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ALKALINITY

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     SUMMARY: Seawater samples are collected at discrete 
     depths using CTD-rosette sampling protocols.  Subsamples 
     for alkalinity are collected and immediately preserved 
     with HgCl2 for subsequent analysis in the laboratory.  
     The alkalinity is determined by a potentiometric titration, 
     and the second end point (V2) is determined with a 
     modified Gran Plot. 
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1.  Principle

    The total alkalinity is defined as the number of milliequivalents 
of H+ required to titrate one kilogram of seawater to the bicarbonate 
equivalence point (~pH 4.5).  The classical chemical formulation 
(Harvey, 1966) of this definition is:

         Alk(t) = [HCO31-] +2[CO32-] +[B(OH)41-] +[OH1-] -[H+]

     In high precision work corrections for other proton acceptors 
(e.g. [H3PO3-] and [SiO(OH)3-), should be taken into account (Edmond, 
1970; Dickson, 1981; Bradshaw and Brewer, 1988).  From the knowledge 
of the total alkalinity, dissolved inorganic carbon, salinity, and 
nutrient content of seawater the entire carbonate "balance" can be 
calculated from the dissociation constants of carbonic acid, boric 
acid and other interacting species.


2.  Precautions

    Samples should be drawn as soon as possible and preserved to halt 
biological activity.  Samples bottles should be completely sealed and 
stored in the dark cool place.


3.  Water Sampling

3.1. Drawing the sample

  3.1.1. Samples are drawn into combusted 300 ml glass reagent bottles 
         in the same manner as dissolved oxygen.

  3.1.2. The drawing tube is completely filled with sample while 
         manipulating the tube to dislodge bubbles.  The drawing tube 
         is flushed and inserted to the bottom of the sample bottle.

  3.1.3. The sample bottle is overflowed with at least two volumes 
         of sample.

  3.1.4. The tube is slowly withdrawn with the sample flowing. 

3.2. Preserving the sample

  3.2.1. Use a pipet to remove water from the neck of the sample 
         bottle of sample.  Enough water is removed so that 
         approximately 1 ml of air is contained in the bottle when 
         the glass stopper is inserted.

  3.2.2. 100 µl of saturated HgCl2 is added to each sample.  The 
         tapered ground glass bottle neck is dried with a Kimwipe 
         wrapped on an applicator stick.  The bottle is sealed with 
         a ground glass stopper coated with a light covering of 
         Apiezon grease.  The stopper is pressed firmly into the 
         bottle to make a good seal, and is secured with polyethylene 
         tape or a large rubber band.                                                


4.  Calibration of Electrode (NBS and SWS)

4.1. NBS

  4.1.1. Soak electrode in storage solution overnight.

  4.1.2. Place electrode in buffer 7 and soak for 15 minutes.

  4.1.3. Pour out old buffer and replace with fresh buffer.

  4.1.4. Record relative millivolt reading when electrode stabilizes.

  4.1.5. Take temperature of buffer.

  4.1.6. Repeat steps 2 through 5 with buffer 4.
        
4.2. Seawater buffer preparation

  4.2.1. 0.4 M Tris and 0.4 M Bis seawater buffers are prepared 
         according to the method of Dickson (1992).

  4.2.2. NaCl, KCl, and NaHSO4 are dried and added gravimetrically.

  4.2.3. MgCl2 and CaCl2 are added volumetrically from stock 
         solutions that have  been standardized with AgNO3.

  4.2.4. HCl is added from a 0.1 M stock solution carefully prepared 
         from a Dilut-it.

  4.2.5. Buffers are stored in tightly capped 250 ml polyethylene 
         Nalgene bottles.

4.3. Calibration

  4.3.1. Place electrode in Tris buffer overnight.

  4.3.2. Pour out old buffer and replace with fresh buffer.

  4.3.3. Record relative millivolt reading when electrode stabilizes.

  4.3.4. Take temperature of buffer.

  4.3.5. Place electrode in Bis buffer for approximately 15 minutes.

  4.3.6. Repeat steps 2 through 6. 


5.  Preparation and Standardization of Acid Titrant

5.1. Volumetrically prepare a solution of 0.1000 N HCl in 0.7 M 
     sodium chloride. 

5.2. Standardize the above solution against recrystalyzed sodium 
     tetraborate (borax) which is stored in a dessicator over a 
     saturated solution of sodium chloride and sodium citrate 
     (Vogel, 1978).

5.3. Prepare at least two concentrations of borax primary standard.

  5.3.1. Make a 0.0035 to 0.004 M solution of sodium tetraborate.

  5.3.2. Weigh out approximately 25 g of the borax solution and 
         titrate in a similar manner to a seawater titration.

