The Notes for
Polymer and Coatings Science-
Chapter Two

Bulk Polymerization of Poly(methylmethacrylate)

An example: Solution Polymerization of Poly(methylmethacrylate)

Suspension Polymerization of Poly(methylmethacrylate)

Emulsion Polymerization of Poly(methylmethacrylate)

Properties of PMMA

Poly(acrylonitrile) (PAN) can be polymerized from acrylonitrile using a monosuspension process. ??So hows does monosuspension compare to general suspension??

The major use for poly(acrylonitrile) is textile (clothes) fibers.

PAN is toxic only if burned, in which case HCN (the "cyanide gas" used for gas chambers) is produced. When PAN is solution polymerized, organic solvent, the solution can be used for fiber spinning. Suitable organic solvents include dimethylacetamide, DMF, DMSO. Fibers prepared from pure PAN are difficult to dye, so a minor portion (~10%) of comonomers such as methyl methacrylate, vinyl acetate, or N-vinyl pyridine are added to improve dyeability.

H   CH3         H   H        H   H
|   |           |   |        |   |
C = C           C = C        C = C
|   |           |   |        |   |
H   C=O         H   O        H   N
|               |           / \
O-CH3           C=O        C   C=O
    	        |          |  /
	        CH3        C-C

Methyl          Vinyl        N-Vinyl
Methacrylate    Acetate      Pyridine
PAN can be polymerized in aqueous solutions of concentrated inorganic salts such as calcium thiocyanate, sodium perchlorate, and zinc chloride.

Emulsion polymerization of PAN is problematic because the monomer has an appreciable water solubility and the formation of polymer in the aqueous phase (for emulsion polymerization, polymerization is supposed to occur in the surfactant droplets!) can lead to coagulation of the latex. The molecular weight of PAN molecules ranges from 80,000 to 170,000.

PAN is extremely soluble in polar solvents such as THF and DMOS.

In PAN, appreciable electrostatic forces occur between the dipoles of adjacent nitrile groups on the same polymer molecule. This intramolecular interaction restricts bond rotation and leads to a stiff chain. As a result, PAN has a high crystalline melting point (Tm) of 317 deg C and is soluble only in the solvents mentioned above.

    C       C       C       C                   C       C       C       C
  /   \   /   \   /   \   /   \   /           /   \   /   \   /   \   /   \   /
C       C       C       C                   C       C       C       C
|       |       |       |    ------->       |   O   |   O   |   O   |
C       C       C       C                   C       C       C       C
\\\     \\\     \\\     \\\               /   \   /   \   /   \    / 
  N       N       N       N                     N       N       N   
  :       :       :       :                     :       :       : 
I believe the above reaction is some kind of oxidation because the notes show oxygen over the reaction arrow. The reaction leads a ladder polymer with aromatic rings.

The heating of this polymer to temperatures of 1500- 3000 deg C (hellacious temperatures which disrupt most organic matter into water and carbon dioxide) result in a graphite carbon skeleton structure with great strength.

Poly(acrylamide) (PAM) is water soluble to infinite molecular weight. PAM is prepared by a free radical reaction, but it also can be prepared via alkoxide (RO-) initiation:
 
      H   H          H   H
      |   |          |   |
RO- + C = C   ---->  C - C- (the second carbon has a negative charge)
      |   |          |   |
      H   C=O        O-R C=O
          |              |
          NH2            NH2


      H   H          And the negatively charged -NH is going to act like 
      |   |          the RO- above, ripping the hydrogen away from 
----> C - C-H  ----> the second carbon of another acrylamide monomer,  
      |   |          and leaving behind a pair of electrons, etc. 
      H   C=O        
          |              
          NH 
         (-)
PAM is hard and brittle. It is readibly soluble in cold water, and is slightly soluble in organic compounds because of its polarity. It undergoes reactions characteristic of the amide group.

Applications: PAM is used as a flocculant in the processing of minerals, the treatment of industrial wastes. Copolymers which incorporate acrylamide increase the dry strength of paper.

Thermosetting Acrylic Copolymers

Usually thermoset acrylics are terpolymers (made from three different monomers.)

