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`UNITED STATES PATENT AND TRADEMARK OFFICE
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`BEFORE THE PATENT TRIAL AND APPEAL BOARD
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`JOHNSON MATTHEY INC.
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`Petitioner
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`v.
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`BASF CORPORATION
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`Patent Owner
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`Patent 9,032,709
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`DECLARATION OF MICHAEL P. HAROLD, PH.D.
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`1
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`JM 1004
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`I, Michael P. Harold, declare as follows:
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`INTER PARTES REVIEW OF U.S. PATENT NO. 9,032,709
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`1.
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`2.
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`I attach my resume as Exhibit 1 to this declaration.
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`Experience and Qualifications
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`I am the Department Chair and M.D. Anderson Professor at the
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`University of Houston Department of Chemical Engineering. From May to August
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`2013, I was the Acting Dean of the Cullen College of Engineering, also at the
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`University of Houston.
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`3.
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`I received my B.S. in Chemical Engineering from Penn State in 1980
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`and earned my Ph.D in Chemical Engineering from the University of Houston in
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`1985.
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`4.
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`I have been a Professor at the University of Houston since 2000. My
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`research focuses on catalytic reaction engineering, including the catalytic reduction
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`of NOx to nitrogen in the oxidizing atmosphere of lean burn and diesel vehicles. I
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`have authored at least 135 peer-reviewed papers.
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`5.
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`In 2014, I was elected a Fellow of the American Institute of Chemical
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`Engineers. In 2013, I received the Esther Farfel Award, which is the top honor to a
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`university faculty member at the University of Houston.
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`6.
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`I am the Founder and Principal Investigator of the Texas Center for
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`Clean Engines, Emissions & Fuels (TXCEF), a UH Center involved in the
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`research, development, testing, and implementation of emission control
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`INTER PARTES REVIEW OF U.S. PATENT NO. 9,032,709
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`technologies. TXCEF involves a partnership between UH, the City of Houston,
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`the State of Texas, and third-party companies. Since 2003 the Center has had
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`grants awarded totaling over $20 million.
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`7.
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` Since December 2011, I have been the Editor-in-Chief of the AIChE
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`Journal, the journal of the world’s leading organization for chemical engineering
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`professionals. Since 2010, I have been on the Editorial Board of Reviews in
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`Chemical Engineering and from 2009 to 2011, I was a Consulting Editor of
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`Industrial & Engineering Chemistry Research.
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`8.
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`In 2004, I served as Editor of a special issue in Catalysis Today on
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`“NOx Reduction for Diesel and Lean Burn Engines.”
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`9.
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`Before joining the faculty of the University of Houston in 2000, I
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`worked for the DuPont Company, ultimately becoming the Research Manager for
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`Chemical Process Fundamentals. I also served as the Global Technology for
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`Polymer & Fiber R&D. During my years at DuPont I was involved in the research
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`and development of polymer intermediates manufacturing and chemical reaction
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`engineering.
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`10.
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`I have reviewed U.S. Patent No. 9.032,709, assigned to BASF
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`Corporation. I have also reviewed at least the following patents and printed
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`publications:
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` S. Hashimoto, Y. Miyairi, T. Hamanaka, R. Matsubara, T. Harada and S.
`Miwa, SiC and Cordierite Diesel Particulate Filters Designed for Low
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`INTER PARTES REVIEW OF U.S. PATENT NO. 9,032,709
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`Pressure Drop and Catalyzed, Uncatalyzed Systems, SAE Technical
`Paper 2002-01-0322.
` U.S. Patent No. 5,516,497 (“Speronello”), assigned to BASF
`Corporation.
` The certified translation of Georg Hüthwohl, Bernd Maurer and Gennadi
`Zikoridse, The SCRT® System – A Combination Particle Filter with SCR
`Catalyst – Enables Both Particle and NOx Emission To Be Reduced
`Simultaneously in Commercial Vehicle Diesel Engines, Proceedings of
`the Dresden Motor Conference, held in May 1999.
