USOO6221448B1

(12) United States Patent (10) Patent No.: US 6,221,448 B1

Baetzold et al. (45) Date of Patent: *Apr. 24, 2001

(54) COLD SEAL COMPOSITIONS COMPRISING (56) References Cited

HOMOGENEOUS ETHYLENE POLYMERS
U.S. PATENT DOCUMENTS
(75) Inventors: John P. Baetzold, North St. Paul; 5,397,843 3/1995 Lakshmanan et al. .............. 525/240
Robert G. Polance, Lino Lakes; 5,530,054 6/1996 Tse et al. ............................. 524/474
Michelle M. Chanak, Forest Lake, all 5,548,014 8/1996 Tse et al. ............................. 524/477
of MN (US)
FOREIGN PATENT DOCUMENTS
(73) Assignees: H. B. Fuller Licensing & Financing,
Inc.; The Dow Chemical Company O 531 618 3/1993 (EP).
WO 97/33921 9/1997 (WO).
Notice: Subject to any disclaimer, the term of this WO 98/03603 * 1/1998 (WO).
patent is extended or adjusted under 35
U.S.C. 154(b) by 0 days. OTHER PUBLICATIONS

This patent is Subject to a terminal dis “A New Family of Linear Ethylene Polymers Provides
claimer. Enhanced Sealing Performance” Tapi Journal pp 100-102,
Feb. 1992.
(21) Appl. No.: 09/200,667
* cited by examiner
(22) Filed: Nov. 25, 1998
Related U.S. Application Data Primary Examiner Paul Thibodeau
ASSistant Examiner D. Lawrence Tarazano
(63) Continuation-in-part of application No. PCT/US97/12366, (74) Attorney, Agent, or Firm Nancy N. Quan
filed on Jul. 21, 1997.
(60) Provisional application No. 60/066,813, filed on Nov. 26, (57) ABSTRACT
1997, provisional application No. 60/022,538, filed on Jul.
22, 1996, and provisional application No. 60/044.909, filed The present invention is a cold Seal composition having
on Apr. 25, 1997. certain rheological properties. The composition comprises
(51) Int. Cl." .............................................. B65D 27/14 from about 10 wt-% to 100 wt-% of at least one homoge
(52) U.S. Cl. ................ 428/35.2; 428/34.3; 428/355 AC; neous ethylene/C-olefin interpolymers. The novel adhesive
428/355 EN; 428/355 BL: 428/523; 229/80; compositions of the present invention may be coated onto a
525/88; 525/240; 526/348; 526/943 variety of Substrates, resist blocking upon being Supplied as
(58) Field of Search ..................................... 524/502,504, a roll-good, and exhibit a wide range of bond Strengths,
524/478,474; 525/240, 88; 526/943, 348; amenable to a variety of cold Seal bonding applications.
428/355 AC, 355 EN, 355 BL, 34.2, 515,
35.2, 523; 229/80 19 Claims, 1 Drawing Sheet

