UNITED STATES PATENT AND TRADEMARK OFFICE
`
`BEFORE THE PATENT TRIAL AND APPEAL BOARD
`
`Sony Corporation
`Petitioner
`v.
`UChicago Argonne, LLC
`Patent Owner
`
` Case IPR2015-01521
`Patent No. 6,680,143
`
`DECLARATION OF KUZHIKALAIL M. ABRAHAM PH.D.
`
`
`
`
`
`
`
`
`
`
`
`
`
`SONY EXHIBIT 1002
`
`Page 1 of 130
`
`

`
`TABLE OF CONTENTS
`
`INTRODUCTION ........................................................................................... 1
`
`QUALIFICATIONS ........................................................................................ 1
`
`
`I.
`
`II.
`
`III.
`
`INFORMATION CONSIDERED ................................................................... 9
`
`IV. LEGAL STANDARD ................................................................................... 11
`
`V.
`
`PRIORITY DATE AND PERSON OF ORDINARY SKILL IN THE
`ART ............................................................................................................... 13
`
`VI. TECHNOLOGY BACKGROUND ............................................................... 13
`
`A.
`
`B.
`
`Battery and Electrochemical Cell ........................................................ 13
`
`Lithium Metal Oxide Positive Electrodes ........................................... 16
`
`1.
`
`Layered LiMO2 structures were well known in the art ............ 16
`
`VII. OVERVIEW OF THE ’143 PATENT .......................................................... 20
`
`VIII. CLAIM CONSTRUCTION .......................................................................... 21
`
`A.
`
`B.
`
`C.
`
`“positive electrode” (claims 1 and 17) ................................................ 22
`
`“prepared in its initial discharged state” (claim 1)/ “having in its
`initial discharged state” (claim 17)...................................................... 26
`
`“both the LiMO2 and Li2M’O3 components being
`layered”(claims 1 and 17) ................................................................... 26
`
`D.
`
`“M and M’ are disordered in the electrode structure” (claim 4) ......... 27
`
`IX. CERTAIN REFERENCES DISCLOSE AND/OR RENDER
`OBVIOUS ALL FEATURES OF CLAIMS 1-4, 8, 9 AND 17 OF
`THE ’143 PATENT ....................................................................................... 28
`
`A.
`
`Neudecker discloses all of the features of claims 1-4, 8, 9, and
`17 ......................................................................................................... 28
`
`
`
`i
`
`Page 2 of 130
`
`

`
`1.
`
`Claim 1 ...................................................................................... 30
`
`a)
`
`b)
`
`c)
`
`d)
`
`e)
`
`f)
`
`a)
`
`b)
`
`“A lithium metal oxide positive electrode for a
`non-aqueous lithium cell” ............................................... 30
`
`“prepared in its initial discharged state” ......................... 32
`
`“having a general formula xLiMO2∙(1−x)Li2M’O3”
` ........................................................................................ 34
`
`“in which 0<x<1” ........................................................... 40
`
`“where M is one or more ions having an average
`oxidation state of three with at least one ion being
`Mn” ................................................................................. 41
`
`“where M’ is one or more ions with an average
`oxidation state of four” ................................................... 42
`
`“both the LiMO2 and Li2M’O3 components being
`layered” ........................................................................... 43
`
`“the ratio of Li to M and M’ being greater than one
`and less than two” ........................................................... 45
`
`2.
`
`3.
`
`4.
`
`5.
`
`6.
`
`7.
`
`Claim 2 ...................................................................................... 46
`
`Claim 3 ...................................................................................... 48
`
`Claim 4 ...................................................................................... 49
`
`Claim 8 ...................................................................................... 50
`
`Claim 9 ...................................................................................... 50
`
`Claim 17 .................................................................................... 51
`
`B.
`
`C.
`
`Alternatively, part 1 of Neudecker combined with the general
`knowledge of one of ordinary skill in the art renders claims 1-4,
`8, 9, and 17 obvious. ........................................................................... 52
`
`Rossen discloses all of the features of claims 1-4, 8, 9, and 17 .......... 55
`ii
`
`
`
`Page 3 of 130
`
`