` Yasutake Teraoka, Kazunori Kanada, Hiroshi Furukawa, Isamu
`Moriguchi, and Shuichi Kagawa, Simultaneous Catalytic Removal of
`Nitrogen Oxides and Soot by Copper-Loaded MFI Zeolites, 30 Chemistry
`Letters 604 (2001).
` Chapters 8 & 9 from Ronald M. Heck and Robert J. Farrauto with Suresh
`T. Gulati, Catalytic Air Pollution Control (2002).
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`11. Although for the sake of brevity this Declaration refers to selected
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`portions of the cited references, it should be understood that one of ordinary skill in
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`the art would view the references cited herein in their entirety, and in combination
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`with other references cited herein or cited within the references themselves. The
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`references used in this Declaration, therefore, should be viewed as being
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`incorporated herein in their entirety.
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`12.
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`I am not, and never was, an employee of Johnson Matthey Plc or any
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`Johnson Matthey company. I have been engaged in the present matter to provide
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`my independent analysis of the issues raised in the petition for inter partes review
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`of the ’709 patent. I received no compensation for this declaration beyond my
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`normal hourly compensation based on my time actually spent studying the matter,
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`INTER PARTES REVIEW OF U.S. PATENT NO. 9,032,709
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`and I will not receive any added compensation based on the outcome of this inter
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`partes review of the ’709 patent.
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`13. Based upon my experience in this area, a person of ordinary skill in
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`the art in this field at the relevant time frame (“POSITA”), a person of ordinary
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`skill in the art of the ’709 patent at the time of the invention is a person who has
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`obtained at least a BS or MS in a chemistry, chemical engineering, material
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`science, or a related field and least three years of experience or training in
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`researching, studying, designing, or manufacturing diesel exhaust treatment
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`systems.”
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`14. Based on my experiences, I have a good understanding of the
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`capabilities of a POSITA. Indeed, I have taught, participated in organizations, and
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`worked closely with many such persons over the course of my career.
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`Interpretations of the ’709 Patent Claims at Issue
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`15.
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`I understand that, for purposes of my analysis in this inter partes
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`review proceeding, the terms appearing in the patent claims should be interpreted
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`according to their “broadest reasonable construction in light of the specification of
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`the patent in which it appears.” 37 C.F.R. § 42.100(b). In that regard, I understand
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`that the best indicator of claim meaning is its usage in the context of the patent
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`specification as understood by a POSITA. I further understand that the words of
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`the claims should be given their plain meaning unless that meaning is inconsistent
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`INTER PARTES REVIEW OF U.S. PATENT NO. 9,032,709
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`with the patent specification or the patent’s history of examination before the
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`Patent Office. I also understand that the words of the claims should be interpreted
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`as they would have been interpreted by a POSITA at the time of the invention was
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`made (not today); because I do not know at what date the invention as claimed was
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`made, I have used the earliest listed priority date of the ’709 patent, August 5,
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`2003, as the point in time for claim interpretation purposes.
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`Obviousness
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`Legal Principles
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`16.
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`I have been informed that a patent claim is invalid as “obvious” under
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`35 U.S.C. § 103 in light of one or more prior art references if it would have been
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`obvious to a POSITA, taking into account (1) the scope and content of the prior art,
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`(2) the differences between the prior art and the claims, (3) the level of ordinary
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`skill in the art, and (4) any so called “secondary considerations” of non-
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`obviousness, which include: (i) “long felt need” for the claimed invention, (ii)
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`commercial success attributable to the claimed invention, (iii) unexpected results
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`of the claimed invention, and (iv) “copying” of the claimed invention by others.
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`For purposes of my analysis above and because I know of no indication from the
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`patent owner or others to the contrary, I have applied a date of August 5, 2003, as
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`the date of invention in my obviousness analyses, although in many cases the same
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`analysis would hold true even at an earlier time than August 5, 2003.
