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TITRATION ALKALINITY

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     SUMMARY: Seawater is collected from discrete depths 
     using PVC sampling bottles attached to the CTD/rosette   
     system.  Subsamples of approximately 50 ml are measured 
     gravimetrically and titrated with 0.1 N HCl using an 
     automated potentiometric titration system.  Total 
     alkalinity is determined using a Gran plot corrected 
     for interference from bisulfate and hydrogen fluoride. 
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1.  Principle

    Titration alkalinity is one of four parameters needed to describe 
the carbonate system in seawater.  Titration alkalinity is therefore 
useful for assessing the magnitude and direction of ocean-atmospheric 
carbon dioxide flux and the saturation state of calcium carbonate 
within the interior of the ocean.  Titration or total alkalinity is 
usually defined as the quantity of hydrogen ions in millimoles (mmol) 
required to neutralize the weak bases in 1 kilogram of seawater 
(Grasshoff, 1983).  A more exact definition (Dickson, 1981) of total 
alkalinity is the quantity of hydrogen ion required to neutralize 
bases formed from weak acids with pKs of a > 4.5.  Our determination 
of total alkalinity employs the potentiometric titration of a seawater 
sample with hydrochloric acid.  Our methods are slight modifications 
of those developed for seawater analysis (Grasshoff, 1983 and references 
therein).  Our titration procedure employs an open cell and a computer-
controlled titration system .  The computer-controlled system 
incorporates an automated high-precision burette and pH meter. 


2.  Precautions

    Alkalinity samples should be drawn directly from the Niskin bottle 
using clean drawing tubes.  Care should be taken to avoid contamination 
from ship's equipment or the atmosphere.


3.  Water Sampling

    Alkalinity samples are collected using the same techniques employed 
when collecting DIC samples (see Chapter 6).

3.1. Drawing the sample

  3.1.1. Samples are drawn into a clean 300 ml glass reagent bottle.

  3.1.2. The bottle should be flushed with at least one volume of water.

  3.1.3. The tube is withdrawn so that the bottle remains brimful when 
         the tube is completely withdrawn.


4.  Preserving the Sample

4.1. Some of the sample is removed from the reagent bottle using a 10 
     ml pipet.  Enough water is removed so that about 1 cc of air is 
     contained in the bottle when the glass stopper is inserted.

4.2. 100 µl of a saturated HgCl2 solution is added to the sample.  
     The tapered ground glass bottle neck is dried with a kimwipe 
     and the bottle is sealed with a ground glass stopper covered 
     with light coating of ApiezonR grease.  The stopper is pressed 
     firmly into the bottle to make a good seal and is secured with 
     polyethylene tape of a large rubber band.


5.  Potentiometric Titration

5.1. The sample is brought to 25°C and approximately 50 ml is placed 
     in a tared 100 cc beaker.  The weight of the sample is recorded 
     to the nearest milligram.

5.2. A clean stirbar is added to the beaker and the beaker is placed 
     on a stirplate.  The antidiffusion burette tip and the 
     potentiometric electrode is placed in the beaker.

5.3. The temperature of the stirred sample is measured to the nearest 
     0.1°C.  The temperature of the sample is recorded and the 
     automated titration is initiated.

5.4. The automated titration procedure adds a 1 to 1.5 ml aliquot of 
     approximately 0.1 N HCl depending upon the anticipated sample 
     alkalinity.  After reaching a stable mv reading, the mv value is 
     recorded and a 15 microliter HCl aliquot is added.  After the 
     electrode output stabilizes a second 15 µl aliquot is added.  
     This process is continued until the mv value reaches a 
     predetermined value beyond the V2 inflection point.  Typically 
     30 to 35 aliquots are added to reach the predetermined mv value.


6.  Computation of Total Alkalinity

    Total alkalinity is determined from the volume of acid required 
to reach the second endpoint and the acid normality.  The inflection 
point (V2) is determined using a Gran plot (Gran, 1952) which corrects 
for the interference from both bisulfate and hydrogen fluoride.  Sulfate 
and fluoride concentrations are calculated from salinity and the 
equilibrium constants for bisulfate and hydrogen fluoride (Khoo et al., 
1979; Dickson and Riley, 1979).


7.  Preparation of HCl

    The accuracy of the total alkalinity measurement is determined, in 
large part, by the uncertainty in the normality of the HCl.  The 
approximately 0.1 N HCl solution is made by dilution of concentrated 
HCl into a 0.7 M solution of high-purity NaCl.  The normality of the 
HCl solution is ascertained by titration of solutions made from dried 
high-purity sodium carbonate and borax.


8.  Precision and Accuracy

    The precision of our total alkalinity determinations is approximately 
+4 µequiv/kg.  This gives a coefficient of variation of approximately 
0.2% for typical seawater samples.  Because we lack a liquid seawater 
standard of known alkalinity, the accuracy of our total alkalinity 
determinations is not well known.  In order to help ensure the accuracy 
of our alkalinity measurements we regularly collect intercalibration 
samples for Dr. Keeling's laboratory at Scripps Institution of Oceanography.  
To date, alkalinity values for replicate samples analyzed in both 
laboratories are typically within 10 µequiv/kg.


9.  Equipment and Supplies

    kimwipes and applicator sticks
    300 ml ground glass stoppered reagent bottles
    10 ml automatic pipet
    Apiezon grease
    analytical balance
    volumetric flasks, 100 ml beakers, 50 ml glass pipets and mercury 
      thermometer
    Automated titration system
      PC and software
      Brinkmann model 655 Dosimat and 5 ml top
      Orion model 940 pH meter
      Orion combination electrode
      stir plate


10.  Reagents

     distilled deionized water (DDW)
     high purity sodium carbonate
     high purity sodium chloride
     reagent grade hydrochloric acid


11.  References

     Almgren, T., D. Dyrssen and S. Fonselius.  1983.  Determination 
     of alkalinity and total carbonate.  In: Methods of Seawater 
     Analysis, M. E. K. Grasshoff and K. Kremling, editors, Verlag-
     Chemie, pp. 99-123.

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

     Dickson, A. G. and J. P. Riley.  1979.  The estimation of acid 
     dissociation constants in seawater media from potentiometric 
     titrations with strong base. TheThe ionic product of water (Kw).  
     Marine Chemistry, 7, 89-99.

     Gran, G.  1952.  Determination of the equivalence point in 
     potentiometric titration. Part II.  Analyst, 77, 661-671.

     Khoo, K. H., R. W. Ramette, C. H. Culberson and R. G. Bates.  
     1977.  Determination of hydrogen ion concentrations in seawater 
     from 5 to 40oC:  standard potentials at salinities from 20 to 
     45 o/oo.  Analytical Chemistry, 49, 29-34.