Professional Documents
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Polymer History
Dorel Feldman
To cite this article: Dorel Feldman (2008) Polymer History, Designed Monomers and Polymers,
11:1, 1-15, DOI: 10.1163/156855508X292383
Review
Polymer History
Dorel Feldman ∗
Department of Building, Civil and Environmental Engineering, Concordia University,
1455 De Maisonneuve Blvd.W., Montreal, Quebec, Canada H3G 1M8
Abstract
During the last century and a half, new families of engineering materials known as polymers have been
discovered and produced, that have not only challenged the classical materials but have also made possible
the realization of new products which have contributed to extend the range of activities of mankind. This
paper is a brief review of the history of the most important groups of polymeric materials, such as plastics,
fibers and elastomers. In the growth of polymeric materials during the last century and a half, plastics are
the leader followed by fibers and elastomers.
Koninklijke Brill NV, Leiden, 2008
Keywords
Polymers, plastics, fibers, rubber, review
1. Introduction
Polymers are at the basis of important industrial goods. Their rapid growth in
production is caused, beside social factors, by the necessity to replace classical
materials.
The word “polymer” was introduced by the Swedish chemist J. J. Berzelius. He
considered, for example, benzene (C6 H6 ) to be a polymer of ethyne (C2 H2 ). Later
this definition underwent a subtle modification [1].
Polymer science is a relatively new discipline which deals with plastics, natural
and synthetic fibers, rubbers, coatings, adhesives, sealants, etc.; all of these materi-
als nowadays have become very common.
The concept of polymers is one of the great ideas of the 20th century. It emerged
in the 1920s amid prolonged controversy and its acceptance is closely associated
with the name of H. Staudinger who received the Nobel Prize in 1953.
Many examples of synthetic polymers can be mentioned; some everyday, like
polyesters or nylons, others less known, like the ones used for medical applications
for organs, degradable sutures, etc.
* Tel.: (1-514) 848-2424, ext. 3202; Fax: (1-514) 848-7965; e-mail: feldman@bcee.concordia.ca
2. Plastics
The first plastic material was based on nitrocellulose and was obtained by Parkes
in 1862 and Hyatt in 1866. The addition of camphor to nitrocellulose led to the
first thermoplastic (a modified natural polymer) known as celluloid. By 1900 this
material was used for movie film.
In about 1897, galalith (gala = milk, lithos = stone) was produced in Germany
by reacting casein (a milk protein), with formaldehyde [2].
The first synthetic thermoset polymer (a phenol-formaldehyde (PF)), known as
Bakelite, was obtained in 1907 by Baekeland through the polycondensation of
phenol with formaldehyde. Bakelite was commercialized in 1909–1910 [3]. The
commercial development of this PF material is considered to be the beginning of
the truly synthetic plastic era and of the plastic industry, although cellulose nitrate
(semi-synthetic) had been known and in use for some time.
The successful use of PF resin catalyzed the development of other polycondensa-
tion products based on formaldehyde (F) with urea (U) and melamine (M), known
as amino resins, aminoplasts or aminoplastics. Such polymers were first described
by Tollens in 1884 and were patented by John in 1918 [4]. Aminoplasts, contrary
to phenoplasts, can be made translucent or in light colors [5]. In 1926 Rossiter pro-
duced aminoplasts based on formaldehyde and mixture of urea and thiourea [6].
The production of MF resins began in the mid-1930s [7].
Unsaturated polyesters (uPES) were discovered in 1933 by Ellis and commer-
cialized around 1942. These polycondensation products are known as alkyds, name
which appears to have been derived from alcohol (alk) and acid (yd); they are used
primarily as coatings. From the same family, glycerophthalic (Glyptal) coatings in-
volve glycerol and phthalic anhydride [5].
The existence of vinyl chloride (VC) was reported by Liebeg and Regnault in
1835, but its ability to polymerize was not fully known at that time. The effect of
sunlight on VC was later investigated by Baumann in 1878, when it was observed
that a white substance formed as a result. Very little progress was then made until
1912–1916 when Klatte discovered the basis for VC photo-polymerization [8]. In
1926 Ostramislenski patented flexible film cast from a solution containing PVC and
a plasticizer [4]. Also it was discovered that PVC became a flexible material that re-
D. Feldman / Designed Monomers and Polymers 11 (2008) 1–15 3
Yet the new polymer could not be fabricated by melt processing. The next two
forms of PTFE, fine powder and dispersion, were also not melt-processible. The
pursuit of more easily processible fluoro-polymer led to fluorinated ethylene–
propylene co-polymer (FEP), which could be melted and processed in an extruder.