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`17.
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`I have been informed that a claim can be obvious in light of a single
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`INTER PARTES REVIEW OF U.S. PATENT NO. 9,032,709
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`prior art reference or multiple prior art references. To be obvious in light of a
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`single prior art reference or multiple prior art references, there must be a reason to
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`modify the single prior art reference, or combine two or more references, in order
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`to achieve the claimed invention. This reason may come from a teaching,
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`suggestion, or motivation to combine, or may come from the reference or
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`references themselves, the knowledge or “common sense” of one skilled in the art,
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`or from the nature of the problem to be solved, and may be explicit or implicit
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`from the prior art as a whole. I have been informed that the combination or
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`modification of familiar elements according to known methods is likely to be
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`obvious when it does no more than yield predictable results. I also understand it is
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`improper to rely on hindsight in making the obviousness determination. KSR Int’l
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`Co. v. Teleflex Inc., 550 U.S. 398, 421 (2007).
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`18. Diesel engine emissions contain nitrogen oxides (NOx) and
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`Background
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`particulate matter, both of which are pollutants that countries seek to restrict
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`through the use of emissions standards. Combustion of fuel in a diesel engine
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`requires the presence of oxygen, which is typically supplied by mixing the fuel
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`with ambient air. A portion of the nitrogen and oxygen from this air will react in
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`the combustion chamber leading to the formation of NOx. Diesel engines also
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`produce a relatively large amount of soot, which is the result of the incomplete
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`combustion of the diesel fuel.
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`19. Due to the negative health and environmental impact of these
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`pollutants, the US government and other governments have set strict emission
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`standards for diesel-powered vehicles. Those emission standards set limits on the
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`permissible amount of NOx or particulate matter that may be released from
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`specific sources over specific timeframes. For example, in 1998 the European
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`Union Environment Council proposed new emission standards that sought to
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`reduce the emissions of NOx and particulate matter in two stages, with the first to
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`begin in 2005 and the second to begin in 2008. See Georg Hüthwohl, Bernd
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`Maurer and Gennadi Zikoridse, The SCRT® System – A Combination Particle
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`Filter with SCR Catalyst – Enables Both Particle and NOx Emission To Be
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`Reduced Simultaneously in Commercial Vehicle Diesel Engines, Proceedings of
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`the Dresden Motor Conference, held in May 1999 (“Hüthwohl”). As Hüthwohl
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`states, these two stages, known as Euro IV and Euro V, respectively, demanded
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`new emission treatment systems that significantly curtailed both particulate matter
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`emissions and NOx emissions, simultaneously. Id. at 2-3.
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`20. As of 2003, wall flow filters were one of the best means to curtail
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`particulate matter emissions. As the ’709 patent states, in 2003 they were a “key
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`aftertreatment technology in use” for “high particulate matter reduction” and were
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`“capable of removing over 90% of the particulate matter from diesel exhaust.”
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`’907 patent, col. 2, lines 4-4, 10-12. Wall flow filters remain one of the most
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`effective means to reduce particulate matter emissions. Hüthwohl recognized the
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`importance of wall flow filters in curbing particulate matter emissions, saying that
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`the Euro IV and Euro V emissions standards “can only [be] achieved by” using a
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`“particle filter.” Hüthwohl at 3. Hüthwohl states that its “particle filter” is the
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`same filter used by the “CRT® system,” id. at 2, which was known to be a wall
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`flow fitler. See Ronald M. Heck and Robert J. Farrauto with Suresh T. Gulati,
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`Catalytic Air Pollution Control 201 (2002) (“Heck”) (“the continuous regenerable
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`trap or (CRT) (trademark)” consists of a “wall flow trap or diesel particulate filter
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`(DPF)”).
