Lecture 4

Bio 451 Molecular Biology Techniques

Electrophoresis

 

History of electrophoresis

1930s First reports of the use of sucrose for gel electrophoresis.

1955 Introduction of starch gels, not very good separation

1959 Introduction of acrylamide gels for 1st time (Raymond and Winstraub) Accuracy of control of parameters such as pore size and stability

1964 Disc gel electrophoresis Ornstein and Davis

1969 Introduction of denaturing agents especially SDS separation of protein subunit (Beber and Osborn)

1970 Laemmli-T4 phage separated 28 components “stacking gel + SDS

1975 2 Dimensional gels O’Farrell isoelectric focussing then SDS gel electrophoresis.

1977 Sequencing gels

Late 1970s agarose gels

1983 Pulsed field gel electrophoresis

1983 Capillary electrophoresis introduced

 

Electrophoretic Process

·       Two pieces of equipment are necessary for electrophoresis: a d.c. power supply and a buffer reservoir system.

·       The system consists of upper and lower buffer reservoirs with provision for suspending the gel.  The only electrical connection between the reservoirs is via the gel.  Platinum electrodes are positioned in each reservoir.

·       The macromolecular samples are dissolved in a glycerol containing buffer to increase the density of the sample.  At pH 9, a commonly used pH for electrophoresis, most proteins are negatively charged.  Hence the anode is placed in the lower reservoir.  Often, a “tracking dye” such as bromophenol blue (BB) is included in the sample as a reference.  BB migrates faster than any of the macromolecules.

·       The reaction that permit current passage from the cathode to the anode are the electrolysis of water, producting hydrogen at the cathode and oxygen at the anode:

 

Cathode reaction:         2e- + 2H2O – 2 OH- + H2

                                                HA + OH- --- A- + H2O

 

Anode reaction:           H2O --- 2H+ + 1/2 O2 + 2e-

                                                H+ + A- --- HA

 

One mole of hydroxyl ions and protons are produced at the cathode and anode, respectively, for every mole of electrons that flow through the system.

 

Types of Electrophoresis

Low voltage thin sheet electrophoresis

·       The supporting medium may be paper, cellulose acetate, or a thin layer of material such as silica.

·       Paper.  Chromatography paper is suitable for electrophoresis.  Low voltage paper electrophoresis has been extensively used in the past for the separation of a range of charged compounds such as amino acids, peptides, proteins, nucleotides, nucleic acids and charged carbohydrate derivatives.  Considerable diffusion of small molecules occurs on paper during low voltage electrophoresis and better resolution may be obtained by applying high voltage, where the time required for separation is reduced and less diffusion of the molecules occurs.

·       Cellulose Acetate.  Cellulose acetate is a suitable medium for the separation of radiolabelled substances and for such microtechniques as immunodiffusion and immunoeletrophoresis.  Cellulose acetate will, in general, separate the same range of compounds as paper but has found particular application in clinical investigations for the separation of blood proteins, including glycoproteins, lipoproteins and hemoglobins.

·       Thin Layer Electrophoresis (TLE).  Thin layers of silica, alumina or cellulose can be prepared on glass plates as for thin layer chromatography (TLC). The plates are placed horizontally into the electrophoresis unit and the thin layer is allowed to saturate with buffer by diffusion from the reservoir.  TLE, like TLC, is rapid and gives good resolution and high sensitivity.  High voltages may also be used in TLE.

Gel Electrophoresis

·       Gels may be prepared from starch, agar and polyacrylamide.  The molecular sieving property of the semi-rigid gel helps to separate large ionic compounds such as proteins.  Smaller molecules can be separated only in Sephadex-type gels.  Sephadex-type gels have small pores that exclude larger molecules from access to the stationary phase inside the particle, thereby causing movement outside the pores whereas small molecules are tightly held within the pores.

·       Starch gels are prepared by heating and cooling a mixture of partially hydrolysed starch in an appropriate buffer.  This causes the branched chains of the amylopectin components of starch to intertwine and form a semi-rigid gel.

