[go: up one dir, main page]

WO2024227121A2 - Upcycling of polyethylene and polypropylene and their mixtures to high-value surfactants - Google Patents

Upcycling of polyethylene and polypropylene and their mixtures to high-value surfactants Download PDF

Info

Publication number
WO2024227121A2
WO2024227121A2 PCT/US2024/026720 US2024026720W WO2024227121A2 WO 2024227121 A2 WO2024227121 A2 WO 2024227121A2 US 2024026720 W US2024026720 W US 2024026720W WO 2024227121 A2 WO2024227121 A2 WO 2024227121A2
Authority
WO
WIPO (PCT)
Prior art keywords
wrn
mrr
mxr
rrn
nnr
Prior art date
Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
Pending
Application number
PCT/US2024/026720
Other languages
French (fr)
Other versions
WO2024227121A3 (en
Inventor
Guoliang Liu
Zhen Xu
Nuwayo MUNYANEZA
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
Virginia Tech Intellectual Properties Inc
Original Assignee
Virginia Tech Intellectual Properties Inc
Priority date (The priority date is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the date listed.)
Filing date
Publication date
Application filed by Virginia Tech Intellectual Properties Inc filed Critical Virginia Tech Intellectual Properties Inc
Publication of WO2024227121A2 publication Critical patent/WO2024227121A2/en
Publication of WO2024227121A3 publication Critical patent/WO2024227121A3/en
Anticipated expiration legal-status Critical
Pending legal-status Critical Current

Links

Classifications

    • CCHEMISTRY; METALLURGY
    • C08ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08JWORKING-UP; GENERAL PROCESSES OF COMPOUNDING; AFTER-TREATMENT NOT COVERED BY SUBCLASSES C08B, C08C, C08F, C08G or C08H
    • C08J11/00Recovery or working-up of waste materials
    • C08J11/04Recovery or working-up of waste materials of polymers
    • C08J11/10Recovery or working-up of waste materials of polymers by chemically breaking down the molecular chains of polymers or breaking of crosslinks, e.g. devulcanisation
    • C08J11/12Recovery or working-up of waste materials of polymers by chemically breaking down the molecular chains of polymers or breaking of crosslinks, e.g. devulcanisation by dry-heat treatment only
    • CCHEMISTRY; METALLURGY
    • C08ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08JWORKING-UP; GENERAL PROCESSES OF COMPOUNDING; AFTER-TREATMENT NOT COVERED BY SUBCLASSES C08B, C08C, C08F, C08G or C08H
    • C08J2323/00Characterised by the use of homopolymers or copolymers of unsaturated aliphatic hydrocarbons having only one carbon-to-carbon double bond; Derivatives of such polymers
    • C08J2323/02Characterised by the use of homopolymers or copolymers of unsaturated aliphatic hydrocarbons having only one carbon-to-carbon double bond; Derivatives of such polymers not modified by chemical after treatment
    • C08J2323/04Homopolymers or copolymers of ethene
    • C08J2323/06Polyethene
    • CCHEMISTRY; METALLURGY
    • C08ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08JWORKING-UP; GENERAL PROCESSES OF COMPOUNDING; AFTER-TREATMENT NOT COVERED BY SUBCLASSES C08B, C08C, C08F, C08G or C08H
    • C08J2323/00Characterised by the use of homopolymers or copolymers of unsaturated aliphatic hydrocarbons having only one carbon-to-carbon double bond; Derivatives of such polymers
    • C08J2323/02Characterised by the use of homopolymers or copolymers of unsaturated aliphatic hydrocarbons having only one carbon-to-carbon double bond; Derivatives of such polymers not modified by chemical after treatment
    • C08J2323/10Homopolymers or copolymers of propene
    • C08J2323/12Polypropene

Definitions

  • rnmrnrn r m wrn w w,w,r mxr wxnr w, nm , n w mxr wxnr.
  • rrn n r rn r m wrn m nm n,rn mxr wxnr.
  • rn rn n m- rrnrnrmnmmnnnn w 1 r 1 r 14 rrn. mn. r ...- 1 nrmnn nnnnnrnnz mxn mrm nnrnnv n r 66 rmn n nnrn mx nrn n.. mm n . -- wn mnxr-wxr. n n r r n mxn rn w n.. rnr rnnnnrn..
  • nn m n mr mrrr nr rrr m n mr r r r n rn nwn nw r.nnrnrn w- r wrm m, nn rrwnn ,rnrvnrmrr..., rn mr n,nnnrnn mrmr, rxn n rr. , w r wn r.
  • nnn mnnrr rrn,nrrn nnrmn. mnr vr rm,r nrrnv mr nr,rn n,nnnm:nn r,n v n mmn n n w nnrrv m mx n n nnr, wrn nn rn mrr r v wx - --- rmrmrrrrvnrrrrr rm rmvn mnnnn v r nr rnrnn vrmr,rmrrrv mx nn mr r.rnn, nn,nnn mrvnnrmn mxnrn wxw r n vnnnnmr,mn n w nnnr r n v r
  • n m mrr mr.nm 3 mr,xn , rmr,r m , n nm m,rxm: m rx nnr.nm , n nnr mrmnn rrn m .nm , nr vrn,rn-n, mrzn,n nn.rn mnmr,nnn rn, n n rmnnr.rn vrnnn w- - rnrw-n n .nr vrnnnn n n nnnnn rr--m r-w n .r- rw-n nnnnn r .
  • nr rnr rm nnmmn nr, rrn rvnvnrn mnn n n nrnrnn wn rz mrnnvrn nx xr n r rmnn r “”n.n “n,” rn, mnnr mr wn n rn nmr mnnnnnvnnnr n nn m. “”n “n” “”r n rn m .
  • n.mrrmr. rvn nn 20 n rn ,--wxn-r- mr r nnw r r.n --wx. 2 --wx wxx - n m rnn mr 2-wx 2 .,n nn mr-r-wrxrwrrnnnrnw 2 n 1rvr mrr rn wmn- ⁇ r r n xn-nnnn r,rn rn n rr, 14 r , 22, 23 .
  • nrn n 2 .,,n . rmr m rmn n w mnr rn,vn rr nn rrm rmn n w-m-- rmn n wr n ,v n . 13 n,m mnrrmnrn m n 1 rn mrrr.mn. m rnr wr xrmnn wnn.-r-wxnn n, ,n r m-nr x-n ., n rn wmr - 2 -wx.
  • nrr r n n nrm nzr r n - nm.
  • n nrrn ⁇ n m.n nm mnxr wn rnrxr mnnrnrr rmn . n ⁇ nnnr , w r r, n n. wr nr nn wrr w wrn v r ⁇ . m rr n n . w rn wm nvr . wr xrrmrnz mn . m r.mw n r n nr w r.
  • n.rrmrrrnm rr wz rnrr w rnr nrnn rmrn ... mrr r r m w ⁇ °C r,. wxnn n.rz wx w w mr r nnn n. n r w w n r r wrxnn r rn , r r,n n r .rwr, m xn w n r w r rxn. rxnxn, wx rn r rrrx wn. wr rxn,.
  • n.zxn n v n -.n . wxrxrn wn mnr n rnnx ⁇ ⁇ r n - , wxr wrv n r x n vr,nxnnnn wx ⁇ mnnr w.. rw. rnnx w mn wrn nr mmrrn . . ⁇ ⁇ /0 nn ./0 m 1 .nrn ⁇ wr r - --- rmn. n m rn m.
  • nmnr nrn -rv wr mrnr :, n w z v -.nr n -, wrx n nn nzn r v wr m n , m rvn n. ⁇ ⁇ ⁇ '02 nn r r m .
  • r nm r ⁇ ⁇ ⁇ 34 ⁇ m r w mrx rmnmrvr nnnrrmnrw nn r n r n, r rnr mrzn,n nmrnnr mnmn.rnnn r rnr , - n r n rmr rmr - nrv nnrrmnn.rrnr,n rmnmnnn . vn r n. nrmn .
  • rm w n n v vr ⁇ r ⁇ ⁇ n ⁇ wr ⁇ " + ⁇ ⁇ + ⁇ n nnr v wr ⁇ ⁇ ⁇ , + ⁇ + ⁇ ⁇ ⁇ , + ⁇ 5 n nn m n r nmr r nn.
  • n nnnrnr m r w r n nnrnzrnn.xm mvnrmrnnn n wx n-r x n rn 7 - rx, 8 r r n r n, 7, 9 nnnnmrrznn mrr w rmn n, rmrnrm v nrmn ⁇ r n v .
  • n nnnrmn -- nrmrmn, n ⁇ w rr n ⁇ n w ⁇ n-r- n ⁇ nrn nmnvr ⁇ n> n - .n rrnr rnn , mrz r n xnm mnnn n n r n m mnr.rr, nnxz wnrrmx ,n rrxn-n nmnnrr-.-wxn,n wx, n nnnrn ⁇ mm, -r- .rr, n wrn rmrn rmn .
  • v- rrmnr 11 nrr-rnx mr,n 12 .nr znn-, rr., 7 nv m - --- z 1 m 4rnvr r rrnrm ° wn.. 7 nr n z m rn wr n .xnr nvrv nrvnn,nnn m r,mn rrnn. 13 n- rm r n.
  • n rwnrmrvzn rrn rv mn - vwr-nn . m. -rm ° mnr n wx. m -nn nn. mnrn nmr vwrrmn nn . m nxrnnvn . r nn n rm rmn nrm- n, w rn r n- , w w nmrvr mrn. nr r vr mr w m ⁇ m nn x . n .
  • n, n- r v vr r nn ⁇ vn,wnnvr mr m ⁇ mr wx mrrmrnrn r .. r, r r vrn mr rmn, xnnnnn nn nrm . n wxr nr rn ⁇ ./. - w n r. mm r- nn °. mm r--° v. rmnm wx-°r,n-nr. r nrrm ⁇ ./.
  • nnn rmnn -n m ,..rrmr,- n m-- n ,, nn nrmrmrrn ,- nrn w -rv-m, mn-r-nr,,nn,n,-,rm,--nnn .. n rm ,n nmnrm -rm xn, wr n m .n , nn n mrr r m rmnn . . r rm nvrrn-wr mxr wn v-mxr mxr, mnnmrrrm.
  • nnn,n,n nrm rm mnn m-rmnnmn rmn n wr -,nnn w nr .,r ,,,,n.rvr, rnrm xnn m..mn m rnn , ,,-n rn. nr x,r w x nrr vr-n mxxn vrrmn n .n rn, rmn rm .r.r.
  • rmnnrn,nnrn °rnvwr.--nnnw wx 1 rm- - --- nrn r rnn r n n r n-r nrn. n-n,n-r rnn rrnrnnrr.nnnzrnr , ,n rnr vnr mnn mr vrn , nr n w vrzn, n rm wrn .. r n r r, n wr r w nnn vr n rnnw . .
  • wn rnnnn w- mn m m.., wn nrm.: ° r r n : rv nnw::w: mmn n n mmn mnvnm: mmnnnm:m.: m °n mnnvvnm : °mn .nrnnrmn:m. ° . : : ° n-.n-: - m °r w rrm n - mrrrrn w r . mmmrn °r wx w m w r .
  • x mmmnn mrn m x , m x , m x n n , r, rmrr w.nrr mn m. mnn- r mrnrrrn nmm,-rn r-r, n - nm,n nm 13 rmxr.rr w 1 n nx. .rmnr w wrrr rmr nnr nzzrnrnvnrrm. rmrrmnn wrn n 13 zrrvn rn wrrr rmxn n n.
  • rnrnr nmrn " 1-2 .” rr m nr mnrnnnnnn wn w nrnr n r n nrrnnrr rrn n . n nnv n nrr rvr nr n wr rrn xr m m n n.
  • nnr nnr,.., n mrnm.,n.rrv,n.n,rnrmmrr nr ,r n,n- .m r wxnnn..rr n rr nrn xnnn w..rn mr nnw-n n -m,.. ,.,x vrr n , , - . .nr nnrn mr r m, r, rnn ,.nn,.. r,..rrnn -.. n,..mm, ,.nnn,. n, mr,..
  • r r,.rn,..,rn- xnn - n r n mn vnnr nr- n,.,r.m m , ,-. r,... ,n.,mrzmnr.znnrn mmnrz.n, -. rx-n mrzn . rvrnn mrnm , ,-.,n rx.rn nnrrn,..mr,.,.,r,m-m.rzn r rn .nr - --- r n rn,.rnn,.rnn,.rnn,.rnn,.
  • nnr nnr,.., n nr.nnrrnnmn rr r ,. n,. nrn mr r , , - . nr r,.. r,..., mrnn , - :r r n m.m m , nr. n,. rrn,r...rnvrr,n.,vnnr rrn ,r n . ,- nn,.r rn,..rnrn,r.,x, ,rm- r nr r,. zr,. z,.rx,. .
  • n n ,, nmnn m .nnm,-.. .,.,.n,,r n rn ,, -. ,.,.,.n,.,.r..n,.n,,.,,-... n r,.,. - --- r .v.,...rn,, Vietnamesemn,,...nv,..z,..r,.... rn vr,..n,..r, rn ,...,n m.r.,.n, ,nz, n,-..n,,.,n-,. ,.nr,..rrr,. :n.vrn w,.rrn,n.
  • n nr r n n n ,,- ,,..nw,.nr,.. m,rn n n r .-..r:nvnr,nm.n.rm,v,-..,nr ,.. vv,..r, .. r,..rrn, -. .:.rv,.nn,.n nmr m nnrn,. x z,vr, ,.-. ... ,r.,n rn r, .

