ࡱ>  npr#` bjbj 758****H+AF,,,,,-.-. @@@@@@@$Ch-Fd@ul4--l4l4@,,9A(7(7(7l4X8,,@(7l4@(7(799,+ Fhm,*4<9>OA0A9,F6 F9F9 ./(70}1...@@ 7...Al4l4l4l4 Simultaneous Underway Measurements of pH, fCO2, and TCO2 during CLIVAR P16N R/V Thomas G. Thompson, 3250TT191 13 February 30 March 2006 Papeete, Tahiti Honolulu, HI - Kodiak, AK, USA  Principal Investigator:Dr. Robert H. Byrne Email:  HYPERLINK "mailto:byrne@marine.usf.edu" byrne@marine.usf.edu Participants:Leg 1:Dr. Xuewu Sherwood Liu, Dr. Renate Bernstein Leg 2:Dr. Robert Byrne, Dr. Zhaohui Aleck Wang, Dr. Johan Schijf, Mr. Ryan Bell Institution:College of Marine Science, University of South Florida 140 7th Avenue South, St. Petersburg, FL 33701. Data Processing:Dr. Zhaohui Aleck Wang Email: awang@marine.usf.edu Summary The automated Multi-parameter Inorganic Carbon Analyzer (MICA) developed by the College of Marine Science at the University of South Florida was used to simultaneously measure underway surface seawater pH, fCO2, and TCO2 during the CLIVAR P16N cruise. The MICA data can be compared to measurements from the PMEL underway LiCOR pCO2 system (surface seawater fCO2) and discrete surface sampling (surface seawater pH and TCO2) to evaluate performance. Technical details and performance evaluation of the MICA system can be found in Wang et al. (2007). The system consists of three seawater channels (surface seawater fCO2, TCO2, and pH). All measurements (three channels) are made at constant temperature (25 C) and are based on similar spectrophotometric principles. The system operates autonomously with a sampling frequency of ~7 per hour. For each sample, all three parameters are measured and recorded simultaneously. The MICA system performed well during both legs of the P16N cruise. Its measurements agree well with conventional state-of-the-art measurements of carbon system parameters. The data are internally consistent based on thermodynamic calculations. Principle of Measurements 1. pH Spectrophotometric pH measurements are based on the method described in Clayton and Byrne (1993), but utilize thymol blue as the pH indicator (Zhang and Byrne, 1996; Wang et al., 2007). Thymol blue is directly injected into a stream of underway seawater and absorbances are monitored spectrophotometrically. Sample pH is linked to the absorbance ratio (R), dissociation constant (KI), and molar absorbance ratios (e1, e2, and e3) of the indicator with the following equation:  EMBED Equation.3 ,(1)where the subscript T denotes parameters expressed on the total hydrogen ion scale. The calibrated constants of thymol blue are given by Zhang and Byrne (1996) as:  EMBED Equation.3 ,(2)e1 = 0.00132 + 1.610-5T, e2 = 7.2326 0.0299717T + 4.610-5T2, and e3 = 0.0223 + 0.0003917T. (3)where T is absolute temperature in K, and S is salinity. 2. fCO2 For seawater fCO2 measurements, Teflon AF 2400 (DuPont) is used as both a CO2 permeable membrane and a liquid-core waveguide (LCW) (Wang et al., 2007). Phenol red is used as the indicator (Yao and Byrne, 2001). During each CO2 measurement, the indicator solution, composed of Na2CO3 with constant total alkalinity (TA), is motionless inside the LCW. The seawater samples are directed to flow outside the LCW. After CO2 molecules equilibrate by diffusion with the LCWs internal solution, the equilibrium pH is determined by measurements of absorbance ratios. fCO2 is then derived from the equilibrium pH with the following equation:  EMBED Equation.3 ,(4)where K0 is the Henrys Law constant, K1 and K2 are carbonic acid dissociation constants, and L = EMBED Equation.3 . Parameters a and b are derived through a calibration procedure using CO2 gases at known concentrations. The pH of the indicator solution is determined spectrophotometrically, and the L term in Equation 4 is then calculated. Since the TA of the internal solution is constant, sample fCO2 has a linear dependence on 1/L with a slope of a and an intercept of b. The calibration constants, a and b, account for all uncertainties in Equation 4 including the absolute value of TA. 3. TCO2 Spectrophotometric measurements of DIC using Teflon 2400 AF liquid core waveguides have been described by Byrne et al. (2002). Water samples are acidified before measurements (pH ( 2.7), whereupon the total  EMBED Equation.3 concentration equals the TCO2 concentration. After the internal Na2CO3 -indicator (bromcresol purple) solution attains CO2 equilibrium with the acidified water samples across the LCW CO2-permeable walls, the TCO2 of the outer solution can be written as:  EMBED Equation.3 (5) EMBED Equation.3 (6)where B is an experimentally derived constant determined via calibration of the TCO2 channel against CRM. The subscript ex refers to the acidified outer solution, i indicates the