Poly(perfluoroalkoxy) (PFA), which was introduced in 1973, offers both melt
processing and high thermostability like PTFE. Some other polymers in this fam-
ily were discovered, such as poly(chloro-trifluoro ethylene) (PCTFE), poly(vinyl
fluoride) (PVF), poly(vinylidene fluoride) and other co-polymers and terpolymers
[15].
Saturated polyesters were first studied by Carothers starting 1929; he was able
to obtain a PES of propylene glycol and 1,16-hexadecanoic acid with an average
MW of 12 × 103 . As the aliphatic PES all had boiling points too low, he turned
his attention to polyamides. Later on studies on PES were done by Whinfield and
Dickson (1941–1946). The most important polymer in this group is poly(ethylene
terephthalate) (PET), produced first in 1955 and used as a plastic, film and fiber.
The original discovery leading to the world-wide interest in all classes of
polyurethanes (PU) was made by Bayer and his co-workers in 1937 as a competitive
response to the work done by Carothers on the polyamides. In 1947 Bayer published
an impressive account of the synthesis of PU and polyureas. In the 1950s the basic
technology used polyesters to obtain the flexible foams and polyether polyols were
introduced in 1957 [16]. Later on, PUs were found to be useful for the produc-
tion of plastics (1961), elastomers, foams, adhesives, fibers and corrosion-resistant
coatings [17, 18]. A new transparent thermoplastic PU was produced recently [19].
In 1909 Prileschajew discovered that olefins would react with peroxy benzoic
acid to form epoxides. Peroxy acid epoxidations play an important role in epoxy
resin production [20]. Epoxy resins (EP) were first synthesized by Schlack (the
inventor of nylon 6), in 1934. Their curing reaction was discovered by Castan and
Greenlee (late in the 1930s) and polymer products were introduced in the market
towards the end of World War II. Although a number of different types are now
commercially available, the major share of the market is still held by systems based
upon the reaction products of epychlorohydrin and bisphenol A [7, 21, 22].
Vinyl ester resins, which may be regarded as hybrids of epoxy and polyester resin
chemistry, were developed in the 1960s. They are made by reacting epoxy resins
with ethylenically unsaturated carboxylic acid in order to give terminal unsaturation
[7].
In the early 1950s, Hogan and Bank discovered that ethylene can be polymerized
under moderate conditions (3–4 MPa and 70–100◦ C) with chromium oxide cata-
lysts on silica support. Manufacture of high-density PE (HDPE) produced by this
procedure started in 1956. Currently HDPE is one of the largest commodity plastic
[23]. Shortly after (1953) Ziegler and Natta independently developed a family of
stereospecific transition-metal catalyst that led also beside HDPE to the synthesis
and commercialization in 1957 of polypropylene (PP) as a major commodity plastic
[8, 24–26].
D. Feldman / Designed Monomers and Polymers 11 (2008) 1–15 5
PEEK, the most important member of the poly(aryl ether ketone)s (PAEK), has
become commercially available in 1978.
After 1980 continuous growth was recorded with the development of a number
of high performance polymers that could compete with traditional materials such
as polyamide 4-6 (1987), sindiotactic PS (1989) metallocene polyolefins, polyph-
thalamide (1991), and styrene–ethylene co-polymer and sindiotactic PP in 1992
[31, 32].
3. Fibers
The defining characteristic of a fiber is its thread-like form, without restriction on
chemical composition. Fibers can be metallic, mineral or organic. Nearly all non-
metallic fibers are polymeric materials, either natural, artificial (modified natural)
or synthetic. Natural fibers such as wool and cotton have aspect ratios in the or-
der of 103 or greater. The organic fibers are carbon or heterochain polymers; the
major mineral fibers like glass and asbestos are macromolecular silicates. Organic
synthetic fibers are mostly thermoplastic, some are elastomeric and very few are
thermosets. Their history covers less than 75 years [33–35].