Landscapes

  • Chemical & Material Sciences (AREA)
  • Physics & Mathematics (AREA)
  • Thermal Sciences (AREA)
  • Life Sciences & Earth Sciences (AREA)
  • Sustainable Development (AREA)
  • Health & Medical Sciences (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Medicinal Chemistry (AREA)
  • Polymers & Plastics (AREA)
  • Organic Chemistry (AREA)
  • Organic Low-Molecular-Weight Compounds And Preparation Thereof (AREA)
  • Investigating, Analyzing Materials By Fluorescence Or Luminescence (AREA)

Abstract

Herein, a method for controlling the thermolysis products molar mass using a coolant fluid (e.g., water) to modulate the final products' condensation temperatures. With this strategy, the thermolysis of polyethylene (PE) and polypropylene (PP) is tailored to generate liquid oil, without any catalysts or additives. Subsequent addition of sulfuric acid across the alkenyl groups, followed by the neutralization with sodium hydroxide affords sulfate detergents with excellent foaming behavior.

Description

- --- - - n “ nmrr,n n ,-nn..rvn n w-rnrr rr”nvnrn.r n. , r, , nn nnvnnn wn mn. w vvrrnnmmnn rrnn rrwnrnvnn.,wr ,rn,nnrrrnr r mn rn n rnrnn xnmnrr n,n nnzrrnnn-r ,n x n rn,nnxnv . rr ,r, n. w rn, nn.1 mnmnnn mrrrnvrnmnnn,nn rrnr rnrrn r n ,n2-3r r, nr w m nrnn mnnmzrnrm wn. mnn r rrnnx rnn mrr rv.., mn rn w , rr nnrr rrn.4 rnr nv rnr r n , , r n .nnn- m-r v nrnx.nr nmr rr n v- m rv rn v r . v mmnr n mn nnnx,nnvrrn.5-6 ,v nm n r-v rr rz nn.7 r nrrnnn r nrrmmrn - --- rmnx mxnrnr wrr rnn8-9nnmrvn . r rn rrn r r ,1r0n n n n n nr ,r rmnnr nnrrn. r wr,rrnr r n . rvr --wx v,n m n vrrrn, rnr nrrvrn m rrvrrn . n wrr m rrn ,rxm m m mn nrz rr nr rn v nn r rn v m r nn n -v r rrmn. wr w nrn vn rrnm.n n w, m r rnnn rnrrnv , n.r nrnmrm n-,rvrn nrn:rnn r m mr rrmrn wx nn r n, n,n mnnr,n v r mmn n w nnrrv m mxr w n nnrr nrn m, wr xnr n v r mrrvrr n nn rn mrr r mrr r mn mnnn v r nr nm r nr m rv mxr wxnr. mrr , n r rn r m wrn rn rr v n n r ° °r mnvr n m. r mmrm, rn,rm r r,rrnm r mr,r,r wmrn rn nm , n r rn r m , wrn r . mrr v n n m n z v r mrrnr wxnnmr n, ° nnnr nr°r mr mn rn. m rrn mxr r n, n,n mnnr rm r nn mmn n w nn rn nn w r n v n wxnr n nrrnrnrnnrnrmmr,v wrnmnn mxrw - --- r nn v r nrr mrrn wrn mr r nmn mrnn mmw r r,n v ,rmnrv r,r mxrrn r wxn mr., wrn r n nm , n rm r,rrm r. mrr r rn r m , wrn r mrnrm°,° °,n°. ° °r, rn r m , wrn r ° °,° ° °,° °,° °, mrnrm ,°.n r rn r m , wrn r nm ,° n°. mrr ° °,r ° r°,rn r° ° m,r, w°rn°r nm , n r rn r m , wr . x mn n mr x nm r. n , n r rn r m , wrn mr nrnnrmnr rn ,n vn. r rn r m , wrnnr x nm. xn,mx wnnnrrnrn r m , wrn mr x nmrmx, wnnnr nr rn v r. m , wrn mr nmm r,r n r v .rn r m , wrn v nrmmr, r.n r rn r m , wrn mr r n,nrnnn,nrmnnnrrn.,rn n,nr nrmmr,nnn -rn rn rn, mw-, wrn mr w-n n, n mr n n,nr rn n. , r n mr,n -n - --- nvrnnm m,r mnxr r rn r m , wrn m ,rrm , wx rm ,rrm rnnmwn v, nnrrm nr rn r. m , wrnmrr °. nrr ° °,r ° mrnrm , n r rn r m , wrn r rnm - mr,° r -n°. ° r° rn r m , wrn nnr °, , -° °, -° °, -°° ° -°°°, -°, -° °, -° °, -° °, -°° °, - -° °, -°°°,°, -° °, -° °, -° °, -° °, nm , -°n °, -r° r°n, r° °, m°, w°,° °. nnr,r n rzr rn v , rnrnmvn,rwrn . rnmrnrn r m , wrn w w,w,r mxr wxnr w, nm , n w mxr wxnr. rrn n r rn r m , wrn m nm n,rn mxr wxnr. wx r rn r m , wrn mxr mnnr nnn rrnn - n r , r wxnnmnr. r r,nnnnnrr rnr rrn, mr, wrrnr mnx,r mnnr. r rrnnm nrz,nn r rn r m , wrn mn nmn ,. mrnxrrmrnr rx. m , wrn nrzn - ---n nmr,n,nn r rn r m , wrn nnr rmnnr wrn wr, , mnr, r , nrnrm ., n r rn r m , wrn wx nmrr,rnnrrrr. mxn m rn r m ,rrnn nmxr w rv mxr rx . mxr ,rxn wr rrnv r r m mx,rrnnrn nm , n r rn r mr, . rx mxr wx wrn mnn rnxm mn,nnr r nrnr r. m , wrn mnn rxnm r,m rn. nnr r-n r- r mx , wnrn r. mnn wxnnmr , n r rn r m , wrn mxr mxr n n wx wnvr wnrvnrnrnn , wrn ,r. nn mnnnm r, n r rn r m , wrn ww r rnrn wm, mx n, m rrx,r nn w xvx mnrm nnrrn. w..r m rn. nn n m wnrwnnn wn mr , m , r,nvn mnn .n, wn rn r,n r rrrn, r rwn, wnrn wnn r r n rvw mnnn rwnr n n r n,nm w nmnnnrwnn. - --- nmrr rnn rrrnnnrrrn r.vrvr,n rwn, rrn m.-r wn rn r nn nn v mmw.rr-rn r r.. n ,w mr n,nn - r n m--nnrn,rm-n rn ,n n zn,rvnn r r. mrr-rn r r nrn nn rmmnrmr . n m m ,n w n n nr nrrnw rrn.nv. nnnm r r wnn wnm .. r r n r r n w .nrm rrrn. r nn nn wr mr nrn vr w nvnn wr n wnrr. nmrrr rmm r r wn w mrrrn.. w rvnr r,nmrn w r , n r v .- rnn nmrnnrmr wnxnr. n . - rmrmnrm wx rnnr .. v n w ,nr.. - r --wxnn n2, xn2n m2rr mr nr . r2 r-- rnr nn m-rn mn-r-wxnr. ,, rnv w. mrrnrn wn wv w . -w vrn w vn rnrm- .. - rm rv .x. x wrxrnrr n wrn.n .-. rnn n mxrnnrm wxn n w v , rm wx nr nn2,22 mxr w.,2nr.. x rm r n mxr w., wnn w.,n w.. nmr mr mxr rr m.. - -2-wxn r -xn n,m mnrnr ,rnr . r -rr n mrn rr n w v r v. mnrn w nn., n w -r- rn vrn w r -xnvn.. - r rnx,rmnrrrnr w mr r . x ..rn r rrrrn wnr mrrn. r r nmznrnr.r nn-rnrnz - --- mn r rn r .r -- r r rr n: , n mr w ,rn r r w w n ℃~r ℃m mn n n wr ,w n m r r “m” ,rnvnnrnn n n mrr .- .rmnnrrnrr wmrr. ~ ℃.. r rmrrrm r r wn m w r “m”, w r r rnm r n. r wx <. - r n w n r . m rm r n.m w r . r n-wn. w mn r w < w.. r v m rn xr rm r n.nr w mz n-r-.wxx mn. n vvwn rmnrr nmw ..rmrm --wx .- rrzn n wn mr -2-wx. rmrm r nr nr, vxn r .. - - rmrm mr . 2n w2,n2.. n,n rv n rr nr n v. 2,r, -2,--wx,-r-wx.,n.- - r -2-wx,--wx,n- n rn2 . r-rrmn.nr w wr m .r w wrn m r wrn. rn ,r n wxn .r--xn n r.-2n-wx m.n. vw-w mrrn-2- n n, r.. rm -2-wx mnnr mrnn vrw n-nm. wr nrvrnrnrnrnnnvn, 2 nmr rn w r wn- .., mr . 3 nmr mn. vw- nnrrn-a n-w.x.n.b nrn nrmr--wxn rnnnx., r w vrv..rn rnrmnvn--wx nnm mn vw - mr nrn rnn , n2m r rnr wn- ..,amr b. 3 r rn w r - --- v n. ---wxn -mn---wrvx wxx n.. mr mrv n2 --wxn m2-xr-wxnxvrnnvrrn.r. w rm r n -- n -r-..,n v n rnn -n -rv wx. n rm rrnr -nnrnx.n.vrn..r n2rm nnr -2-wx =.. 2 r vw .nnrn n-r-wxrx nvrrnnr r. mn . rvrm--wx. x, r v. n.r n- xnr. nrmrwr n mn vrwr. wrn n.m wr . r n-wn. w mn r w < w.. m rn. xr rm r n.nr w mz 2r-rwx w.- r -2-wx.. rm - n w mnrn.n mnrn13.nr rn13n - n1vr .,.,n ~.n mr13--rrnnrrr n13 , . –.1, ,n vrn rmn n r n , –, ,. rr n wrn, n n.. rmw rn .- -mr ---rr-wnx..rmrrm rmrnm n-r-. wx wrm mn v-wr-wx wn mnr vnwrnnx nn,.. rr n2 wrn,mr wnnnrn n-- -2-wx. n r -r-wx .wx rmr-m-r--w-rxxnzrrr.n mrmn n. nr nrn n vw n. x n. r n x n.rvrm-r-wx. mn vw - --- n..-mrvrv wxnwnrnnnrnnnrnx n. nr xnnn r n nnn n n-rv wx. . m rnn-r-wxn-r-wx. n r rnrw-r- rnrn,12-19nmrr wm rmn rm wr.r . .- nrn rrnr r nrm rm . r rwn w zn r nxrmn.. mr n mrr nnn rn r r.. -wxr - nr nrm r n n wr, r v.. vrn -n-wxnr rmw nn.. rr .,- nm n mr m ,n nr , . rm .. n mr m rrnr rm n mx rm r n n,,nn n n vr r nr n r n wr mxrmx r = w. n w. . r, r r rr w., w.,n w. rmn,,, mxr, r v.. r n n nn r rn rm , rvn nnrn nn n wxr wrnmrmnrn mxrnnr.rn rnn.nn.r rn nmn r n wr v nr n wr °. rrn r r wr vn-- 1 ..- n n rm n rn. 1m n .. nnn 3.nrm n nrznn rn... -n nr wr r vn rr n rn n 3 n .rn-n n r n. rn rmnn w -,-,n -rn.. rnr n r rrnvn mrmn.. r r wnnrn rn r w rm.n , n n -,-,n -r nnrn.. n n nn .- nnnrn. , m rr rn.. m n-n,n m-xrn.