`U.S. Patent No, 7,60L662
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`IN THE UNITED STATES PA TENT AND TRADEMARK OFFICE
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`Examiner; DfAMOND, ALAND
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`Group Art Unit: 3991
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`Confirmation No: 2755
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`In Inter Parte.\' Reexamination of:
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`BULLET AL.
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`Reexamination Control No. 95/00 l,453
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`Patent No. 7,601,662
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`Issued: October 13, 2009
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`For: COPPER CHA
`ZBOLITE CATALYSTS
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`Mail Stop Inter Partes Reexam
`Central Reexamination Unit
`Commissioner for Patents
`P.O. Box 1450
`Alexandria, 'VA 22313-1450
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`DECLAlL<\'IION OF STACEY I. ZONES, PH.D. UNllER37 C,:F,R. § 1.132
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`1, Stacey Zones, do declare and say as follows:
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`r have a Ph.D. in Chemistry from the University ofCaWbmia at San Diego, I am a
`1.
`Research Felknv at Chevron Energy Technology Company) a division ofChevn.m U.S.A. Inc. a
`whol.ly owned subsidiary of Chevron Corporation (ETC). I have been involved in research and
`development of molecular sieves and zeolites at ETC for more tfom thirty year~, ln 200 l, I
`rec,eived the Donald "l/V, Breck RVr'.ard from the International Zeolite Association for my '\VOt'k
`related to nioiecular siev~s. In 2007~ I received the Eugene J, Ho~1dry award in Applied
`Catalysis frtHn the North American Catalysfa society for my work on zeolite catalysts. lam
`named as an inventor on 115 United States granted patents pertaining to the synthesis and/or use
`of molecular sieves. I am the first~named inventor on lJnited States patent number 6, 709,644
`("the 1644 patene').
`
`I am infomied that United States patent number 7,601,662, ("the '662 patenC), assigned
`2.
`on its face to BASF Catalysts LLC ("BASF"), is currently under reexamination in the United
`States Patent and Trademfirk Office. I mn also i.nfom1ed that the '644 patent is cited as a
`reforence in rejecting the clahus of the '662 patent io: the above captioned reexamination of the
`r662 patent.
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`Exhibit 2009.001
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`inter Path>,~ Reexarnhrnt1t}!1 No, 95/001 ,453
`lLS, Patent No .. 7,60~.664
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`Representatfoes of RASF Corpi:Yrntk:;.rh the m,vner (>f ~'he '662 p~\tent, ;;.:ontackd me and
`3,
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`I nm. ~~\VHre and u.nderst~md th~t Jny ~~rnploy~r~ Chevmn US.A, Ini:;,, and Hi\SF
`4,
`0Jl1J()nttion *lre in several bmdness relationships related to the sale and manufacture t1f catalysts,
`inc1u.dinga license to the '644 patent
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`l have nzn: renuestecl and I'm nQt rei:;dving any ~medal or additional com.pensation from
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`my empkiyer h1 cmmoctfon with this Decfai\~don tUJd I have not n.~tH:::st.ed arid: l MJ not befog
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`regarding fa~ t.~~Khings $Jf the '644 patent, Tht: '644 patent pertf;tbs tQ a zediw having fae cryst~1l
`strrn .. :ture of c.hahazite (CHA} fo.tving sm.aH crystallite siz~\ pnit~esses u.sing the sntaH crysta.ffite
`CHA. as il catatyst and gas sep.aration proce%t~s using the snnlH crystu!fae CHA,
