes. In establishing
`
`obviousness, one must avoid the temptation to read into the prior art the teachings
`
`of the invention at issue and guard against slipping into the use of hindsight. The
`
`prior art itself, and not the applicant’s achievement, must establish the obviousness
`
`of the combination. That is, a claim cannot serve as a motivation to combine prior
`
`art references.
`
`14.
`
`I understand that even if all aspects of the claimed invention were
`
`individually known in the art, this is not sufficient to establish obviousness without
`
`some objective reason to combine the teachings of the references as arranged in the
`
`claim under consideration. On this point, I understand that mere statements to the
`
`effect that a combination was obvious are not sufficient in the absence of
`
`articulated reasoning with rational underpinning to support the conclusion of
`
`obviousness.
`
`15.
`
`I understand that a mere combination of references disclosing
`
`individual elements itself does not satisfy the burden of proving invalidity by a
`
`preponderance of the evidence.
`
` 9
`
`
`
`Exhibit 2018.009
`
`

`
`16.
`
`If a proposed modification to a reference would render the prior art
`
`invention being modified unsatisfactory for its intended purpose, or if the prior art
`
`teaches away from the proposed modification, there is no suggestion or motivation
`
`to make the proposed modification.
`
`17.
`
`If a proposed modification or combination of prior art references
`
`would change the principle of operation of the prior art invention being modified,
`
`then the teachings of the references may not be sufficient to render the claims
`
`obvious.
`
`18.
`
`I understand that obviousness does not require absolute predictability,
`
`however, at least some degree of predictability is required. Evidence showing
`
`there was no reasonable expectation of success may support a conclusion of
`
`nonobviousness. I understand that whether an art is predictable or whether the
`
`proposed modification or combination of the prior art has a reasonable expectation
`
`of success is determined at the time the invention was made.
`
`19.
`
`I understand an invention that is obvious to try is not necessarily
`
`considered obvious. For example, an invention may not be obvious when the prior
`
`art gives only general guidance as to the particular form of the claimed invention
`
`or how to achieve it, or if one of skill in the art could simply try each of numerous
`
`possible choices until one arrived at a successful result. Likewise, a claimed
`
`invention may not be obvious even if it was obvious to explore a new technology
`
`
`10
`
`Exhibit 2018.010
`
`

`
`or general approach that seemed to be promising for experimentation, but the range
`
`of options available to a person of ordinary skill would not have been finite, small,
`
`or easily traversed. And, even then, where the prior art does not give an indication
`
`as to which options or parameters were critical, or does not give direction as to
`
`which of many possible choices may have been successful, then a claimed
`
`invention may still be non-obvious. In other words, an invention may not be
`
`obvious when the prior art does not provide a reason to select the route that
`
`produced the claimed invention.
`
`IV. The Person of Ordinary Skill in the Relevant Field in the Relevant
`Timeframe
`
`20.
`
`I have been informed that “a person of ordinary skill in the relevant
`
`field” is a hypothetical person to whom an expert in the relevant field could assign
`
`a routine task with reasonable confidence that the task would be successfully
`
`carried out. I have been informed that the level of skill in the art is evidenced by
`
`the prior art.
`
`21.
`
`I understand that Petitioner has asserted that one of ordinary skill in
`
`the art as of February 2007 would “have at least a Master’s degree in chemistry or
`
`a related discipline, and have knowledge of the structure and chemistry of
`
`molecular sieves like zeolites, including factors that impact their stability and
`
`activity.” Exhibit 1008 at ¶ 66.
`
`
`11
`
`Exhibit 2018.011
`
`

