Hi Jacob, high-pressure cryocrystallography methods may be useful in this case. 
I copied your question to Chae Un Kim here at MacCHESS and he forwards this 
suggestion:

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Hi Richard,

I think pressure cryocooling might be useful.

They may want to check the following reference.

JF Domsic et al (2008), Entrapment of carbon dioxide in the active site of 
carbonic anhydrase II, J. Biol. Chem. 283, 30766-30771

Best regards,
chaeun

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On Oct 2, 2011, at 6:22 PM, Roger Rowlett wrote:


You can't change the pKa of CO2, which is 6.3. Any attempt to grow bicarb 
complexes below pH 7.5 will be problematic due to CO2 bubble formation, which 
may crack the crystal. What we do in these situations is to soak crystals in a 
cryo solution at a higher pH for as long as practical, then transfer to 
another, identical solution with bicarbonate fo li and soak. This can be 
tricky, because crystals may take a long time to pH equilibrate, crack, or 
dissolve. At pH 7.5 or above, CO2 formation at chemical equilibrium is minimal. 
At low pH, you can also consider using acetate as a bicarbonate analog.

Roger Rowlett

On Oct 2, 2011 4:56 PM, "Jacob Keller" 
<j-kell...@fsm.northwestern.edu<mailto:j-kell...@fsm.northwestern.edu>> wrote:
> Dear Crystallographers,
>
> I would like to soak my crystals in bicarbonate (a possible
> substrate), but the crystals have grown--and only grow--in pH 5.2-6.0,
> so the bicarb/CO2 will just keep evolving out of the solution and
> reliquishing its hydroxyls until the pH is elevated sufficiently out
> of range. Does anyone have a clever way of getting bicarb into these
> crystals? Grow them under CO2? Transfer them to higher pH, and hope
> for the best?
>
> Jacob Keller

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