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ORTHOPHOSPHATE AND DISSOLVED ORGANIC PHOSPHORUS

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     SUMMARY:  Seawater is collected from known depths using 
     CTD- rosette sampling protocols.  Subsamples are drawn and 
     stored in acid-washed polyethylene bottles.  Soluble 
     reactive phosphorus (SRP) is measured spectrophotometrically 
     following the formation of phosphomolybdic acid.  Total 
     dissolved phosphorus (TDP) is measured in a separate 
     sample after exposure to ultraviolet (UV) light and dissolved 
     organic phosphorus (DOP) is estimated by difference. 
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1.  Principle

    Phosphorus (P) is one of several macronutrients required for the 
growth of marine organisms.  In open ocean marine ecosystems, P is 
often present in low and, perhaps, limiting concentrations for 
microalgal and bacterial populations.  Therefore, P is a central 
element in oceanic biogeochemical cycles.

    In seawater, inorganic phosphorus (also referred to as 
orthophosphate or soluble reactive phosphorus, SRP) occurs chiefly 
as ions of HPO42-, with a small percentage present as PO43-.  
Dissolved organic phosphorus (DOP) exists in a variety of forms 
(primarily P-esters) which result from excretion, decomposition, 
death and autolysis.

    In this analytical procedure, we make direct measurements of 
SRP and total dissolved phosphorus (TDP).  The latter includes all 
organic and inorganic phosphorus compounds.  Bound phophorus is 
released from organic matter by ultraviolet light (UV) oxidation 
and the liberated orthophosphate is reacted with an acidified 
molydate reagent and potassium antimonyl tartrate.  The resulting 
compound, a heteropoly acid (phosphomolybdic acid), is reduced to 
the intensely colored molybdenum blue by ascorbic acid and measured 
spectrophotometrically.  SRP samples are prepared in the same manner 
as TDP samples, but without the prior UV oxidation step.  DOP is 
calculated by difference (i.e., TDP-SRP).


2.  Precautions

    Contamination is the primary concern with P determinations.  
This is particularly true with samples collected from the euphotic 
zone, where SRP concentrations are extremely low (<0.2 µM).  In 
order to avoid contamination, sample bottles must be meticulously 
cleaned with dilute HCl and rinsed with deionized distilled water 
(DDW) before use.  


3.  Sample Collection and Storage

3.1. Sample collection (also see "NOTE" in Chapter 7, section 3)

  3.1.1. Rinse the nutrient sample bottle (acid-washed, 125 ml 
         polyethylene bottle) 3 times before filling.  Fill to 
         approximately 2/3 full, tighten cap and freeze.

  3.1.2. Record cruise, cast and Niskin bottle number on the 
         bottle and data sheet.      


4.  Sample Analysis

    Currently, GOFS and WOCE nutrient samples collected during 
the Hawaii Ocean Time Series cruises are analyzed by the Hawaii 
Institute of Marine Biology Analytical Facility.  Mr. Ted Walsh has 
provided us with the following procedure for the analysis of phosphate.

    Phosphorus analyses are performed on a four-channel Technicon 
Autoanalyzer II continuous flow system.  The automated wet chemistries 
generally follow the standard methods of seawater analysis as given 
by Technicon (1973).  Slight modifications have been incorporated to 
achieve the optimum range and sensitivity for each nutrient at 
concentration levels specific for the Station ALOHA seawaters.

4.1. Soluble Reactive Phosphorus (SRP)

     This method employs a single color reagent consisting of an 
     acidified solution of ammonium molybdate, ascorbic acid and 
     antimony-tartrate.  The blue phosphomolybdenum complex formed 
     is read colorimetrically through a 50 mm pathlength flowcell 
     at 880 nm (Murphy and Riley, 1962).  The specific automated 
     method used is described in Technicon (1973) with the following 
     modifications:  
     sample pump tube size is increased to allow for a flow rate 
     of 0.8 ml min-1, and the color reagent 
     solution concentration is diluted by a factor of 2.