`
`22.
`
`In my opinion, I agree with the characteristics of a person of ordinary
`
`skill in the art that are proposed by the Petitioner. Based on my experience, I have
`
`a good understanding of the capabilities of a person of ordinary skill in the relevant
`
`field. I have trained, supervised, directed, and advised many such persons over the
`
`course of my career.
`
`V.
`
`Summary of Opinions
`I understand that inter partes review has been instituted on the
`
`23.
`
`following claims of the 662 Patent:
`
`• Obviousness of claims 1-8 and 30 based on Zones in view of
`Maeshima
`
`• Obviousness of claims 1, 2, 5, 6, and 30 based on Maeshima in
`view of Breck
`
`• Obviousness of claims 1, 2, 5, 6, and 30 based on Dedecek in view
`of Breck
`
`• Obviousness of claims 12-24 and 32-50 based on Zones in view of
`Maeshima and Patchett ‘843
`
`• Obviousness of claims 12-24 and 32-50 based on Maeshima in
`view of Breck and Patchett ‘843
`
`• Obviousness of claims 12-24 and 32-50 based on Dedecek in view
`of Breck and Patchett ‘843
`
`24. As explained in detail in this declaration, it is my opinion that these
`
`claims of the 662 Patent are not obvious in view of the prior art.
`
`25.
`
`I also understand that inter partes review has been instituted on the
`
`following claims of the 203 Patent:
`
`
`12
`
`Exhibit 2018.012
`
`

`
`• Obviousness of claims 1, 14, 15, 17-22, 26 and 27 based on Zones
`in view of Maeshima
`
`• Obviousness of claims 1, 14, 15, 19, 20, 26 and 27 based on
`Maeshima in view of Breck
`
`• Obviousness of claims 1, 14, 15, 19, 20, 26 and 27 based on
`Dedecek in view of Breck
`
`• Obviousness of claims 2-13, 16, 23-25 and 28-31 based on Zones
`in view of Maeshima and Patchett ‘843
`
`• Obviousness of claims 2-13, 16, 23-25 and 28-31 based on
`Maeshima in view of Breck and Patchett ‘843
`
`• Obviousness of claims 2-13, 16, 23-25 and 28-31 based on
`Dedecek in view of Breck and Patchett ‘843
`
`26. As explained in detail in this declaration, it is my opinion that these
`
`claims of the 203 Patent are not obvious in view of the prior art.
`
`VI. U.S. 7,601,662 and U.S. 8,404,203
`A. The 662 Patent
`27. The 662 Patent describes a novel catalyst comprising a copper-
`
`exchange zeolite having the CHA structure (“CuCHA”) that can be used as part of
`
`exhaust gas treatment system for an internal combustion engine, in particular a
`
`diesel engine. More specifically, the CuCHA catalyst is used in the selective
`
`catalytic reduction (SCR) of nitrogen oxides (NOx) in the presence of ammonia
`
`(NH3) (also referred to as “NH3 SCR of NOx”). As explained in the 662 Patent, it
`
`was known in the art that metal-exchanged zeolite catalysts used for the NH3 SCR
`
`of NOx declined in activity when exposed to harsh hydrothermal conditions. 662
`
`
`13
`
`Exhibit 2018.013
`
`

`
`Patent at 1:35-38. The invention claimed in the 662 Patent was the result of efforts
`
`to develop a zeolite catalyst that exhibited improved hydrothermal stability over
`
`existing zeolites. 662 Patent at 1:47-51.
`
`28.
`
`I have reviewed the declaration of Dr. Ahmad Moini regarding the
`
`invention of the 662 Patent. Exhibit 2003. I understand that the inventors tested
`
`over 900 zeolite materials including over twelve different framework types.
`
`Exhibit 2003 at ¶ 4. In my opinion, this broad experimentation is contrary to
`
`Petitioner’s argument that the claimed invention was a routine optimization that
`
`was predictable based on prior art teachings.
`
`29. Claim 1 of the 662 patent claims a catalyst comprising an
`
`aluminosilicate zeolite having the CHA structure, a silica to alumina ratio (“SAR”)
`
`of 15 to 150, and a copper to aluminum atomic ratio between 0.25 and 1, where the
`
`catalyst is effective to promote the reaction of ammonia with nitrogen oxides
`
`(NOx) to form nitrogen and H2O selectively (i.e., NH3 SCR of NOx).
`
`30. Dependent claim 2 requires a SAR from about 15 to 100, and
`
`dependent claim 30 requires an exhaust gas treatment system comprising the
`
`catalyst of claim 2 effective for the NH3 SCR of NOx.
`
`31. Dependent claims 3-8 are directed to an aluminosilicate zeolite having
`
`the CHA crystal structure, a mole ratio of silica to alumina from about 25 to about
`
`40, and/or an atomic ratio of copper to aluminum from about 0.30 to about 0.50.
`
`
`14
`
`Exhibit 2018.014
`
`

