Dear François,

You have not made me rest any easier.   Yes, there is a discussion about 
the ChromHD and brine samples in Morrison et al., but there is only 
discussion and no solution to the problem.

I am still concerned about recommending the TC/EA technique or ChromHD 
technology for delta H-2 measurements to those who analyze ground waters, 
saline waters, or brines containing ions whose salts have water of 
hydration.

Ty




Francois Fourel <[log in to unmask]> 
Sent by: Stable Isotope Geochemistry <[log in to unmask]>
02/20/2006 10:13 AM
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Re: Gas Bench hydrogen measurements






Hello Ty,
There is a discussion regarding ChromHD and brine samples in the paper 
we did with John Morrison:
"On-line high precision stable hydrogen isotopic analyses on nanoliter 
water samples - J. Morrison, T. Brockwell, T. Merren, F. Fourel and A.M. 
Phillips - Analytical Chemistry Vol 73, Number15, Pages 3570-3575".
I am not running brine samples here with my MultiPrep, but I remember 
from the numerous equilibration experiments we did with John, we 
sometimes had surprises with H2O-H2 equilibration reactions. If the 
water to equilibrate is not pure, the catalysts seem to be sometimes 
affected and the D/H numbers can become very erratic.
We even had the case once on waters extracted from plants where 
equilibration got us nowhere whereas EA-ChromHD on the same waters gave 
beautiful numbers.
Regards,



-- 
François FOUREL

UMR CNRS 5125 PEPS
Université Claude Bernard Lyon 1
2 rue Raphaël Dubois - Bât. Géode
F-69622 VILLEURBANNE Cedex - FRANCE

Tél : +33 (0) 4 72 44 62 42
FAX : +33 (0) 4 72 43 16 88
Email : [log in to unmask]


Tyler B Coplen a écrit :
> 
> Dear Paul and Wolfram,
> 
> I was not issuing a concern about memory due to sample carryover in the 
> syringe from one sample to the next, which has been discussed on 
> ISOGEOCHEM, nor about analysis of precipitation samples.
> 
> Rather, unless the proper precautions have been taken, I am concerned 
> about recommending the TC/EA technique or ChromHD technology for delta 
> H-2 measurements to those who analyze ground waters, saline waters, or 
> brines containing ions whose salts have water of hydration.  Luckily for 

> some laboratories, they never analyze such waters and this e-mail does 
> not apply to them.
> 
> Unfortunately, many of the most interesting waters in geochemistry and 
> geology are saline waters or brines composed of salts having waters of 
> hydration.  Some of these salts can be dehydrated.  Calcium sulfate 
> dihydrate (gypsum) dehydrates completely at 163 degrees C.  Calcium 
> chloride hexahydrate and magnesium sulfate septahydrate both dehydrate 
> completely at 200 degrees C.  But some salts with waters of hydration 
> are more problematic.  Magnesium chloride hexahydrate does not dehydrate 

> with increasing temperature.  Rather, it decomposes, giving off HCl at 
> 116 degrees C.
> 
> One can imagine that putting calcium/magnesium chloride/sulfate waters 
> into a reactor can provide the opportunity for large between-sample 
> memory unless all salt formed during flash evaporation of a sample is 
> maintained above its dehydration temperature.  The more samples that are 

> analyzed, the larger the memory.  What one would like to do is to 
> maintain the bottom of the septum and the injection volume at a 
> temperature greater than degrees C.  In this manner, only magnesium 
> chloride will be a problem and most other salts will be dehydrated. 
> 
> What I am wondering is how Willi and Giorgio tackle this problem.
> 
> I should mention that because we analyze such brines and saline waters, 
> we prefer dual-inlet Pt equilibration.
> 
> Ty
> 
> 
> 
> *Paul Brooks <[log in to unmask]>*
> Sent by: Stable Isotope Geochemistry <[log in to unmask]>
> 
> 02/17/2006 05:53 PM
> Please respond to
> Stable Isotope Geochemistry <[log in to unmask]>
> 
> 
> 
> To
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> cc
> 
> Subject
>                Re: syringe memory
> 
> 
> 
> 
> 
> 
> 
> 
> Ty,
> 
> We were able to eliminate the memory effect of syringe injection on an 
> H/Device by using a dry ethyl ether rinse between samples.  I think 
> since we started this others are now using alcohol or carbon 
> tetrachloride, but the principle is the same.  Rinsing the syringe with 
> a dry compound that is an azeotrope and injecting the waste to a modest 
> house vacuum dries the syringe completely.  We keep the ethyl ether in a 

> vial with a septa to stop it evaporating, then inject to a waste 
> position that is a septa with the house vacuum on the other side of the 
> septa.  Even as the syringe goes into the waste septa one sees the ethyl 