COLD SEAL RHEOLOGICAL PARAMETERS

O

0.1
100E06 100E07 OE-08 1.OOE-09
Blocks
G' (25 C, 10 radisec)
A Seals and resists blocking
Does not sea
at 100 psi
 US 6,221,448 B1
1 2
COLD SEAL COMPOSITIONS COMPRISING Tse et al., U.S. Pat. No. 5,530,054, claims a hot melt
HOMOGENEOUS ETHYLENE POLYMERS adhesive composition consisting essentially of: (a) 30-70
weight percent of a copolymer of ethylene and about 6 to
RELATED APPLICATIONS about 30) weight percent of a C to Co C-olefin produced
in the presence of a catalyst composition comprising a
This application is a Continuation-In-Part of provisional metallocene and an alumoxane and having an M of from
patent application Ser. No. 60/066813 filed Nov. 26, 1997 about 20,000 to about 100,000; and (b) a hydrocarbon
and a Continuation-In-Part of PCT patent application Ser. tackifier which is selected from a recited list. Exemplified
No. U.S. 97/12366 filed Jul. 21, 1997 which claims priority are compositions consisting of 45 weight percent of
to provisional patent applications 60/022,538 filed Jul. 22, 1O
ethylene/butene-1 copolymer having a specific gravity of
1996 and 60/044,909 filed Apr. 25, 1997. either 0.898 g/cm or 0.901 g/cm.
Tse et al., U.S. Pat. No. 5,548,014, claims a hot melt
FIELD OF THE INVENTION adhesive composition comprising a blend of ethylene/O-
The present invention is a cold Seal composition having olefin copolymers wherein the first copolymer has a M.
certain rheological properties. The composition comprises 15 from about 20,000 to about 39,000 and the second copoly
from about 10 wt-% to 100 wt-% of at least one homoge mer has a M. from about 40,000 to about 100,000. Each of
neous ethylene/C-olefin interpolymer. The novel adhesive the hot melt adhesives exemplified comprises a blend of
compositions of the present invention may be coated onto a copolymers, contains 45 weight percent copolymer, with at
variety of Substrates, resist blocking upon being Supplied as least one of the copolymerS having a polydispersity greater
a roll-good, and exhibit a wide range of bond Strengths, than 2.5. Furthermore, the lowest density copolymer exem
amenable to a variety of cold Seal bonding applications. plified has a specific gravity of 0.894 g/cm.
Lakshmanan et al., U.S. Pat. No. 5,397.843, teaches
BACKGROUND OF THE INVENTION blended polymer compositions comprising an admixture of
A “cohesive adhesive” or “cold Seal” is an adhesive which
a copolymer of ethylene and an O-olefin and an amorphous
25 polypropylene and/or amorphous polyolefin, or mixtures
is nontacky to the touch, yet adheres to itself with pressure. thereof. The Single ethylene and C-olefin exemplified,
Cold Seals are employed for a variety of uses, particularly in FLEXOMER 9042, is described as having a 1-butene con
various packaging applications Such as for food (i.e. flexible tent of 15 weight percent, a melt index of 5.0 g/10 minutes,
packaging for candy wrappers, chips etc.), Sterilizable medi a crystallinity level of 26 percent and a density of 0.900
cal packaging, Self-seal and tamper evident envelopes, band g/cm.
ing for paper money, napkins, and clothing, and protective Hence, Single-site catalyzed or metallocene polyolefins
packaging Such as fold over “blister' packages for hardware have found utility for use in hot melt adhesive compositions.
and Small parts. Additionally, cold Seal adhesives have found However, the hot melt adhesives exemplified in Tse et al.
utility as anti-skid coatings and for release-paper free tapes and Lakshmanan et al. employ relatively high density met
Such as tableSS diaper tapes. 35 allocene polyolefins causing Such compositions to be unsuit
Natural latex based products have dominated the cold seal able for use in cohesive cold Seals.
market for quite Some time, Since natural lateX is inherently Industry would find advantage in cold Seal compositions
cohesive. Natural latex based cold Seals have several defi that overcome the disadvantages of the natural lateX and
ciencies. For example, in the medical packaging area, natu amorphous polyalphaolefin based compositions.
ral lateX has been identified as a skin Sensitizer due to it 40
containing certain proteins. Natural latex is also Susceptible SUMMARY OF THE INVENTION
to aging effects Such as yellowing and changes in the bond The present invention is a cold Seal composition having
Strength because of oxidation. Another deficiency of natural certain rheological properties. The cold Seal composition is
latex relates to the effect of irradiation, which is required for characterized as having a storage modulus (G") at 25 C.
the Sterilization of packaged medical bandages and devices. 45 ranging from about 1x10° dynes/cm to about 1x10' dynes/
Irradiation causes the natural lateX to crosslink, Significantly cm, and preferably ranging from about 1x107 dynes/cm to
changing the bond properties. about 8.5x10' dynes/cm’.
Certain hot melt adhesives have also found utility as cold In one embodiment, the present invention is a hot melt
seals. EP531618 published Mar. 17, 1993 teaches cohesive cold seal comprising from about 10 wt-% to 100 wt-% of at
cold seal compositions which include about 60 to about 95 50 least one homogeneous ethylene/C-olefin interpolymer.
parts by weight of an amorphous polyalphaolefin (APAO) Accordingly, the present invention provides formulated cold
polymer and about 1 to 30 parts of a crystalline aliphatic Seal compositions as well as uncompounded compositions,
hydrocarbon wax. Exemplified are compositions based on consisting entirely of metallocene or Single-site catalyzed
REXTAC and VESTOPLAST APAO derived from Ziegaler polyolefin(s) exhibiting improved Sealing and bonding char
Natta catalysis. Such polyalphaolefins characteristically 55 acteristics. The polymer preferably has a melt indeX ranging
have a relatively broad polydispersity (MW/Mn). Further, from about 200 g/10 min. to about 2000 g/10 min. and a
Rextac 2280 and Rextac 2315 are ethylene-propylene density ranging from about 0.855 g/cm to about 0.880
copolymers containing relatively low concentrations of eth g/cm. Alternatively, the cold Seal composition may com
ylene. These APAO based compositions are compounded prise a blend of metallocene polyolefins, wherein the blend
and disadvantageously exhibit poor Self Seal properties and 60 of polyolefins has the previously described melt index and
low peel Strengths. density characteristics.
Homogeneous linear and Substantially linear ethylene In another embodiment, the cold Seal composition com
polymers are prepared using Single-site or metal locene prises from about 30 wt-% to about 80 wt-% of a single-site
catalysts. Homogeneous ethylene/C-olefin interpolymers catalyzed metallocene polyolefin in combination with a wax
differ from APAO, with regard to homogeneity, molecular 65 and/or tackifier.
weight distribution (M./M.), as well as comonomer The present invention also embodies a variety of articles
(C-olefin) content. wherein the novel adhesive composition of the present
 US 6,221,448 B1
3 4
invention is coated onto a Substrate. Once coated the adhe In addition or in the alternative, the homogeneity of the
Sive composition resists blocking upon being Supplied as a polymer may be described by the SCBDI (Short Chain
roll-good and provides a wide range of Self-sealing bond Branching Distribution Index) or CDBI (Composition Dis
Strengths at room temperature. Further, the adhesive of the tribution Breadth Index), which are defined as the weight
present invention can be formulated to be Substantially percent of the polymer molecules having a comonomer
entirely Saturated, providing excellent oxidative resistance. content within 50% of the median total molar comonomer
content. The SCBDI of a polymer is readily calculated from
BRIEF DESCRIPTION OF THE FIGURE data obtained from techniques known in the art, Such as, for
The FIGURE depicts the theological properties of cold example, temperature rising elution fractionation
Seal compositions according to the invention. (abbreviated herein as “TREF'), which is described, for
example, in Wild et al., Journal of Polymer Science, Poly.
DETAILED DESCRIPTION OF THE Phys. Ed., Vol. 20, p. 441 (1982), in U.S. Pat. No. 4,798,081
INVENTION (Hazlitt et al.), or in U.S. Pat. No. 5,089,321 (Chum et al.).
The cold Seal composition of the present invention exhib The SCBDI or CDBI for the homogeneous ethylene/C-olefin
its certain rheological characteristics as depicted in the 15 interpolymers useful in the invention are preferably greater
FIGURE. Accordingly, the cold Seal composition is charac than 50%, more preferably greater than 70%, with SCBDI’s
terized as having a storage modulus (G') at 25 C. ranging and CDBI of greater than 90% being easily attained.
from about 1x10° dynes/cm to about 1x10' dynes/cm’. Homogeneous ethylene/C-olefin interpolymers differ