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`21. At the time, Selective Catalytic Reduction (SCR) of NOx was the
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`most efficient means to curtail NOx emissions from diesel engine exhausts. As the
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`’023 patent states, in 2003 a “proven NOx abatement technology … [was]
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`Selective Catalytic Reduction (SCR),” ’023 patent, col. 2, lines 41-44, a
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`technology that was “capable of NOx reduction greater than 90%, and … thus
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`represents one of the best approaches for achieving aggressive NOx reduction
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`goals.” Id at col. 2, lines 46-49.
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`22. Known SCR catalysts at the time included platinum loaded onto high
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`surface area alumina, vanadium loaded onto high surface area titania, and copper
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`loaded on nanoporous particle zeolite. These SCR catalysts were well studied and
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`their properties well documented. For example, it was well known that these three
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`catalysts could convert NOx at different operating temperature ranges as
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`documented.
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`23. Other properties of these catalysts, such as their hydrothermal stability
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`(i.e., the catalyst’s ability to withstand high temperature without becoming
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`irreversibly deactivated) or their susceptibility to sulfur poising were well known.
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`24.
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`It was also well known that these catalysts could serve more than one
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`function in an exhaust gas treatment system. For example, the soot oxidation
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`capacity for platinum on alumina and for copper on zeolites were both studied and
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`documented. See Yasutake Teraoka, Kazunori Kanada, Hiroshi Furukawa, Isamu
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`Moriguchi, and Shuichi Kagawa, Simultaneous Catalytic Removal of Nitrogen
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`Oxides and Soot by Copper-Loaded MFI Zeolites, 30 Chemistry Letters 604
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`(2001) (“Teraoka”) (teaching that “Cu-loaded MFI zeolites showed the catalytic
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`activity for the oxidation of soot and reduction of NOx simultaneously”).
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`25. Accordingly, those skilled in the art could have easily selected an
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`appropriate catalyst for a particular function based on well documented properties
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`of that catalyst. For example, one could have selected a particular type SCR
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`catalyst based on factors such as the desired efficiency of the system and the
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`acceptable cost and complexity of the system. If an SCR process were chosen, a
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`INTER PARTES REVIEW OF U.S. PATENT NO. 9,032,709
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`person of ordinary skill in the art could have then matched known catlytic
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`materials to specific applications based on known properties of the catalysts.
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`A Person of Ordinary Skill in the Art Would Have Been Motivated To
`Permeate the Walls of a Wall Flow Filter with an SCR Catalyst
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`26. Diesel engine exhaust catalysts are heterogeneous and thus typically
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`have an active metal on a high surface area support (on a microscopic scale) to
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`increase the rates of the chemical reactions and the selectivity to the desired
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`product(s). Those catalysts are typically coated onto a honeycomb monolithic
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`substrate which provides a high geometric surface area of the active material.
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`Honeycomb substrates are those which have multiple parallel walls that define
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`channels which run along the axial length of the substrate. Examples of
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`honeycomb substrates include flow-through monoliths and wall-flow filters.
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`27. Shown below is a flow-through-monolith, where each channel is
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`unblocked and open at both the inlet and outlet ends.
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`28. Shown below is a wall-flow filter, with each channel blocked at one
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`end of the substrate body and alternate channels blocked at opposite end-faces.
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`See Heck at 217:
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`29. As of 2003, vanadium, copper or iron were all well-known SCR
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`catalysts. Copper and iron containing catalysts were commonly loaded on a
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`zeolite. A zeolite is a microporous crystalline material comprising aluminosilicate.
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`Copper and iron can be loaded onto the zeolite by ion exchange or similar process.
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`As of 2003, ZSM-5 and beta zeolites were well known as being suitable for SCR
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`applications. Supporting the iron or copper catalyst in a zeolite was known to
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`improve the selectivity in converting NOx to the innocuous (benign) byproducts of
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`the SCR reaction.
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`30.