> ether blow out of the syringe even before the plunger comes down.
> 
> Having said that, the syringes we use gradually oxidize and have to be 
> replaced every 200 injections.  I have also only run a few sets of sea 
> water, but saw no memory effect going from the sea water to the 
> standards in fresh water.
> 
> I can provide more details if anyone is interested.  Paul Brooks
> 
> 
> 
> 
> At 09:35 AM 2/17/2006, you wrote:
> 
> Dear François,
> 
> With the ChromHD technology, how are you solving the between-sample 
> memory problem for brine and sea water samples?
> 
> Ty
> 
> *
> Francois Fourel <[log in to unmask]>*
> Sent by: Stable Isotope Geochemistry <[log in to unmask]>
> 
> 02/17/2006 03:33 AM
> 
> Please respond to
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> 
> 
> To
> 
> [log in to unmask]
> 
> cc
> Subject
> 
> Re: Gas Bench hydrogen measurements
> 
> 
> 
> 
> I'd like to add a few comments to Willi's email.
> As far as D/H is concerned I fully agree that continuus flow is now
> giving the best precision for water analyses. My experience is that a
> Eurovector EA with ChromHD technology generates D/H precisions better
> than 0.5permil which is better than what we get with our MultiPrep/DI
> system (usually 1permil). As far as 18O is concerned our experience here
> is that we get reproducibilities better than 0.05permil using CO2-H2O
> equilibration with our MultiPrep-DI system. For some applications going
> from 0.1 to 0.05 can make a significant difference.
> Another parameter to take into account when doing 18O with an EA is that
> as soon as you will mention the name "carbon monoxide", the health and
> safety officer of your university will be on your back. Depending on the
> legislations, there are almost always solutions, but CO2 equilibration
> is more "health and safety-friendly".
> Our experience in short is that for best isotopic determinations with
> waters we prefer D/H with an EA but 18O with DI equilibration.
> 
> Regards,
> 
> -- 
> François FOUREL
> 
> UMR CNRS 5125 PEPS
> Université Claude Bernard Lyon 1
> 2 rue Raphaël Dubois - Bât. Géode
> F-69622 VILLEURBANNE Cedex - FRANCE
> 
> Tél : +33 (0) 4 72 44 62 42
> FAX : +33 (0) 4 72 43 16 88
> Email : [log in to unmask]
> 
> Willi A. Brand a écrit :
>  > Hi,
>  > I just would like to comment to Anindya's remark that "/certainly 
TCEA
>  > cant be an alternative to more precise gas bench/".  The daily 
routine
>  > precision in our TC/EA is 0.5 per mill for D/H from water samples. We
>  > run more than 200  injections per day with a net of 30 samples, each 
of
>  > them injected 3 times. The other half of the injections is standards
>  > (the sequences are optimized for performance, not throughput; given 
the
>  > precision we could afford to inject each sample only once, increasing
>  > the net number of samples processed for D/H to 90 on a single mass
>  > spec). For 18O, precision is in general better than 0.1 per mill with
>  > fewer injections due to the longer elution time of the CO. With a 
single
>  > glassy carbon tube we have made more than 3000 injections.
>  > My conclusion: This is my method of choice for the times to come. It 
is 
>  > so much more convenient compared to all other techniques (I think I 
have
>  > tried them all) with zero compromise in precision.
>  > Willi
>  >
>  > Anindya Sarkar wrote:
>  >
>  >> Hi Penny
>  >> With a relatively new machine and gas bench we get typically 1.5 %o 
SD
>  >> that is the kind of SD one gets in dual inlet as well. But we have
>  >> been able to bring it down to even 1 %o level also. I hope u are 
using
>  >> a fixed volume of water (we use 500ul and our experiments show that 
if
>  >> you go below 200ul, values systematically change). we also bake the
>  >> column after say about every 100 samples. But ur problem it looks 
more
>  >> with platinum catalyst. The sticks supplied by thermo are not like
>  >> hokko beads but a thin coating. we have reused each for at least 10
>  >> analyses and yet got very good results. but we also noticed that 
from
>  >> some sticks coatings are peeling off. why not try with absolutely 
new
>  >> sticks and run several of ur lab standards and see the
>  >> reproducibility? as i understand TCEA will have more errors than gas
>  >> bench (~2%o) but we got ~3%o on limited analyses; possibility of 
water
>  >> evaporating in up part of furnace b4 it reacts. certainly TCEA cant 
be
>  >> an alternative to more precise gas bench.
>  >> 
---------------------------------------------------------------------
>  >> Anindya Sarkar
>  >> Associate Professor
>  >> National Facility of Stable Isotope Geochemistry
>  >> Department of Geology and Geophysics
>  >> Indian Institute of Technology
>  >> Kharagpur 721302
>  >> West Bengal, INDIA
>  >> Tel.: 0091-3222-283392 (O) 283393 (R) 220184 (R)