4.2. Total Dissolved Phosphorus (TDP)
              
     The method for TDP involves initial UV digestion of a seawater 
     sample followed by autoanalysis of the digestion product (SRP; 
     see Chapter 8, section 4.1).  The modified photoxidation technique 
     (Armstrong et al., 1966) utilizes a 2 hour UV irradiation period.  
     Exact details of the photoxidation unit are described in Walsh 
     (1989).  Periodic calibration checks of the UV lamp efficiency 
     are made using dissolved organic phosphorus (β-glycerol-
     phosphate) standards.  As a general rule, the UV lamp is replaced 
     after approximately 700-800 hr of use.

4.3. Low-level procedures

     We have recently developed a method for the determination of P 
     dissolved in seawater at low concentrations (<0.1 µM; Karl and 
     Tien, in preparation).  The method is based upon the quantitative 
     removal of SRP by co-precipitation with magnesium hydroxide which 
     is formed by the addition of high purity sodium hydroxide to 
     selected seawater samples.  The precipitate is collected by 
     centrifugation, washed with a solution of weak sodium hydroxide 
     (0.01 M) and then dissolved in a known volume of high purity 
     hydrochloric acid.  At this point, the concentrated samples are 
     treated as above (see Chapter 8, section 4.1) for the determination 
     of SRP.  The detection limit is determined by the volume of 
     seawater initially used (50-250 ml for our routine assays), but 
     P concentrations as low as 5 nM can be easily and reproducibly 
     detected.  All low level P determinations are corrected for 
     arsenic interference by thiosulfate reduction of dissolved 
     arsenate (Johnson, 1971).
 
 
5.  Calibration, Data Reduction and Calculations

5.1. Calibration stocks and regression standards

     The calibration of dissolved inorganic nutrients in the 
     autoanalysis of seawater samples is performed using standard 
     solutions containing N, P and Si.  A nutrient stock solution 
     is prepared by dissolving dried (65°C, 72 hours) analytical 
     grade reagent chemicals with distilled-deionized water in 1 
     liter glass volumetric flasks containing 1 ml of chloroform.  
     Once dissolved, this stock solution is immediately transferred 
     into 1 liter amber  polypropylene bottles and stored at 4°C.  
     The reagent chemicals and concentrations are:  phosphate (KH2PO4, 
     1 mM), nitrate (KNO3, 5 mM) and silica (Na2SiF6, 4 mM).  

     Working standards are prepared daily by volumetric dilutions 
     of the stock using glass pipettes and a plastic (polymethyl-
     pentene; PMP) volumetric flask.  All pipettes and PMP flasks 
     are acid-washed (1M HCl) and gravimetrically calibrated prior 
     to use.  The daily regression standards are prepared by diluting 
     the working standard with low nutrient natural seawater diluent  
     (SWDIL).  The SWDIL is filtered open ocean surface seawater that 
     is stored in a carboy at room temperature.  By using this technique 
     all standards are matrix-matched with the seawater samples and any 
     cross-nutrient interference effect should be accounted for.

     Cross-nutrient interference and reagent contamination was evaluated 
     by preparing separate solutions, as above, but with one of the three 
     standards omitted.  Only phosphate showed a slightly measurable 
     increase (+0.014 µM) in the presence of 40 µM-NO3 and 160 µM-Si.  
     The linear regressions of the standards were applied to all seawater 
     sample peaks for calculating each batch of cruise samples.  Typical 
     correlations produced r2 values that were between 0.9999 and 0.99999.

5.2. Blank corrections

     All seawater standard absorbance peaks were corrected for the 
     absorbance of the seawater diluent (SWDIL).  All seawater sample 
     peaks were corrected for the refractive index absorbance for each 
     unique nutrient detection system.  The refractive index corrections 
     (in apparent µM units) ranged from approximtely 0.13 (for P), 0.23 
     (for N) to 2.41 (for Si), and represent the increase in absorbance 
     that is due strictly to the presence of dissolved salts in seawater 
     when compared to the distilled-deionized water baseline.  These 
     corrections are made by running sampling seawater (35 o/oo salinity) 
     through the autoanalyzer with DDW only in reagent lines and also with 
     all reagents except the color producing reagent.  The Levor surfactant 
     used routinely in the phosphate channel was omitted from the DDW lines 
     during the refractive index measurement.