`
`1.
`
`Claim 1 ...................................................................................... 57
`
`a)
`
`b)
`
`c)
`
`d)
`
`e)
`
`f)
`
`g)
`
`h)
`
`“A lithium metal oxide positive electrode for a
`non-aqueous lithium cell” ............................................... 57
`
`“prepared in its initial discharged state” ......................... 58
`
`“having a general formula xLiMO2∙(1−x)Li2M’O3”
` ........................................................................................ 61
`
`“in which 0<x<1” ........................................................... 67
`
`“where M is one or more ions having an average
`oxidation state of three with at least one ion being
`Mn” ................................................................................. 68
`
`“where M’ is one or more ions with an average
`oxidation state of four” ................................................... 70
`
`“both the LiMO2 and Li2M’O3 components being
`layered” ........................................................................... 70
`
`“the ratio of Li to M and M’ being greater than one
`and less than two” ........................................................... 73
`
`2.
`
`3.
`
`4.
`
`5.
`
`6.
`
`7.
`
`Claim 2 ...................................................................................... 73
`
`Claim 3 ...................................................................................... 74
`
`Claim 4 ...................................................................................... 75
`
`Claim 8 ...................................................................................... 77
`
`Claim 9 ...................................................................................... 78
`
`Claim 17 .................................................................................... 78
`
`D.
`
`Rossouw discloses all of the features claims 1, 2, 3, 8, and 9 ............. 79
`
`1.
`
`Claim 1 ...................................................................................... 82
`
`
`
`iii
`
`Page 4 of 130
`
`

`
`a)
`
`b)
`
`c)
`
`d)
`
`e)
`
`f)
`
`g)
`
`h)
`
`“A lithium metal oxide positive electrode for a
`non-aqueous lithium cell” ............................................... 82
`
`“prepared in its initial discharged state” ......................... 83
`
`“having a general formula xLiMO2∙(1−x)Li2M’O3”
` ........................................................................................ 86
`
`“in which 0<x<1” ........................................................... 87
`
`where M is one or more ions with an average
`oxidation state of three with at least one ion being
`Mn ................................................................................... 88
`
`where M’ is one or more ions with an average
`oxidation state of four ..................................................... 89
`
`both the LiMO2 and Li2M’O3 components being
`layered ............................................................................. 90
`
`the ratio of Li to M and M’ being greater than one
`and less than two ............................................................. 93
`
`2.
`
`3.
`
`4.
`
`5.
`
`Claim 2 ...................................................................................... 93
`
`Claim 3 ...................................................................................... 94
`
`Claim 8 ...................................................................................... 94
`
`Claim 9 ...................................................................................... 95
`
`Rossouw renders claims 1-3, 8, and 9 obvious.................................... 95
`
`Rossouw in view of Linden renders obvious claim 17........................ 96
`
`E.
`
`F.
`
`X. Declaration ..................................................................................................... 98
`
`
`
`iv
`
`Page 5 of 130
`
`

`
`
`
`I.
`
`I, Kuzhikalail M. Abraham, declare as follows:
`
`INTRODUCTION
`
`1.
`
`I have been retained by Sony Corporation (“Petitioner”) as an
`
`independent expert consultant in this proceeding before the United States Patent
`
`and Trademark Office. Although I am being compensated at my usual rate of
`
`$450.00 per hour for the time I spend on this matter, no part of my compensation
`
`depends on the outcome of this proceeding, and I have no other interest in this
`
`proceeding.
`
`2.
`
`I understand that this proceeding involves U.S. Patent No. 6,680,143
`
`(“the ’143 patent”) (Ex. 1001).
`
`3.
`
`I have been asked to consider whether certain references disclose or
`
`suggest the features of claims 1-4, 8, 9, and 17 of the ’143 patent. My opinions are
`
`set forth below.
`
`II. QUALIFICATIONS
`
`4.
`
`I received a Bachelor of Science degree in chemistry from Kerala
`
`University, Kerala, India in 1965 and a Master of Science degree in Chemistry
`
`from the same university in 1967. I then obtained a Ph.D. degree in chemistry from
`
`Tufts University, Medford, Massachusetts, USA in 1973. Following my graduation
`
`from Tufts University, I conducted post-doctoral research at Vanderbilt University
`
`in Nashville, Tennessee and Massachusetts Institute of Technology in Cambridge,
`
`
`
`1
`
`Page 6 of 130
`
`