Preferably, the cold Seal composition exhibits a Storage from amorphous polyolefins also described as amorphous
modulus (G) at 25°C. ranging from about 1x107 dynes/cm polyalphaolefins (APAO), with regard to homogeneity,
to about 8.5x10' dynes/cm and more preferably from about molecular weight distribution (M./M.), as well as comono
1x107 dynes/cm to about 8x10 dynes/cm. As the G' mer (C.-olefin) content. APAO’s are homopolymers,
approaches the upper limit, the tan Ö is preferably greater copolymers, and terpolymers of C-C C-olefins which are
than about 0.15. At a G' of greater than about 8.5x10 typically polymerized by means of processes which employ
dynes/cm, the composition tends not to seal at pressures 25 Ziegler-Natta catalysts, resulting in a relatively broad
ranging from 10 psi to 100 psi. On the other hand, when the molecular weight distribution, typically greater than 4. In
storage modulus is less than about 1x107 dynes/cm’, the contrast, the homogeneous ethylene/C-olefin interpolymers
composition is pressure Sensitive to the extent that at high useful in the inventive adhesive composition are character
coat weights the composition tends to block to lacquer ized as having a narrow molecular weight distribution. The
coated Surfaces after being coated and wound onto a roll. homogeneous ethylene/C-olefins have a M/M of less than
Homogeneous linear and Substantially linear ethylene 4, preferably less than 3, more preferably from 1.5 to 2.5,
polymers are prepared using Single-site or metallocene cata even more preferably from 1.8 to 2.2, and most preferably
lysts. Homogeneous ethylene polymers are characterized as about 2.0. Further, whereas amorphous polyolefins produced
having a narrow molecular weight distribution and a uni from Ziegler-Natta catalysis typically have an (C-olefin
form short-chain branching distribution. In the case of 35 concentration greater than 50 wt-%, homogeneous ethylene/
Substantially linear ethylene polymers, Such homogeneous C-olefin interpolymers useful in the present invention are
ethylene polymers are further characterized as having long predominantly ethylene, having a greater ethylene content
chain branching. Substantially linear ethylene polymers are than comonomer content.
commercially available from The Dow Chemical Company Substantially linear ethylene interpolymers are homoge
as Affinity TM polyolefin plastomers, which are produced 40 neous interpolymers having long chain branching. Due to
using Dow’s Insite TM technology. Homogeneous linear eth the presence of Such long chain branching, Substantially
ylene polymers are available from Exxon Chemical Com linear ethylene interpolymers are further characterized as
pany under the trade name ExactCE plastomers. havin(g a melt flow ratio (I/I) which may be varied
The cold Seal composition of the present invention is a independently of the polydispersity index, and the like, the
thermoplastic composition comprising at least one homoge 45 molecular weight distribution M/M. This feature accords
neous ethylene/C-olefin interpolymer which is an interpoly Substantially linear ethylene polymers with a high degree of
mer of ethylene and at least one C-Co C-olefin. The term processability despite a narrow molecular weight distribu
“interpolymer is used herein to indicate a copolymer, or a tion.
terpolymer, or a higher order polymer. That is, at least one It is noted that Substantially linear interpolymers useful in
other comonomer is polymerized with ethylene to make the 50 the invention differ from low density polyethylene prepared
interpolymer. in a high pressure process. In one regard, whereas low
The homogeneous ethylene/C-olefin interpolymer is a density polyethylene is an ethylene homopolymer having a
homogeneous linear or Substantially linear ethylene/C-olefin density of from 0.900 g/cm to 0.935 g/cm, the homoge
interpolymer. By the term "homogenous”, it is meant that neous linear and Substantially linear interpolymers useful in
any comonomer is randomly distributed within a given 55 the invention require the presence of a comonomer to reduce
interpolymer molecule and Substantially all of the interpoly the density to the range of from 0.855 g/cm to 0.910 g/cm.
mer molecules have the same ethylene/comonomer ratio The long chain branches of Substantially linear ethylene
within that interpolymer. The melting peak of homogeneous interpolymers have the same comonomer distribution as the
linear and Substantially linear ethylene polymers, as interpolymer backbone and can be as long as, or about the
obtained using differential Scanning calorimetry, will 60 Same length as the length of the interpolymer backbone.
broaden as the density decreases and/or as the number When a substantially linear ethylene/O.-olefin interpolymer
average molecular weight decreases. However, unlike het is employed in the practice of the invention, Such interpoly
erogeneous polymers, when a homogeneous polymer has a mer will be characterized as having an interpolymer back
melting peak greater than 115 C. (Such as is the case of bone substituted with from 0.01 to 3 long chain branches per
polymers having a density greater than 0.940 g/cm), it does 65 1000 carbons. Methods for determining the amount of long
not additionally have a distinct lower temperature melting chain branching present, both qualitatively and
peak. quantitatively, are known in the art.
 US 6,221,448 B1
S 6
The molecular weight of the ethylene/C.-olefin interpoly lar weight by at least about 5000, preferably at least about
mer will be selected on the basis of the desired performance 10,000, and more preferably at least about 20,000. In
attributes of the cold Seal composition. Typically, however, addition or in the alternative, the first homogeneous
the ethylene/C.-olefin interpolymer will preferably have a ethylene/(C-olefin interpolymer may be blended with a
number average molecular weight of at least 3,000, prefer Second homogeneous ethylene/C.-olefin interpolymer,
ably at least 5,000. Typically, the ethylene/C-olefin inter wherein the first and second interpolymers differ in density
polymer will preferably have a number average molecular by at least about 0.005 g/cm, preferably by at least about
weight of no more than 100,000, more prefcrably no more 0.01 g/cm. In this embodiment, as the density differential
than 60,000, and even more preferably less than 40,000. increases, the relative proportion of the higher density
Ultra-low molecular weight ethylene/O-olefin interpoly interpolymer will typically decrease, as the increased levels
mers are either ethylene homopolymers or interpolymers of of crystallinity would otherwise tend to decrease Storage
ethylene and a C-Co C-olefin. Such interpolymers are modulus at 25 C. and probe tack to levels which would
Surmised to be particularly useful as diluents in combination render them unsuitable for use as cold Seals.
with higher molecular weight metallocene polyolefins and In one embodiment, the cold Seal composition will com
for low application temperature (<135 C.) applied compo 15 prise a blend of two homogeneous ethylene/C-olefin, the
sitions. When the ethylene/C-olefin interpolymer has an first interpolymer having a density of about 0.870 g/cm or
ultra-low molecular weight, and the like, a number average leSS and the Second interpolymer having density greater than
molecular weight less than 11,000, the ethylene/C.-olefin about 0.900 g/cm. In this instance, the homogeneous
interpolymer leads to a low polymer Viscosity but is char ethylene/(C-olefin blend will fall within the density and MI
acterized by a peak crystallization temperature which is preferred ranges previously described.
greater than that of corresponding higher molecular weight In addition to the homogeneous ethylene/C.-olefin
materials of the Same density. The ultra-low molecular interpolymer, the cold Seal adhesive of the present invention
weight ethylene/(O-olefin interpolymers will have a number may further comprise at least one block copolymer present
average molecular weight less than about 6000, preferably in an amount ranging from about 1 wt-% to about 40 wt-%
less than about 5000. Such homogeneous interpolymers will 25
and preferably from about 2 wt-% to about 30 wt-%. At 1
typically have a number average molecular weight of at least wt-%, the effect is Subtle but detectable. At concentrations
about 800, preferably at least about 1300. below 1 wt-% the effect of the block copolymer tends to be
The density of the ethylene/C-olefin interpolymer will So Subtle that it is difficult to detect with most adhesive
likewise be Selected on the basis of the desired performance performance testing. At concentrations greater than about 40
attributes of the cold Seal compositions. In the case wherein wt-%, the viscosity tends to be too high for the majority of