internal solution, and is ionic strength. Materials and Measurements 1. Reagents For each of the three indicators used, three wavelengths are chosen for measurement of absorbances. Two wavelengths assess the absorbance peaks of acid and base forms of the indicator, while a third wavelength serves as a reference wavelength. Absorbances vary at the acid and base wavelengths in response to pH changes, but not at the reference wavelength. Absorbance measurements at acid and base indicator maxima are used for determination of all CO2 system parameters. The wavelengths chosen for the three channels are listed in Table1. Table 1. Wavelengths used for spectrophotometric determination of inorganic carbon species.ChannelIndicatorAcid WavelengthBase WavelengthReference WavelengthSeawater fCO2 Phenol red434 nm558 nm700 nmTCO2Bromcresol purple432 nm589 nm700 nmpHThymol blue435 nm596 nm730 nmThe indicator solution for CO2 measurements consists of a solution of 2 M phenol red, 225 mol kg-1 total alkalinity (Na2CO3), and 0.2 M sodium lauryl sulfate. For TCO2 measurements, the indicator solution is made of 2 M bromcresol purple in 1000 mol kg-1 total alkalinity (Na2CO3) and 0.2 M sodium lauryl sulfate. The reference solutions of the CO2 and TCO2 measurements are similar solutions that contain no indicator. For pH measurements, the thymol blue stock solution is made in Milli-Q water with a concentration of 1.5 mM. The R ratio of thymol blue solution is adjusted (R~0.77) to minimize the magnitude of indicator-induced pH perturbations. All indicator and reference solutions are stored in gas-impermeable laminated bags. 3N HCl in Milli-Q water is stored in a 250 ml glass bottle and used to acidify TCO2 samples. 2. MICA system Three Ocean Optic 2000 spectrophotometers are used to determine indicator absorbances for each of the three measurement channels. The light assemblies, spectrophotometers, and optical cells are connected with optic fibers. The light assembly of each channel consists of a high-temperature tungsten lamp with blue and short-pass filters in order to achieve an improved balance of spectral intensity between 430 and 700 nm. The optical cells of the CO2 and DIC channels are custom-machined from PEEK rods. The PEEK optical cell has a 27 mm O.D. and a 2 mm I.D. with a length of 15 cm. A Teflon AF 2400 LCW is located inside this optical cell. The sample inlet and outlet, and two optical fibers that connect the optical cell with the light source and spectrophotometer, are inserted into the ends of the LCW with two custom-made PEEK connectors. The ends of the LCW are sealed with two O-rings that are housed inside the connectors. The PEEK connectors allow both reagent and light to pass through the LCW. The pH optical cell is machined from a PEEK rod, but does not require special connectors since no LCW is used. Indicator and reference solutions are pumped through separate lines into their respective channels by digital peristaltic pumps. Surface seawater is obtained continuously with a shipboard pumping system. It first flows through a SBE 49 CTD that records salinity and temperature, and is then pumped through three seawater channels (fCO2, TCO2, and pH). Before entering the TCO2 channel, seawater samples are acidified with ~3 N HCl using a digital peristaltic pump. The mixing ratio is approximately ~700 (seawater to HCl). An in-line coil is used to facilitate mixing. For pH measurement, thymol blue is mixed with seawater sample at a mixing ratio of ~700 (seawater to thymol blue), whereupon the final thymol blue concentration in the mixed sample is ~ 2 M. This low indicator concentration results in very small indicator-induced pH perturbations (< 0.001 pH units). An in-line mixing coil is also used in this case. All channels are thermostated in a Lauda E100 water bath that is set to 25 0.1C. All samples, reference and indicator solutions are temperature pre-equilibrated to 25 C in the water bath using PEEK and glass coils. All measurements, as well as calibrations, are taken at this temperature. All components of the system are connected to a custom-made electronic motherboard that is controlled by a PC. The interface program cycles to operate the MICA autonomously. The time required for each measurement cycle depends on the equilibration time (7 minutes for the seawater fCO2 and TCO2 channels) and flushing time selected for the indicator/reference solution and samples (~2 minutes). The equilibration time required for pH measurements is very short. The following sequence is used during a measurement cycle: Flush pH reference (seawater samples without indicator solution). Flush reference for seawater fCO2 and TCO2. Read and store reference readings. Flush indicator solutions for seawater fCO2 and TCO2; mix thymol blue with seawater samples (pH measurements); acidify TCO2 samples. Seawater fCO2 and TCO2 equilibration (7 minutes). Read and store measurements. Repeat Steps 4-6 five times. End of one measurement cycle and repeat from the beginning. 