6.  Accuracy and Precision

    The detection limit for phosphorus is approximately 0.02 µM with a 
coefficient of variation for field-collected replicates of 0.3%  For DOP 
the detection limit is 0.02 µM with a coefficient of variation of 1%.


7.  Equipment/Supplies

    Niskin bottles and rosette/CTD unit
    acid-washed, 125 ml polyethylene sample bottles 
    Autoanalyzer (Technicon Corp.) and accessories


8.  Reagents

    glass distilled deionized water (DDW)
    HCl (1M) for cleaning
    concentrated H2SO4
    ultrapure NaOH and HCl for low-level P determinations
    Ammonium molybdate solution: Dissolve 40 g of ACS grade ammonium 
     paramolybdate [(NH4)6Mo7O24. 4H2O into 800 ml DDW and dilute 
     to 1 liter in a volumetric flask.  Store  in plastic bottle in
     the dark.  Solution is stable indefinitely.
    Ascorbic acid solution (Prepare fresh):  Dissolve 1.8 g of ACS 
     ascorbic acid into 100 ml DDW (1.8% wt/vol).
    Antimony potassium tartrate solution:  Dissolve 3.0 g of ACS 
     antimony potassium tartrate (C8H4K2O12Sb2 . 3H2O) into 800 ml 
     DDW and dilute to 1 liter in a volumetric flask.  Solution is 
     stable for several months.
    Mixed reagent (Prepare fresh):  Mix together in the following 
     order 15 ml ammonium molybdate, 50 ml 5 N sulfuric acid, 30 ml 
     1.8% ascorbic acid and 5 ml potassium antimony tartrate.
    Stock phosphate standard solution (1 mM):  Dissolve 0.1361 g of 
     dry (65°C for 72 hours) potassium phosphate monobasic (KH2PO4) 
     into 800 ml of DDW and dilute to 1 liter in a volumetric flask.  
     Store in a dark bottle with 1 ml of chloroform.
    Working phosphate standard (40 µM):  Dilute 4.0 ml of the stock 
     standard to 100 ml (use volumetric flask).  Then dilute the 
     working standard to prepare a series of standards to cover 
     a range of P concentrations.


9.  References

    Armstrong, F. A. J., P. M. Williams and J. D. H. Strickland.  1966.  
    Photo-oxidation of organic matter in seawater by ultraviolet radiation, 
    analytical and other applications. Nature, 211, 481-483.

    Grasshoff, K., M. Ehrhardt and K. Kremling.  1983.  Methods of Seawater 
    Analysis.  Verlag Chemie.

    Johnson, D. L.  1971.  Simultaneous determination of arsenate and 
    phosphate in natural waters.  Environmental Science and Technology, 
    5, 411-414.

    Murphy, J. and J. P. Riley.  1962.  A modified single solution 
    method for the determination of phosphate in natural waters.  
    Analytica Chimica Acta, 27, 30.

    Strickland, J. D. H. and T. R. Parsons.  1972.  A Practical 
    Handbook of Seawater Analysis.  Fisheries Research Board of Canada, 
    167.

    Technicon Industrial Systems.  1973.  Orthophosphate in water and 
    seawater.  Autoanalyzer IIR Industrial Method No. 155-71W.  W. 
    Tarrytown, New York 10591.

    Walsh, T. W.  1989.  Total dissolved nitrogen in seawater: A new 
    high temperature combustion method and a comparison to photo-
    oxidation.  Marine Chemistry, 26, 295-311.

    Walsh, T. W., R. E. Young and S. V. Smith.  Seawater nutrient 
    storage and analysis.  Manuscript.