the ethylene/C-olefin interpolymer is compounded with adhesive applications.
additional ingredients Such as waxes, plasticizers, and A wide variety of block copolymers are useful in the
tackifiers, the ethylene/C-olefin interpolymer will have a present invention including A-B-A triblock Structures, A-B
density of at least 0.855 g/cm, preferably at least about 35 diblock structures, (A-B), radial block copolymer
0.860 g/cm. Typically, the ethylene/c-olefin interpolymer Structures, as well as branched and grafted versions of Such,
will have a density less than about 0.890 g/cm, preferably wherein the A endblock is a non-elastomeric polymer block,
less than about 0.885 g/cm, more preferably less than about typically comprising polystyrene and/or vinyl, and the B
0.880 g/cm, and even more preferably less than about 0.875 block is an unsaturated conjugated diene or hydrogenated
g/cm. 40 version thereof. In general, the B block is typically isoprene,
In the case of compounded compositions, the ethylene/ butadiene, ethylene/butylene (hydrogenated butadiene),
C-olefin interpolymer will be present in the cold Seal com ethylene/propylene (hydrogenated isoprene), and mixtures
positions of the invention in an amount of at least about 10 thereof. Commercial embodiments include the Kraton(E) D
wt-%, and typically in an amount of at least about 20 wt-%, and G series block copolymers, available from Shell Chemi
preferably in an amount of at least about 30 wt-%, and more 45 cal Company (Houston, Tex.), Europrene(R) Sol T block
preferably in an amount of about 40 wt-%. At amounts less copolymers available from EniChem (Houston, Tex.), Vec
than 10 wt-%, the composition is disadvantageously brittle tor(R) block copolymers available from Exxon (Dexco)
and tends to lack Sufficient cohesive Strength. (Houston, Tex.), as well as others.
Advantageously, the ethylene/O-olefin interpolymer may be In general, block copolymers range in Ablock (styrene or
100 wt-% of the cold seal composition of the invention, 50 vinyl) content from 0, as in the case of multi-arm (EP)n
eliminating the need to further compound the polymer. 100% diblock polymers, to about 50 wt-%. Typically, the
Typically, however, the ethylene/O-olefin interpolymer is non-elastomeric Ablock concentration ranges from about 5
present in an amount of not more than 80 wt-%, and wt-% to about 45 wt-% with respect to the weight of the
preferably less than about 70 wt-%. block copolymer. Block copolymerS also range in diblock
The homogeneous linear or Substantially linear interpoly 55 contents from 0, wherein the block copolymer is 100%
mer preferably has a melt index (MI) ranging from about coupled, to 100% diblock, as previously mentioned. prefer
200 to 2000 g/10 min., more preferably ranging from about ably from about 0 to about 50% and most preferably from
300 to about 1500 g/10 min., and most preferably ranging about 0% to about 30%.
from about 400 to about 1200 g/10 min. For uncompounded The preferred diblock content of the block copolymer
cold Seal compositions, the ethylene/C-olefin interpolymer 60 depends on the Selection of the homogeneous ethylene/O-
most preferably has a density between about 0.860 g/cm olefin. When employed with a homogeneous ethylene/C.-
and 0.880 g/cm in combination with a melt index between olefin having a melt index greater than about 500 g/10 min.,
about 400 and about 600. preferably the block copolymer is predominantly triblock,
In another embodiment, a first homogeneous ethylene/O- having a low diblock content, less than 50 wt-% with respect
olefin interpolymer may be blended with a second homo 65 to the weight of the block copolymer. For this embodiment
geneous ethylene/O-olefin interpolymer, wherein the first the block copolymer contributes Significantly to the cohesive
and Second interpolymers differ in number average molecu Strength of the adhesive composition. Alternatively, when
 US 6,221,448 B1
7 8
employing a homogeneous ethylene/C-olefin having a melt Suitable ethylene/unsaturated carboxylic acid, Salt and
indeX leSS than about 300 g/10 min., increasingly higher ester interpolymers include ethylene/vinyl acetate (EVA)
concentrations of diblock may be employed since the adhe including, but not limited to, the stabilized EVA described in
Sive Strength is contributed primarily by the homogeneous U.S. Pat. No. 5,096,955, incorporated herein by reference;
ethylene/C-olefin, rather than by the formation of styrene ethylene/acrylic acid (EEA) and its ionomers, ethylene/
domains by the block copolymer. methacrylic acid and its ionomers, ethylene/methyl acrylate;
The molecular weight of a block copolymer may be ethylene/ethyl acrylate; ethylene/isobutyl acrylate; ethylene/
related to its solution viscosity at 77 F. of a given weight of n-butyl acrylate, ethylene/isobutyl acrylate/methacrylic acid
polymer in toluene. The amount of block copolymer and its ionomers, ethylene/n-butyl acrylate/methacrylic acid
employed for determining the Solution Viscosity depends on 1O and its ionomers, ethylene/isobutyl acrylate/acrylic acid and
the molecular weight. For the higher molecular weight block its ionomers, ethylene/n-butyl acrylate/acrylic acid and its
copolymers, the Solution Viscosity may be expressed as a ionomers, ethylene/methyl methacrylate; ethylene/vinyl
function of a 10 wt-% or 15 wt-% block copolymer solution, acetate/methacrylic acid and its ionomers, ethylene/vinyl
whereas for more conventional and lower molecular weight acetate/acrylic acid and its ionomers, ethylene/vinyl acetate/
block copolymers, a 25 wt-% block copolymer solution is 15 carbon monoxide, ethylene/methacrylate/carbon monoxide;
employed. For 10 wt-% or 15 wt-% the range of solution ethylene/n-butyl acrylate/carbon monoxide; ethylene/
viscosity may be from about 300 cPs to about 2000 cPs at isobutyl acrylate/carbon monoxide, ethylene/vinyl acetate/
about 177 C. For a 25 wt-% block copolymer solution, the
solution viscosity may range from about 100 to about monoethyl maleate; and ethylene/methyl acrylate/
100,000 cps, preferably from about 200 to about 50,000 cps, monoethyl maleate. Particularly Suitable copolymers are
more preferably from about 200 to about 25,000 and most EVA; EAA; ethylene/methyl acrylate; ethylene/isobutyl
preferably from about 200 to about 10,000 cPs. Solution acrylate; and ethylene/methyl methacrylate copolymers and
Viscosities may also be reported at a plasticized polymer mixtures thereof.
concentration of 25 wt-%. Hence, the molecular weight of AS used herein, the term "tackifier” means any of the
the block copolymer determines the most convenient and compositions described below which are useful to impart
most accurate measurement method. 25 tack to the hot melt adhesive composition. ASTM D-1878
Preferably, the block copolymer employed in the adhesive 61T defines tack as “the property of a material which enables
composition of the present invention is Substantially fully it to form a bond of measurable Strength immediately on
hydrogenated in which the midblock is typically ethylene/ contact with another Surface'.
butylene, ethylene/propylene, or mixtures thereof. Hydro
genated block copolymers tend to be most compatible. In general terms, tackifying resins are useful in the cold
Further, the addition of such block copolymers does not Seal compositions of the invention. Tacklifying resins com
diminish the outstanding thermal stability contributed by the prise resins derived from renewable resources Such as rosin
homogeneous ethylene/O-olefin. The majority of commer derivatives including wood rosin, tall oil, gum rosin; rosin
cially available hydrogenated block copolymers are pre esters, natural and Synthetic terpenes, and derivatives of
dominantly linear. Branched versions such as Kraton(R) 35
Such. Aliphatic, aromatic or mixed aliphatic-aromatic petro
GRP-69A having a styrene-ethylene/butylene-styrene back leum based tackifiers are also useful in the cold Seal com
bone with isoprene side chains, as well as Kraton(R) G1730, positions of this invention. Representative examples of
an S-EP-S-EP block copolymer having a terminal ethylene useful hydrocarbon resins includes alpha-methyl Styrene
propylene block rather than terminal polystyrene are most resins, branched and unbranched Cs resins, Co resins, Co
useful for increasing tack. The Styrene content of the hydro 40
resins, as well as Styrenic and hydrogenated modifications of
genated block copolymers typically varies from about 5 Such. Tackifying resins range from being a liquid at 37 C.
wt-% to about 40 wt-% and preferably from about 10 wt-% to having a ring and ball softening point of about 135 C.
to about 30 wt-% with respect to the weight of the block Solid tackifying resins with a Softening point greater than
copolymer about 80 C., more preferably with a softening point gtreater
The cold Seal composition of the present invention may 45