·       Agar/Agarose gels consist of two galactose-based polymers, agarose and agaropectin.

 

Electrophoresis: Acrylamide Gel Electrophoresis

·       Polyacrylamide gels are made from acrylamide monomers copolymerised with the cross linker N,N’methylenebisacrylamide in the presence of ammonium persulphate and TEMED as catalyst.  Prior degassing of solutions is required since molecular oxygen inhibits chemical polymerization.

 

The Tools of Biochemistry by Terrance G. Cooper, Univ. of Pittsbrugh, Wiley-Interscience Publications, John Wiley and Sons, NY, 1977.

 

Make up of the Acrylamide gel

The migration of macromolecules through acrylamide gel is influenced by the structure of the gel itself.

·       The compounds used to construct the polymer matrix are acrylamide, N,N’-methylene-bis(acrylamide), tetramethylenediamine (TEMED), and ammonium persulfate (ammonium persulfate dissolved in water it forms free radicals).

·       If the ammonium persulfate free radicals are brought into contact with acrylamide, the free radical is retained within the acrylamide molecule.  The “activated” acrylamide can then react with successive acrylamide molecules producing a polymer chain. To obtain a gel, the acrylamide needs to be cross-linked with N,N’-methylene-bis(acrylamide).  TEMED or b-(dimethylamino) propionitrile is usually added at at concentration of 0.4% to serve as a catalyst of gel formation because of its ability to exist in a free radical form.

 

·       The size of the holes or pores in the gel is determined by two parameters: (1) the amount of acrylamide used and (2) the degree of cross-linkage.  The average pore size reaches a minimum when 5% of the total acrylamide used is N,N’-methylene-bis(acrylamide).  Therefore, in many formulations the bis(acrylamide) content is fixed at 5% of the total acrylamide and is not altered.  In the lab, we used 30% Acryl+0.8% Bis (2.6% bis). The pore size is manipulated by varying the total content of acrylamide.

 

The following are other considerations in the production of polyacrylamide gels. 

·       The buffer serves (1) to maintain a constant pH within the reservoirs and within the acrylamide gel and (2) as the electrolyte which conducts current across the electric field.

·       A buffer must be chosen that does not interact with the macromolecules being separated.  Such interactions might change the rate of molecule migration. This would occur if the interaction adds or neutralizes the charge on the macromolecule.

·       The pH of the environment must allow the macromolecules to be charged not denatured.  In the case of proteins the usual outside limits are 4.5 and 9.0.  However, a broader or more restricted range may be necessary.

·       The ionic strength and concentration of the buffer must be considered.  If the electrolyte concentration within the acrylamide gel is too low, the migrating macromolecules conduct a large portion of the current.  As a result they are not found in a sharp band but rather spread into diffuse zones and thus greatly decrease the resolution of this method.  Alternatively, if the electrolyte concentration within the gel is too high, the amount of current conducted increases while voltage decreases.  This usually results in a decreased rate of macromolecular migration and the generation of heat, which can denature the proteins being separated.

·       The extent to which a macromolecule migrates into the gel depends on both the size of the molecules and the average size of the pores thorough which it must pass.  It is this sieving effect that enhances the resolution obtained with acrylamide gels.  Logarithms of the relative mobilities for a group of proteins decrease linearly as the total gel concentration is increased.

 

Discontinuous Gel Electrophoresis

·       Disc pH or disc electophoresis is a modification of the zone electrophoretic technique described above.  The significant differences are (1) the use of a two gel system and (2) the unique buffer systems used in the gel matrix and in the buffer reservoirs.  The lower-separating or running gel is prepared using about the same amount of acrylamide (5-10%) as would be used for an analogous zone electrophoretic experiment.  The buffer used in this gel is usually an amine such as Tris which is adjusted to the proper pH (e.g., pH 8.8) using hydrochloric acid. 

·       After the separating gel has polymerized, a second, small layer of gel is polymerized on top of it.  This is the upper or stacking gel.  A total acrylamide content of 2-3% acrylamide is common.  The buffer used in the stacking gel is also an amine such as Tris, but in this case the pH is adjusted with HCl to 2 pH units lower than that of the running gel (pH 6.8). 