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`In the SCR process, NOx is reduced with a reductant, such as
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`INTER PARTES REVIEW OF U.S. PATENT NO. 9,032,709
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`ammonia (NH3), into two innocuous byproducts, nitrogen gas and water, over a
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`catalyst. The reaction (unbalanced), in general terms, is depicted below:
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`NH3 + NOx + O2 → N2 + H2O
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`31. Diesel engine exhaust gas generally does not contain ammonia, and
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`thus an ammonia-based SCR process to reduce NOx emissions requires a source of
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`reductant supplied to the exhaust stream. The most prevalent source of reductant
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`as of 2003 was a reductant dosing system that injected the reductant into the
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`exhaust stream. Such dosing systems were well known in the art as of 2003, as the
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`’709 patent describes. See ’709 patent, col. 10, lines 19-32. It was known in the
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`art that such dosing systems could inject ammonia directly into the system, or
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`instead some type of ammonia precursor like aqueous urea solution.
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`32. There would have been, as of 2003, a strong desire to combine an
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`SCR catalyst with a wall flow filter. Specifically, there would have been a strong
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`desire to use a single substrate—a wall flow filter—to remove two known
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`pollutants—particulate matter and NOx. As of 2003, both pollutants were the
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`subject of tightening emissions standards, and industry was seeking to develop a
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`diesel exhaust treatment system that could aggressively reduce the emissions of
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`both simultaneously.
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`33. Hüthwohl taught that exactly such a solution was needed to achieve
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`the aggressive emission reductions required by the newly proposed Euro IV & V
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`emissions standards. Specifically, Hüthwohl states that “excellent emission
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`values” can “only be achieved” by combining a particle filter with an SCR catalyst.
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`Hüthwohl at 3.
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`34. Combining a wall flow filter with an SCR catalyst would have had
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`many well-known advantages, including a decrease in the amount of space needed
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`to accommodate the dual functions of particulate matter removal function and NOx
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`reduction. Performing the SCR and particulate filtration functions using separate
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`substrates, (e.g., loading the SCR catalyst on a substrate other than the particulate
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`filter) would likely require more space than using one substrate for both functions
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`For example, Hüthwohl teaches about how “[c]urrent SCR catalysts cannot be
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`accommodated in the physical volume of today’s city buses,” Hüthwohl at 3, and
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`furthermore, that “[i]t is disproportionately more difficult to integrate a[n
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`additional] particle filter” into that same system. Id. Space is a valuable
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`commodity in all diesel exhaust treatment systems. Thus, a lower system volume
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`would have many known benefits.
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`35.
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`In light of the newly proposed emissions standards, industry would
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`have followed the teachings of Huethwohl so that products could effectively serve
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`two needed functions—particulate matter removal and NOx reduction—using only
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`a single substrate, a wall flow filter. The selection of specific SCR catalytic
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`materials would have been mere optimization of known catalyst features with
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`known filter substrates.
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`36. Hüthwohl provided a person of ordinary skill the reasonable
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`expectation that the resulting emission treatment system would work as intended—
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`i.e., to simultaneously reduce NOx and particulate matter emissions—because the
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`Hüthwohl system did in fact achieve the reduction of both pollutants. That is,
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`there would have been a reasonable expectation of success because the Hüthwohl
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`system had already accomplished the simultaneous reduction of both NOx and
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`particulate matter emissions.
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`The Iron and Copper Zeolites Taught By Speronello Would Have Been the
`Preferred Candidates To Load Inside A Wall Flow Filter
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`37. Speronello describes iron and copper zeolites as SCR catalysts and it
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`is clear that SCR catalysts of the ’709 patent are nothing more than the Speronello
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`catalysts loaded into a wall flow filter. The teachings of Speronello suggest that
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`these copper and iron zeolite catalysts would be just as applicable to a wall flow
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`filter as to a conventional flow through substrate. In fact, the catalytic material in
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`the claims of the ’709 patent are often almost identical to the teachings of
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`Speranello.