than about 100° C. are preferred.
further comprise one or more interpolymers of ethylene The cold Seal composition of the invention may comprise
having at least one comonomer Selected from the group from up to about 75 wt-% of a tackifying resin. Typically,
consisting of vinyl esters of a Saturated carboxylic acid and particularly when it is desired to employ less than about
wherein the acid moiety has up to 4 carbon atoms, unsat 80 wt-% of the polymer, the cold seal composition will
urated mono- or dicarboxylic acids of 3 to 5 carbon atoms, 50 comprise from about 10 wt-% to about 70 wt-%, more
a Salt of the unsaturated acid, esters of the unsaturated acid preferably from about 20 wt-% to about 60 wt-% tackifier.
derived from an alcohol having 1 to 8 carbon atoms, and In the alternative, in cases where it is desirable to employ
mixtures thereof. Terpolymers of ethylene and these at least about 30 wt-% of the homogeneous ethylene/O-
comonomers are also Suitable. Ionomers, which are com olefin interpolymer, the present invention advantageously
pletely or partially neutralized copolymers of ethylene and 55 provides cold Seal compositions containing minimal tacki
the acids described above, are discussed in more detail in fier. For such embodiments the cold seal composition of the
U.S. Pat. No. 3,264,272. In addition, terpolymers of present invention comprises less than about 30 wt-%
ethylene/vinyl acetate/carbon monoxide or ethylene/methyl tackifier, preferably less than about 25 wt-% tackifier, more
acrylate/carbon monoxide containing up to 15 weight per preferably less than about 20 wt-% tackifier, and most
cent carbon monoxide may also be employed. 60 preferably less than about 15 wt-% tackifier. In such
The ethylene to unsaturated carboxylic comonomer instances, cold Seal compositions containing less than about
weight ratio is preferably from 95:5 to 40:60, more prefer 10 wt-% tackifier, and even cold Seal having no tackifier,
ably from 90:10 to 45:50, and even more preferably from exhibit adequate hot tack.
85:15 to 60:40. The melt index (I at 190° C.) of these For the cold Seal composition of the invention, the pre
modifying interpolymers of ethylene may range from 0.1 to 65 ferred tackifying resin is predominantly aliphatic. Commer
150, preferably from 0.3 to 50, and more preferably from 0.7 cially available tackifying resins for use in the present
to 10 g/10 min. invention include ESCOREZ 5000 series hydrogenated
 US 6,221,448 B1
9 10
dicyclopentadiene hydrocarbon resins available from EXXon ture (from 150° C. to 200° C) under an inert gas blanket
Chemical Company (Houston,Tex.) and EASTOTAC series until a homogeneous mix is obtained. Any mixing method
cycloaliphatic hydrocarbon resins available in various producing a homogeneous blend without degrading the hot
degrees of hydrogenation from Eastman Chemical melt components is Satisfactory, Such as through the use of
(Kingsport, Tenn.). a heated vessel equipped with a Stirrer. Alternatively, the
Waxes may be usefully employed in the cold seal com homogeneous ethylene/C.-olefin interpolymer, optional
positions of the present invention, particularly to increase tackifier(s) and optional plasticizer(s) may be provided to an
blocking resistance. Waxes are commonly used to modify extrusion coater for application to the Substrate.
the Viscosity and reduce tack at concentrations up to about When the cold seal composition comprises a blend of two
30 wt-%, preferably from about 3 wt-% to about 20 wt-% or more ethylene/C.-olefin interpolymers, it will be preferred
and most preferably from about 3 wt-% to about 5 wt-%. At to prepare the cold Seal compositions using a dual reactor
concentrations greater than about 30 wt-%, the wax tends to configuration, with one of the polymers being produced in
disadvantageously hinder the ability of the cold Seal com the first reactor, the other of the polymers being produced in
position to Seal. Waxes useful in the cold Seal compositions a Second reactor, and the tackifier(s) and optional plasticizer
of the present invention range in melt point from about 80 15 (s) being optionally provided, typically at a point after the
C. to about 120° C. and include paraffin waxes, microcrys Second reactor, via a Side-arm extruder. In this embodiment,
talline waxes, Fischer-Tropsch waxes, polyethylene and cold Seal compositions can be provided in forms Such as
by-products of polyethylene wherein M is less than about pellets, pillows, or any other desired configuration.
3000. Examples of commercially available waxes include Examples of Such a proceSS which may be adapted in
Bareco C-4040, an ethene homopolymer and PX-100, a accordance with the teachings of this disclosure to prepare
Fischer-Tropsch wax, both available from Bareco Products blends of a homogenous linear (higher molecular weight or
(Rockhill, S.C.). ultra-low molecular weight) or Substantially linear ethylene/
C-olefin interpolymer, wax, and optional tackifier, are dis
Also Suitable are ultra-low molecular weight ethylene/(C.- closed in WO 94/OO500 and WO 94/O 1052.
olefin interpolymers having a density greater than about 25 The viscosity of the hot melt cold seal compositions of the
0.920 g/cm prepared using a constrained geometry catalyst, present invention varies widely and will be chosen based on
and may be referred to as homogeneous waxes. Such homo the intended method of application. For slot coating, the
geneous waxes, as well as processes for preparing Such viscosity may be as high as 100,000 cPs at the coating
homogeneous waxes, are Set forth in the examples below. temperature, whereas for pattern coating, gravure coating
Homogeneous waxes, in contrast to paraffinic waxes and and roll coating the Viscosity is typically less than about
crystalline ethylene homopolymer or interpolymer waxes, 5,000 cps at the coating temperature. The application tem
will have a M/M of from about 1.5 to about 2.5, preferably perature ranges from about 100° C. to about 180° C., with
from about 1.8 to about 2.2. lower application temperatures being preferred.
Homogeneous waxes will be either ethylene homopoly The cold Seal composition of the present invention can be
merS or interpolymers of ethylene and a C-Co C-olefin. 35 cast from Solution or advantageously applied molten by any
The homogeneous wax will have a number average molecu of a variety of hot melt coating processes well known in the
lar weight less than about 6000, preferably less than about art including knife coating, roll coating, slot coating, gravure
5000. Such homogeneous waxes will typically have a num coating, curtain coating, etc onto a Substrate. Useful coat
ber average molecular weight of at least about 800, prefer weights range from about 0.01 g/in’ to about 0.1 g/in. For
ably at least about 1300. 40 Some applications, for example when the cold Seal is applied
Homogeneous waxes lead to a low polymer and formu to an uneven Substrate, thicker cold Seal coatings are not
lation Viscosity, but are characterized by peak crystallization uncommon. However, in most instances, to reduce cost,
temperatures which are greater than the peak crystallization lower coating thicknesses ranging from about 0.2 to 1 mil
temperatures of corresponding higher molecular weight are preferred.
materials of the same density. In hot melt cold Seal 45 A “cohesive adhesive” or “cold Seal” composition is
applications, the increase in peak crystallization temperature essentially non-tacky to the touch, yet adheres to itself. The
translates to an increased heat resistance, and the like, coated Substrates may be bonded to themselves at ambient
improved creep resistance, and improved Shear adhesion temperatures at pressures ranging from about 5 to 100 psi
failure temperatures (SAFT). (for 1 second), preferably from about 5 to about 60 psi, and
An incremental amount of other ingredients Such as other 50 more preferably from about 5 to about 40 psi. Lower
thermoplastic polymers and liquid plasticizers may be use preSSures are required when longer dwell times, in excess of
fully employed in the present invention provided the result 1 Second, are employed. The peel Strength may range from
ing adhesive composition exhibits the required rheological 0 to 2,000 g/linear inch, are preferably from about 50 to
characteristics. AS is known in the art, various other com 1000 g/linear inch and more preferably from about 100 to
ponents can be added to modify the tack, color, odor, etc., of 55 about 500 g/linear inch for the majority of applications. The
the cold Seal thermoplastic composition. Additives Such as desired peel Strength depends on the end-use application.
antioxidants such as hindered phenolics (IrganoxTM 1010, For example, in the case of candy wrappers the cohesive
IrganoxTM 1076), phosphites (for example, IrgafosTM 168), cold Seal bond Strength should be equal to or greater than the