·       The buffer used in the protein sample should be identical to that used in the stacking gel.

·       The reservoir buffer is made up of 0.025M Tris, 0.192 M Glycine, pH 8.8).

·       Glycine exists as both a zwitterion with a net charge of zero and a glycinate ion with a charge of minus one:

 

NH3CH2COO- ------ NH2CH2COO- + H+

                       

·       When the electric field is established, chloride, protein, bromophenol blue, and glycinate anions all begin to migrate toward the anode.  However, as glycinate ions enter the sample buffer and stacking gel they encounter a low pH, shifting the equilibrium toward formation of zwitterions, which are immobile.  Failure of glycine zwitterions to move into the sample and stacking gel creates a deficiency of mobile ions, which in turn decreases current flow.  However, a constant current must be maintained throughout the entire electrical system.  This is accomplished in the area between the leading chloride ions and the trailing glycinate ions by an increase in voltage.  The result is a very high localized voltage gradient occurring between the chloride ions and the glycinate ions.  In this condition the relative ion mobilities are glycinate< proteins<BB<Cl-.

·       In this strong local electric field the anionic proteins all migrate rapidly.  The stacking gel has large pores so as not to impede their progress.  If any of the proteins overtake the leading chloride ions, they slow down because wherever there are chloride ions there is no ion deficiency, and hence the large field strength disappears.  The rapid movement of the proteins behind the chloride front and the decreased rate of protein migration as they approach the front result in a piling up or concentration of the protein sample in a tight disc between the glycinate and chloride ions.  As the disc of proteins encounters the running gel their migration is slowed by the small pores of the gel.  This permits the small glycinate ions to catch up with the proteins.  Crossing the interface between the stacking and running gels, glycinate ions become fully charged once again, and there is no longer an ion deficiency.  Hence from this point on there is a constant field strength throughout the gel, and separation of the protein proceeds just a with zone electrophoresis.  The advantage of this modification is that the protein sample enters the separating gels as a narrow zone.  The resulting protein bands are therefore much more compact, and this increases resolution.

 

SDS Acrylamide Gel Electrophoresis

·       Molecules which are tightly, but not covalently, bound together do not usually separate from one another during electrophoresis.  Thus, the anionic detergent sodium dodecyl sulfate (SDS) is used to separate a mixture of proteins.  SDS binds to the hydrophobic regions of proteins and separates most of them into their component subunits.  1.4g SDS binds to 1 gram of protein.  SDS binding also imparts a large negative charge to the denatured, randomly coiled polypeptides.  This charge largely masks any charge normally present in the absence of SDS.

·       If component subunits of protein are held together by disulfide bonds, these bonds may be broken before electrophoresis by heating the preparation in the presence of SDS and b-mercaptoethanol, a reducing agent.

 

Two Dimensional Gel Electrophoresis

·       This powerful technique involves first subjecting the mixture of proteins to isoelectric focusing on a 1 mm diameter gel in a capillary tube.  Isoelectric focusing is carried out in much the same way as elecrtrophoresis with the exception that ampholytes are electrophoresed through the gel prior to sample addition in order to establish a pH gradient within it.  As a protein moves down the tube it continuously encounters a higher and higher pH environment.  As the protein traverses this pH gradient it reaches a pH corresponding to its isoelectric point.  At this pH the net charge of the protein is zero and it therefore stops moving in the electric field. 

·       At the end of isoelectric focusing, the gel is removed from the capillary tube and placed on top of a slab gel.  The sample is now subjected to SDS acrylamide gel electrophoresis.  Since the isoelectric point and molecular weight of a protein are unrelated it is possible to obtain an even distribution of proteins using these parameters in two dimensions.