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`38. When selecting an SCR catalyst to load onto a wall flow filter, the
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`iron and copper zeolites disclosed by the Speronello patent would have been
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`preferred catalyst. Those catalysts were known to be stable at high temperatures,
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`resistant to sulfur degradation, and active and selective over a wide range of
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`temperatures—all crucial considerations for use in a diesel exhaust treatment
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`system. Further, as of 2003, industry appreciated that these three catalyst
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`characteristics were crucial when developing a diesel exhaust treatment system.
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`As of 2003, catalysts of the type taught by Speronello had been the subject of
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`extensive research and were well-known to be active for SCR.
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`39. With respect to stability at high temperatures, the filter often must be
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`heated to high temperatures in order to “regenerate” the filter, i.e., to burn off the
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`trapped soot. This property is distinct from the catalyst’s operating temperature
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`which is the temperature range within which the catalyst effectively converts NOx
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`into N2 and water. These two properties of a catalyst are independent of each
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`other.
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`40. The ’709 patent acknowledges that “the catalyst composition must be
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`durable so that it maintains its SCR catalytic activity even after prolonged
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`exposure to higher temperatures that are characteristic of filter regeneration.” ’709
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`patent, col. 3, lines 3-6, and states that iron or copper zeolites display “thermal
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`resistance to temperatures greater than 650° C.” Id. at col. 7, lines 51-53.
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`Speronello teaches that its “promoted zeolite materials demonstrate sufficient
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`thermal and hydrothermal stability to … provide an acceptably long life and
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`efficiency of the catalysts.” Id. at col. 6, lines 22-25. Speronello also teaches
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`catalyst compositions capable of “effective[ly] … reduc[ing] nitrogen oxides with
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`ammonia” “at a temperature of from about 200° C. to 600° C.”). Id. at claim 5.
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`There appears to be no material difference between the copper and iron zeolite
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`catalysts described in Speronello and the copper and iron zeolite catalysts
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`encompassed by the claims of the ’709 patent. The ’709 patent does not suggest
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`any special treatment or modification of the SCR catalyst described by Speronello.
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`Thus, the catalyst thermal durability claimed by in the ’709 patent is an inherent
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`feature of the catalyst described in Speronello. A skilled artisan would have
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`recognized that the Speronello catalysts would have adequate thermal durability
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`for use in a catalyzed wall-flow filter.
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`41. With respect to resistance to sulfur degradation, diesel emissions were
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`known to include sulfur. The sulfur present in diesel exhaust was known to be able
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`to poison the catalyst, decreasing its activity and necessitating more frequent
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`regeneration of the catalyst. Thus, it would have been desirable for the selected
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`SCR catalyst to be resistant to sulfur poisoning. The ’709 patent acknowledges
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`this common sense principle, saying that resistance to degradation by sulfur is an
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`important consideration, ’709 patent, col. 8, lines 3-5, and recognizing that
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`Speronello teaches that its iron or copper zeolites “are resistant to sulfur
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`poisoning.” Id. (referring to zeolites used in the “[s]uitable SCR compositions”
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`described by Speronello and another other prior art patent, see id. at col. 7, lines
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`58-61).
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`42.
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`In general, the more active the catalyst, less catalyst is needed to
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`adequately reduce the emissions of pollutants. This is beneficial for a number of
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`reasons, including to lower the overall cost of the system and to use a smaller
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`system volume. A lower system volume has many known benefits, including to
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`save space in the diesel exhaust aftertreatment system; space is a valuable
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`commodity in all diesel exhaust aftertreatment systems. With respect to the
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`activity and selectivity of the Speronello catalysts, the reference teaches that its
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`catalysts “provide a simple and relatively inexpensive means for efficiently
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`catalyzing the reduction of nitrogen oxides.” Speronello at col. 16, lines 44-49.