antiblock additives, pigments, and fillers, can also be tear Strength of the wrapper itself. If the wrapper has very
included in the formulations. It is generally preferred that the 60 low tear Strength the peel Strength may be less than the
additives should be relatively inert and have negligible or detection limit of the measuring device employed. In
Synergistic effects upon the properties contributed by the contrast, for medical packaging applications peel Strengths
essential ingredients. in excess of 1,000 g may be required to insure the packaging
The cold Seal compositions of the invention may be does not burst open under pressure, resulting in contamina
prepared by Standard melt blending procedures. In 65 tion of the medical device. Regardless of the peel Strength,
particular, the first polymer(s), tackifier(s), and optional the cold seal bond preferably exhibits a smooth peel or fiber
plasticizer(s) may be melt blended at an elevated tempera tearing bond, rather than a Zippery peel.
 US 6,221,448 B1
11 12
The cold Seal composition of the present invention may be Bohemia, N.Y.). The samples were heat sealed to uncoated
coated onto a wide variety of Substrates Such as polymeric release paper as well as to the release lacquer coated paper
films and foils which in turn are used to package food and at 120° F. and 50 psi for 16 hours.
Sterilizable medical device, Self-seal and tamper evident 4. Rlieology Testing
envelopes, banding for paper money, napkins, and clothing, The storage modulus (G') and tan delta were determined
and protective packaging Such as fold over “blister' pack in accordance with ASTM D4440-93. A test frequency of 10
ages for hardware and Small parts. Additionally, cold Seal radians/sec and a temperature ramp or Step test was per
adhesives have found utility as anti-skid coatings and for formed with a 10 mm diameter parallel plate test geometry
release-paper free tapes Such as tableSS diaper tapes. with a gap of 1 to 4 mm.
The invention can be further illustrated by the following 5. Density is measured in accordance with ASTM D-792.
non-limiting examples. The Samples are annealed at ambient conditions for 24 hours
before the measurement is taken.
EXAMPLES
6. Melt index (I), is measured in accordance with ASTM
Test Methods
15
D-1238, condition 190° C./2.16 kg (formally known as
1. Self-Seal Test “Condition (E)”).
The adhesive compositions were coated onto Standard 7. Molecular Weight is determined using gel permeation
copy paper with a Pamarco Precision Hand proofer using an chromatography (GPC) on a Waters 150° C. high tempera
85Q Quadragravure engraved roller. The roller is specified ture chiomatographic unit equipped with three mixed poros
to apply 34.6 CBM/in' of material. (CBM=cubic million ity columns (Polymer Laboratories 103, 104, 105, and 106),
micron) The coat weights were measured to verify the operating at a System temperature of 140 C. The Solvent is
amount deposited. Coated sheets of paper were Sealed 1,2,4-trichlorobenzene, from which 0.3 wt-% solutions of
adhesive side to adhesive side in a Sentinel press. The the Samples are prepared for injection. The flow rate is 1.0
conditions used were room temperature sealing (78. F., 25 mL/min. and the injection size is 100 microliters.
C.), 1 second dwell time, and variable pressure from 10 to 25 The molecular weight determination is deduced by using
100 psi. The bond was then characterized in accordance with narrow molecular weight distribution polystyrene Standards
the following descriptions: (from Polymer Laboratories) in conjunction with their elu
tion volumes. The equivalent polyethylene molecular
weights are determined by using appropriate Mark-Houwink
coefficients for polyethylene and polystyrene (as described
Bond Rating Description by Williams and Word in Journal of Polymer Science,
1. No Cling Samples did not stick together, i.e. freely fall Polymer Letters, Vol. 6, (621) 1968, incorporated herein by
apart. reference) to derive the following equation:
2. Cling Substrates stick together but a very small
amount of force is required to pull apart. Mpolyeihylene=a*(Mpolystyreneb.
35
3. Cling/Zippery Peel Same as "Cling except accompanied by a
Zippery noise. In this equation, a =0.4316 and b=1.0. Weight average
"Zippery denotes a stick-slip phenomena molecular weight, M, is calculated in the usual manner
which often results in the generation of noise. according to the following formula: M=X w. M, where w,
4. Seal/Zippery Peel Samples stick together and a reasonable amount and M are the weight fraction and molecular weight,
of force is required to pull apart, accompanied
by a zippery noise. 40 respectively, of the ith fraction eluting from the GPC col
5. Seal? Smooth Peel Samples stick together and a reasonable amount U.
of force is required to pull apart resulting in 8. Melt Viscosity is determined in accordance with the
a smooth separation and no noise associated following procedure using a Brookfield Laboratories DVII+
with debonding.
6. Seal/Fiber tear Samples stick together and paper fiber tearing Viscometer in disposable aluminum Sample chambers.
results upon separating the sheets. 45 The spindle used is a SC-27 hot-melt spindle, Suitable for
measuring Viscosities in the range of from about 10 to about
100,000 centipoise. The sample is placed in the chamber,
For Examples 35 to 38, a pressure of 100 psi was which is in turn inserted into a Brookfield Thermosel and
employed, whereas for Example 39 the cold seal coated locked into place. The Sample chamber has a notch on the
surfaces were bonded to each other with a pressure of 50 psi. 50
bottom that fits the bottom of the Brookfield Thermosel to
The peel Strength was determined by Separating the bonded ensure that the chamber is not allowed to turn when the
paper with an Instrumentor’s Bench Peel Tester Spindle is inserted and Spinning. The Sample is heated to the
(Instrumentors Inc., Cleveland, Ohio) at a rate of 12 inches/ desired temperature, with additional Sample being added
minute, averaging the readings over 20 Seconds. until the melted sample is about 1 inch (2.5 cm) below the
2. Sentinel Press Blocking Test 55
top of the Sample chamber. The Viscometer apparatus is
The tendency of the Samples to adhere to Flexcon release lowered and the Spindle Submerged into the Sample chamber.
lacquer, 82-3-90017 was also characterized. A No. 6 Myer Lowering is continued until brackets on the Viscometer
rod was used to apply the release lacquer onto medical grade align on the Thermosel. The Viscometer is turned on, and Set
to a shear rate which leads to a torque reading in the range
kraft paper at a coat weight of 0.0054 grams/in. The of 30% to 60%. The reading is taken after about 30 minutes,
adhesive coated copy paper, prepared in accordance with the 60 or after the value has stabilized.
Self Seal Test was pressed against the release-lacquer coated The Synthesis of the ultra-low molecular weight polymers
paper in a Sentinel PreSS for 1 Second. The preSSure was and waxes is described in WO 98/0360, published Jan. 29,
varied until either fiber tear occurred or 100 psi was reached. 1998, incorporated herein by reference. Table I depicts the
The same bond ratings as for the Seal test were used. density and melt indeX or Viscosity of the homogeneous
3. Koehler Blocking Test 65 ethylene/C-olefin interpolymers employed in the examples.
Examples 35 to 39 were also tested using the Koehler K The exemplified Polymers 1 to 8 are substantially linear
53000 IC Block Tester, (Koehler Instrument Company Inc., ethylene-octene polymers.
 US 6,221,448 B1
13 14
Examples 1 to 39 of Tables II and III depict several
TABLE I embodiments of cold Seal compositions of the present inven
tion based on metallocene or Single-site catalyzed polyole
Density Melt Index Viscosity at fins. Abroad concentration range of homogeneous ethylene/
Designation g/cm (g/10 min.) 350° F (cPs) 5 C-olefin interpolymers are employed ranging from 40 wt-%
Polymer 1 O.87O 1OOO
to 100 wt-% as depicted in Example 39. Although Polymer
Polymer 2 O.859 1OOO
7 (Example 28) and Polymer 8 (Example 27) do not possess
Polymer 3 O.87O 500
the desired properties uncompounded, the properties can be
Polymer 4 O.87O 2OO enhanced with tackifier and wax, as depicted in Examples 30
Polymer 5 O.87O 5OOO and 31. Likewise, Example 7 employing Polymer 2 is not
Polymer 6 O.864 2OO desirable due to its tendency to block. However, the appli
Polymer 7 O.88O 5OOO cants Surmise that by decreasing the polymer concentration
Polymer 8 O.890 1OOO and adding Some wax this disadvantage can be overcome.
Further, Examples 35 and 36 are surmised to be suitable to
form cold Seal tapes which do not require the tape backing
to be coated with lacquer.
TABLE II
Test 1 Test 2
Self-Seal Sentinel Press
Coat Characterization Block Test