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`The '644 patent discloses that (.t zeoUtc having the CHA crystal structure c~m be used for a
`7,
`variety of process.es intfodi.ng. separation of gasses~ such as separating carbon dioxide from
`natural. gas (cot 5, lines 66~67), as c.atalysts used for tbe reduction of oxides 1..1fnhrogen in a gas
`siri;:am in the pre~ence of'1xygen (c1..)L 1., lines 54-66}, converting 1o\vcr ~kdwts ~md other
`oxygem~td hydrocarbons h':} a gasolinz~ b·oiHng point hydrocatlx}n pmduct (coL 5, lines 18 .. 14),
`and frw pi:t:<duch~g dhnetbykirnim.~ (cnL 5.~ lb~~ 36-40). Add.itinrm!ly,. the ~544 patent sfate8 that <-S
`zenliN.~ hmd.ng the CI{A i.::rystal. strm:ture rn~ry z:onH!1n a md~~l. or meta!. ions {sm:~h .as c:dx.Jt,
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`fo my viev,:,. the phrn~•z: '*reductkm of z\xid~s uf nitn~gz:n z:tmw;ned in a pis. strernn in. tJw
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`\xesl!nce of t.\KV?'en'l in the '644 patent: refors to and teaz:hcs a numher of diffon.mt ri..Mi;.~t.Ions,
`including thz~ redm::tion t)fNO '\\"lthout nxludng agents, such as ln the presencz~ of CO (for
`example~ a three-way (:.atalyst), the decornpo;:;ition of NO in the pn.isem~e of oxygen, a11d N20
`decomr1ositfon, the sek~i:ti\:t: c~talytic re<ltittiNl of NO in the presence of an i.umwJnia n::ducing
`.agent and oxygen, and the st~kctive cata1yrk. reductkm of NO in the presence ofa hydrnc.atbon
`red'lCh<~ ·:wer<t ''!l,.l •ww~'"ll Th;:.. ~644 l'P~.,.n· <j<)e • .;;: 'Y'* t"'•~ch ~fl«t:::ifl··, """'.fl.c.l°i"ll'l'-: {.-l ... th; ~ednc:6r<n ,,t
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`h fa: tM,me:r.af!<." knov.in §n thz~ art dmt zed!iws that tx.inh~in mekd or metaJ fon~., s:uch as
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`these. rt~~cti~)fts ~1f retit~e.ln~~ ~J.f o·xhJes c~f n.~tt\>;ge:n h1 a gas strt~n1 tr1 t~~e .f"'S:l\~se1lce: ~)f {.$Xy·gen ..
`Sevz~rnl p~tems ass:igt~zxl tz1 Chevron U.S,i\. Inc. pert;;il:nfog to m>:ikcular skvt~s Ci..'>ntain
`statemz~nts drnt the molecular sieve in the pnH.~nt is useful for the n.~ductfon of QXkks of nitrogen
`in the presence of excess oxygen~ and that the molecular skvc cm1 contain rrwt%~! kms such as
`C{}pper, cobalt, mixtures th~~rcof mid other r:n~h'lls. Fot example,. tlnited States patent Nos,
`?J 38,099 (SSZ:-73, SAS fa1me\vf.lrk: t.yp~); 6/~76~732 (SSZ~St\ RT11 Frarnew\)tk Type); and
`6,540,903 (SSZ-47, Ne<.v FranK·.vcn·k Type) m-ejust a fo,v C'::.:<.unpk1s of such patents,
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`Exhibit 2009.002
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`Inter Partes Reexamination No. 95/001 ,453
`U.S. Patent No, 7,601,662
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`The i544 pateM does not specifically disclose or suggest that the zeolite having the CHA
`HJ.
`crystal structure is useful for selective catal)1k reduction ofoxides ofnitrogen in the ptesence of
`a reductant~ such as ammonia, There is Ill) discussion) sugges:tjon or example in the '644 patent
`indkatingthat a zeolite having the CHA crystal structure containing copper exhibits improved
`sefoc.tive catalytic reduction of oxides of nitrogen at temperatures below 350° C compared to
`otlli~r zeolltes, or that a zeolite having the CHA crystal structure and containing copper maintains
`excellent conversion of oxides of nitrogen after hydrothermal aging at teinperntures in excess of
`650° C a11d 10~:10 H20. hmderstand that many zeolites containing copper and other metals have
`had limited application as selective catalytic reduction catalysts in diesel engines becaus·e of
`problems related to maintenance of good nhrngen oxide conversion uptm hydrothermal exposure
`at temperatures in excess of650° C.