3. Standards and Calibration Prior to the cruise, the CO2 channel was calibrated against five standard CO2 gases ranging from 280 to 550 ppm (XCO2). TCO2 was also calibrated before the cruise using a Certified Reference Material (CRM). Thymol blue has been calibrated previously for seawater pH measurements (Zhang and Byrne, 1996). During the cruise, CO2 gas standards and CRM were used periodically to evaluate calibration consistency for CO2 and TCO2 measurements. Re-calibration was performed if necessary. Results 1. Precision The precisions of all measured parameters, estimated by replicate measurements at the concentration ranges encountered, are given as follows: pH 0.001Seawater fCO2 1 atmTCO2 1-3 mol/kg 2. Corrections The calibration for the CO2 channel is related to XCO2 readings of the standard CO2 gas tanks, even though it is fCO2 that drives equilibrium across the LCW membrane. Based on DOE (1994), XCO2, pCO2 and fCO2 can be calculated from each other at various measurement conditions (temperature, salinity, and pressure). The MICA seawater fCO2 measurements reflect fCO2 at 25C with 100% water vapor content. The fCO2 at 25 C was corrected to in-situ temperature to compare with PMEL LiCOR underway pCO2 measurements. The temperature correction used in this case is given by (Millero, 2007):  EMBED Equation.3 (7) No correction was required for the MICA TCO2 measurements since TCO2 is expressed in mol kg-1. The MICA pH measurements give pH values on the total scale at 25 C. The auxiliary salinity, temperature and pressure data used for these corrections and calculations were obtained from underway measurements using shipboard instruments. 3. Quality control Quality control analysis was performed in three steps. First, suspect data were removed, as necessary, following reported cruise log malfunctions (e.g. possible sample contamination and observed malfunction of the thermostat) and spectrophotometric anomalies (e.g., sudden decrease of baseline light signal indicating entrapment of air bubbles). Secondly, data points with deviations > 3 standard deviations (p < 0.01) from the running average of the data were removed. Finally, two of the three measured carbonate parameters (fCO2, TCO2, pH) were used to calculate the third parameter, which was compared with direct MICA measurements of the parameter. Suspect data were eliminated based on this internal consistency check. 4. Data Display Figures 1 and 2 show the longitudinal distribution of surface water fCO2, TCO2, and pH obtained with the MICA underway system. For comparison, pHT data calculated from fCO2 and TCO2 measurements (using the K1 and K2 constants of Mehrbach et al. (1973) refit by Dickson and Millero (1987)) were also plotted.  Figure 1. USF underway measurements of fCO2 (a), TCO2 (b), and pH (c) during the P16N Leg 1.  Figure 2. USF underway measurements of seawater fCO2 (a), TCO2 (b), and pH (c) during the P16N Leg 2. References Byrne, R. H.; Liu, X.; Kaltenbacher, E.; Sell, K. 2002. Spectrophotometric measurement of total inorganic carbon in aqueous solutions using a liquid core waveguide. Analytica Chimica Acta, 451, 221-229. Clayton, T.D., and R.H. Byrne. 1993. Spectrophotometric seawater pH measurements: Total hydrogen ion concentration scale calibration of m-cresol purple and at-sea results. Deep-Sea Res., 40: 2315-2329. Dickson, A.G. and F. Millero. 1987. A comparison of the equilibrium constants for the dissolution of carbonic acid in seawater media. DeepSea Research, 34, 17331743. DOE Handbook. 1994. 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G. Dickson & C. Goyet, eds. ORNL/CDIAC-74 Mehrbach, C. Cuberson, C.H., Hawley, J.E. and Pytkowicz, R.M. 1973. Measurement of the apparent dissociation constants of carbonic acid in seawater at atmospheric pressure. Limnol. Oceanogr., 18, 897-907. Wang, Z. A., Liu, X., Byrne, R. H., Wanninkhof, R. H., Bernstein, R. E., Kaltenbacher, E. A., Patten, J. 2007. Simultaneous spectrophotometric flow-through measurements of pH, carbon dioxide fugacity, and total inorganic carbon in seawater. Analytica Chimica Acta, 596: 23-36. Yao, W.; Byrne, R. H. 2001. Spectrophotometric determination of freshwater pH using bromocresol purple and phenol red. Environmental Science and Technology, 35, 1197-1201. Zhang, H.; Byrne, R. H. 1996. Spectrophotometric pH measurements of surface seawater at in-situ conditions: absorbance and protonation behavior of thymol blue. Mar. 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