Weight Viscosity Pressure Bond Pressure Bond

Example Polymer Tackifier Wax (g/m) 350° F. (psi) Rating (psi) Rating
Ex. 1 40% 55% 5% O.O149 1535 3O 4 60-100 3
Polymer 1 E5380 PX-100 40 5
Ex. 2 40% 55% 5% O.O191. 2120 3O 4 60-100 3
Polymer 3 E5400 PX-100 40 5
50 6
Ex. 3 40% 55% 5% 1140 50-100 4 60-90 2
Polymer 4 E5400 PX-100
Ex. 4 40% 60% 30-40 5 80-1OO 3
Polymer 3 E5400
Ex. 5 40% 55% 5% OOO84 40-50 5 60-100 3
Polymer 1 E5400 PX-100
Ex. 6 60% 30% 10% 40 2 30-50 1.
Polymer 1 E5400 PX-100 60-80 2 60-80 2
Ex. 7 50% 50% O.O157 2O 6 50-100 4
Polymer 2 E5400 1O 6
5 5
Ex. 8 80% 20% 60-100 2 50-100 1
Polymer 1 E5400
Ex. 9 80% 20% 60-80 2 50-100 1
Polymer 3 E5400
Ex. 60% 20% 20% 50 2 SO-90 1.
Polymer 1 E5400 PX-100 60-90 3 1OO 2
Ex. 55% 40% 5% O.O121 4260 20-60 5 70-90 3
Polymer 3 Eastotac PX-100
H-100-R
Ex. 60% 30% 10%
Polymer 3 Eastotac PX-100 O.O122 4190 30-50 2 80-1OO 3
H-100-R 60-80 5
Ex. 50% 30% 20% O.O1O3 2105 40-60 2 70-1OO 2
Polymer 3 Eastotac PX-100 70-100 5
H-100-R
Ex. 40% 40% 20% O.O137 1240 50-100 3 70-1OO 2
Polymer 3 Eastotac PX-100
H-100-R
Ex. 70% 20% 10% 6130 40-80 2 80-1OO 2
Polymer 3 Eastotac PX-100 90 2
H-100-R
Ex. 65% 24% 11% O.O132 4785 30-60 2 60-70 1.
Polymer 3 Eastotac PX-100 70-90 5 80-90 2
H-100-R
Ex. 45% 35% 20% 1712 30-70 3 60-80 1.
Polymer 3 Eastotac PX-100 (1665)
H-100-R 80-100 4 90-1OO 2
Ex. 50% 45% 5% O.O1OS 3.556 30-60 2
Polymer 3 Eastotac PX-100 70-90 5
H-100-R
Ex. 65% 30% 5% 6400 30-50 2 60-90 3
Polymer 3 Eastotac PX-100 60-90 5
H-100-R
Ex. 20 54.33%. 38.83% 11.83% 3490 30-60 2 60-80 2
Po ymer 3 Eastotac PX-100 70-90 5 90 3
 US 6,221,448 B1
15
TABLE II-continued
Ex. 21 57.5% 37.5% 5% 54OO 30-50 5 60-90 3
Polymer 3 Eastotac PX-100 60-90 6
H-100-R
Ex. 22 56% 24% 20% OOO66 2885 3O 2 60-80 1.
Polymer 3 Eastotac PX-100 40-90 2 90 2
H-100-R
Ex. 23 45% 45% 10% O.O1O2 2265 30-50 3 60-90 3
Polymer 3 Eastotac PX-100 60-90 4
H-100-R
Ex. 24. 45% 35% 20% O.O112 2610 30-90 3 60-70
Polymer 3 Eastotac PX-100 (2510)
H-100-R 80-90 2
Ex. 25 56% 24% 20% O.O171 3O15 30-90 2 60-90 2
Polymer 3 Eastotac PX-100
H-100-R
Ex. 26 54.33%. 38.83% 11.83% O.OO96 33OO 30-50 2 60-100 3
Polymer 3 Eastotac PX-100 60-90 5
H-100-R
Ex. 27 100% 70-100 1.
Polymer 8
Ex. 28 100% 70-100 1.
Polymer 7
Ex. 29 40% 60% O.O122 1400 2O 5 70-100 2
Polymer 1 Escorez 30-70 5
54OO
Ex. 30 40 w %, 60% 90-100 2
Polymer 8 Escorez
54OO
Ex. 31 40 w %, 60% 60-100 3 50-100 3
Polymer 7 Escorez
54OO
Ex. 32 40% 60% 60-100 3
Polymer 1 Eastotac
H-130-R
Ex. 33 40% 60% 60-100 3
Polymer 5 Eastotac
H-130-R
Ex.34 40% 55% 5% 30-40 5
Polymer 3 Escorez PX-100 50 6
54OO
Ex. 35 80% 20% O.O116 10660 1OO 5
Polymer 3 Escorez
54OO
Ex. 36 80% 20% O.OO9 5840 1OO 5
Polymer 1 Escorez
54OO
Ex. 37 55% 40% 5% O.O145 3700 1OO 6
Polymer 3 Escorez Bareco
54OO C-4040
Ex. 38 65% 30% 5% O.O.194 6047 1OO 6
Polymer 3 Escorez Bareco
54OO C4040
Ex. 39 100% O.OO8 16475 50 3
Polymer 3
Comp. 15% O.OO)4 1OO 1.
A. Vestoplast
608/75% 10%
Vestoplast Polywax
408 2OOO
Comp. 40% O.OO)4 26SO 1OO 2
B Rextac 10% 10%
2280/40% Wing- Polywax
Rextac tack 2OOO
2315 95