`
`Massachusetts from 1973 to 1975. My curriculum vita, which includes a detailed
`
`summary of my background, experience, and publications, is attached in the
`
`Appendix A.
`
`5.
`
`After my education and post-doctoral research training, I began my
`
`professional career at EIC Laboratories Inc., Norwood, Massachusetts in 1976.
`
`During the twenty-one years of my tenure at EIC Laboratories, I held the positions
`
`of Senior Scientist (1976-1979), Group Leader (1979-1984), Head of Lithium
`
`Battery Research (1984-1992), and Vice President and Director of Research (1992-
`
`1997). All of my work at EIC was concerned with research and development of
`
`lithium and lithium-ion battery materials including cathode and anode active
`
`materials and electrolytes, and the design, fabrication, testing, and characterization
`
`of battery prototypes. In 1997, I was appointed president of Covalent Associates
`
`Inc., Woburn, Massachusetts, where I remained until 2000. At Covalent I
`
`continued my research and development activities on lithium batteries along with
`
`my administrative duties.
`
`6.
`
`In 2000, I started my consulting company, E-KEM Sciences, in
`
`Needham, Massachusetts, to provide technical advice on the research and
`
`development of battery technologies with an emphasis on lithium and lithium-ion
`
`batteries. My clients have included private companies, government agencies,
`
`
`
`2
`
`Page 7 of 130
`
`

`
`research organizations and attorneys’ clients. I have continued my consulting
`
`activities to the present time.
`
`7.
`
`In 2006, I became a Research Professor on a part time basis at the
`
`Northeastern University Center for Renewable Energy Technology (NUCRET) at
`
`Northeastern University, Boston, Massachusetts. In this position, I supervise the
`
`M.S. and Ph.D. degree thesis work of graduate students conducting research on
`
`materials for advanced lithium and lithium-ion batteries.
`
`8. My areas of expertise include materials processing and fabrication,
`
`with applications in energy, such as electrochemical cells, including rechargeable
`
`lithium and lithium-ion batteries. My various technical contributions in lithium and
`
`lithium-ion battery technology are summarized in 209 technical publications and
`
`15 United States patents which are listed in my curriculum vita. (Appendix A). I
`
`have also made numerous meeting presentations worldwide on my research results
`
`including the 57 invited talks listed in my resume. Appendix A.
`
`9.
`
`During my thirty-eight year career in the lithium battery technology
`
`area, in both industry and university research, I have made many pioneering
`
`contributions to the development of rechargeable lithium and lithium-ion batteries.
`
`These include, but are not limited to:
`
`- Being among the first to demonstrate a practical rechargeable lithium
`
`battery with long cycle life. These batteries are the precursors to today’s
`
`
`
`3
`
`Page 8 of 130
`
`

`
`lithium-ion batteries. See Appendix A (Publication Numbers 16 and 25 in
`
`Abraham Resume: “Secondary Lithium Cells,” Proceedings of the
`
`Symposium on Power Sources for Biomedical Implantable Applications
`
`and Ambient Temperature Lithium Batteries, B. B. Owens and N.
`
`Margalit, eds., the Electrochemical Society, 80-4, 384 (1980), and
`
`“Rechargeable Li/Vanadium-Oxide Cells Utilizing 2Me-THF/LiAsF6,”
`
`Journal of the Electrochemical Society, 128, 2493 (1981));
`
`- Being among the first to demonstrate a rechargeable Lithium-Sulfur
`
`battery which is currently developed world-wide. See Appendix A
`
`(Publication Number 13: “A Lithium/Dissolved Sulfur Battery with an
`
`Organic Electrolyte,” Journal of the Electrochemical Society, 126, 523
`
`(1979));
`
`- Studied the various factors affecting the performance of high power
`
`lithium batteries leading to the demonstration high rate lithium cells with
`
`LiCoO2 cathodes and nonaqueous liquid electrolytes, and high pulse
`
`power Li-ion cells with LiNiO2 cathodes and gel polymer electrolytes.
`
`Appendix A (Publication Numbers 127, 108 and 131: “Discharge Rate
`
`Capability of the LiCoO2 Electrode,” Journal of the Electrochemical
`
`Society, 145, 482 (1998); “Solid-State Carbon/LiNiO2 Pulse Power
`
`Batteries,” in Proceedings of the 36th International Power Sources
`
`
`
`4
`
`Page 9 of 130
`
`