 

·       Gradient Gel Electrophoresis

 

·       Isoelectric focusing.  This technique, also called electrofocusing is based on moving boundary rather than zone electrophoresis.  Amphoteric substances such as amino acids and peptides are separated in an electric field across which there are both voltage and pH gradients.  The anode region is at a lower pH than the cathode region and a stable pH gradient is maintained between the electrodes.  Amphoteric substances thus become focused into narrow stationary bands.  The carrier ampholytes are usually synthetic aliphatic polyamino-polycarboxylic acids and are available commercially in mixtures covering a wide pH band (e.g. 3 to 10) or various narrow bands (e.g. 4 to 5).  The anode end of the column is connected to a reservoir containing an acid solution (e.g. phosphoric acid) and the cathode end is connected to a reservoir containing an alkaline solution (e.g. sodium hydroxide).  On opening the two reservoir valves the two solutions diffuse into the column setting up a pH gradient between the acidic anode and the alkaline cathode.  The valves are then closed and the current switched on, causing the carrier ampholytes to migrate until they reach the pH regions where they have no net charge.   The sample is then allowed to enter the upper end of the column by opening a valve, and the charged sample component migrate until they reach the pH regions of the tube at which they have no net charge. Vertical columns containing polyacrylamide gel impregnated with carrier ampholytes can also be used, reducing the time required for separation.

·       Isotachophoresis.  This technique is another form of moving boundary electrophoresis.  The principle underlying isotachophoresis is utilized in the stacking gel system in SDS polyacrylamide electrrophoresis.  In greek, isotachophoresis means travel (phoresis) at the same (iso) speed (tacho).  Any charged substances can be separated by isotachophoresis.  For the separation of a mixture of anions, a leading anion (e.g. Cl-) is chosen which has a higher mobility than the sample ions, and a trailing anion (e.g. glutamate) is also chosen which has lower mobility than the sample ions.  All the anions must have a common cation (e.g. Tris).  When the current is switched on, the leading ions will move towards the appropriate electrode, the sample ions will follow in order of their mobilities and the trailing ion will follow behind the sample ions. 

·       Pulse-Field Gel Electrophoresis.  When a DNA molecule is larger than the pore size, the DNA can no longer be sieved by the gel according to its size but must instead migrate “end-on” through the matrix as if through a sinuous tube.  This mode of migration is known as “reptation.” Gels of 0.1-0.2% agarose can resolve extremely large DNA molecules, but they are very fragile.  Even then, these gels are incapable of resolving linear DNA molecules larger than 750kb.  DNA molecules in the individual chromosomes of lower eukaryotes may be 7000 kb or more in length. 

·       In 1984, Schwartz and Cantor reported the development of pulse-field gel electrophoresis.  In this method, pulse, alternating, orthogonal electric fields are applied to a gel.  Large DNA molecules become trapped in their reptation tubes every time the direction of the electric field is altered and can make no further progress throughout the gels until they have reoriented themselves along the new axis of the electric field.  The larger the DNA molecules, the longer the time required for this realignment.  Molecules of DNA whose reorientation times are less than the period of the electric pulse will therefore be fractionated according to size.  The original method described by Schwartz and Cantor was capable of resolving DNAs up to 2 megabase pairs in length.  However, as a consequence of improvements to the technique, resolution of DNA molecules larger than 5000kb can now be achieved. 

·       In 1986, Gardiner et al used a vertical gel apparatus with platinum wire electrodes positioned on opposite sides of the gel.  The DNA moves first toward one set of electrodes and then toward the other as the electric fields are switched.  The net result of these zigzag movements is a straight line from the loading well toward the bottom of the gel.  Because all the lanes in the gel are exposed to equivalent electric fields, there is no horizontal distortion of the DNA bands.  As with other pulsed-field gel electrophoresis systems, the size of the molecules resolved at a given voltage is a function of the angle between the electrodes and the pulse time.  Typically, the electrodes are arranged at a 90o angle and 10 second pulses are used to separate molecules between 50 kb and 450kb in length; 50 to 60-second pulses are used to fractionate molecules larger than 1000 kb in length.  The upper limit of resolution of the system appears to be approx. 9000kb.