In the beginning, textile fibers came from nature: animal skins, hair, wool, silk
from silkworms, and plants like flax, cotton, hemp, etc.
The utility of flax and hemp twines was recognized even in the Stone Age. Flax
fabrics were used in pre-dynastic Egypt (fine linen cloth being woven in 3800 BC)
and in Neolithic lake dwellings in Switzerland.
References to hemp and ramie (fibers cultivated in temperate latitudes, and un-
known to ancient Egyptians and Hebrews or to early Greeks) occur in Chinese
writings dating 2800 BC and in early Sanskrit literature. Jute appears to have been
cultivated in Bengal from the most ancient times.
Traditionally the culture of silk began in 2640 BC in China, where for many
centuries its origin and the art of manipulating it were kept secret (it did not reach
Japan until AD 300). There are Sanskrit records dating from 1000 BC that refer to
the working of silk in ancient India.
Wool sheep appear to have originated as mountain animals in Mesopotamia. It is
well known that their wool was employed for clothing at least 5000 years ago [10].
For centuries, all textiles came from fibers that were harvested from a plant,
animal or insect. Then, at the end of the 19th and beginning of the 20th century,
people discovered that they could create textile fibers of their own. Those early
fibers still originated from a natural source, cellulose from wood pulp, but soon
enough, in the 1930s, 1940s and 1950s, a stream of synthetic fibers came on the
scene that owed their origin in chemical plants instead of plants that could be grown
in the field [36].
The idea for producing artificial fibers seems to have been advanced first by
R. Hooke in his Micrographia, published by the Royal Society in 1665. In 1833
Braconnot described the nitration of various celluloses and Liebeg established the
D. Feldman / Designed Monomers and Polymers 11 (2008) 1–15 7
The first polyamide that was mechanically spun from a melt was nylon 9, which
had a moderately high melting point of 196◦ C. Considerably work was also done
with nylon 5-10 with a melting point of 200◦ C. Nylon 66 decomposes just above
its relatively high melting point of 265◦ C [43].
The derivation of nylon 11 from castor oil was developed by Zeltner, Genas and
Kastner in 1944, and its production started in 1949 [4]. Nylon 12 first came to the
market in Germany in 1959 [44].
Several polyesters were investigated by Carothers during a DuPont program that
started in 1929. These polyesters were mostly linear aliphatic and they were char-
acterized by low melting points, considerable solubility in organic solvents and
poor resistance to hydrolysis. In 1941 Whinfield and Dickson obtained a aromatic
polyester, PET, and found it to have great promise as a fiber- and film-making poly-
mer. Its large-scale manufacture started in 1953 [10, 27, 45, 46]. Hill, Carothers
co-worker, also contributed to the preparation of fiber-forming polyesters [47].
Acrylonitrile (AN) was prepared by Moreau in 1893. Poly(acrylo nitrile) (PAN)
was developed for fibers in 1940; patents based on the utilization of concentrated
aqueous solutions (in Germany) and organic liquids (USA) were obtained in 1942.
Pilot production of PAN started in USA in 1943, and the first acrylic fiber (Orlon)
was made in 1948 and put into commercial production in 1950. By definition acrylic
fibers contain 85% or more AN. Along with PAN was developed a class of fibers
known as modacrylic. By definition they are based on co-polymers containing less
than 85% but more than 35% AN by weight. Their production started in 1949.
Such kind of fibers often contain as co-monomer a high amount of vinyl chloride,
vinylidene chloride or vinylidene cyanide [10, 48].
Poly(vinyl alcohol) (PVA) was produced in 1924 by the saponification of
poly(vinyl acetate) (PVAc). PVA fibers (Vinylon) were produced in 1951 in Japan
by coagulating the extrudate from an aqueous PVA solution in an aqueous sodium
sulfate solution. Their insolubilization is done by treatment with formaldehyde [49].
Based on the discovery of heterogeneous stereospecific catalysts by Ziegler,
Natta obtained in 1954 crystalline polypropylene (PP). Commercial production of
PP fibers and filaments started in 1957. The excellent wear and resistance to stain-
ing associated with low cost led to the use of such fibers for various applications
[14].