`
`Symposium, published by IEEE, New York, NY (1994); and “Synthesis
`
`and Characterization of LiNiO2 as a Cathode Material for Pulse Power
`
`Batteries,” in Proceedings of the Symposium, Materials For
`
`Electrochemical Energy Storage and Conversion II - Batteries,
`
`Capacitors and Fuel Cells, Fall Materials Research Society Meeting,
`
`Boston, MA. December 1-5, 1997;
`
`- Synthesized and characterized lithium manganese oxide spinel cathode
`
`materials and studied their electrochemical performance in lithium and
`
`lithium-ion cells. Appendix A (Publication numbers 119, 129 and 130:
`
`“Preparation and Characterization of Micron-sized Spinel LiMn2O4,’
`
`Journal of the Electrochemical Society, 143, 1591 (1996); “The
`
`Li4Ti5O12//PAN Electrolyte//LiMn2O4 Rechargeable Battery with
`
`Passivation-Free Electrodes,” Journal of the Electrochemical Society,
`
`145, 2615 (1998); “Preparation and Electrochemical Characterization of
`
`Overlithiated Spinel LiMn2O4,” Journal of the Electrochemical Society,
`
`145, 1131 (1998);
`
`-
`
`Invented a non-aqueous rechargeable Li-air battery which is being
`
`pursued worldwide. Appendix A (Patent Number 12: U.S. Pat. No.
`
`5,510,209);
`
`
`
`5
`
`Page 10 of 130
`
`

`
`- Synthesized and characterized Li-rich layered metal oxide cathode
`
`materials with improved electrochemical properties. These include the
`
`preparation of a new sodium substituted cathode material in which the
`
`voltage decay and the layer to spinel conversion during long-term cycling
`
`have been mitigated, and another Li rich cathode material with a new
`
`morphology exhibiting high rate cycling capability. Appendix A
`
`(Publication Numbers 188, 200, 208 and 209: “Mitigation of Layered to
`
`Spinel Conversion of a Li-rich Layered Metal Oxide Cathode Material
`
`for Li-ion Batteries,” Journal of the Electrochemical Society, 161, A290
`
`(2014); “A Li-rich Layered Cathode Material with Enhanced Structural
`
`Stability and Rate Capability for Li-on Batteries,” Journal of the
`
`Electrochemical Society, 161, A355 (2014); “A High Rate Li-Rich
`
`Layered MNC Cathode Material for Lithium-ion Batteries,” Royal
`
`Society of Chemistry Advances, RSC Adv., 5, 27375 (2015); “A Search
`
`for the Optimum Lithium Rich Layered Metal Oxide Cathode Material
`
`for Li-ion Batteries,” Journal of the Electrochemical Society, 162, A1236
`
`(2015).
`
`10.
`
`In my consulting activities I have advised clients on lithium primary
`
`and secondary battery technologies. These included research, development and
`
`characterization of advanced electrode, electrolyte and separator materials for Li-
`
`
`
`6
`
`Page 11 of 130
`
`

`
`ion batteries, battery design and optimization, lithium battery performance and
`
`safety, prototype development, battery manufacturing, and applications of Li-ion
`
`batteries.
`
`11.
`
`I have provided expert opinions before the Board in proceedings
`
`related to separators in Li-ion batteries, in proceedings involving allegations of
`
`patent infringement, and in court cases involving allegations of product liabilities
`
`liability resulting from cellphone and laptop computer Li-ion battery fires.
`
`12.
`
`I have won many awards for my contributions to the field of lithium
`
`and lithium ion batteries. These include:
`
`- Battery Research Award from the Electrochemical Society, Pennington,
`
`NJ, the premier society for battery chemists and engineers in the world,
`
`for my contributions to primary and secondary lithium batteries;
`
`- National Aeronautics and Space Administration (NASA) Group
`
`Achievement Award for the Rechargeable Battery Team, 1995, for my
`
`contributions to the development of NASA’s rechargeable battery
`
`technology; I also won NASA Certificates of Merit for Invention in 1983
`
`and 1997;
`
`- Elected Fellow of the Electrochemical Society, Pennington, NJ; elected
`
`in 2000;
`
`
`
`7
`
`Page 12 of 130
`
`