 

Detection of Macromolecules

·       Coomassie Brilliant Blue Staining for proteins

·       Alcian blue, Toluidine blue for glycoproteins

·       Amido black, Wilson sudan black for lipoproteins

·       Fluorescent Staining Techniques: Pluorescamine

·       Specific Enzyme Visualization: lactate dehydrogenase-reduction of nitroblue tetrazolium chloride (yellow to blue); Periodic acid-Schiff for glycoproteins.

·       Detection of Radioactive Macromolecules: X-rays, liquid scintillation, sepctrophotometry.

 

Capillary Electrophoresis (CE).  This type of electrophoresis can separate a wide variety of molecules of biological interest such as metabolites, drugs, amino acids, nucleic acids, carbohydrates, peptides and proteins based on their sizes and ionic properties.  CE separations of proteins and peptides are based on charge-to-mass ratios.  While PAGE separations are restricted to polyacrylamide matrices and a relatively small number of buffer systems, CE separations can be achieved in a variety of matrices and buffers.  Consequently, there is much greater flexibility in the design of the optimal separation protocols.

·       CE employs as fused-silica capillary column, which may or may not be derivatized, either in free solution or in the presence of a fluid matrix.  The CE separation is more analogous to HPLC than PAGE.  However, CE separation is based on electrophoretic parameters.  CE is most useful for separations of peptides because it offers great flexibility in separation parameters.  It can be used to monitor proteolytic digestions and optimize digestion conditions for the production of a representative peptide fingerprint of a protein.

·       The capillaries are generally 30 to 50 cm long with 50-75 µm internal diameter.  The net total volume of these capillaries is in the low microliter range.  The capillaries are thin-walled; this allows rapid and efficient exchange of the Joule heating that results from the high voltages that are necessary for electrophoretic separations.  The maximum Voltage and current that can be run are 300µA and 30kV.  As the protein and peptide molecules are swept through the capillary, they pass through the detector light path and are registered on the UV monitor.  With respect to sensitivity, speed, and versatility, CE can offer some advantages over gel electrophoresis for the separation of proteins and peptides.

·       In CE, buffer flow is generated inside the column when the electric field is applied.  This flow is from the cathode electrode to the anode electrode in a a fused-silica capillary column; this movement of the buffer is called the electroosmotic flow (EOF)

·       Isoelectric focusing can be performed by CE.  A pH gradient is generated in a coated capillary column by filling the column with asample solution that contains ampholytes.  A high pH solution (NaOH) is placed in the cathode reservoir and a low pH solution (phosphoric acid) is placed in the anode reservoir.  After separation by IEF in the absence of electroosmotic flow, mobilization of the proteins past the detector is necessary.  A simple replacement of the anode reservoir with the buffer in the cathode reservoir established EOF and causes the sample zone to migrate pass the detector.

·       The selection of an appropriate separation protocol for a protein depends on the specific properties of that protein.  However, there are separation approaches that utilize specific properties of proteins.  IEF-CE separates on the basis of charge alone; CE in the presence of ionic detergents such as SDS separates on the basis of size alone; and CE using underivatized capillaries at low pH or derivatized capillaries at high salt and high pH separates on the basis of both size and charge.

 

Factors affecting electrophoresis

The electric field

·       Voltage.  If the separation of the electrodes is d (cm) and the potential difference between them is V volts, the potential gradient is V/d.  The force on an ion bearing a charge q coulombs is then Vq/d newtons.  The force causes migration and the rate of migration is proportional to Vq/d.  The rate of migration under unit potential gradient is called the mobility of the ion.  An increase in the potential gradient will therefore increase the rate of migration proportionally.

·       Current. When a potential difference is applied between the electrodes, a current is generated, measured in coulombs sec or amperes.  The size of this current is determined by the resistance of the medium and is proportional to the voltage.  The current in the solution between the electrodes is conducted mainly by the buffer ions with a small proportion being conducted by the sample ions.  An increase in voltage will increase the total charge per second conveyed towards the electrode.  The distance migrated by the ions will be proportional to both current and time.

