Dissolving Carbonate Rocks

[Josh Perfetto]

Hi all,

I have a question I'm hoping some OAE folks on the list could help with. We have some HCl we wish to neutralize by dissolving carbonate rocks, with effluent discharge into the ocean. We want to do this as fast as possible, but without degassing CO2.

What conditions should we optimize for (e.g. maintaining a certain pH or DIC level)? Or does anyone have any pointers to papers that would be helpful in figuring this out?

Thanks for any tips,

-Josh

[Greg Rau]

The neutralization of a mineral acid with mineral carbonate (always) leads to CO2 emissions. Eg:

CaCO3 + 2HCl —-> CaCl2 + H2O + CO2

How about using silicate rocks for the neutralization?: https://pubs.acs.org/doi/abs/10.1021/es0701816

G

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On Jun 3, 2023, at 11:43 PM, Josh Perfetto <jo...@snowrise.com> wrote:



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[Dennis Amoroso]

Gentlemen,

     We at Advanced Materials Processing Inc. can take your acid, blend it with a mixture of rock powder and biomass, and turn it into a balanced fertilizer which is then a revenue stream and does not need to be a waste product.  Bacteria and fungi are both powerful means to change the chemistry and characteristics of many kinds of toxic waste.

We currently deliver our fertilizer to farmers in California, Colorado, Alberta, Chile, and Peru.

Let me know what you think!

Dennis Amoroso President and Chairman

To view this discussion on the web visit https://groups.google.com/d/msgid/CarbonDioxideRemoval/3280CA64-E2DE-4C63-A7A8-6F36F1AA98EF%40sbcglobal.net.

[Ken Caldeira]

Josh,

As Greg alludes, then the carbonate eventually reprecipitates (time scale ~ 4000 years), the CO2 will be released back to the atmosphere, but if you are concerned about the centennial time scale, then you want to add alkalinity and CO2 in a ratio that avoids crossing the pCO2 isolines in a direction from smaller to larger:

If you want to do more precise calculations for your conditions, there are a number of online calculators available, such as this one:

https://biocycle.atmos.colostate.edu/shiny/carbonate/

Best,

Ken

To view this discussion on the web visit https://groups.google.com/d/msgid/CarbonDioxideRemoval/CAPk76MWkLsRB0Pfy6xiE2vFbicEH4MDT3fy17FPcwnFTP8_wYA%40mail.gmail.com.

[Josh Perfetto]

Hi Greg and Ken,

I'm sorry I don't think I was clear enough in my question (or otherwise I am misunderstanding something big :) )

In the questioned situation, I have produced the HCl through an electrochemical process and already released the alkalinity to the ocean for OAE (lets just say HCl was extracted from the sea and NaOH returned). Now I am simply trying to get rid of this HCl without affecting alkalinity. I realize if I dissolve CaCO3 with HCl on land it will release CO2. So I am trying to do it in an aqueous solution, and retain the carbon as HCO3- as the rock dissolves, with direct release of the effluent into the ocean. In my view this would be the same outcome as in Greg's 2008 paper, just done differently. Is it not?

The reason I wanted to avoid CO2 temporarily degassing in the acidic dissolution environment was to avoid complications with re-equilibration. So I was trying to explore what conditions that would require (i.e. dissolve rock as fast as possible in order to minimize reactor size, minimize the water volume which must be passed through).

Greg - thanks for the suggestion and paper on silicates - I'm trying to explore everything that could possibly be done with HCl or Cl2. One thing I'm not clear on is if release of silica into the ocean would be viewed as a problem.

Dennis - thanks for your commercial offer, I'll follow up with you separately.

-Josh

[Tom Goreau]

Silica is an essential element for diatoms, and deficient in all surface waters except Antarctic waters in winter when there is no light for phytoplankton.

 

Thomas J. F. Goreau, PhD
President, Global Coral Reef Alliance

Chief Scientist, Blue Regeneration SL
President, Biorock Technology Inc.