  1. the first monomer confers hardness and rigidity to the polymer (examples below)
    • acrylonitrile
    • methyl methacrylate
    • styrene
    • vinyl toluene
  2. the second monomer contributes flexibility to the polymer (examples below)
    • ethyl acrylate
    • 2-ethylhexyl acrylate
    • butyl methacrylate
  3. the third monomer provides pendant reactive groups which are the sites for crosslinking (examples below)
    • acrylic acid
    • butoxymethylacrylamide
    • glycidyl acrylate
    • hydroxyethyl acrylate


Most thermoset acrylics are prepared by solution polymerization. Solvents used include butanol and xylene. In order for 1) the solution to have the right viscosity and 2) the solution to have a satisfactory solides content (40 to 60% by weight), the molecular weight of the thermoset acrylic must be kept down to about 20,000 to 30,000 by the use of a relatively high initiator concentration and high temperature. Applications of thermoset acrylics range from very flexible coatings needed for strip metal to the hard chemical resistance needed for domestic appliances.

Poly(vinyl acetate)

vinyl acetate is prepared from acetylene and acetic acid.
          			    H   H
      -                             |   |
H - C - C - H  + H C - C - OH  -->  C = C
      -           3                 |   |
	         		    H   O
acetylene        acetic acid            |
		         		C=O
			        	|
			         	CH3
There is a problem with acetic acid reacting with the vinyl acetate to produce ethylidene diacetate, shown below:
    H   H       O
    |   |       || 
H - C - C - O - C - CH 
    |   |             3
    H   O
        |
        C=O
        |
        CH3
This side reaction is minimized by:
  1. using a molar axcess of acetylene
  2. short reaction times
  3. low temperature
Poly(vinyl acetate) (PVAc) can be prepared from ethylene, starting with the oxidation of the ethylene. Below, [O] is a generic term for 'oxidation' that appears again and again in the notes.
H   H            H   O                           H   H       O
|   |  [O]       |   ||     [O]     Co(Ac)       |   |       ||
C = C -----> H - C - C - H ----->, --------> H - C - C - O - C - CH3 
|   |            |                               |   |
H   H            H                               H   O
		         			     |
ethylene     acetaldehyde                            C=O    
			        		     |
        H   H                                        CH3
  H+    |   | 
----->  C = C                               ethylene diacetate
        |   |
            O
            |
            C=O
            |
            CH3

vinyl acetate
In the above, ethylene is oxidized to acetaldehyde with aqueous palladium chloride. This reaction is carried out as a liquid phase at a temperature of 100 deg C and a pressure of 1 to 3 atm.
H   H                           H   O
|   |                           |   ||
C = C + PdCl  + H O  ---->  H - C - C - H  + Pd  + 2HCl
|   |       2    2              |
H   H                           H
Vinyl acetate is a colorless liquid with a boiling point of 73 deg C, and a pleasant sweet odor (note that it is an ester.) Before shipment, the monomer is usually inhibited by cupric acetate or hydroquinone.

Poly(vinyl acetate) may be polymerized by bulk, solution, suspension, or emulsion techniques. Commercially, emulsion polymerization is the predominant method.

The emulsion polymerization of PVAc is carried out batch wise in a stirred reactor which is jacketed for heating and cooling. Below is a typical formula (recipe.) Note that the numbers below, to which no specific units have been assigned, refer to mass.
Vinyl Acetate                   100      monomer
water                           100      carrier
hydroxyethylcellulose             2.5    protective colloid
poly(ethylene glycol ether 
of lauryl alcohol                 2.5    surfactant
sodium doelecylbenzenesulphonate  0.1    surfactant
sodium bicarbonate                0.5    buffer
potassium persulfate              0.5    initiator

reaction temperature:  75 to 80 deg C
reaction time:         2 hours
The reaction is highly exothermic, and it is common to polymerize first only a portion of the monomer, and then to add the remainder of the monomer slowly over the 2 to 4 hours.
The resulting latex is used "as is" (as opposed to decanting the water and then drying the solid polymer.) The solid polymer is not isolated, because the end use is for surface coatings and adhesives.
With regard to tacticity, a head to tail structure is expected.
PVAc is soluble at room temperature in a wide range of solvents:



Last Update- May 28, 1995- wld