“PX-100 - Polywax 100

“ES380 - Escorez 538O
Test 3 Block Test
Label Paper Dow Release Lacquer Multiweb Release Lacquer Test 4 Peel Test
Ex. 35 Slight; adhesive transfer None None 240 + 18 g
Ex. 36 Slight; adhesive transfer None None 215 + 9 g
Ex. 37 Severe blocking None Slicks, but no 458+ 193g
FT or transfer Paper Tear
Ex. 38 Blocks; 30-50% FT None Slicks, but no 310 + 202 g
FT or transfer Paper Tear
 US 6,221,448 B1
18
TABLE II-continued
Ex. 39 Cling Less than 50
Comp. A Og
Comp. B 3g

7. The cold seal composition of claim 1 wherein the

TABLE III homogeneous linear or Substantially linear cthylene/C-olefin
1O interpolymcr has a melt indeX ranging from about 400 g/10
Peel Values of Example 11
min. to about 1200 g/10 min.
Seal AVg Actual 8. The cold seal composition of claim 1 wherein the
Pressure Peel Width Peel polydispersity of the homogeneous linear or Substantially
Sample (psi) (grams) Observation (inches) (grams/inch) linear ethylene/C-olefin interpolymer is less than 4.
15
Ex. 11 2O 71.0 Legging 1. 71.0 9. The cold seal composition of claim 1 wherein the
40
60
218.6
339.9
Legging
Legging
1.
1.
218.6
339.9
polydispersity of the homogeneous linear or Substantially
linear ethylene/C-olefin interpolymer is less than 2.5.
10. The cold seal composition of claim 1 wherein the
The peel values of Example 11 were also evaluated. The 2O density of the homogeneous linear or Substantially linear
peel Strength is Suitable for the packaging of IV tubing. ethylene/C-olefin interpolyrner ranges from about 0.855
Tapes having a paper backing coated with a cold Seal g/cm to about 0.890 g/cm.
composition are commonly employed for packaging medi 11. The cold seal composition of claim 4 wherein said
cal devices. In the case of IV tubing, the tape is wrapped composition further comprises at least one tackifying resin.
around bundles of IV tubing to reduce the volume of 12. The cold seal composition of claim 11 wherein the
packaging required as well as the keep the tube from 25 tackifying
tangling. The cold Seal composition forms Sufficient bond 10 wt-% toresin is present in an amount ranging from about
about 70 wt-%.
Strength with light pressure applied by hand.
What is claimed is: 13. The cold seal composition of claim 4 wherein said
1. A cold Seal composition comprising from about 10 composition further comprises at least one wax.
wt-% to 100% wt-% of at least one homogeneous linear or 14. The cold seal composition of claim 13 wherein the
Substantially linear ethylene/C-olefin interpolymer. wax is present in an amount ranging from about 3 wt-% to
2. The cold seal composition of claim 1 wherein said about 20 wt-%.
composition has a storage modulus (G") at 25 C. ranging composition 15. The cold Seal composition of claim 4 wherein said
from about 1x10" dynes/cm to about 8.5x10" dynes/cm. 35 from the group further comprises at least one polymer Selected
3. The cold seal composition of claim 1 wherein the consisting of block copolymers, ethylene
homogeneous linear or Substantially linear ethylene/C-olefin Vinyl acetate, ethylene-methyl acrylate, ethylene-n butyl
interpolymer is present in an amount greater than about 30 acrylate, and mixtures thereof.
wt-%. 16. A package, envelope or tape comprising a Substrate
4. The cold seal composition of claim 1 wherein the coated with the cold Seal composition of claim 1.
homogeneous linear or Substantially linear ethylene/C-olefin 40 17. The package, envelope or tape of claim 16 wherein the
interpolymer is present in an amount ranging from about 40 coated Substrate is bonded to itself forming a Smooth peeling
wt-% to about 80 wt-%. or Substrate failing bond.
5. The cold seal composition of claim 1 wherein the 18. The package, envelope or tape of claim 17 wherein the
homogeneous linear or Substantially linear ethylcne/O- 45 force to Separate the bond ranges from about 100 g to about
olefini interpolymer has a melt indeX ranging from about 500 g/linear inch bond width.
200 g/10 min. to about 2000 g/10 min. 19. A cold Seal composition consisting essentially of one
6. The cold seal composition of claim 1 wherein the or more homogeneous linear or Substantially linear ethylene/
homogeneous linear or Substantially lincar ethylene/O- C-olefin interpolymer.
olefilin interpolymer has a melt indeX ranging from about
300 g/10 min. to about 1500 g/10 min.
 UNITED STATES PATENT AND TRADEMARK OFFICE
CERTIFICATE OF CORRECTION

PATENT NO. : 6,221,448 B1 Page 1 of 2

DATED : April 24, 2001
INVENTOR(S) : Baetzold et al.

It is certified that error appears in the above-identified patent and that said Letters Patent is
hereby corrected as shown below:

Column 1
Line 54, "Ziegaler” should be -- Ziegler --.
Line 63, “metal locene' Should be -- metallocene --.
Column 2
Line 4, “30)” should be -- 30 --.
Column 4
Line 43, “havin(g” should be -- having --.
Column 6
Line 4, “ethylene/(o. -olefin” should be -- ethylene/o, -olefin --.
Line 19, “ethylene/(o. -olefin” should be -- ethylene/o, -olefin --.
Line 56, “mentioned.” Should be -- mentioned, --.
Column 9
Line 23, “ethylene/(o. -olefin” should be -- ethylene/o, -olefin --.
Column 12
Line 4, “Rlieology” should be -- Rheology --.
Line 18, “chiomatographic' should be -- chromatographic --.
Column 16
Table II, EX.24, Bond Rating Column, “blank space' should be -1 --.
Column 15-16
Table II-continued, Third Column, “Test 3 Block Test” should be -- Test 3 Koehler
Block Test --.
Table II-continued, EX. 37, Fourth Column, “Slicks,’ Should be -- Sticks, --.
Table II-continued, Ex. 38, Third Column, “None FT or transfer” should be -- None --.
Table II-continued, Ex. 38, Fourth Column, “Slicks, but no Paper Tear” should be --
Sticks, but no FT or transfer --.
Table II-continued, Ex. 38, Fifth Column, “310+202 g” should be -- 310 + 202 g Paper
Tear --.

Column 17-18
Table II-continued, Fourth Column, “Less than 50, 0g, 3 g should be in Fifth
Column, -- LeSS than 50, 0g, 3 g --.
Line 34, “8.5x10" dynes/cm” should be -- 8.5x10' dynes/cm--.
Lines 44 and 45, “ethylcine/o, -olefini” should be -- ethylene/o, -olefin --.
 UNITED STATES PATENT AND TRADEMARK OFFICE
CERTIFICATE OF CORRECTION

PATENT NO. : 6,221,448 B1 Page 2 of 2

DATED : April 24, 2001
INVENTOR(S) : Baetzold et al.

It is certified that error appears in the above-identified patent and that said Letters Patent is
hereby corrected as shown below:

Column 17, cont.

Line 49, “lincar' Should be -- linear --.
Column 18
Line 9, “cthylene/o, -olefin” should be -- ethylene/o, -olefin --.
Line 20, “interpolyrner” should be -- interpolymer --.

Signed and Sealed this

Twenty-ninth Day of April, 2003

JAMES E ROGAN
Director of the United States Patent and Trademark Office