-rv. rmn.n-wrrnrxn nrm rrn - --- nn vr.n.m m- wrrm rn-wr mxr.., r . rnn . -rnnnrnr rmnn .. nvn n n-rv rmr . nxm xn r w r n nrz w mrx wx, mrmnrr. n, mxr n .nr- mn vr rmmrr. m rmnn nnnrnn rm r .. rm nnrrnnnrnr-rn-nwx. rv zrnnn 1rnn n n zn mn nnrn.. n66 . rrn rm n. - .. rmrmn n vrr . m nnm rnrrn wn v rr, xnn n.r wn rm r rm.. rrn, rn rrnmn r ° v.rz rr vnrz rnr wnxn rnrw rnm rnn. = mrr rn mnn wxm r w, w = °, vrzr nw.. rn r =.r-.m°.nnrnrrrr, nv rrn.. zn m °.r w rrzn. xrmn wr rnn,,- xrmn wrn rnmrm-m wrxrr wnnr,, = °.mr, °. rmrm r wn -rrnzn nn- = °. xrmn wrrrmn .wn r r .rrmnnmrrrm. .rmrmn - r v nn mn vr wn.. m n.rr m.rn n , nr.1rn. rn66rmn n nnn rnn wr n nnrmn n rx r. .m rn, wrnrn nr - --- m . - -r . r rm m m rm- nn n. rrn nrn ~. - .. rrr.n mxmr rm .rmrmn rrn n nn n w m n. m rnn-n n mmxrnr ,n w mnn . r r . rn rn n, m- rrnrnrmnmmnnn w1r1r 14 rrn. mn. r ...- 1 nrmnn nnnnnrnnz mxn mrm nnrnnv n r66 rmn n nnrn mx nrn n.. mm n . -- wn mnxr-wxr. n n n r r n mxn rn w n.. rnr rnnn nnrn.. r wn r rnvr w n n v .vr, . nrm n mr r-rv rn. n nm n rnn wr rn. m rn n. m m rrnn nnrr nrm. mmxnrz mxwmnn r r m rn n n m nm. r rnm . m. m nrr w- rn. rn nnnr mx wnrxrmxnn w rr nn nrnn rmn r r z .r-rmr rnnnrrr wr r-. mnnznnrwn. - nnrnn n r nn ..w rn nnn w. r . vr, rnrm n -rv x rn mr .r-n n. rmrm r r n n r nr wr.. n n mnmrn wr r nn. rrn nnm nmrrn rnr.n - --- rrmrrmn nmxrnxr nr rn .nn wr rv . nn-n wnrrnrm n -. . n - nr xxrr rrmm .. . n - nr xr rm mx w. , w.. rnrw m w mm , n n r n n n.1 n,r mn rn wr’ nr n~ w,rmrrrn-rrm r-mrmnmn rnnn wnrn nnnnnn3rn mn.2 w nnrnr m nm n. r n4, r r v v r n r r mwnr v,n m n w r n. n n r rmvr-m wrmr v n- n- n r n nr n nn m w wrrmr mrmr n.,nrr.nr wnr,n m mrnmnrnnrnn m m nnn rxnvn mwzrmrrr.5 v vr 3, 6-8 n wnrn nr r vrnnr r rmnr-vm. n nmr n.rrmrm m n vr vrz wx rrrnn r r “n” nvr -nnnvrnmrnr-nrrnnn mnr m . m r rn nnm. w n nnvrnmn vn r rnn. nn m n mr mrr nr, rrr m n mr r r r n rn nwn nw r.nnrnrn w- r wrm m, nn rrwnn ,rnrvnrmrr..., rn mr n,nnnrnn mrmr, rxn n rr. , w r wn r. n - --- xr rnn n rn r rm.,nnrnn,rmn,n rr nnmrrm n nvnnnrv,n , nrr nx mnn r nmr v x rn nn nm r m rn, n nv rr v r-rn nm wn rn nmr v n -nnrrxn r n. r, nmr rn “ . ”nv v ..,,n,x,n rn v - . , n . wnn r rn ..,.,.,.,.,n xn rr n.nrmr rnn nr m, rn “x”n rnrm ‘x’ n n r,.., r ‘’. rn n xr ‘’ wn rm rn..,r ‘r x,n, ‘x z’,nr’ rnn n ‘nrrn x’,n n’,n ‘ rnn z’. ‘w x’,, ‘ r’,n ‘ ‘ z’ w rnnrr n rn ‘ x’, x,, z,rrr’ ‘rrn x’,rr ‘ ’,n ‘ z’ w rnr n rnn rnn’,nn ‘rnrrn z’.nm nmr v,.rnm “n”,nn “ ‘x’ ‘’”, wr ‘x’n ‘’r n r r nrnzmr w v ,n “ ‘x’ ‘’”. nvnnn r ,n n nr vr n n, w r r m. m m,nmnn,nnrn w mn rr n.nn m r nrrn r nn rnr nm nn m , w rr wr rnr w rnnnnrr n m m rnwnrn nnr nnn . rrm w nr n r n r,nnnn xrmr,n r nnn m r rn nr r mnrnnvrvnrrn. nnn mnnrr rrn,nrrn nnrmn., mnr vr rm,r nrrnv mr nr,rn n,nnnm:nn r,n v n mmn n w nnrrv m mx n n nnr, wrn nn rn mrr r v wx - --- rmrmrrrrvnrrr rm rmvn mnnn v r nr rnrnn vrmr,rmrrrv mx nn mr rr.rnn, nn,nn mrvnnrmn mxnrn wxw r n vnnnnmr,mn n w nnr r n v r nrr mvrr wrn nn w nn w r n v r mxnr wrn .mr r nmn nrnmnr,n vr nr,n. rn,nr m,nnmrzr rn mnmr,nn r n n rr r n rrnmn r n n m r rrn mnr 3 rnnnrn r n n r3nn m rn rrnmn. n m mrr mr.nm 3 mr,xn , rmr,r m , n nm m,rxm: m rx nnr.nm , n nnr mrmnn rrn m .nm , nr vrn,rn-n, mrzn,n nn.rn mnmr,nn rn, n n rmnnr.rn vrnnn w- - rnrw-n n .nr vrnnn n n nnn rr--m r-w n .r- rw-n nn r . nn mm-n n , nm,rn ,n-m,r-w n , m n nnr mrmnn rrn.mnnr.nm , r vrn.rnnx,mn v,n r v,n nnnrn m n mrr,nzrrrn m v z,rxm ,n rnnr,rr,rnvnrr.nrnmnn r . v n nr nnr mr mr rm w n-m :nnm nn-m zrnmrmn m rrrr m mrr.., - --- rrz.rmnnr.rr mr nn ,rxm,mnn n nm °mrr r mn, mrr v n n r °n n rvr r°r,°,m.°n,m° , mrr v °,°,°,°,°,° ,°,°,°,°,°,°, mrn rn ,°,°,°,°,r°r mnvr rr m , rnwnmnrwrmrr r mnvr rr m.n r mrrnr z v n n m v , rn m ° °r mn.nm mrrnr rr z v n°,°n,°,m°,°, v r °,°,°,°,°,°,°,°,° °,°,°, °,°,°,°,°,° ,°,°,°,°,°,°, °,°,°,°, ,°,°,°,°,°,°,°, r mn °r mnrn rn wnnwmrr mrn. rm ,°,r°,mr°,r°,°°,°°.nm , r °,°,°,°,°,°,°,° ,°,°,°,°, °,°,°,°,°,°,° ,°,°,°,°,°, °,°,°,°,°,° ,°,°,°,°,°,°, °,°,°,°, ,°,°,°,°,°,°,°, °,°,°, °,°,°,°,°,°,°,°,°, °,° °,°,°,°,°,°,°,°,°,°, ° ,°,°,°,°,°,°,°,°,°,°,°, °,,°°,,°°,,°°,,°°,,°°,,°°,,°°,,°°,,°°,,°°,,°,°, °,°,°,°,°,°,°,°,°,°, °,°, °,°,°,°,°,°,°,°,°, °,°,°, °,°,°,°,°,°,°,° °,°,°,°, °,°,°,°,°,°,° ,°,°,°,°,°, °,°,°,°,°,° ,°,°,°,°,°,°, °,°,°,°,° ,°,°,°,°,°,°,°, °,°,°, ,°,°,°,°,°,°,°,°, °,°, °,°,°,°,°,°,°,°,°,°, °,°,°°,,°°,,°°,,°°,,°°,,°°,,°°,,°°,,°°,,°°,,°°,, - --- °°,,°°,,°°,,°°,,°,°,°,°,°,°,°,°,°, .n °,°,°,rn rn wnnwmrr ° m°,°, r°mrr ° °,° °,° °, mrr ° ,°.n°m°,° °.nm , r ° °, ° °,r ° ,°.r mrr ° °,rn nnmr mrm,n vn.nrxm, nrnnrnm.mnnnrn:nrm mrn mmnrrnnr mrrnr mxrnnrr-rnmrnr mrnrrnr mrnr mrrnrn nr mr r r rnmnnr. vvnr n rm .rxm,nr mnnn nr nrmnr mr.nm , v nr nrn mn nm . rvnm , mr r nmn nn w r n v n w mxr v . r nmnn m mr wnrn nvr rm rnvrnn mxr , mnm rr m . r nn mrn mxr ,rrn m rrm r mnn mn vr nnn mr w ..,,, r,rm rr.nm , r nm rm r,rm ,,,,,, ,rrm r.nm , r nm ,, ,,,,,,,,,,,,,,,,,,,,,,,,,,,,,,,,,,,,,,, ,,,,,,,,,,,,,,r r.,,,,,,,,,, mxrn wmx , vn nnnr.mnmmn n w,nnnnrrv m w v m mxr wx.nm ,r vn mmn n nmnr. wrr n w m rn v . w nxm, nn nwnnnr n v nn r nn nrrn n nnrnr rrw nn v n n nn nr n v n ,mn mxnrrn wxr rv mmn n v n nr nr.nn vn wrn, nnr. n vmn w nnnr rv r r n.nmn r, - --- nrnnrr.rxmrn, vnn.rnnnr,n,,nr, w v r ,, ,,rnmnwn n v .,n, , , nrv rmrrrnn v .rxm, nr r znn v rn rr z nnrnrvnr m v r mrr wn n vn.r w nxm, m v rn v v m n v mrrwrn m v r n v .rxmr,r m m v . mxr wx n v n mmn n nxnrr wxnn v n w wxr , rn mxr w n wxm nnr. nnr rr, mmn nn r nn nrrn nnr rwrwnnn v n n nn nr nn wx, nnrn n rvmrr n m mxr v n mrr n m mxr wx mmn nwn m mxr wx n r nnrrr . mrr n nnrnn , ,n,v,r nnr.nm , nr, -n- m, nnr,mr,rr, nm ,,rzn ,x -n- r vrnr.n nr n nnrmr r n.rxm, r n mmn n nnr. nnr r rm v , v n rm v .n rmvrm nnrr rmvnn nnr.nmm,, r r r n nw nr nn rnr n nnr mvrm nnr, , rnm , w.r, , mnr, r ,r mnn xm., r nnrnnr n r nrr.r v n rn v rmnrnrrrn wn rn xmn, r mrr rnmrrn . vrxmrn,nr. w n n rn r rn, rn n nv.nmmrr,.n w nxm, rm nnrr mrnrmrr -° °.nm , °° °, -° °, -r° -°°, -°°, -°°, -°°, -°°, -°°°, - - --- °°,, - -°° °°,° -, -°°°,° -,° -°°°, -° °, -° °, -° ° °.nm , nnrm , -° °,° °,° °, -°, -°, - rr -°, -°, -°, -°, -°, -°, -°°,, - -°°,, - -°, -°, -°, -°, -°, -°, -°, -°, °, -°, -°, -°, -°, -°°, -°, -°, -°, -°, -°, -°, -°, -°, - °,°,°,°,°,°,°,, -°°,, -°°,, -°°, -°,°,°,°,°,°, °,°,°,°, ,°,°,°,°,°,°, °,°, °,°,°,°,°,°,°,°,°, °,°,°°,,r°°,r°n, rn°,w°,nn°w,m°,rr°,°.,°,°, mr wnrmrn, r mrrrn. mrrrnn vn v n w nnnnr.r.rnxm, m v wnm ,rr,,,,, m ,rrw mrrrn. wnnwnn ,,,r mrrrn.mrrrn n r mrr.nmnnmrrwnr rmrrn mrrnnnrmrr ,°m,rr rn wn v °,°,°,°°,,°°,,°° °,°,°,°,°, °,°,°, ,,°°,,°,°°,,r°n,m°,n°n,r°.,n°m, °,,rmr°r rn wn v n nnrr ° ,°. nm , mx,r rnrv rrrn wx,, ,r rvmnrmnnr.nxr m r rnn rrn mnn r r.nr wxnrnrnnr m. rn r rnn rrnrv r m m r rm n n. rrnn r . r n mmnnr rrnnrnrrrnnn n n. rm n rvrm nn m r nn rx rrn r .nm , mnxrm wnxnn r rnr nn vr rnnn , wrn mxrr mr wmxr wn - --- nr wnrvr r mnnnr rnrx,zrn.nm. , wx r rnnr rnmn mn,. mrr rrrrnnrrrn r mrn, w r n r w vr rn r mn, ,mr rn .xm rnrrrnnn r n, ,r 3•rr2,3•mrrn,n wr rn nm3,rn3•n,-26,. rnrx. r x r ,rxm, r nm .,n , wx,,r mnnr nr n w r r rrx m.nn r mnn r,x wxzn,,r,m wnx,n,r mnnr n rn xz , wx,,r r r r r rrx. n r rn mnnr w r r nn rz. nn rmn n n,r mz.rr rnrrn nrz.nm , wnr n r nx mmxr, n n.xnmrn.xmrvnrnn +, nr +z ,r4z+n ,2+,r2+n r ,n2+rrn nnnn nmrn r