The first aromatic polyamide (aramid) fiber based on poly(m-phenylene isoph-
thalamid) (MPD), known as HT-1 and later re-named, was commercialized under
the trade name Nomex by DuPont in 1967. It was also produced in Japan and USSR
in 1970. These aromatic polyamides have at least 85% of the amide linkages at-
tached directly to two aromatic rings.
In 1973, DuPont started production of another aromatic polyamide fiber, a
poly(p-phenylene terephthalamide) marketed as Kevlar; this fiber has exceptional
strength competitive with glass, steel and carbon fibers [11, 50].
Aromatic polybenzimidazoles (PBI) were synthesized by Vogel and Marvel in
1961, with anticipation, later justified, that these polymers would have exceptional
D. Feldman / Designed Monomers and Polymers 11 (2008) 1–15 9
thermal and oxidative stability. In 1983 PBI fiber, spun from solutions of poly(2,2 -
(m-phenylene)-5,5 -bibenzimidazole) for a wide range of textile applications, was
commercialized [51].
Carbon fibers, first used as light bulb filaments in 1879, trace their modern his-
tory back to about 1942. The first commercially produced carbon filament was made
from a cellulosic precursor for its application as incandescent lamp filament. Sys-
tematic work regarding carbonization of rayon and PAN yarns and fabrics was ini-
tially investigated by Union Carbide during World War II. Two processes for manu-
facturing high-strength and high-modulus carbon fibers from rayon and PAN were
invented almost simultaneously in 1959 and 1961. Later, in 1963, a high-modulus
fiber made from pitch as precursor was invented. Since 1980, ultra-high-strength
fibers from PAN and ultrahigh-modulus fibers from pitch have been developed and
are used extensively in the aircraft and spacecraft structures [52–55].
Spandex fibers, which by definition consist of at least 85% of segmented
polyurethane, were invented in the 1950s to improve on the process and proper-
ties of rubber fibers; they became commercial around 1960 [56].
4. Elastomers (Rubbers)
The first mention of rubber trees is to be found in De Orbe Nuovo by Pietro Martire
d’Anghiera, published in latin in 1516. The outstanding source of natural rub-
ber, the large forest tree Heveea Brasiliensis, occurs in the southern equatorial
region, mainly in Malaysia, Indonesia, Thailand, Ceylon, India, Cambodia, Viet-
nam, Brazil, Africa and some other countries from Asia and South America. Such
trees were called “Cau-uchu” or “weeping wood” in South-America. The name was
derived from the use of the material as an eraser, “rub off pencil marks”, an applica-
tion introduced by Priestley in 1770. The original name of caoutchouc is still used
to denote rubber in many languages other than English, where it is reserved for the
rubber hydrocarbon [57, 58].
Until 1823, when Macintosh patented the use of coal tar, the lack of a satisfactory
solvent delayed the progress of rubber utilization and the natural rubber remained
little more than an academic novelty.
In 1839 Goodyear found that heating rubber with sulfur and white lead gave it
far superior properties. Hancock exploited this process, termed vulcanization by
Brockeden, to provide an elastic material insoluble in common solvent, from the
initial thermoplastic one [48]. The so-called cure, namely treatment with sulfur
chloride, which is now obsolete, was discovered by Parkes in 1840 [57].
Page reported the results of his studies on natural rubber in 1847. This endeavor
may well represent the onset of interdisciplinary research activity involving macro-
molecules [59].
Faraday showed in 1826 that natural rubber was a hydrocarbon of empirical
formulae (C5 H8 ) and Williams gave the name isoprene to the volatile liquid ob-
tained by destructive distillation of natural rubber of composition C5 H8 . A reversing
10 D. Feldman / Designed Monomers and Polymers 11 (2008) 1–15
5. Conclusion
Polymers initially tended to be viewed as a chemist specialty, but they are now
strongly associated as plastics, fibers and elastomers with engineering as well,
through design, fabrication and testing of products.
The last decades have shown an increasing important requirement in the polymer
industry; it is the rapid development and introduction of new and improved prod-
ucts. In the growth of this family of engineering materials during the last century,
plastics are the leader, followed by fibers and elastomers.
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