`
`32. Dependent claims 12-14 and 32 require that the catalyst is deposited
`
`on a honeycomb substrate, where the honeycomb substrate comprises a wall flow
`
`filter substrate, a flow through substrate, or a high efficiency open cell foam filter.
`
`33. Dependent claims 15-20 require that at least a portion of the substrate
`
`(wall flow or flow through) is coated with CuCHA to reduce oxides of nitrogen, or
`
`coated with Pt and CuCHA to oxidize ammonia.
`
`34. Dependent claims 21-24 require that the catalyst is disposed
`
`downstream of a diesel engine and an injector that adds a reductant to the exhaust
`
`gas stream from the engine.
`
`35. Dependent claims 33-38 are directed to an exhaust gas treatment
`
`system including a catalyzed soot filter and a diesel oxidation catalyst that are
`
`located upstream of the CuCHA catalyst.
`
`36. Dependent claims 39 and 40, which depend from claim 3, are directed
`
`to depositing the catalyst on a wall flow filter substrate or flow through substrate.
`
`37. Dependent claims 41-46 include the same limitations as claims 15-20.
`
`38. Dependent claims 47-50 require the same limitations as claims 21-24.
`
`The 203 Patent
`
`B.
`39. The 203 patent is a divisional of the 662 patent and contains the same
`
`specification as the 662 patent. Independent claim 1 of the 203 patent is directed
`
`to a process for the reduction of oxides of nitrogen contained in a gas stream
`
`
`15
`
`Exhibit 2018.015
`
`

`
`wherein the gas stream is contacted with a catalyst comprising a zeolite having the
`
`CHA crystal structure, a mole ratio of silica to alumina from about 15 to about 100,
`
`and an atomic ratio of copper to aluminum from about 0.25 to about 0.50.
`
`40. Dependent claim 14, which depends from claim 1, further requires
`
`that the process includes adding a reductant to the gas stream. Dependent claim 15
`
`requires that reductant comprises ammonia or an ammonia precursor, while
`
`dependent claim 16 requires that the reductant comprises urea.
`
`41.
`
`Independent claim 26 includes the same limitations as claims 1 and
`
`14. Dependent claims 27 and 28 include the same limitations as claims 15
`
`(ammonia reductant) and 16 (urea reductant).
`
`42. Dependent claims 17-22 depend from claim 15, and require SAR from
`
`about 25 to 40, Cu/Al ratio from about 0.30 to about 0.50.
`
`43. Dependent claims 23 and 24, which depend from claim 15, require
`
`that the catalyst is disposed on a honeycomb flow through or wall flow filter
`
`substrate. Dependent claim 25 also depends from claim 15, and requires that the
`
`gas stream is from an internal combustion engine, and the process includes
`
`contacting the gas stream with a catalyzed soot filter and oxidation catalyst that are
`
`upstream from the CuCHA catalyst.
`
`
`16
`
`Exhibit 2018.016
`
`