nrnn mrxr mrx. nnn r rm , m r rnrrn rnn, w rr nrrnr rrnr m r rn. r rrn,rxm,nn nnr mrr nrnrm rnnr rnnnrnnrn.nnr,nrnnnnnrn nr r..,rrnr m r rnmr rrnrn .rnnn rr rn, rn rrn, w mrrn r n ,rm ,nrnr,nnrnvrn. .nrn mn r2rn . nn nm, m, r r rnm, rm, n. r xm, n nm, - --- mr,rr-rr-n, nnnr'nm,,rr' , n r m r rx nr ,nn n. ,nm rx, m rrm rrnrnn r-x- r.nm nmnnr.rxm, wx,, , x m r rnnr rx n. r mnnr r rx mxr wx,, ,nm , mnn m r.rx r mrmnrnrrnnr rnmnn r r mnr nr nn r . mnnm rmnr rnnr,n vmr, w.x,n,r ,r mnnr x m , ,rxm,nn nrnrrn.n mx wnnrmnr w vx,,r ,mrr wmx,n,nr,rx xn x rmx wnnr n v . mnnr mnnnmn rw, n n n rm rnv m w r mnnr n rnr n r w r n. nr rnr rm, nnmmn nr, rrn rvnvnrn mnn n nrnrnn wn rz mrnnvrn nx xr n r rmnn r “”n.n “n,” rn, mnnr mr wn n rn nmr mnnnnvnnnr n nn m. “”n “n” “”r n rn m . r r nrrr nnr nnr n r r rr nxnr w rn m v nrrr nn n nn n nmmn nmrn,, n.mn,rrmn,nnrnmn,n vn mr r m rrr,nr, rn-nmm-nrn rr nrmnrr. nnr mn r rnn rrrm mrrn, vn nmn,,nr .mnmrn r nr - --- mnrrmrn nmnnvnn,r mmr v wr, n m rrn,.... wr ,,rrr,,rrrr rr. m nr ,,,r,-, ,,r,- .xm - n , rr m rmn ,vn n. wrm “ ” mn rmn, n,- , nr,- r rn,rn, x,- n,- n,,-rr- x, n,- n,r- n,rx,-,mnn,- n,- mn,- x-rnm ,x,rx,rn - xmn, n,- xrnmn,- xmn,- rn,rn,r- nmn,r rn r n m rrmn,- - x ,x,rx,rn n n. r,rm,rvmn,r m,nn nnr .., mrnnr,nrrrm n,.., r n,.,-n n,rx, x,rx,r n mmn, mnn . vnr n n x,.., , vnr. rn mnr vrnn, rmn “n,” “rxm,” “r ,”n “ n” mn r n mr xrn v. r, v rv vn r r rm n,rmr,n rn n nr mn,z, m rxm nrrrr rr r nn n n x, rnn mr, r, r n rn,nvrn r, v, mrmnrrrn ,n r rnwn n r vn rn rrr r n.nmrmn, v rv nr , rn,nn rn rmn.n , nr vrnn rw “ ”n “r ” mn nmn v n rrnrrnr “rn,r”r “.nrxmnr,,nmn,z,rm n,rmr . nr wr “ ,”r “r ” w rr nxr nv v, rmr ” “rxm,”r “r ” r rw. n nv v ,n , wrn nrn w wrnmr.nmnn rnn, wn nmw mr - --- mrnn wnmrn mnrxmn. vr wr r r wrnvr n nnmnnrnn r. mn nnrr.rnr wxn,nr nn,nn:mnnnmrr rm n mmn n w nnrrv m ,n v n nnr, wrn mxr wxnr r mrrvrr nn rn mrr v r mrrr nrrmmrnv mn mxnnr w vxnrr n.r . m rn nn - wrn rn mrr r v mn. n r ° °r mn vr r rm. m mn rn mnnn,rm - mn wrn r mnr,rmrm rm. mn mr,rmrn mnn. rn,rm -r w,rn nr m . m rn nn - wrrrm r. v n n m v r nm rrnr mrr z ° °r m nr . m rrn n n. r nn r n, nnnr n mr rm nn w r n v n ,n mnnrn m mxr w mmn n w nnr rv w r n v xrn nrrr mnrrnnn wr,r wnrnmnrn r.nmn nn w r n v rv mxr wxnr . r m,rm rnr,nrmn r- wrn r nmrm . m rn nn ,r-rm wr r. ° ° n r mrr °. m . °,°rn°,n°n ° - wrn r mrr °,° ,° °,° °,° . m °. ° °.rn nn - wrn r mrr - --- °. m°,r r°n n°,n ° - wrn r mrr . m rn nn -°,r ° °. mn wrn mrx nnr.r. mn rn nn - wrn mrx rn.. m v r.n nn - wrnnr nrnr xn. mmx wrnn nn - wrn mrx rm.x m wnnrrnnr nnnn v .- wrn mrx m. m rn n vn. - wrn v rm.r r mrr. nnrnrnnn r n-, wrn mr r n,nr n, rn n,nr . m rn nnnmnn-r.rm r nn -n n, wrn mr - w-n n,n .n rx mrn mrxnr wnn. xnrm -. wrn ww. r mnn mxr. m wrn nrvn mxr - rrrn. xnm.xn . mrx rn wnnrv -rr mxrnrnrn. mxr .mr m mxrrn wxnrnm - w,rrnr m nvrnrm , m ,r . m rrrm . w n nn - wrnmrr rn °.n v n nnrr ° °,r ° -.° m °.rn nn - wrn r mrr m.r mr -°rn°,n -n° °, -- w°rn°, -n°n°rr°, - - --- °° °°°, -° °, -° °, -° °, -°° °, - °, -° , -°,° -°°,° -° °, -° °, -° °, -° ° ° , -° °, -° °,° °,° °, rz.r m. rn nn - wrn nnrn vn.r m. wrrnrn nn - wrn w rrn w, mn mxr wxnr w,w, .r m n w mxr wxnr. n r rn nn - wrn m rrn m. m r mnxrn wnxnr.- wrn mxr .xr m rn. n nn - wrn mxr wxnr mnnnn rrnn - n r , r r.n mr. nnnrnrnnrrn,- wrn mxr wxnr r r rrn,rmnn nr.. z m rn nn - wrn m rrn n. mn. mrxrn nn - wrn nrznn . m r mrx. r n rn nn - wrn nnrn mnn,r.n wrn wr, , mnr, r ,r rr.r mn rrnrrnn - wrn wxnr r rx. m rn n.n - wrn mnn rx. m r mnxrnn . - wrn mnn . m mnnr r. rm r nnnnn - wrn rx . m rn -- rx nmnnr.n wx wnvr rnnnnn - wrn, w mxrnr m wxxr - --- r. n wnvr rnnn , xmwrvnmr rn r,nnr, w nnnnn w r n rr r wnnxmr.n rrnnrxn r,r nnnm rn r rn.n n nn vr rnv, m n, nrr, rn r.rv nn vnn wn rn ..,mn, m nr r w r nmrn rwm,rrrr,.r, wm,rrmrrnrvn n r.n rr r nr n °r mnmrr,n xx -m --r.v , , rnn,nn,r w rnnvrr n,nvrnnm,nnnnmrn,.n rr n r nmrn r r .., r r w ,rr, rv r rr.nvrn n,rnn w n -v,-v n w m rnvrn n m m.rn n rr wnvr nn n r n nr nvrn rn n n r mx ~-. r n nrn nn,r rnr .rm, rrrrn-r nnrm ,rnn rnrn r r nrr n. nmx n-r r n rx nvr mnn r n n, wxr rmnm nn , vr rn n n. -nmr ^- nr mr n wxn r vmrn,nnnn.vnnrrnnvrn w r -nv r-mr- r n,m,nn,m n,mn,n wrrmn. mr nn -nmmr w nnnr-v mr, v..,nnvnrvnn nrnrxnvr - --- nmrrrn.12.9-1r1vrm, nrmn wn,wvrm,r n rn rv n v n- n .r nr w n ,.., nn. n, r-n n- r-m nrn rx n rmzn r nvrrm13-n n14 n - nmrv vwrr m nm- n , r v,nr r n v rnnnnmmrz .15n nvr nm rnr r v nnrzn n . nrn n- n -v n , nvrn nr. rnrn n n r n nnmn,rnr v mr mn..,mr .m v .., rn , wx,n r rrm mn nrrnn,nrnr r mrm vrn nn r ,16 nn w n rn rn n r n m rrn n. r nnvmrvn nn n mrr n nr n®> r n m,nr.17rmnmn,r nvnr m rn rrm r n wrnxn r r n r 18-n n rrr r nnn, rn nr 2n r. rn, mzn vrrn mnmr r- m-rr r rnrn.r19,nrnv rrr -,nmrn- rn m mnr-,nn m w nrn-nrrrv2,m2,n, n nr-mr-vm n,nrr nrnrm rn rn r w n r n rn w vnnvrn. r n nn rnr rnn-mrr rm m n v . . mr vr rn nmr ~-nrm rrr rrr rrnn r rw “n” vrz wxn xz nnn m wr m nv .. nrm r r n nvrn -nnvrnmn- rnn v n . nnm. nnnrnn n w nnvrnmn nn nrnnn,n n nnr.m mxnr xm w v ..,rrn nr mmr rn rn nr rnm..10, w v r mr v n m r - --- r w~ m wnr mn m- n rz r r nn n m r rn ~2, ℃ v 2n2,rr. r n w mn. mr “m” . r,n nn vrr z ~ ℃r wx. wx wrnn n n zrn rrmr,n nrrmnn rrrrn. wx rm r rvnnrr v --wx,rr-r-w nn2-2-wx, ,2x.2-,- x wr w., w.,n w. . n , ,n , r v.nnrxrmn w mrrrnnr ..rn nmr nrm wx wr r-nrrn n w -,.rmr-m rmr w rrz wxm n n w,,wn mn wx w mnrr rrn~ w. w mrn. n.mrrmr. , rvn nn20n rn ,--wxn-r- mr r nnw r r.n --wx.2--wx wxx - n m rnn mr 2-wx2.,n nn mr-r-wrxrwrrnnnrnw2n 1rvr mrr rn wmn- ~ r r n xn-nnn r,rn rn n rr,14 r, 22, 23. r-r-wx wrnrnw rrzn -rwnrmr n rn . rr, nrr - nrm r r-wx w n . -mrr rmnrmr rv x m r w mnr w rn wnx .n. - nn rrnn> ,24m rrr m nznn w-v n wm nz v rn. r m--wxrnmr--- w vr wx vr mznr nr n , r v2.nwx . nm nmrnv ~r nnn ~ w ,vrrrnwn mnrv wr rn n-m2-wrx ~ wr. -n2-rwx,nv-r-wxr wnr nmw rrrr--rwzx w n ~r mn ~ nw ~ . rr nn rnxrmr mn .n,rr n nnr rnnnrnrnm nrm , nv wxrr. -rn rnnnn1r r.nnn.,13-2-wxnn--wx,n mwnnrrnmrnr - --- nn,13 , - . rn 2 xz --wxnr nrn n nn wnxr w. nn. vmvnrn-mn r n r 25, 26. wrn vn2xzn4- r r nrnx n, r rn n r rv. w.x,r w m ,wn n -xrvn w rx mvrnr nnr,nr z xz rnnrnr rn n rn m.2n7 wnnn r n--wnrw, wn rnnx, rn v n 2xr--wx.--wxw rn vrn -2-wx. r , x n13--wx -,rrnnnr rnnnrnn r . n, mnn mnrr n mnr r, n,nrx . wr mrrxrn, w w wrnm n r w. x nn 13 vr n r n n n n ., . n n w -r-z w w r,rrzn ,wn--rm.rr wrxnnrnnn mnrr vnm, wr nnr .. r . rn .1 xn rr ww nmr , --.n.,n n n rx n-r. . n wxrmn rrn v,vnnrnr m m mnrx . ~ m r r nnrn, vnvrnn,nr.,rrnr wn --nrmr --wx,n2r-r-2 2 2 2wx, v r2 v . wx w wx w., w.,n w., r ..nn ,,x.-,-,n, w mmn n nr n r n w mx rmn n r,mnn n r r n n v w nnvn mr nm rv. rr, wr mm r2n rm rr.- n -rv wx nmr n wr m m rrnnr n- .. rn n,n,nn wr mnn+ n rn - ,n r rmr r n mnm n. nnrnn nmnn r nrnm -rr-wxrnmrwr w n rm nrmnzn.w..mrrrrnv, - --- rnr,28-r2-wxwn-r-w mxr wrr-rrrzrn- nr- - . , r n,--wxn -r-wx wrrm n x n. nrn n 2.,,n . rmr m rmn n w mnr rn,vn rr nn rrm rmn n w-m-- rmn n wr n ,v n .13n,m mnrrmnrn m n 1rn mrrr.mn. m rnr wr xrmnn wnn.