`
`- Elected Fellow of the American Institute of Chemists; elected in 1986;
`
`and
`
`- Elected Fellow of the Royal Society of Chemistry, United Kingdom,
`
`elected in 2013.
`
`13.
`
`I served as a member of the Editorial Board of the Journal of Power
`
`Sources from 1982-2010.
`
`14.
`
`I served as a reviewer of lithium battery proposals for several
`
`international organizations including Canada Research Council (Canada Research
`
`Chair Selection), Netherlands Foundation for Fundamental Research on Matter,
`
`and Exact Sciences & Technology Israel Science Foundation.
`
`15.
`
`I am a reviewer for battery articles submitted for publication in many
`
`journals including: The Journal of the Electrochemical Society; Electrochimica
`
`Acta; Electrochemistry Communications; Journal of Applied Electrochemistry;
`
`Journal of Power Sources; Chemical Communications; Science; Nature; Journal of
`
`The American Chemical Society; Journal of Physical Chemistry; and Ionics.
`
`
`
`
`
`
`
`8
`
`Page 13 of 130
`
`

`
`III.
`
`INFORMATION CONSIDERED
`
`16. The opinions summarized in this Declaration are based on the
`
`documents I reviewed and my knowledge and professional judgment. In forming
`
`my opinions, I reviewed the documents listed below:
`
`• The ’143 patent (Ex. 1001);
`
`• The prosecution history of the ’143 patent (Ex. 1003);
`
`• The prosecution history of U.S. Patent No. 6,677,082 (“the ’082
`
`patent”) (Ex. 1004);
`
`• Patent Reexamination History of the ’082 patent (Ex. 1005);
`
`• Neudecker et al., “Lithium Manganese Nickel Oxides Lix(MnyNi1-y)2-
`
`xO2, Part 1 Synthesis and Characterization of Thin Films and Bulk
`
`Phases, and Part 2 Electrochemical Studies on Thin-Film Batteries,” J.
`
`Electrochem. Soc., vol. 145, pp. 4148-4168 (1998) (“Neudecker”)
`
`(Ex. 1010);
`
`• Rossen et al., “Structure and Electrochemistry of LixMnyNi1-yO2,”
`
`Solid State Ionics, Vol. 57, pp. 311-318 (1992) (“Rossen”) (Ex. 1011);
`
`• the ’082 patent (Ex. 1012);
`
`• Thackeray et al., “Li2MnO3–stabilized LiMO2 (M=Mn, Ni, Co)
`
`electrodes for lithium-ion batteries,” J. Mater. Chem., Vol. 17, pp.
`
`3112-3125 (2007) (“Thackeray 2007”) (Ex. 1013);
`
`
`
`9
`
`Page 14 of 130
`
`

`
`• Thackeray, “Lithiated Oxides for Lithium-Ion Batteries,” The 186th
`
`meeting, the Electrochemical Society Symposium, October 9-14,
`
`1994, Miami Beach, Florida, published in January 1, 1995
`
`(“Thackeray 1994”) (Ex. 1014);
`
`• Bruce, “Solid-state chemistry of lithium power sources,” Chem.
`
`Commc’n, 1817-1824 (1997) (“Bruce 1997”) (Ex. 1015);
`
`• Armstrong et al., “Synthesis of Layered LiMnO2 as an electrode for
`
`rechargeable lithium batteries,” Nature, vol. 381, pages 499-500
`
`(1996) (“Armstrong”) (Ex. 1016);
`
`• U.S. Patent No. 6,214,493 to Bruce et al. (2001) (“Bruce”) (Ex. 1017);
`
`• U.S. Patent No. 5,153,081 to Thackeray et al. (1992) (“Thackeray
`
`1992”) (Ex. 1018);
`
`• Rossouw et al., “Synthesis and Structural Characterization of a Novel
`
`Layered Lithium Manganese Oxide, Li0.36Mn0.91O2, and its Lithiated
`
`Derivative, Li1.09Mn0.91O2,” Journal of Solid State Chem., vol. 104,
`
`pp. 464-466 (1993) (“Rossouw”) (Ex. 1019);.
`
`• Japanese Laid-Open Patent Publication No. JP-A-8-37007, published
`
`on February 6, 1996 (“Yoshio”) and a certified English-language
`
`translation thereof. (Ex. 1020);
`
`
`
`10
`
`Page 15 of 130
`
`