>  >>        Cell: 09434043377
>  >> Fax.: 0091-3222-282268
>  >> _http://anindya-sarkar.tripod.com_ <
http://anindya-sarkar.tripod.com/>
>  >> ------------------------------------------------------------------
>  >> ----- Original Message ----- From: "Penny Higgins"
>  >> <[log in to unmask]>
>  >> To: <[log in to unmask]>
>  >> Sent: Friday, February 17, 2006 3:57 AM
>  >> Subject: [ISOGEOCHEM] Gas Bench hydrogen measurements
>  >>
>  >>
>  >>> Hello Isotopers,
>  >>>
>  >>> We've been attempting to use our Gas Bench to do hydrogen analysis 
of
>  >>> waters using platinum catalysts and headspace equilibration at 
about
>  >>> 32degreesC. When we started, we got acceptable numbers with good
>  >>> within analysis (10 peaks) standard deviations. Values plotted
>  >>> sensibly along (or very near) the meteoric water line. As time went
>  >>> on, our standard deviations have gotten much worse (as much as 7
>  >>> permil) and our data very seldom plot reasonably close to the
>  >>> meteoric water line. Often, hydrogen data plot well above the
>  >>> meteoric water line. We have gotten great results from oxygen
>  >>> analyses of the same samples.
>  >>>
>  >>> We've just spent a great deal of time and effort to ensure that our
>  >>> sample gas is totally dry before it enters the mass spectrometer. I
>  >>> also let the catalysts sit in our oven (60degreesC) for two days
>  >>> before placing them into the vials with our water samples. We got
>  >>> better standard deviations for our analyses this time (between 2 
and
>  >>> 3), but still have unreasonable scatter around the meteoric water 
line.
>  >>>
>  >>> Questions:
>  >>>
>  >>> 1) What is a generally acceptable standard deviation for d2H from 
> water?
>  >>>
>  >>> 2) Could the problem be with our catalysts? I thought that, by
>  >>> definition, catalysts were reusable .. but maybe not. We've only 
done
>  >>> about 5 analyses with each catalyst.
>  >>>
>  >>> 3) Are we going to have this same problem when we start running
>  >>> waters using our TC/EA instead? or are we going to be happy that we
>  >>> made the change?
>  >>>
>  >>> If anyone out there in cyberspace has dealt with and corrected this
>  >>> problem, we would love to hear from you!
>  >>>
>  >>> Thanks,
>  >>>
>  >>> ~Penny
>  >>>
>  >>> *******************************************************************
>  >>>                       Dr. Pennilyn Higgins
>  >>>                        Research Associate
>  >>>
>  >>>                             "SIREAL"
>  >>>   Stable Isotope Ratios in the Environment Analytical Laboratory
>  >>>
>  >>>         Department of Earth and Environmental Sciences
>  >>>         University of Rochester
>  >>>         227 Hutchison Hall
>  >>>         Rochester, NY 14627
>  >>>
>  >>>                    [log in to unmask]
>  >>>
>  >>> Office: 209b Hutchison Hall               Lab: 209 Hutchison Hall
>  >>> Voice : (585) 275-0601              Outer lab: (585) 273-1405
>  >>> FAX   : (585) 244-5689              Inner lab: (585) 273-1397
>  >>>
>  >>>           _http://www.earth.rochester.edu/SIREAL/index.html_
>  >>> *******************************************************************
>  >>>
>  >>>
>  >>>
>  >>> --
>  >>> No virus found in this incoming message.
>  >>> Checked by AVG Anti-Virus.
>  >>> Version: 7.0.344 / Virus Database: 267.15.6/257 - Release Date:
>  >>> 2/10/2006
>  >>>
>  >>>
>  >>
>  >>
>  >
>  > --
>  > .....................................................................
>  > Willi A. Brand, Stable Isotope Laboratory      [log in to unmask]
>  > Max-Planck-Institute for Biogeochemistry (Beutenberg Campus)
>  > Hans-Knoell-Str. 10, 07745 Jena, Germany      Tel: +49-3641-576400
>  > P.O.Box 100164,      07701 Jena, Germany      Fax: +49-3641-577400
>  > _http://www.bgc-jena.mpg.de/_
>  > _http://www.bgc-jena.mpg.de/service/iso_gas_lab/_
>  > .....................................................................
>  > GASIR 2005 in Jena:
>  > 
_http://www.bgc-jena.mpg.de/service/iso_gas_lab/gasir2005/index.shtml_
>  > .....................................................................
>  >
> 
> -- 
> François FOUREL
> 
> UMR CNRS 5125 PEPS
> Université Claude Bernard Lyon 1
> 2 rue Raphaël Dubois - Bât. Géode
> F-69622 VILLEURBANNE Cedex - FRANCE
> 
> Tél : +33 (0) 4 72 44 62 42
> FAX : +33 (0) 4 72 43 16 88
> Email : [log in to unmask]
> 
> Center for Stable Isotope Biogeochemistry
> Valley Life Science Building Room 3060
> Integrative Biology - MC3140
> Berkeley CA-94720
> Phone: (510)-643-1748
> Fax: (510)-643-1748
> 

-- 
François FOUREL

UMR CNRS 5125 PEPS
Université Claude Bernard Lyon 1
2 rue Raphaël Dubois - Bât. Géode
F-69622 VILLEURBANNE Cedex - FRANCE

Tél : +33 (0) 4 72 44 62 42
FAX : +33 (0) 4 72 43 16 88
Email : [log in to unmask]