-r-wxnn n, ,n r m-nr x-n ., n rn wmr -2-wx. r rv wx, n -2-wxn-r-wx w n n ~. ℃rvrrnrr.x-2-nwxx n w wrn-r-wx, w wnr , .. rn - , x n r wr rr,zn n-rn, .. r n -r- r rn n n--. rnwn nr rr n w rnrn ,n n -rxr rmnrr.-r-xrnn . , n rn r v m r mn m m , n rx r nv rn . n r rnn mxrn wx w.n, w nvrn, nrn , w., n wx n.., wx w wr., ,vnnvr nm 2 r n-nnn r . m . n . vn r v ,rnnnn r .nr,29nn mn n r .16n nn r rrn rn mrn vn n m r , n r n nnnnr rn30,r 31nn r. n"r" ^^! n v ^- mn ^^! ^=v. nr r ^^! =.m.rmnm,nrm "# mn ^- n rm.nmvvrmr.nrr xnrmn,n nnrm n ^-n ,n r mvr nnnrn rnr n r nv r ^^"",% =.mn ^^n = -. m ^^ =. mn ^^ &&' "",%&&' ^""v,r&' =r.."n#,%&& mn' nr ^^n"",&' =m "#,%&&' ^=. m.wvr, ^ -.rrm ^^"#,,&' =.nmvnv ^^"r#, ^&'- ^= -.n - --- mv. mn rmn mrn rnnn. ^-.32n wr r n r nr n rn nn ^- nw wrvn rmnrm ^ n mrr .nnr, n xrmnnm- nn mvr.vrrnvnrnnrm ^- nr wn w mrr r w w rr, wr n rm nnrm r ~r –mr ~r ..2v0, 33-40, w rm r r nr> rnr wr rr vr nr rnm n n n r rm n nr . r r w mrr-rn v w rn n,nn,rww x nr . w mr v vrn , r nrmrnr r w zn.n n rnnnnm mvr w , rrnn v,mr-mn mv mrr vm w m rmnv. nn-r- nrrnn nmrrr w-rxn rnr m nrn m .n wxrrx, r ,19 r r xnn rr nxnv n nn.rmrn, r n rrnn r n r w r-n- mxr, rmvn n v r- m wnr-mmrv . r n w r mn vr rn m 41.-43 nn r n -v -mr-vm rnnr w . nrr r n n nrm nzr, r n - nm. mn n w nr rn r x >.nr rwnzn ,,.m, wnrr,.,rmn-xm-nr w,.r r rmmr 66 rr,n.7n8 810 44, 4 rv.nrn wnr xm w-rnnzrz rwrn mnr rrn rrr.z5.r n w n n - ---nrmnn r mrnm mr n wrrrmn w - mnn, n nm xnzmn.. wrm.nwn.mrm n r n : rnrmr wr nrnrm. ° rmv m mn-1 nnnw m nw . mn m m mnn-1 -1 mnvnm , : mmnvnnn mm. m °n mnnvnm ° mn-1 ° mnvvnnnnmm. m ° w rmrv-m rrmrn rm-n.n wrrrrmn n . rn w rrm n m m r w nn. rnrnmr n m rn nrrnvnvrn nrmr mrnr r wn ˚. znn -1r vnr w r wxrrm n n. rrzn --wx nm r n r n 2 wrn n r -xn wr vn r znnz.n r n-rv wx,xz wx,n rn r m n rrnn rwn. rn xrmn w rn rn nmn r vn, w rxrnrmrmn,rrnvn rmr z rrrnrmnrr r w,rnrmz rnmnrmmn . rnmr - m r –1 rrn r n m-1 m n rn – m w n ® w rxn. rmrnr w..rmn n rmmnmr TM - --- mrmn r wrrrm wnrnrrmrmnnw- m rmr nrmn. r °n n mm mnm m n mmrn:z. mz rrnr m nzn m r - w rrmn n mnvnr- w,rmm- wn mr- nvnmrr °. z. w r w mnn mn mmmrmnm wr vn : wr: nr nnn mmnm rm n vn : rn: nr nnn m w m, mxn wnr rnn:nn:..mrm wrr.rn xn,nn wn nznwn n m n nn vn m. wr r r m n m rn - mzn nm ..nz rnr n nznr w rn n v .nn w nrrm . zn w:.mn, n w:.mn,n r °, vnmrr : °,rn r:mrr: : ° w :.mn, mrr: °, n . rr n w nn22 mxr r w,n r nn2nr ..mrr r. r ~ m w m- n rz r r r r r r w w rz n w rn rr-rn. nx m wn rn,r wm. n w w rn m n r mn w mxr n wrn n ., . r r rv n nrr 2 .mn , nn n wr wr vn n wr rr w mnrr n: n r rn r v. r n w vr-rrzn rrz r r, r ~ ℃ rr ~r m wn ., w.~2n ℃r mwn, wnr nrrnnmrrnr mm r mrn r rr “m”., . “m” rn nrnnmr..rmn. r rm m w rnrmmnrx m mnr.r n rwrz w, . r wr w r r m w , . n,n r n w ,rn, rnr rnrrr w wn nwn wr r nmr rmmrmr.rr. - --- n n n. m mnnnn rw w...x .n xrmn, m wx r rn w r w r wx m wrrnrr nr r. nnwr w n r r r ~ m. .mrr w ℃,n r nr r .. wxn rx n, xzr wr n nn. n nrrn,, ~n m.n nm mnxr wn rnrxr mnnrnrr rmn . n ~nnnr , w r r, n n. wr nr nn wrr w wrn v r ~. m rr n n . w rn wm nvr . wr xrrmrnz mn . m r.mw n r n nr w r. n.rrmrrrnm rr wz rnrr w rnr nrnn rmrn... mrr r r m w ~ ℃ r,. wxnn n.rz wx w w mr r nnn n. n r w w n r r wrxnn r rn , r r,n n r .rwr, m xn w n r w r rxn. rxnxn, wx rn r rrx wn. wr rxn,. wxxnn wrn wrr rnr n m,w vn rmv n rr rr r-w xn0n rr vrr ℃, mr.n r rr v mn wrnrmw w vxmr1-zm0.vrn. n m m1 w rrmm.rr. nvrzrn. rr rr w rnn, rmnr w rn2 - n -n.. nn rrr wr wmrm mn n,rrnrrzrnn n v. w:rn-,rv wxm, n mnn wr,mnrnnm-nrn - --- vn,-rv wxnvnmwxmrn n rvmmrr.nr r rrzn r wx n.r - rrnn xn, wxv wrmrvr.n xn r mm.vn --wxn xn w nnnrn wr r . v. 2 w,n rr ℃n rmn nmrnvr nn w vr m r w w wx wr ^^ * = ^ ^^ ^n ++ = * *, ^ ^ ^^ ^ ^ ^ ^ ^ ^ ^^ + + =* *, ^^ ^ ^^^++ wr ^^+n ^^+
Figure imgf000035_0003
Figure imgf000035_0001
-.m nnrnn.n rn rr 2 ^^* = ^ ^^ ^+ = , ^^ × * ^ ^ ^ ^ + * + × × ^^ ^^+ wrm ^^+ nnn
Figure imgf000035_0004
rn rrn nrmr.-.. n.zxn n v n -.n . wxrxrn wn mnr n rnnx ^^ ^^ r n - , wxr wrv n r x n vr,nxnnnn wx ~ mnnr w.. rw. rnnx w mn wrn nr mmrrn . . ^^ ^ /0 nn./0 m1.nrn
Figure imgf000035_0002
^ = wr r - --- rmn. n m rn m. nmnr nrn -rv wr mrnr, :, n w z v -.nr n -, wrx n nn nzn r v wr m n , m rvn n. ^^ ^^'02 nn r r m . r nm r ^^ =^
Figure imgf000036_0001
^^34 × m r w mrx rmnmrvr nnnrrmnrw nn r n r n, r rnr mrzn,n nmrnnr mnmn.rnnn r rnr , - n r n rmr rmr - nrv nnrrmnn.rrnr,n rmnmnn . vn r n. nrmn . ^- nn m n vr mrr w 4, 5n m rnrrmnnrr nn n .nrmn v n1 9 nm n . r rmn v m , n mr x 1 9 n r m n mrrw. rm w n n v vr ^r ^ = ^^ n ^^ wr ^^ "
Figure imgf000036_0002
+ ^^ ^^ + ^^ n nnr v wr ^^ × ^^, + ^^ + ^^ × ^^, + ^^5 n nn mnr nmr r nn. n ^^ × n ^^, n n + r r ^^ × ^ v v ^ + ^^ × ^^6 + ^ r ^ + ^^ × ^^, + ^^ × ^^ + ^^ × ^^6 + ^^ ^^ × ^ n rv rm r ^- n n nnr v ^, +n ^^ + ^r^&v + ^^7rm r ^- n - --- n nnr ^^ v × ^^, + ^^ × ^^ + ^^ × ^^6 + ^^ + ^^8 + ^^7 ^^ − × mr r rvrm r ^- n n nnr v m ^^, + r r ^^ + ^^% ^^ − × ^^, + ^^ − × ^^ + ^^ − × r ^^ v 6 + r ^^ m + ^^ r ^- n r rmnmrmr 5 . wrmmrzn . n- r w n r vv m.6 ^-nnnr - m r n. rn ,, nrrn rrnnnn r nrn r n, m r n1 2n3rmnr r xrnnmrr n vnnrmrn r v .nnr mn.r- m nr a wr n n . rmr wrnr mnr n r nr n, n n v vnnr. w mrr rn – , nnr v r v v rr-xEamrn m m,n nn .6mrvnn nn r lgA mrn. . nv n e wnmr mn n r-xnn r. . v.nrnnnrn r rnzn66n r-xrnn m810n. r m nzn6r6n-xn810 wr mr nnxrn rr vn66r810, ~ mnnxrn rn v3n wr r mr nnn n.r n 3 wr nmm, mxrrr wzr w n.wrnnnrrnr6 mxnn. mxnr r vn wr . mn. m, r v6.810 nnr.n nr n r rr n wnx n w . nnxrn rrn m . r rnz r rmn r vn wr z x n66n-xn810n nr n r vrnn r wrrn. m r nn v wr w n wrm ℃rrm mrnn v.mm rrz w vn n vr n. mxr wr nnrnm wr rmn n . zn. nr' m ^^ =91:!;<=*> × ^^ ^^ 2 × ^ - --- ^^ ?@=*1 ^ wr ^^ n ./. ^^91:!;<=*> .2 × ^^=*=12 × ^^ ^^91:!;<= ./. mr m
Figure imgf000038_0001
^^ 66 r n *> -xn n 8 v 10 r r ^^ n @= m *12 66 810 n 66 810=*=12
Figure imgf000038_0002
r r , r mn, r v ^^ m -nxr n. -rv wx r r rn x. nnrn nr n nnrnn--wxr rm ~ mm ~.n mmvrnr-rx.n,nn mmm zrr,r .n.n-r-wxnrwnmr r nrm ~ mm ~. nrn nrn rvr ~ mm r rmn m n. n nnnrnr m r w r n: nnrnzrnn.xm mvnrmrnnn n wx n-r x n rn7- rx,8r r n r n,7, 9 nnnnmrrznn mrr w rmn n, rmrnrm v nrmn~ r n v . m r w nrmn -- nrmrmn, n ~ w rr n ~ nw ~ n-r- n ~ nrn nmnvr<n>
Figure imgf000038_0003
n - .n rrnr rnn , mrz r n xnm mnnn n n r n m mnr.rr, nnxz wnrrmx ,n rrxn-n nmnnrr-.-wxn,n wx, n nnnrn~ mm, -r- .rr, n wrn rmrn rmn . nrmrn vr nx n,n r x n w .rnrrrnrrxrn.n r.
Figure imgf000038_0004
- --- c nn n a brrn wrx
Figure imgf000039_0001
c rnzrn, n,n xn. ,r w v. , r r nrm , ,n d er r wv.nrm ,nvrrm v. fr n n wr nrm mm mr, vr r rn n.- w nrm gvrnrmm , w,r , ,nnzr. .rm rnmrrrnnnr,nrvnrxrmn ^v .. x x x x vva b 2 - --- - - r - - - - - 2 a bxxn v wm r w nr 2 nrw r. .vr m rn w w - wnx m-rvr wxnnnn .n.
Figure imgf000040_0001
- --- 2
Figure imgf000041_0001
c wr r.nn n nnr nrmnn. xmr . v x
Figure imgf000041_0002
w bx. nmnr w. n ℃ wnrw r ~ m,vn w . =nnrnn wx,xz wx,n . x =
Figure imgf000041_0003
- --- a 2 . 0 1 . p n
Figure imgf000042_0001
- --- b c ‘-’n ‘-’ wr xz wxn nrm wxx n. d- w m r x n. e- m w mnnrnr xn wnr. rmn n . .nnr nrmn v m -r , ,n . rnxnrrrnmrmnr-r nn,,n mr r 298 K.5 . ^^ /mol K rou lael ^^, ^^ ^^ ^^ ∆ ^^ ^^ ∆ ^^ ^^ 600 800 K
Figure imgf000043_0001