`
`• Numata et al., “Synthesis of Solid Solutions in a System of LiCoO2-
`
`Li2MnO3 for Cathode Materials of Secondary Lithium Batteries,”
`
`Chemistry Letters (1997), pp. 725-726 (“Numata”) (Ex. 1021);.
`
`• Thackeray’s Presentation to the USPTO of April 15, 2013 during ex
`
`parte reexamination of the ’082 patent. (Ex. 1005 at 538-563);
`
`• Excerpts from Linden, Handbook of Batteries, 2nd Edition (1995), pp.
`
`1.3-1.5, 14.7, 36.4-36.17, 36.22-36.27, 36.42-36.59, A.1, A.2, A.7,
`
`A.8 (“Linden”) (Ex. 1023);
`
`• Web page, Oak Ridge National Laboratory,
`
`(http://web.ornl.gov/sci/physical_sciences_directorate/mst/pcm/public
`
`ations.shtml) (Ex. 1025).
`
`IV. LEGAL STANDARD
`
`17.
`
`In formulating my opinions and conclusions, I have been provided
`
`with an understanding of the prevailing principles of U.S. patent law that govern
`
`the issues of patent invalidity.
`
`18.
`
`I understand that assessing the invalidity of a patent claim involves a
`
`two-step analysis. In the first step, the claim language must be properly construed
`
`to determine its scope and meaning. In the second step, the claim as properly
`
`construed must be compared to the prior art to determine whether the claim is
`
`invalid.
`
`
`
`11
`
`Page 16 of 130
`
`

`
`19.
`
`I am informed that a claim is invalid as anticipated under 35 U.S.C. §
`
`102 if a single prior art reference discloses every element of the claimed invention
`
`to a person of ordinary skill in the art.
`
`20.
`
`I am informed that even if a single prior art reference does not fully
`
`anticipate a patent claim, the claim may be invalid as obvious if the differences
`
`between the claim and one or more prior art references are such that the claim as a
`
`whole would have been obvious at the time the invention was made to a person of
`
`ordinary skill in the art. In arriving at a conclusion of whether a claim is obvious, I
`
`understand that several factors are to be considered: (1) the scope and content of
`
`the prior art; (2) the differences between the art and the claims at issue; (3) the
`
`level of ordinary skill in the art; and (4) objective evidence of non-obviousness.
`
`21.
`
`I have also been informed that determining whether there are any
`
`material differences between the scope and content of the prior art and each
`
`asserted claim of the challenged patent requires consideration of the claimed
`
`invention as a whole to determine whether or not it would have been obvious in
`
`light of the prior art. If the prior art discloses all the limitations in separate
`
`references, consideration should be given to whether it would have been obvious to
`
`combine those references. I understand that a claim is not obvious merely because
`
`all of the limitations of that claim already existed in the prior art. Further, a person
`
`
`
`12
`
`Page 17 of 130
`
`

`
`of ordinary skill in the art who is combining references should have a reasonable
`
`expectation of success of the combination.
`
`V.
`
`PRIORITY DATE AND PERSON OF ORDINARY SKILL IN THE
`ART
`
`22.
`
`I understand that in a related case before the U.S. International Trade
`
`Commission (ITC), the Patent Owner asserted that this patent has a priority date of
`
`June 22, 2000. I have used this priority date in my analysis, and I have viewed the
`
`prior art from the perspective of one of ordinary skill in the art as of that date.
`
`23.
`
`I have been informed that in the related ITC proceeding, the Patent
`
`Owner proposed that a person of ordinary skill in the art for the asserted patents
`
`would have a Ph.D. in a field such as chemical engineering, physics, materials
`
`science, or chemistry, and one to two years of experience studying, analyzing, or
`
`preparing electrochemical materials. I have used this definition in my analysis
`
`below.
`
`VI. TECHNOLOGY BACKGROUND
`
`A. Battery and Electrochemical Cell
`24. The ’143 patent concerns lithium metal oxide positive electrodes,
`
`commonly referred to as cathodes, for use in electrochemical cells and batteries.
`
`25. Those of ordinary skill in the art would have been very familiar with
`
`Li-ion electrochemical cell and battery operation. General facts about these types
`
`
`
`13
`
`Page 18 of 130
`
`