`
`44. Dependent claims 2-4 require that the gas stream is an exhaust gas
`
`stream of an internal combustion engine, and depositing the catalyst on a
`
`honeycomb flow through substrate.
`
`45. Dependent claims 5-7 require that the gas stream is an exhaust gas
`
`stream of an internal combustion engine, and depositing the catalyst on a
`
`honeycomb wall flow substrate.
`
`46. Dependent claims 8-13 are directed to an exhaust gas treatment
`
`system including a catalyzed soot filter and a diesel oxidation catalyst.
`
`C.
`47.
`
`Properties of the Claimed CuCHA Catalyst
`
`In addition to the experimental results disclosed in the 662 Patent,
`
`there are also several third party publications that have verified the properties of
`
`the claimed CuCHA catalyst. These papers are briefly discussed below.
`
`48.
`
`In 2006, BASF supplied (under a non-disclosure agreement) the Ford
`
`Motor Company with catalyst samples for evaluation that had a washcoat of
`
`CuCHA (copper exchanged SSZ-13) having a SAR of about 30 and a Cu/Al ratio
`
`of about 0.45. Exhibit 2004 at ¶¶ 4-8. The results of the evaluation were published
`
`in a paper in the SAE Journal of Fuels and Lubricants in 2008 that I will refer to as
`
`the “Ford paper.” Exhibit 2002; see also Exhibit 2004 at ¶¶ 4-8. The Ford paper
`
`describes the “state-of-the-art Cu/zeolite” as having “remarkable high temperature
`
`hydrothermal stability up to 950° C while maintaining stable low temperature NOx
`
`
`17
`
`Exhibit 2018.017
`
`

`
`activity.” Exhibit 2002.001. The paper further notes that “[t]he enhanced
`
`durability of the 2007 SCR formulations has been mainly attributed to advances in
`
`the zeolite type and composition.” Exhibit 2002.005.
`
`49.
`
`In 2010, a paper published in the Journal of Catalysis by individuals
`
`from the Institute for Interfacial Catalysis (“Kwak paper”) also confirms the
`
`properties of the claimed CuCHA catalyst. The Kwak paper explains, with citation
`
`to the 662 Patent, that “[i]n the very recent patent literature, Cu2+ ion-exchanged
`
`SSZ-13 (Cu-SSZ-13) has been reported to exhibit NOx conversions of 90-100%
`
`over a wide temperature range in the NH3-SCR process, and its activity exceeded
`
`80% even after extensive high-temperature hydrothermal aging…Our results
`
`confirm that the activity and selectivity of the Cu-SSZ-13 catalyst for both NOx
`
`SCR with NH3 and NH3 oxidation are superior to those of both Cu-beta and Cu-
`
`ZSM-5.” Exhibit 2014.001.
`
`VII. Claim Construction
`In the present proceeding, I have been advised that the claims are to
`50.
`
`be given their broadest reasonable interpretation in view of the specification.
`
`A.
`51.
`
` “Catalyst”
`
`I disagree with Petitioner’s position that the term “catalyst” is
`
`indefinite. In my opinion, the term “catalyst” is a well understood and frequently
`
`used term by persons of ordinary skill in the art. I have no dispute with Dr.
`
`
`18
`
`Exhibit 2018.018
`
`

`
`Lercher’s opinion that a catalyst is generally understood to refer to a material that
`
`increases the rate of chemical reaction without itself undergoing a permanent
`
`chemical change. IPR2015-1121 Lercher Decl. at ¶ 42.
`
`“[Z]eolite having the CHA crystal structure”
`
`B.
`52. Dr. Lercher asserts that “a zeolite with the CHA crystal structure”
`
`refers to chabazite materials with the crystal structure set forth in the IZA’s data
`
`sheet for the CHA framework. Chabazite is a naturally occurring material that has
`
`the CHA framework, however, there are other materials that also have the CHA
`
`structure. For example, U.S. 4,544,538 to Zones (Exhibit 1016) and U.S.
`
`6,709,644 to Zones (Exhibit 1004) respectively describe the synthesis of SSZ-13
`
`and SSZ-62, both of which have the CHA structure. Accordingly, I believe a more
`
`appropriate definition of “a zeolite with the CHA crystal structure” is materials
`
`with the crystal structure set forth in the IZA’s data sheet for the CHA framework.
`
`C.
`
` “[T]he catalyst effective to promote the reaction of ammonia with
`nitrogen oxides to form nitrogen and H2O selectively”
`53. Petitioner has stated that the phrase “the catalyst effective to promote
`
`the reaction of ammonia with nitrogen oxides to form nitrogen and H2O
`
`selectively” should be interpreted to mean that “the catalyst be able to promote the
`
`selective reaction of NH3 with NOx to form N2 and H2O, i.e., that it be an SCR
`
`catalyst.” IPR2015-1121 Petition at 6. I presume Petitioner did not intend to
`
`change the meaning of the claim by substituting “be able” for “effective.”
`
`
`19
`
`Exhibit 2018.019
`
`