. ^
Figure imgf000043_0002
- --- 2 -. -. armnrnm
Figure imgf000044_0001
’w. ^^ ^^, ^^ ^^ ^^ w .rmnm. rmr ^- nn n rnmrr.
Figure imgf000044_0003
^^ ^^ . . . . . . ^^ ^ ^ ^^ ^^ ^^ ^^ ^^ ^^ ^^ ^^ ^^ . . . . -. . . -. . -. rnmr.rr v v r ^- n r nnn rmr v
Figure imgf000044_0002
- --- b a a
Figure imgf000045_0001
. x - m . rr, nnmnmmrvn v w n,n mnmn m m n.rrn, r r w nrn rm r ’ mr m n n rr m r n ’.., wr mr m r n n,n n r n m °rr. wn r , rm n rn -, w w r nr w rrnnn mxr r wnr r v. , rm ,n r wx.n n nnrn n -nr nn nrzn w, mn r r nr n ,w vrvn rmmrr.mrx, r, nrrn wn-rxrmnmnn mn..,rnnrnnnr nrrn n w rrm. v- rrmnr,11nrr-rnx mr,n12.nr znn-, rr.,7nv m - --- z 1m 4rnvr r rrnrm ° wn..7nr n z m rn wr n .xnr nvrv nrvnn,nnn m r,mn rrnn.13n- rm r n.15rm rn n n rnn -rz- r nmn rrnnn nvr vwrnrnrrnnrnrnrm . wxn2 n vr rrn. , wrn ,r rnrr r, r nn --wx nmr rn .11 wnwrr n r xnv mr nrrrn, rn-m nnr rn rr v rrn, m r m r 2m2.16n nwrrn n2 n m2r nrrwr rnrmrr .nr, v m rn mx , v rr,nmm n r nm n .rr, mn n-r r r --wx rn nrm r nnn-.nrnnm r,wrnnrrxnnnmrnrr.1mrn, zrnnr m 1n rrnmnrn,,nnrm r-rrvnrnr.7 , rnnn n.8-21 mnnrr, r v rn r rrn nv n, n rrr. m n rrrmnrvnn mrr-rnrm rrm wx,w x n nr .22 rm r mr m nvr,rn nm m n mrrrn, n v n.mn wr n nr wx .rrmr, n v w nr rrn rv w mr v,n nrm n-r r , w nrzn.nr n rnr r rmn w rm r r nmnr m mrrrnnnr mrr-rnrm vr , vn,nr rr. rn-rvnrrrrmw- w - --- nnrrnrmn rn rnn.nnmrrrrn-rnnrmnn, rn nr n r r m , wrm mrr n r r n rnr .n n rnn n mrn n,n w nn r mr m, nrnnnn r . nr r n z nnm nnnnxnnnnn r n, n’rv rr,22nn nnn zn.n nrn rm nrm wrr nn r r r rn xrn mrr n..nnr r . rvn rn r nr n , wr rmr m rn nmr n nr rm rn. =-rv °nn =, ° ww,n. rm-m wrrr w rm nn . r n r nr w. wxn nrnn r r . r nnr rrn .,. rmrn znnn xn rv nm r nnr ~. mn m wxn rv.nnr,wn wrr r r ,vn . r zn . r. r n rn,mrr ~ °n w. n r r . , r °r.nn, wr rn r nnn, mnn wr nm,vn r r- nr . r rv.rrrrzn rm r-n rv r rrrnnrrn wrn n,n wn m nnrnnrnm rnrnnrm.r nr r rmrnnmnrr- r rnn.nnn.r2m3 , r, wx w w. m n wx = ° rv mrm n, xnr = ° mnn.n n n wx, rm rrn nn n r nn mnrn,--n,nnn ~ w. r w n vrz rrn w..wrm, -° m,rn rx- nmnn.n v . , r r --wx v n r mr n nv nrvrnn r nr r nm =- °.nnr, -° r n n mn nn r n rrn “rx w”. n, - --- v mnrrzr r mr wrr ~n °nn °mnnr w r.vrwnxmn rrr rvnn rrn-rvnn. n rwnrmrvzn rrn rv mn - vwr-nn . m. -rm = ° mnr n wx. m -nn nn. mnrn nmr vwrrmn nn . m nxrnnvn . r nn n rm rmn nrm- n, w rn r n- , w w nmrvr mrn. nr r vr mr w m ~ m nn x . n . , n - rrn rm n m rn rrn,nn n rn n v n.n nrr, rm = ° r nwr- r r - nvn rv rr r nm rr m . nrvnrzn mx n.m wr ,n wx w r mrnnr wnr =m °nrw rn nrn °,rm mr mnr w ., m, . rv 24 mr mrr ., m “ r °mrrmr nnr . m ,-m-- nn rn .”, ̶mrrr wmnnv9rn w rrrnrv, r .25r-26 rn w.rr n,rr . wrmr m mn,nn-- rnnn,n-m--nn . rn w n r nn n -.n n, n wx w rm r rr rrn . nrm nrrwrr r nn , m r mr m.n. n, n- r v vr r nn ~ vn,wnnvr mr m ~ mr wx mrrmrnrn r .. r, r r vrn mr rmn, xnnnnn nn nrm . n wxr nr rn ^^./. - w n r. mm r- nn = °. mm r--° v. rmnm wx-°r,n-nr. r nrrm ^^./.nw-nnn m mrmn - --- vrnnnrrnn.27nrrr,, vnr nnrnrv r mrvn r .nrn, m nn- m n 1 mr m rm rn nrn n n. wrm -n. w nnn rmnn -n, m ,..rrmr,- n m-- n ,, nn nrmrmrrn ,- nrn w -rv-m, mn-r-nr,,nn,n,-,rm,--nnn .. n rm ,n nmnrm -rm xn, wr n m .n , nn n mrr r m rmnn . . r rm nvrrn-wr mxr wn v-mxr mxr, mnnmrrrm. rm n vrrnrmn . mxrrnrn w m n.28 mxr r wrm r mr n n m w. mmr r,. m , w. mnnnr,wrm nn. wnx w. w rrnr wx = °, wr r nnn . w nnr r nnn r . r. nr = = ° °rn wr. ~ mr n w mr n,nnrnn--nn w. r .. n n mrrm ,r w wn mnvr n r r n w mr m r r n m nnrn mrr rvnn znr .. rvnrr r n- w . n~ mr mxr-rv wxn ~ mr .n nrrnnr w mnnr rr n rm . nnn,n,n nrm rm mnn, m-rmnnmn rmn n wr -,nnn w nr .,r ,,,,,n.rvr, rnrm xnn m..mn m rnn , ,,-n rn. nr x,r w x nrr vr-n mxxn vrrmn n .n rn, rmn rm .r. rmnnrn,nnrn = °rnvwr.--nnnw wx1rm- - --- nrn r rnn r n n r n-r nrn. n-n,n-r rnn rrnrnnrr.nnnzrnr , ,n rnr vnr mnn mr vrn , nr n w vrzn, n rm wrn .. r n r r, n wr r w nn vr n rnnw . . rn wr n nrz wr r rmr rn nr n rn .. n2 4 - nvr x-n, n.rmnn 1 vn. rn n .-. m r rvnv . w nw rnn .n. m— rnn wn.nnn.-nrvnv 1-1r3 , r v—.wr.nrrrr - rnn,rr, mnrnr mn rnn.n mnmn . wwrvrn,n nr n rnnn mn nrrnrmrnnn rn nrrrn r .n mrznrr,29rnrm -n -n rrnn r n r n v wvr, nr nrn nr . m n r,. rm wr n n .vnn mx rr r rm nrzn w n r ~ rr,rrrrn wr rnrr wrnv n vr nrm zn. w n rn rmn w w r nnrnn n . r. rmn w r r rn , n mr n n r r wnrnrn rnnrm . n r r. r ,n -rn, wrnn rn rrmr wnnrn r.nn.nrrn-,-. ...rn w rr w mr mxn nrr nnmrvr w r vr nrnwn rn’ mn- nn-, mrmnr-n,n-rm. rrv mnnrnn mx rnrmrnnx wr.30 -n-vrn,,nnrrrnm n , wnnrrrn -. - --- , w.v.vr , w w mnn w w n m n-n.. r-mrvmrnr.-rnrnx x wnnmnmvrrvn r . , w.nnr,-nnn rn n nr rmn m r3.,nd rdw,rm mn xrr rn n.1n , w-m r -rnn rrmnrrmnr mxn.32rrnrmrr,nnnxvnr wn nv mn wrnrn n, vm ..,r n rnrr rmn m n w-rv rn,3 rnmr. mrn, wrrrmn wrwn-nw rr mrxr w rr m. w.r3rnm n . n -n-rn w nnrn. m mxr . m nm n , r v.mr , -rmnr m r r m nrrmn mr r -rn, rn nr rnnrnnr mx n w n n m r. rn, xnmnn. m mx w w xn, w rrrrr r r rnrrnr n’ . w vrw. nrnnrrnnnnxm wr, nrr nmrnnnr m.-rn r n rn n wnr, r n. mm r m rnn n r-wr m,..-rn rnCMC =. mm, = nnrwn mznrrn mnnmrnnCn =.w mm,rn =nnr mn,n. r,n, n n rr n rMCn r n.34 m nn n. m wm.r n mxrrrr v n C,MCr -rn . , rnr -rn. x rnnnrvr =m mx w nnn w. rn . , w CMC. rv w mnr w r- mnmr r’ r “mrm35r".mr mxr-rvrnr,n mrmv w > n wnnrn. r,rn r rrrrmnvn - --- rrnr vm-rnwnrrzm r r wn.n znn n v r r rr n .,rn. rnn -r rrn vnn rrnr 36-37n mn, nrrm rn nnrmxrnnnrmrn-vnrrn . nr rrrnnnmnrm v vn- m.38-39rvr, rv m rm rm 40nrn w v r, w n rr zmrr wr °. nn mrv rm nrnn rrnr wn n m vm . n rn.41 nrwrn, n rm n rm n,n n n rvn rnrmn mn ~ m n.42 r-r wwxnr nn -rv n xvn n r n. , - w nn wr nvr rmr r rrn, ,.v 3 mxr . rrmnr r n n n rn,rn nnrr-rr-nn. r nvv mr x ,nn-r rrvnn m n nrnvrnmnr rmn r n nrn nrm.mn m m nr, zwnn w rrrn vr rr nr rn n . m rnm nrz n.., wr v. m n mrrrnn nrmn v vr mr m nrm rrnrn nr n rm n wx. rr vrz wr , n v-r wm rr w rnn nrn n-vrnr.mrm, w, wxnrn vn rrnm. r . r nzn ,.,mr rr,n., r m-rr, wrnr,xn66 n. w rmr,r n.mrxmr, - --- wm,nnnr,n nr wr n n r,.n r nr.r,mrvrzn. mmr®r wr w rr ✕ r wrvrznwrn mn vrzrr mn mn,nrmnrrm . --n r. mn w rr n r rmr w wnnn wrn m x:. mm x.mn mnzn r . ° rmrr, ° mmnw r, mmnn nrmrr, mnmrr, ° n mnmrr, ° rm r, °mnn n-mn.n,-. .nrn w wrrrrnm n rm m n .m. wn rnnnn w- mn m, m.., wn nrm.: ° r r n : rv nnw::w: mmn n n mmn mnvnm: mmnnnm:m.: m °n mnnvvnm : °mn .nrnnrmn:m. ° . : : ° n-.n-: - m °r w rrm n - mrr rrn w r . mmmrn °r wx w m w r . mmnn w ,,-rrnzn n,, r wn rrvnx r. m rrm n mn n- wnrr.r, xmr rrn wmn - --- mmn . mm.,.n x. xm. ,- x . mm.. xm . mm.. x -.- m m wr vn v nmnnrn ~. mmnrr r mn. n w r r .mrn rnn v. m wn nn wr . x mmmnn mrn: m x , m x , m x n n , r, rmrr w.nrr mn m. mnn- r mrnrrrn nmm,-rn r-r, n - nm,n nm 13rmxr.rr w1 n nx. .rmnr w wrrr rrmr nnr nzzrnrnvnrrm. rmrrmnn wrn n13 zrrvn rn wrr rrmxn n n. xrmnr n n zrnrvn rxnrn n.- wr n,n znnrmn . mr w rxnm , rmmw .n nnr nn mrmn wrn rrmnrrnr mn wnr vmwn ~m,r.rn r nx,nrmn r wr ~.r nn mrmn wrv nnnr nm ~ ,rr r m w r vm rm ,n rnm ~. n ,.r m- nvrzrz r rrnzr,. w mm nrrnr z,. mm wr rn, mrr w w rm r, °r mn.r m r r w ~ °,n °mn rnmrr rn rmmrr wrr r m w ~ °. mm, znmr wr wrr n r rr .r mn, r n rr.z ~ °n ~ °, r v. rm r n w rnnmnn, nrm. wnx w n xnw m ,rnr v, wxr rm r r w -n - n w rmn .rn rn, m w w n °,nrr m mn-nrr-m vr w wr rrr.w w wrrn.nr mn, v - --- n. mnnr wrnrrr rnm.mrrr mnn nrz w n nnvr nmn rn n wr m wr. m,✕. mn xn w wn r n w m xn w r n mnmxr wrrrnvr-24,rnrznrn.n rr v,n xnn r rn n, mr vm m mv r rn v °. m w mnr x nnrnnr mr z rrnv1r nnn n rmn r r wvr nx .n nnm n2 m, vnr n rnrrrrmrm . n n, m nvrnmnn m v n w rnn rnnnmrn.n nr vmr nrnm rnnrrnnrn.3m-4n r, rrnvrrn rnrrrnnrrn r.nnw r rr n rw mr nr nr rm n rr nr,rnv rnv rnn nr .wvr, n mrv n n r r , nw r rnn w v nnxnvn r r nn .rnz r-wr w nr n rrm.rr. w nnrr nrrvn.nnvr,nnr nnw rnnn .mrn, n’mrr nrn r v r n wr mrr wn °n °n r wxr . rmnn r,mnn n rrxn v m r r znr n , nv w n .rr,n rrm r rn nrvr r r nnr n r xr nnrn nr n mr mn. wx wv 1 6m6nn nnnnwnmn r . r nn66 : nrn nr, nnnr66n ^^./. w,,rmn. nn