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`As Figure 2 of Speronello shows, the efficient means of catalyzing the reduction of
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`NOx worked over a wide range of temperatures. See id. at Figure 2 (showing high
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`NOx conversion efficiency from about 350 to 600° C). Importantly, the range over
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`which the Speronello catalysts work efficiently in reducing NOx matches the
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`temperature of needed for use in a diesel exhaust system. The ’709 patent—in
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`“EXAMPLE 4: Evaluation of NOx Conversion and Particulate Removal for
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`Coated Soot Filters”—demonstrates the NOx conversion efficiency of its claimed
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`catalysts at a “controlled” “filter inlet temperature of 370° C.” See ’709 patent,
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`Example 4. As Figure 2 in Speronello demonstrates, the base metal zeolite
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`INTER PARTES REVIEW OF U.S. PATENT NO. 9,032,709
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`catalysts disclosed by Speronello would have been expected to provide very
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`efficient NOx conversion at that temperature, with a NOx conversion efficiency
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`approaching 90%. Further, those same base metal zeolite catalysts would have
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`maintained a satisfactory NOx conversion efficiency (i.e., above 80% NOx
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`conversion efficiency) all the way up to 550° C. See Speronello, Figure 2. The
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`Speronello catalysts, therefore, would have been a preferable option when
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`selecting an efficient catalyst, and their activity would have directly led to cost and
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`space savings in the diesel emission aftertreatment system.
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`43. Furthermore, the Speronello catalysts were active over a wide range
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`of temperatures, which is a factor when selecting a catalyst for use in diesel
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`exhaust treatment systems. See Speronello, Figure 2; see also id. at claim 5
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`(claiming a base metal zeolite catalyst capable of “effective[ly] … reduc[ing]
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`nitrogen oxides with ammonia” “at a temperature of from about 200° C. to 600°
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`C.”). Such systems were known to experience a wide range of temperatures, based
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`on how hot the emissions were from the diesel engine. If an SCR catalyst only
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`worked effectively at a limited temperature range, then NOx would escape when
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`the engine is operated at a temperature outside that limited range. This would be
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`undesirable, because it would prevent the SCR catalyst from achieving the
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`aggressive NOx reduction goals required by the impending emissions standards.
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`INTER PARTES REVIEW OF U.S. PATENT NO. 9,032,709
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`44. Another routine design parameter is the space velocity (SV), that is
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`the ratio of the volumetric flow rate to the total volume of the monolith catalyst
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`(units of inverse hours, h-1). This factor determines the residence time that the
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`exhaust gas is in contact with the catalyst and is provided in units independent
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`from the dimensions of the filter. For example, a highly active catalyst will
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`convert NOx more quickly, thus the SV of the exhaust gas may be increased while
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`maintaining adequate catalyst contact time for good conversion. The Speronello
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`catalysts were active at a very high space velocity of 1.2 x 106 cc/g h for a powder
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`catalyst. This is equivalent to a space velocity of about 220,000 h-1 were the power
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`supported as a washcoat on a monolith substrate at a typical loading of 3 g/in3. For
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`example, both Cu- and Fe-exchanged beta zeolite catalysts achieved over 80%
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`conversion above about 350o C at the stated space velocity. A person of ordinary
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`skill in the art would recognize these catalysts to be active SCR catalysts.
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`45.
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`It is clear that SCR catalysts of the ’709 patent are nothing more than
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`the Speronello catalysts loaded into a wall flow filter. As described above, the
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`claims of the ’709 patent are often almost identical to the teachings of the ’709
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`patent. For example, the ’709 patent requires catalyst washcoat loadings of up to
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`2.4 g.in3 or of at least 1.3 g/in3, whereas Speronello teaches at least seven SCR
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`catalyst compositions, all following within those claimed ranges:
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` col. 8, lines 57-60 (Catalyst I: 1.6 g/in3 of a copper zeolite catalyst);
` col. 9, lines 26-29 (Catalyst II: 1.7 g/in3 of a copper zeolite catalyst);
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`INTER PARTES REVIEW OF U.S. PATENT NO. 9,032,709
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` col. 9, lines 60-64 (Catalyst III: 1.5 g/in3 of a copper zeolite catalyst);
` col. 10, lines 26-30 (Catalyst IV: 2.0 g/in3 of a copper zeolite catalyst);
` col. 10, lines 64-67 (Catalyst V: 1.8 g/in3 of a copper zeolite catalyst);
` col. 11, lines 39-42 (Catalyst VI: 1.5 g/in3 of a copper zeolite catalyst);
` col. 12, lines 45-48 (Catalyst VII: 1.7 g/in3 of a copper zeolite catalyst).