·       Resistance.  Ohm’s law expresses the relationship between current I (measured in amperes, A), voltage V (measured in volts, V) and resistance R (measured in ohms, W) in which:

V/I=R

·       The current, and hence the rate of migration are thus inversely proportional to the resistance, which in turn is a function of the medium, the buffer and its concentration.  Resistance will increase with the length of the supporting medium but will decrease with its cross-sectional area and with increasing buffer ion concentration.  During electrophoresis the power dissipated in the supporting medium (W, measured in watts) is such that:

W=I2R

·       An increase in temperature will cause the resistance to fall.  Part of this effect is due to an increase in the mobility of the ions as a result of a decrease in the viscous resistance offered by the liquid to the motion of the ions through it as the temperature rises.  The heating will produce evaporation of the solvent from the supporting medium causing a decrease in resistance.  Although the rate of migration and the total charge per second conveyed towards the electrode will increase, the increase in buffer ion concentration will result in slower migration of the sample.

·       When constant voltage is applied, the current will increase during electrophoresis due to a decrease in resistance of the medium with the rise in temperature.  Consequently, more heat will be produced resulting in more evaporation of solvent and a decrease in resistance.  A constant current avoids these problems but may lead to a drop in voltage due to decreased resistance, resulting in reduced rate of migration.

·       If a number of gels are run in parallel with one power supply, then:

1/R= 1/r1 +1/r2+…. 1/rn

where R is the total resistance and r1,r2, etc. are the resistances of each gel.  The total current supplied must be increased in proportion to the number of gels used, assuming that they all have the same resistance.

 

The resistance does decrease as the temperature increase for semiconductors.  Since the gel is a semiconductor so it make sense for the decrease in resistance.  This is  because increasing temperature means increasing the velocity of charged particles so conductivity will increase.  However, the resistance in metals does increase as the temperature increase.  When the temperature of a metal is increased its resistance also increases this is because the increased vibration of the matel lattice makes it harder for the free electrons to flow easily through the material.  When a semiconductor is heated its resistance goes down as more electrons have the energy to become free from the lattice.

 

The sample

·       Charge.  The rate of migration increases with an increase in the net charge.  The magnitude of the charge is generally pH dependent.

·       Size.  The rate of migration decreases for larger molecules, due to the increased frictional and electrostatic forces exerted by the surrounding medium.

·       Shape.  Molecules of similar size but different shapes such as fibrous and globular proteins exhibit different migration characteristics because of the differential effect of frictional and electrostatic forces.

 

The buffer

·       Composition.  The buffers in common use are formate, acetate, citrate, barbitone, phosphate, Tris, EDTA and pyridine.  The buffer should not bind to the sample.  In some cases, however, binding can be advantageous, for example borate buffers are used to separate carbohydrates since they produce charged complexes with carbohydrates.  Since the buffer acts as a solvent for the sample, some diffusion of the sample is inevitable, being particularly noticeable for small molecules such as amino acids and sugars.  The extent of diffusion can be minimized by not overloading the sample.

·       Concentrations  As the ionic strength of the buffer increase, the proportion of current carried by the buffer will increase and the share of the current carried by the sample will decrease, thus slowing the sample migration.  High ionic strength of the buffer will also increase the overall current and heat will be produced.  At low ionic strengths the proportion of current carried by the buffer will decrease and the share of the current carried by the sample will increase, thus increasing its rate of migration.  A low ionic buffer strength reduces the overall  current and results in less heat production, but diffusion and the resulting loss of resolution are higher.  The compromise is to use between 0.05 to 0.1 M.

·       PH determines extent of ionisation.

 

The supporting medium

·       Adsorption.  This is the retention of sample molecules by the supporting medium.  Adsorption causes tailing of the sample and reduces the rate and resolution of the separation.

·       Electro-osmosis.  This results from a relative charge being produced between water molecules in the buffer and the surface of the supporting medium.  The charge may be caused by surface adsorption of ions from the buffer and the presence of stationary carboxyl groups on paper or sulphonate groups on agar.  The effects of electro-osmosis can normally be ignored.

·       Molecular Sieving.  Molecular sieving occurring in agar, starch and polyacrylamide gels is that the movement of large molecules is hindered increasingly by decreasing the pore size since all molecules have to traverse through the pores.