Figure imgf000055_0001
^^ = ^ ^ ^ ^ ^^ ^ ^ ^ ^ ^^ - --- w mrrn ^^:!; ^ r<=*> ^M=Nr =nz m ^^nn rvn ^ nrn^z:!; nn<=*> r ^^M=N12 mr nv n m rm6r6 ^^r66n ^^^n m nmvrn rnnn12nr ^^= =rrmn n n ^^ m=*=12 m.n mr,n wrmx.rmnz*=12 x rnrnnnrn nr nn xn n n ^^./. r vrn n nrr mrnr w rm nn. n nr wn,n v znrz =r °rn wrxn mrm nnnn m r r r nn =.-.°.vn , m nn.rn m r r = - ° wr nv r r nn.mnnnr mm wrrn.nnz. r w nv w nnr m n2n4 r rr24 n. rn rn wr nrz n rm rn. n, rnmnrnn w wnxn.- nrmnnnxrnrmxr wn rrn wn ~ rn .-. r m r rm nrv 7rn26 , nr rn .rrn v w n rnnrmn. m r r nrmrv rrn wra. ,r rrn m2 2 2nn rn n m r °.,r, 11-24 1r6n 2-72 -3 2n3 °,- 6-36 15 rrrmn 2- °r,, 5-21 11 , rmnrrmr- n zn °:,- 7-26 wr - --- znr- arn nmr r °,m v w1.nnrnnrrn nnrnnnr mrm.r . nnrn wr
Figure imgf000057_0001
nn- .nr m- wrrrzznrmrmn mrr m .nrm w . wr.rrrm m nr-rz.n m n r nxrmn. nmr nw. rn mwrnrnnr, rrmrn rrnn nmrnrr - --- rn rrnrnn nr mr wn nmr rrn. rn mmm rnnw rnrrmn.rxmr, n. rnrnr nmrn "1-2." rr m nr mnrnnnnnn wn w nrnr n r n nrrnnrr rrn n . n nnv n nrr rvr nr n wr rrn xr m m n n. nrrn nn nxn nxr r mr r n nn nxr nnn nnrm nn n.nnn n n rnn nn n n xr r rnn mnn m.rrmr,nnrrn r rrnnnnnrmn xnr nn wnn nnnn nnmrnrn nrnrnnxn nn r mn nr nnmnmnn n nm. rnr rr nrnr n n n vr rr r.rr, nrv n n n m n rnrm xnnn nrm. nr,v.m,..w,..,r n,,n vr m. n,n , , . rn .m.rnrr,..rnr,.. m,..,n rnnrn w,.vr w nmn. , ,-. r ,. r,., r n: n n rn. . n n : n , , - nn,v.rn,. wn,.r,n.,., nrmnn.rnnvrn nnn mnvw mnm ,..nr,, . rvr- vn,m.rz.n,..,.mn r, rm,-.rm - --- v rn,..n. ,..,r m,.. n,..,wr mr n-n nn,.r,.r..nn,, ,-. ..r . r,.v,.. n,.. r, r n,.,r vn n r rn n nmm mr n.,n,., . n, n-,r.. rn,.,r.m :mm, ,nn- m n,. nmm,.,.r ,.nn, . .. z-nz,.. r,.. nn,...,...,.,n,.m rrr, rn m v v - z n .rn m r x nnr ,.n,.nr,n.,m. , , -. r n nnz,..r,.. ,.,., n mn nn ,rn w, -v. m.r n mmrnn,.rmn,x.-.n,.vr,r. n,r.n, n.r, x.nr nn ,.,.,, n,rm, -. .r mr.r rn.:wr, .. r n n rr,. n,. n,., nn v , , . n n wxnr m nn.n vn . -mr,n.,..n,,..., r,n..n,n. ,.. n,.. r, rn rmzn.n , ,n-n rm nm n,..nn,. ,..n,.-,. v,. ,. ,. , ..,. mr,.. n w n rm ..rw,.., nrn w r ,. ,r.rnrm.nn , , -. nnnn rmr n,.,w r rrn n nr rmnm mxr nr w -rrm- mr mn.vrnrrn rn , ,-. rvw.rn nnv,rn.mn,.,mrnnrrnn,w,n-. n : - --- .rm,..,r, x,-n -n n.rn m nr,.n,. r . wn,..rr,..n,. nw,,...., r,r. r,.. rr,. rn-mnnrmn n-rnn v n , , v nw r n r rn.m r--v. mrrnrz,.r. n,.m.nrmrn-rvr,.. nnr,.., n mrnm.,n.rrv,n.n,rnrmmrr nr ,r n,n- .m r wxnnn..rr n rr nrn xnnn w..rn mr nnw-n n -m,.. ,.,x vrr n , , - . .nr nnrn mr r m, r, rnn ,.nn,.. r,..rrnn -.. n,..mm, ,.nnn,. n, mr,.. w,....rr,n,.,. rnr,n.-.r,. ,.. r . nr n nn - rrv,. v , , -. m ,.v,.,rrzn nr wxr - ,m.nr.rn rmr , ,-.n r rmnr, , mr r,., .x n rm .nr nnrn r,,.,-,. nrm .. rn,., x n rrn.. nn.rn.rrx n r m n.r n vn,..mrnrn,. n , ,-..rnnr,..r,. ,...mnrz,,... n,.. r,.. ,... nr,.. ,.r,. wr,..,..,n.r.m,m.n.nv,. ,.. m,..,x w vrz - v,x nn nnn.n , ,-n.r nmm - --- n.zrn,. r,.r,. ,.nz,.,-rnrr nnn,.. r,.. , ,-. rmnmrr , v r mn rrr. r n,..r.w rn m , ,-. m n,..,rrnrr r v .n rn- ,,.n.rm,n.r.,..r,n..,r.,. r r,. nnnr r nn rn,..,r-x - n r n: mn vnnr n r n rnr,r..m nrnnn,.mrnnn, .,.,- rnw. nr,.,n n rm ,-. n r , nrn,. rrn,..vrr,.,v nr rn r n . r.rn n n r , ,- ,. n,. r,.. r,.., mrnn , -nr :r r n m.m m , n. r ,r..n..mn,r.. n,..., mr r n—r:rm mrm,....rm,n.nrmn,.,,r,-.r n:. rn n,mnn r n r n.rn n n nn,,.-. r rn,..rnrn,r.,x, rm r nr r,. zr,. z,.rx ,-. m nn nn r - ,. ,.,r n r.nr nnrn mr rn nn n ,.wr,., rzn , , - . r,nrvnn n ,, n w wr . vn,,...xvnznrnx nrr- rn..rn. ,,.. - --- n,,....r,n.n,,...,xrnr . , . ., . r ,... ,. n,. n, nn.nvnxn r rm rnn n r ,.r rn-nr,.,n.,. rr,.. n,.n,., n rn nr.nmn nr m n nn x r r , , - .nn,..r,.. .nvn m,xmrnnz mxnr.nr rnmrrrm,n, - nzrnnn,.r r.n,.r.rm ,..,r n rmr m -. m m rrr.n mr , ,.nz,.n,n.,n.m,,...,nm,.rnnn,m. ,r.rmrnz,m.nnzm, n nzn rmrr n r r rr n m , , - n.n nn,.. ,.. rmnmr ., v r mn rrr. n,..rwr. rn m , ,-. mr ,nn,r.m,.,..rrr,n..r,r. r v .n nr r,.. nnrn,..n r,. r r,.rn,..,rn- xnn - n r n: mn vnnr nr- n,.,r.m m , ,-. r,.. ,n.,mrzmnr.znnrn mmnrz.n, -. rx-n mrzn . rvrnn mrnm , ,-.,n rx.rn nnrrn,..mr,.,.,r,m-m.rzn r rn .nr - --- r n rn,.rnn,.rnn,. wr,.,n n rm ,- r nn n.rn n n r ,rnnnr.,r.mwr ,n.nrn,-.mr,., nmrn-n , - n n.rm , r n,. r..n..mn,r..rn,n.n.., mr, r,n—-r:rm mrm,....m,.rmn . .r , ,- ,.,r r n..n. mrr-vrz,... ,.. rmn-vr,.. nnr,.., n nr.nnrrnnmn rr r ,. n,. nrn mr r , , - . nr r,.. r,.., mrnn , - :r r n m.m m , nr. n,. rrn,r...rnvrr,n.,vnnr rrn ,r n . ,- nn,.r rn,..rnrn,r.,x, ,rm- r nr r,. zr,. z,.rx,. . m nn nn r -n n,n.,r n r.nr nnrn mr r , , -n r,n,r.vwnrn,., rzn n w .wr . x n ,,-. .n,.,..m.m,nn.,.n,...rr,r.,.rrrnn,,..nnn,.n,... w,. rr, . ,.. mr,. . ,.vrnn,nr n ,, -. . r,.vn,..nnr,,nmnr,m.,r.zn ,,-. - --- ,.-,. nr,.n,. ,.. n,mmn nr nvrnmn n..mn. nr,r,n,.n,...n ,..r,nr nvrnn .. nrn,,...wm,,- .rrn. nn,.mnrn ,, -. r ..r,nn,, ,.zr,rn n n .z .-m.r,.-. n,.rn .n,.rm, ,nnr,., . - .rmnn,.mnn,nr ,, ,,.-,. mr,. ,. ,.rnz,.r,nr mmn.n,.. ,... r ,.,.-.,. n, r ...,., ,n.,, ..rr. ,.r.r,.nw,n,...rnm,n,.n.vr,n.,, ... m, n mr nnrn mn- v, .m,..nn,.,.. ,,-. :nvrnmn .r,.. ,.. , ..,.,n,,.r.rr,. n,. n, n vn ,,.. . .r,n.nnn,,...,w.n.,.rn,.n,.,.. n,..mm, w, . ,. rr,. r,.n,.. rn..rr,,.rnr, ,,-. m . v,.nw,..m,nn nr .. n,..:..,n.,rn,r., ,n,nvr, ,. -. n ,, nmnn m .nnm,-.. .,.,.n,,r n rn ,, -. ,.,.,.n,.,.r..n,.n,,.,,-... n r,.,. - --- r .v.,...rn,,.....mn,,...nv,..z,..r,.... rn vr,..n,..r, rn ,...,n m.r.,.n, ,nz, n,-..n,,.,n-,. ,.nr,..rrr,. :n.vrn w,.rrn,n. ,nn . r , r,n.n-r w .m,..n,.n,. ,.r . rn rnn ,.,.m,nrnn ,,. ,r.m,r,,m-.nnrnnr n:r nn n ..-. - ,.r ,.x,rn n n r ,, ..,r,..wr,nr,.r,wn,r.vnn n ,,-. r,rn r n nmnrr,,.r,nzn-r,..mrr,..wr,..r ,.,..mn n,..m,.mz,.n,. n, .. nn,..n,n ,., . . ,. r,.rn,m m ,,- .,n,,.,.n, nr : m nnnrn ..,,..,.,.. n,,..nn,nmr ,, - . . ,.n,rn r ,,-.r .,m,rn....nmr,..,nmr,.. ,..,..rm, ..rrn,..rnn,..rrrnnn,nrn,,n-. ,, mr r .-. ,,rm,-..,. rnn,nr nnrn mr - --- m ,.,n-,... r,.n,.nz,.. rm,..rw, ...nm,n.,vrn,.rr, vw ,,-. . n nr r n n ,,- ,,..nw,.nr,.. m,rn n n r .-..r:nvnr,nm.n.rm,v,-..,nr ,.. vv,..r, .. r,..rrn, -. .:.rv,.nn,.n nmr m nnrn,. x z,vr, ,.-. ... ,r.,n rn r, . m .n mr,.n,.n,.n,..n,nnn ..mn, r n nrn r .:..mr,.nnn, . m.m,r., mrrn,,..,m.m-. . ,. n,n r,., . mr xmmr,zrrn mmnn,vn-. rrrnr rrnnrnnrr rn rr. wn vrnrnn mnnr mm m v-r r. m nn vr rnrn r.n nrnn n rn wn w r nrn rnnnnxm wnnrm.xmrn,

