ࡱ> b jbjb "D\DDD8|l\ "....T},RR......}4:"}m Dd0,""\\d \\ Report on alkalinity measurements on P02 (6/04 8/04) Method Samples for total alkalinity were collected in glass bottles made from Schott Duran glass. They were preserved by the addition of 0.02% by volume of a saturated mercury(II) chloride solution (DOE, 1994 SOP 01), and analyzed typically within 24 hours on board ship. Total alkalinity measurements were made using an open-cell, two-stage, potentiometric titration procedure similar to that used to certify reference materials for total alkalinity (see Dickson et al., 2003), except that samples were not weighed into the titration vessel but instead were dispensed using a 120mL glass syringe. A metal frame attached to the syringe barrel and plunger controlled the maximum extent the plunger could be withdrawn in the barrel. This ensured that a reproducible amount of seawater was dispensed. The analytical procedure was as follows: An aliquot of seawater was dispensed into the titration vessel (a jacketed glass beaker with its temperature controlled to 0.02 C at about 20.0 C ), a stirrer bar added, and the temperature probe and burette tip inserted in the solution. The solution was then acidified to a pH of about 3.6 with a single aliquot of the titration acid, stirred vigorously, while bubbling CO2free air through for about 6min so as to remove CO2. The main titration was then started and the solution was titrated using 0.05 mL increments to a pH of about 3.0. Data from the pH range 3.53.0 were used in a non-linear least squares process that corrects for the reactions with sulfate and fluoride ions to estimate the total alkalinity of the samplesee Dickson et al. (2003) for more details. The equipment used for this is listed in Table 1. Table 1: Listing of equipment used for alkalinity titrations for A20120-cm3 glass syringe with custom frame to ensure reproducible dispensing250-cm3 capacity glass jacketed beakerThermostat bath (Fisher model 9110)Magnetic stirrer and stir barCalibrated thermometer 0.01 C for cell temperature (Guildline model 9540)Digital voltmeter (Kethley model 199)Custom high-impedance voltage-follower amplifierRoss-Orion combination pH electrode (model 1802)Calibrated thermometer 0.1 C for acid temperature (YSI model 4600)Metrohm Dosimat model 665 burette with calibrated 5 mL exchangeable burette unit, and anti-diffusion tipThe hydrochloric acid used for the titration was made up in bulk and then stored in 1L Pyrex bottles with greased ground-glass stoppers. The acid strength was approximately 0.100molkg1, and it was made up in a 0.6 molkg1 sodium chloride background so as to approximate the ionic strength of seawater. Selected bottles of the acid are then analyzed coulometrically (Dickson et al., 2003) to assign a concentration to the batch. Quality Control and Calibration of Reported Results The at-sea repeatability of the method was estimated by analyzing duplicate samples, collected on each cast. These results after rejecting pairs where one or both values were considered questionable were used to estimate a standard deviation using the standard expression (DOE, 1994 SOP 23). The repeatability was 0.91molkg1, based on 232 pairs of analyses. In addition, analyses were made of the alkalinity of CO2 reference material. These analyses were carried out regularly throughout the cruise, typically a pair of analyses for every station. The results are shown in Figure 1.  Figure 1. Plot of the results of analyses of reference materials (Batch 65: certified value = 2206.00 mol kg1 plotted as dashed line). Values depicted by open circles are considered outliers. An examination of Figure 1 suggests that there were meaningful changes in the system calibration during the course of the cruise. The data from the start of the first leg of the cruise up until station 57 (July 4th, 2004) appear to follow a quadratic pattern, however there are no comments in the laboratory notebook that suggest an explanation for this trend. The data from the rest of the first leg, for stations 58-108 (July 24th, 2004) are stable with an average value that is below the certified value for Batch 65. The second leg of the cruise also appears to be stable but with a somewhat higher average value. It seems appropriate to treat the data in Figure 1 as consisting of three groups: for stations 156 the CRM results can be represented by a quadratic expression in the station number N: , with a root mean square deviation of about 1.18 mol kg1 (114 data points); for stations 57108 by the average value ; and for stations 109190 by the average value . A decision was made to treat the cruise data as being in the same three groups, and to calibrate the reported data by adjusting the measured results so as to correct these CRM results to the certified value of 2206.00 mol kg1. The adjustment chosen was multiplicative (as would be expected if the deviation was indeed due to the dispensing system). Data for each station was thus multiplied by to correct for the observed calibration trends. Finally, the adjusted alkalinity data results were multiplied by a factor of 1.0002 to correct for the dilution inherent in adding mercury (II) chloride to the sample to preserve it for analysis. Once the at-sea alkalinity measurements had been adjusted in this fashion, they were salinity normalized to a salinity of 35 and the resulting values plotted in Ocean Data View (ODV) to help identify any questionable data. As a result of this analysis, 55 points were identified as either questionable or bad, and flagged accordingly. (Outliers found at this stage in replicate data were thus identified.) References Dickson, A. G., Afghan, J. D. & Anderson, G. C., 2003. Reference materials for oceanic CO2 analysis: A method for the certification of total alkalinity. Marine Chemistry 80, 185197. DOE, 1994. Handbook of methods for the analysis of the various parameters of the carbon dioxide system in sea water. Version 2, Dickson, A. G. & Goyet, C. (Eds.), ORNL/CDIAC-74. 189 pgs. PAGE  PAGE 3 "6 2 4 5 q w    Z [ K+-/0Z|~B jءhch!H*hiSh!5jh!UhM*bh!CJh8_h!H* hWh!hWh!H*hUh!H*hUh!5 hUh!hM*bh!CJH* h!CJ h!6hyh!H* h8_h!h!67>O^ x 7  $Ifgd!lxgd! & Fgd!gd!gd!gd!  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