  5.3.3. Calculate the endpoint using a Gran Plot.                                         

5.4. Calculate normality of the acid titrant using the known quantity 
     and concentration of borax primary standard.

5.5. As a final check on the accuracy of our acid standardization, 
     a subsample is sent to Dr. Andrew Dickson's laboratory at 
     Scripps Institution of Oceanography for high precision 
     coulometric determination of the acid normality.


6.  Titration of Samples
  
6.1. Turn on computer, Dosimat, printer, and pH meter.  Load the 
     alkalinity program.  Dispense approximately 20 ml of acid 
     through the Dosimat to purge any air bubbles and to pump fresh 
     acid into the lines.                                                          

6.2. Throughly rinse and dry a 50 ml beaker.

6.3. Place beaker on balance and tare.  Weigh out approximately 
     50 grams of sample.      

6.4. Rinse electrode with seawater and gently dry by touching the 
     bottom of the electrode with a Kimwipe.  Do not wipe the 
     electrode dry.

6.5. Place sample on magnetic stir plate.  Put stir bar into sample 
     taking care not to splash any sample out of the beaker. Adjust 
     to moderate stirring.  Arrange electrode and buret tip as to 
     not interfere with the stir bar but to make sure electrode 
     junction and tip are submerged in sample.          

6.6. Start titration program.  The program will request a preadd 
     volume.  This volume should be sufficient to adjust the pH of 
     the sample to about 4.  The program will then add HCl in 0.015 
     ml increments and record the millivolt reading after each 
     increment is added.  The titration will automatically terminate 
     when a specified millivolt reading (equivalent to pH 3.0) is 
     reached.                

6.7. After the titration has terminated, check and record the sample 
     temperature.

6.8. Remove beaker from stir plate and pour out sample.  Rinse with 
     tap water for approximately 3 minutes and then rinse with 
     deionized distilled water.  Dry beaker for next sample. 


7.  Calculations

    Data is fit by a modified Gran Function (f2=(Vo+V)([H+]+[HS04-]+[HF])) 
using Matlab.  A best fit Eo and slope are obtained by minimizing the sum 
of the residuals for those points in the range pH 3-3.5.  The accuracy 
of the calculated slope is determined by comparing to the measured slope 
for the buffers described above.


8.  Quality Control

    As a safeguard on the quality of our results, we maintain a set of 
secondary standards which are run with each analysis.  These are made 
from a large surface seawater sample, which is preserved with HgCl2 
and subdivided into 300 ml reagent bottles.  These are sealed as 
described above and stored in a cool dark place.


9.  Precision and Accuracy

    The precision of our titration procedure is approximately 3 µeq/kg.  
An absolute alkalinity standard is not yet available, and the accuracy 
of the procedure is determined primarily by the standardization for 
the normality of the titrant.  We  intercalibrate the determination 
of the acid normality with Dr. Andrew Dickson's laboratory at Scripps 
Institution of Oceanography, where high-precision coulometric methods 
are used to determine the acid normality.


10.  Equipment and Supplies

     Niskin bottles and rosette
     300 ml combusted reagent bottles
     Apiezon grease
     Computer interfaced 665 Dosimat and Orion EA 940 Ion Analyzer
     Calibrated volumetric glassware
     Analytical and topload balance
     Magnetic Stirrer
     Thermometer
     Glass Electrodes     


11.  Reagents

     Hydrochloric acid (0.1000 N)
     Sodium tetraborate (borax)
     Distilled and deionized water
     NaCl
     HgCl2 (saturated solution)


12.  References

     Bradshaw, A. L. and P. G. Brewer.  1988.  High precision 
     measurements of alkalinity and total carbon dioxide in 
     seawater by potentiometric titration:  Presence of unknown 
     protolytes?  Marine Chemistry, 23, 69-86.

     Dickson, A.  1981.  An exact definition of total alkalinity 
     and a procedure for the estimation of alkalinity and total 
     inorganic carbon dioxide from titration data.  Deep-Sea 
     Research, 28A, 609-623.

     Dickson, A.  1992.  pH buffers for seawater media based on 
     the total hydrogen ion concentration scale.  Deep-Sea Research, 
     submitted.

     Edmond, J. M.  1970.  High precision determination of titration 
     alkalinity and total carbon dioxide content of sea water by 
     potentiometric titration.  Deep-Sea Research, 17, 737-750.

     Harvey, H. W.  1966.  The Chemistry and Fertility of Sea Waters.  
     Cambridge Univ. Press, 240 pp.

     Vogel, A. I.  1978.  Textbook of Quantitative Inorganic Analysis, 
     4th Ed., pp. 300-301. Longman, New York.