Claims

- --- .m: mnrmrnr wxnrr rmn-rvr mrn: n,n m m r nn r n, nnrrv nmn mrx,n v n mmn n w nnrr nrn m, wrrn wxnnrmr n mrr v r mrr rn mnnn vrrr mn rv mx vr wxr nnrrr.mrrr nr m. mn r m wr°n rn °mrr mnrvr vrmrr m.. rm m r,mrmr, wrnr,rrmnr rm.rm r,. m mr rn m, wrn rn mrr v z n °m v°r mnr.mrrnr. m rmrrrn mxnr wxnr mrnnr n mr mnnr n r n, n,n w nnrrnnnnnr w r n v n mmn n nr n nnrrmnrvnr mm, mxr wx nn w r n v r wrn m nrr mrrn wrn rvr m rxrn wxmnnrn.n w r n v - ---. r m,rm rnr,rmmr, wrr,nrr rmnmr.rm . m°. rn mr, wrn r mrr °. ° m,° rn°,°mr,° w,rn° r°,m°rr ° °,° °. °,°. m°. rn mr, wrn r mrr ° . ° m,r °rn°,mr°, wrn°,rr°mrr°. ° . r. m rn mr, wrn mrx mn . mn v .rn mr, wrn mrx nnr . m rn m, wrnnr nrnrrn. . m mx wnrnnr nm vr, w.rn mrx xn - ---. m mx wnrnnr nm vr, w.rn mrx r. r mr. rn mr, wrn v m r. r mnnnrn ,nrrnmr, w n,nrrn mr rm r mn,nrnnr. n,nr. r mnnrn-mnr, wrnn,w-mnr rm w-n n, n mr, r nn,mnr,r -n rn n. n. m mxr wrxn rmmr, wrn, mrrmnvrn ,mr rm ,rrm . r. v mn rnnnrrmr, wrn°mr°,rrrn°wn °. . ° m °.rn mr, wrn r mrr -. m mr rn mr, wrn nnrr °,r -° °, -° °, -° °, -°° °° -°°, -°°, -°°°, -°,° -°°, -°°, -°°, -°°, - - --- °°,, - -°°°,°°, -°°,°°, -°°,°°, -°°. °, -°. m mr rrznr.mr, wrn v ,nnr,r. r mwrrnrmnnm mxrr, w wrxnn wr rwrnvn w,r n w mxr wxnr,.w,. mr r mnxrm wxr,n wrrn. m rrmr n.n mnn rnrrmr, wrn mxr wxnr mnnr. nn - n r , r.n m rn mr, wrn mxr wxnr r rn.nnr rrn,r rrn,rmnn. nr mzn.rn mr, wrn m rrmr . mmrxrrn mm, wrxr.n nrznmr n - ---. r mn, nrn wrnmr, w wrnr,n,nrmr rmnnr. mnr, r ,. r mn rrnrrm.r, wrn wxnr rrr. mx mr rn w m,,r,v,r mx,rrrmrnrmxxn .. mx mr rnrxm,, w,,r,rrvrmrnrn . r mxr. m mxrrn wxmnrr, w.rn mnn rx . mn mn rrn. m, wrn mnn rx . mr nrnn -m-r, wrrxn nrmxnnr.rm. m m rn mr, wrn mxr wxnr mrxr wx wnvr rnnn , wrn ,rm.r wnvr rnnn - ---. r mx r mnxrm wxr, wrmrn w.w r mn.n.
PCT/US2024/026720 2023-04-28 2024-04-28 Upcycling of polyethylene and polypropylene and their mixtures to high-value surfactants Pending WO2024227121A2 (en)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
US202363462863P 2023-04-28 2023-04-28
US63/462,863 2023-04-28

Publications (2)

Publication Number Publication Date
WO2024227121A2 true WO2024227121A2 (en) 2024-10-31
WO2024227121A3 WO2024227121A3 (en) 2025-01-16

Family

ID=93257451

Family Applications (1)

Application Number Title Priority Date Filing Date
PCT/US2024/026720 Pending WO2024227121A2 (en) 2023-04-28 2024-04-28 Upcycling of polyethylene and polypropylene and their mixtures to high-value surfactants

Country Status (1)

Country Link
WO (1) WO2024227121A2 (en)

Family Cites Families (6)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US3420916A (en) * 1965-10-04 1969-01-07 Dow Chemical Co Pyrolyzed blend of polyethylene and polypropylene
WO2014060082A1 (en) * 2012-10-20 2014-04-24 Clariant International Ltd Waxy oxidation products of rice bran
EP3286283A1 (en) * 2016-03-31 2018-02-28 Trifol Resources Limited PROCESS FOR THE PREPARATION OF A C20 to C60 WAX FROM THE SELECTIVE THERMAL DECOMPOSITION OF PLASTIC POLYOLEFIN POLYMER
PL3470440T3 (en) * 2017-10-10 2021-10-25 Thai Polyethylene Co., Ltd. Oxidized polyethylene wax
EP4244264A1 (en) * 2020-11-13 2023-09-20 Braskem, S.A. Processing of polypropylene and products therefrom
CN117886720B (en) * 2024-01-10 2025-11-25 西北工业大学 Methods for preparing aliphatic sulfonate surfactants from polypropylene, polyethylene, or a mixture of both plastics

Also Published As

Publication number Publication date
WO2024227121A3 (en) 2025-01-16

Similar Documents

Publication Publication Date Title
WO2024227121A2 (en) Upcycling of polyethylene and polypropylene and their mixtures to high-value surfactants
WO2024154061A1 (en) Compositions and methods for stabilizing rna
AU7010798A (en) Semipermeable encapsulated membranes with improved acid and base stability process for their manufacture and their use
JPH0485301A (en) Amylose particle and its production
US20220041638A1 (en) Method for separating biomass from a solution comprising biomass and at least one oligosaccaride
WO2024144945A9 (en) Methods to produce high strength aluminum and high-strength aluminum articles produced therefrom
Pan et al. Edible polyelectrolyte microcapsules with water-soluble cargo assembled in organic phase
WO2025058551A1 (en) Device and related methods for debridement of wounds
WO2025011852A1 (en) A method for enabling simultaneous transmission of power to a first wireless device and of data to a second wireless device using the same set of available resources, related radio network node, and related wireless device
EP4638497A1 (en) Il-2 fusion protein
WO2025257416A1 (en) Enhanced tnpb polypeptide and use in genomic editing
WO2024231578A1 (en) Digital-analog quantum computing method of fermion-boson models in superconducting circuits
WO2025016964A1 (en) Method for solving an electronic structure problem based on hybrid digitized counterdiabatic quantum computing
JP6922161B2 (en) Method for manufacturing stretched porous film
WO2024223127A1 (en) Methods for enabling positioning of a wireless device, related nework node, related radio network node, and related wireless device
US7204258B2 (en) Method for cleaning and/or disinfecting the vacuum channels of a sealing station
Mautner Negotiable Instrument Delivered as Security: Contract Subject to Condition Precedent, Mortgaged Asset and the Issue of Consideration and Value
WO2024200062A1 (en) A method for enabling mitigation of interference at a wireless device, a related network node, and a related wireless device
Harper Factors affecting the application of ultrafiltration membranes in the dairy food industry
WO2025054605A1 (en) Improved pcr primers for sars-cov-2 viremia
EP4638473A1 (en) Means and methods to target endogenous condensates
JP3513193B2 (en) Method for producing soybean β-amylase preparation
EP4602870A1 (en) Methods for sidelink communication, related wireless devices and a related network node
Harari Using the Law of Negligence to Reduce Political Appointments in Government Companies
WO2025202503A1 (en) Extracellular vesicles carrying cancer specific splice variants

Legal Events

Date Code Title Description
WWE Wipo information: entry into national phase

Ref document number: 2024798152

Country of ref document: EP

ENP Entry into the national phase

Ref document number: 2024798152

Country of ref document: EP

Effective date: 20251128

ENP Entry into the national phase

Ref document number: 2024798152

Country of ref document: EP

Effective date: 20251128