`
`of cells and batteries are provided in Exhibit 1023, Linden’s Handbook of
`
`Batteries.
`
`26. The positive electrode is one of three primary parts of an
`
`electrochemical cell. In particular, lithium-ion electrochemical cells must include:
`
`(1) a positive electrode (cathode); (2) a negative electrode (anode); and (3) a
`
`nonaqueous electrolyte. Other types of cells may have aqueous electrolytes, but
`
`lithium cells must have non-aqueous electrolytes due to the high reactivity of Li
`
`ions with water.
`
`27. Lithium batteries operate using the flow of Li ions between the
`
`positive and negative electrodes through the nonaqueous electrolyte in conjunction
`
`with the flow of electrons through the external circuit. The positive electrode
`
`releases Li ions and electrons during charging and receives them while the battery
`
`is discharging (i.e., while the battery is in operation). The negative electrode
`
`receives Li ions and electrons during charge. The opposite process occurs in the
`
`negative electrode during discharge.
`
`28. Li-ion cells are generally prepared in the discharged state, i.e., using a
`
`discharged (lithiated) positive electrode.. The cell is “charged” using an external
`
`power source to transfer Li ions from the positive electrode to the negative
`
`electrode. This process of transferring Li ions to the negative electrode (charging)
`
`
`
`14
`
`Page 19 of 130
`
`

`
`occurs, for example, whenever you plug your cell phone in to an electrical power
`
`source to recharge the battery.
`
`29. For illustration, I have included a figure showing the flow of Li ions
`
`and electrons during charge and discharge below.
`
`
`
`
`
`30. The figure above shows a positive electrode having an LiCoO2 active
`
`cathode material, and a negative electrode based on LixC6. In general, negative
`
`electrode materials include lithium metal or carbon, and these materials can
`
`reversibly accept and donate lithium. Ex. 1023, 36.7-36.9; Ex. 1015, 1817.
`
`Transition metal compounds in which lithium ions can be inserted and extracted
`
`also may be used as the negative electrode. Ex. 1023, 36.9.
`
`
`
`15
`
`Page 20 of 130
`
`

`
`31. As I mentioned above, due to the high reactivity of Li ions with water
`
`or water-containing compounds, lithium cells require a non-aqueous electrolyte as
`
`the medium through which lithium ions flow between the electrodes. Non-aqueous
`
`electrolytes include: (1) a liquid organic electrolyte such as a lithium salt dissolved
`
`in an organic solvent, and (2) a solid polymer electrolyte, which is a lithium salt in
`
`a polymer matrix. See Ex. 1023, 36.13-36.16. Suitable solvents for liquid
`
`electrolytes include ethylene carbonate (EC), dimethyl carbonate (DMC), and
`
`diethyl carbonate (DEC). Ex. 1023, 36.15; Table 36.9. Suitable lithium salts
`
`include LiClO4, LiPF6, LiBF6. Id., 36.15, 36.26; Table 36.9. A nonaqueous
`
`electrode can also be a solid electrolyte, for example, lithium phosphorous
`
`oxynitride (LiPON).
`
`B.
`
`Lithium Metal Oxide Positive Electrodes
`Layered LiMO2 structures were well known in the art
`1.
`32. As I previously mentioned, LiCoO2 is a suitable active cathode
`
`material for use in a positive electrode. This is an example of an LiMO2-type
`
`material, where M is a transition metal. Other transition metals may be used to
`
`form LiMO2-type cathode active materials.
`
`33. For over twenty years, researchers have investigated LiMO2-type
`
`positive electrode materials due to their known layered structures, which allow Li
`
`
`
`16
`
`Page 21 of 130
`
`