`
`54.
`
`I disagree that the 662 Patent does not claim the properties that are
`
`described in the specification. For example, the 662 Patent shows that a CuCHA
`
`catalyst having a SAR of 30 and a Cu/Al ratio of 0.38 (Example 3) exhibits certain
`
`NOx conversion percentages shown in Table 1. This same catalyst, and therefore,
`
`its properties, is claimed in the 662 Patent because claim 1 requires a catalyst
`
`comprising an aluminosilicate zeolite having the CHA structure, a SAR between
`
`15 and 150, and a Cu/Al ratio between 0.25 and 1. Example 3 is also covered by
`
`claims 2 through 8.
`
`55. Dr. Lercher refers to Example 1 of the 662 Patent to suggest that the
`
`claims cover CuCHA catalysts that do not have enhanced properties. While
`
`Example 1 does not perform as well as Examples 2 and 3, it still performs better
`
`than other samples. Specifically, Example 1 has significantly better aged activity
`
`than the Cu-Beta sample (82% compared to 53% at 460° C, and 43% compared to
`
`23% at 210° C).
`
`VIII. Overview of Zeolites
`56. Zeolites are crystalline framework materials that contain pores of a
`
`molecular size. The technical definition of a zeolite has traditionally only referred
`
`to porous aluminosilicate materials. However, over the 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-
`
`
`20
`
`Exhibit 2018.020
`
`

`
`aluminophosphates. There are a boundless number of zeolite compositions that
`
`can be made through the combination of different framework types with various
`
`SAR and ion-exchange contents.
`
`57. The International Zeolite Association currently recognizes 231
`
`different zeolite framework types (i.e., structure types). This list of known zeolites
`
`continues to grow. The CHA framework, which is a key aspect of the claimed
`
`invention in the 662 and 203 Patents, is one framework type recognized by the IZA
`
`and has been known for more than 50 years.
`
`58. Each zeolite framework has its own structural characteristics. Each of
`
`these characteristics will impact the performance of the zeolite in a system. Below
`
`are the images from the IZA for the BEA, FAU and CHA framework types that
`
`illustrate the fundamental difference between these three framework types. As the
`
`images show, there are several differences between the framework types, including
`
`pore size, pore shape, and pore connectivity.
`
`BEA
`
`FAU
`
`
`
`
`
`
`21
`
`
`
`Exhibit 2018.021
`
`

`
`CHA
`
`
`
`59. Pore size defines the maximum size of a molecule that can be
`
`
`
`adsorbed, separated, or diffused by the zeolite. Zeolites can be grouped into four
`
`basic pore size classifications: small, medium, large, and extra-large. CHA, which
`
`is an eight-ring structure, has a small pore size of approximately 3.8 Angstroms
`
`(0.38 nm). Exhibit 2033.022. FAU, which has a 12-ring structure, has a large
`
`pore size of approximately 7.4 Angstroms (0.74 nm). Exhibit 2033.019. VFI is an
`
`example of an extra-large pore size zeolite (12.7 Angstroms). Exhibit 2033.018.
`
`60. The crystal structures of aluminosilicate zeolites are built of AlO4 and
`
`SiO4 tetrahedra that are linked by the sharing of oxygen atoms. The tetrahedron
`
`containing the aluminum atom is charge balanced by association with a cation,
`
`which is most commonly Na+ or K+. 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