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`The 1644 patent doe-s not descdbe or suggest an arnount of copper to be used in the zeollte
`11.
`having the CHA crystal stmcture. Ccdu.mn 5, lines 25-28 of the 1644 patent states that the
`catalyst may contain an ammonium or metal cation complement, preferably in the range frnrn
`about 0.05% to 51J.1o by \\··eight. This statement appears unde.r the heading of ncondensation of
`Lower Alcohols" at col. 5, line 17, and the discussion under this heading pt~rtains to a catalyst for
`the condensation of lower akohois. In this regard, the '644 patent actually states at column 5,
`lines 25~33:
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`The catalyst may be in the hydrogen fonn or may be base
`exchanged or impregnated to contain ammonium or a metal
`catfon com.p!etne11t, preferably in the :range of frt1m about
`0.05 to 5% by vveight The metal cations that may b(! present
`include any of the metals of the Groups 1 through vm of the
`Periodic. Table. Hmvever, in the case of Group IA metals, the
`cation content should in no case be so large as to effectively
`inactivate the catalyst, nor should the exchange be such as
`to eliminate au acidity,
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`This passage quoted above teaches that a catalyst for the condensation of alcohols can include:
`0,05 to 50..\--i by •veight can include metals from Groups I to VHl of the pedodktah!e, which
`includes an Ineta!s in the Periodic Table, The quoted passage of the '644 patent makes reference
`to group IA metals specifically, hut Group IA metals do not include copper. This passage is not
`related to the passage earlier in the '644 patent at col. l, lines 61 ~65 pertaining to reduction of
`oxides of nitrogen., and thel'e is no teaching in the '644 patent of the amount ofcopper, cobalt or
`mixtures therenfthat can be used ihr a rntalvst for the reduction of oxides of nitrogen.
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`The '644 patent teaches a small crystal 1.:eolite vdth the CHA crystal structure having a
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`crystanite size of 0.5 ~l or less. AdditionaIIy, the '644 patent teaches a method for making the
`srnall crystal zeoHte, teaches that it is useful for c.onverting lov.rer alcohols and oxygenated
`hydrm::arbons into liquid products and teaches that it is usefol for the reduction of oxides of
`nitrogen in a gas stteam in the presenc.e of oxygen, as examples runongst a variety of potential
`applications of this new materiaL The' 644 patent does not leach a person having ordinary skill
`in the art a specific zeolite having the CHA crystal strncture, a silica to alumina rnole ratio
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`3
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`Exhibit 2009.003
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`Inter Part.es Reexamination Nli. 95/001 A53
`U.S. Patent No .. 7,.601,662
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`greater than I 5 and a Cu to A! atomic ratio exceeding 025 that vvould be any better than any
`other zeolite for the reductii.:)n of nitro{;:en oxides in an exhaust r.::as. strearn of an internal
`.....
`cornbustion engine at temperatures belo'iv 350° C. The !644 patentdoes not teach a specific
`zeollte having the CHA crystal structure that has especially good hydrothermal stability in
`retaining NOx conversion perfonnance after aging under hydrothe.mw.t conditions.
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`~
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`I hereby declare that·aH statements made herein of my O'>-Vn knowledge are true and that
`13.
`all .statements made herein on inforrnation and belief are believed to be true; and further that
`these statements were made with the kno\.vledge that '-ViHful false statements and the like so
`nmde are punishabk by fine or imprisonment; or both, under Section l 001 of Ihle 18 of the
`United States Code, and that such willful false statements may jeopardize the validity ofthe
`patent at issue in this proceeding, US patent number 7,6 0 l ,662,
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`Dated: February 7, 2011
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`4
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`Exhibit 2009.004