`
`ions to intercalate or insert easily into and de-intercalate or extract from these
`
`structures. See Ex. 1009, 36.11.
`
`34. The layered structure of LiMO2-type electrode materials was well-
`
`known by June 22, 2000 (the priority date asserted by the Patent Owner).
`
`35. For example, LiNiO2 and LiCoO2 contain alternating layers (or
`
`sheets) of oxygen, transition metal, and lithium. See Ex. 1014 (Thackeray 1994), 5,
`
`Fig. 1; see also Ex. 1015 (Bruce 1997), 1819.
`
`36. These alternating sheets or layers of Li, O, and M can also be
`
`described as layers or slabs of MO6 octahedra alternating with layers or sheets of
`
`Li ions. The Li ions move relatively freely between the layers of MO6 octahedra,
`
`making these materials attractive for use as positive electrode materials in Li and
`
`Li-ion batteries.
`
`37. Layered LiMnO2 adopts the LiMO2-type layered structure. Layered
`
`LiMnO2 has alternating layers of MO6 octahedra and Li ions, which form
`
`alternating layers of Li, Mn, and O (Li-O-Mn-O-Li-O-Mn-), as shown in the figure
`
`below. Ex. 1017, Fig. 3.
`
`
`
`17
`
`Page 22 of 130
`
`

`
`
`
`38.
`
`In the figure above, the blocks represent MnO6 octahedra (with Mn in
`
`the center and oxygen atoms above and below in an octahedral pattern) and the
`
`filled circles represent Li ions. Ex. 1017, 4:52-54.
`
`39. Other publications similarly reported this structure of LiMO2-type
`
`materials. See, e.g., Ex. 1019 (Rossouw), 465; see also Ex. 1016 (Armstrong), 499.
`
`40. Additionally, LiMO2-type materials with mixtures of transition metals
`
`as “M” may also adopt this layered structure. For example, LiMO2-type materials
`
`having a mixture of nickel (Ni), cobalt (Co), and manganese (Mn) as the transition
`
`metal have the same layered structure. See e.g., Ex. 1020 (Yoshio), ¶ [0031]
`
`(disclosing a lithium-containing metal composite oxide with a layered structure
`
`LixMnyCozNi1-(y+z)O2 having a same space group R-3m structure as in a layered
`
`structure LiNiO2). Also, when the transition metals are a mixture of cobalt (Co)
`
`
`
`18
`
`Page 23 of 130
`
`

`
`and manganese (Mn), LiMO2 adopts this layered structure. Ex. 1021 (Numata,
`
`abstract), Figs. 1-2.
`
`41. The structure of Li2MnO3 is very similar to LiMO2, and the prior art
`
`disclosed that Li2MnO3 and LiMO2 have compatible structures. Ex. 1021
`
`(Numata), abstract, Fig. 1, 725, left col., third para.; Ex. 1010 (Neudecker), pages
`
`4151-4152.
`
`42. Specifically, Li2MnO3 has the same layered structure as LiMO2
`
`consisting of alternating sheets or layers of Li, M, and O, except one third (1/3) of
`
`the transition metal ions are replaced by Li ions. The layered structure of Li2MnO3
`
`can be noted as Li-O-(Li1/3M2/3)-O-Li-O-(Li1/3M2/3), and the formula for Li2MnO3
`
`may therefore also be written as Li(Li1/3M2/3)O2.
`
`43. Although the structure of LiMO2 and Li2MnO3 are quite similar, the
`
`prior art disclosed that X-ray diffraction (XRD) can detect Li2MnO3 in LiMO2–
`
`type materials. Specifically, the prior art disclosed that peaks between 2θ = 21-25°
`
`do not exist in pure LiMO2-type materials, but peaks (or, more commonly, one a
`
`broad peak) in this region indicate the presence of Li2MnO3. See Ex. 1011
`
`(Rossen), 314; Ex. 1010 (Neudecker), Fig. 7; Ex. 1021 (Numata), Fig. 2, page 726
`
`I understand that later publications by named inventor Dr. Thackeray confirm that
`
`peaks in this region are characteristic of Li2MnO3 and can be used to determine
`
`
`
`19
`
`Page 24 of 130
`
`

`
`whether Li2MnO3 is present in LiMO2-type materials. Ex. 1013 (Thackeray 2007)
`
`at 3117.
`
`VII. OVERVIEW OF THE ’143 PATENT
`
`44. The ’143 patent concerns lithium metal oxide positive electrodes
`
`having two components, LiMO2 and Li2M’O3. Ex. 1001, abstract.
`
`45. The ’143 patent acknowledges that LiMO2-type materials were well
`
`already known as suitable materials for positive electrodes. Ex. 1001, 1:56-61. The
`
`’143 patent thus focuses on the contribution of Li2MnO3 to the structural stability
`
`of LiMO2-type electro