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`46.
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`In addition to knowing that an SCR catalyst could be applied to a
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`wall-flow filter and that metal zeolites are obvious choices for such catalysts, a
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`POSITA would have readily known the amount of metal zeolite catalyst washcoat
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`necessary for good NOx conversion in most applications would be between 1.6 and
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`2.4 g/in3, as shown in Speranello. Moreover, a POSITA would have known that
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`the amount of catalyst washcoat required for effective NOx conversion would be
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`the same whether it was applied to a flowthrough substrate or a wall-flow filter.
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`Due to the fast response time of the SCR catalyst, the kinetics of the SCR reaction
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`would not be that different for a flow-through SCR compared to an SCR catalyst
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`on a filter. Thus, a POSITA would know that metal zeolite catalyst could be
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`applied to a filter at the same loadings disclosed in Speranello.
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`47. Having reviewed all claims of the ’709 patent, it is thus clear that the
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`’709 patent does nothing more than take the SCR catalyst composition taught by
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`Speronello and load it onto a wall flow filter. The ’709 patent makes no advances
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`of its own with respect to the activity or selectivity or durability of the SCR
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`catalyst composition.
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`INTER PARTES REVIEW OF U.S. PATENT NO. 9,032,709
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`It Was Known That Copper Zeolites Could Simultaneously Catalyze the
`Oxidation of Soot and the Reduction of NOx
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`48. As of August 5, 2003, it was known that several metal catalysts—
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`including copper zeolites—could catalyze the oxidation of soot. The Teraoka
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`article, in fact, is entitled “Simultaneous Catalytic Removal of Nitrogen Oxides
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`and Soot by Copper-Loaded MFI Zeolites.” Teraoka concludes that “Cu-loaded
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`MFI zeolites showed the catalytic activity for the oxidation of soot and reduction
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`of NOx simultaneously in the soot–NOx–O2 reaction system.” Teraoka at
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`Abstract.
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`49. Copper can oxidize soot via the production of NO2. NO2 is a strong
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`oxidant and will readily react with carbon soot to convert it into CO2 and water.
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`Copper was well-known as a catalyst for the oxidation of NO to NO2. See, e.g., M.
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`Shelef et al., NO2 formation over Cu-ZSM-5 and the selective catalytic reduction
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`of NO, 26 Catalysis Letter 277 (1994). (Thus a typical SCR reaction not only
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`reduces NO and NO2 to N2 and water, but also converts a certain amount of NO to
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`NO2 as a by-product.) NO2, in turn, was known to “oxidize the dry carbon soot
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`held within the trap [i.e., wall flow filter]….” Heck at 202. In fact, using NO2 to
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`oxidize the soot trapped in a wall flow filter was—as of 2002 when Heck was
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`published—the “most successful approach to date for combusting … dry soot.” Id.
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`Heck describes the process and the reactions through which NO2 can combust
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`accumulated soot (where C in the equation below is the soot).
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`INTER PARTES REVIEW OF U.S. PATENT NO. 9,032,709
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`50.
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`In addition to the copper catalyst, it is often desirable to increase the
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`ratio of NO to NO2 via an upstream diesel oxidation catalyst. This NO2 could then
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`oxidize the accumulated soot:
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`51. Heck discusses these general principles specific
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