Technical Advisor, Blue Guardians Programme, SIDS DOCK

37 Pleasant Street, Cambridge, MA 02139

gor...@globalcoral.org
www.globalcoral.org
Skype: tomgoreau
Tel: (1) 617-864-4226 (leave message)

 

Books:

Geotherapy: Innovative Methods of Soil Fertility Restoration, Carbon Sequestration, and Reversing CO2 Increase

http://www.crcpress.com/product/isbn/9781466595392

 

Innovative Methods of Marine Ecosystem Restoration

http://www.crcpress.com/product/isbn/9781466557734

 

No one can change the past, everybody can change the future

 

It’s much later than we think, especially if we don’t think

 

Those with their heads in the sand will see the light when global warming and sea level rise wash the beach away

 

Geotherapy: Regenerating ecosystem services to reverse climate change

 

 

 

From: <carbondiox...@googlegroups.com> on behalf of Josh Perfetto <jo...@snowrise.com>
Date: Sunday, June 4, 2023 at 7:14 PM
To: Ken Caldeira <kcal...@carnegiescience.edu>
Cc: Dennis Amoroso <dennis....@gmail.com>, Greg Rau <gh...@sbcglobal.net>, Carbon Dioxide Removal <carbondiox...@googlegroups.com>
Subject: Re: [CDR] Dissolving Carbonate Rocks

 

Hi Greg and Ken,

 

I'm sorry I don't think I was clear enough in my question (or otherwise I am misunderstanding something big :) )

 

In the questioned situation, I have produced the HCl through an electrochemical process and already released the alkalinity to the ocean for OAE (lets just say HCl was extracted from the sea and NaOH returned). Now I am simply trying to get rid of this HCl without affecting alkalinity. I realize if I dissolve CaCO3 with HCl on land it will release CO2. So I am trying to do it in an aqueous solution, and retain the carbon as HCO3- as the rock dissolves, with direct release of the effluent into the ocean. In my view this would be the same outcome as in Greg's 2008 paper, just done differently. Is it not?

 

The reason I wanted to avoid CO2 temporarily degassing in the acidic dissolution environment was to avoid complications with re-equilibration. So I was trying to explore what conditions that would require (i.e. dissolve rock as fast as possible in order to minimize reactor size, minimize the water volume which must be passed through).

 

Greg - thanks for the suggestion and paper on silicates - I'm trying to explore everything that could possibly be done with HCl or Cl2. One thing I'm not clear on is if release of silica into the ocean would be viewed as a problem.

 

Dennis - thanks for your commercial offer, I'll follow up with you separately.

 

-Josh

 

On Sun, Jun 4, 2023 at 10:25 AM Ken Caldeira <kcal...@carnegiescience.edu> wrote:

Josh,

As Greg alludes, then the carbonate eventually reprecipitates (time scale ~ 4000 years), the CO2 will be released back to the atmosphere, but if you are concerned about the centennial time scale, then you want to add alkalinity and CO2 in a ratio that avoids crossing the pCO2 isolines in a direction from smaller to larger:

To view this discussion on the web visit https://groups.google.com/d/msgid/CarbonDioxideRemoval/CA%2BL%3DET3dUwXn5Ow2bXaRwWSkEHhiedz-WJaJe4uWXQzz0BsWbw%40mail.gmail.com.

[Michael Hayes]

Josh, if you want to look at biotics, the HCL can likely be used to extract bio oil from microalgae:

https://bmcplantbiol.biomedcentral.com/articles/10.1186/s12870-018-1614-9

As this process needs to be confined, any CO2 outgassing can be monitored for, and any CO2 generated can be used in other biotic systems. I don't believe that there will be much outgassing, yet that needs to be demonstrated at the field level.

I'm setting up large thick walled HDPE tanks to test this biotic path, PM me if your want to get deeper into the tech.

Best

--

[Josh Perfetto]

Hi all,

A bunch of people wrote me privately asking why not use silicate rocks and why not sell HCl. Let me share my reasoning to ask you all to pick at this; I’m not trying to be right but to learn anything and everything wrong so I sincerely thank you for anything you point out about why this might not be a good idea or whatever else I should think about before I waste time executing it :)

I think it’s clear that alkalinity in the ocean can be generated by removing acidity. I realize there’s a market for HCl but I am thinking about the long-term where there is way more need for CDR than HCl.

I think it’s also energetically easier to generate dilute acidity than concentrated - but this makes the acidity more expensive to transport for neutralization. So I started to think it would be better to transport the (way more concentrated) rock to the site of ocean operations for dissolution, with effluent release into the ocean, than the other way around. Let's consider it a site of megaton removal alkalinity generation.

This leads to my concerns about silicates (and I am new at this so again please correct any mis-assumptions):

1. I’m worried Fe in silicates would cause massive ocean fertilization in this scenario, which is not agreed on as a good thing

2. Similarly I’m concerned that any trace metals would cause major concern in this scenario, given the concentrated point-source release of effluent

3. I’m unsure about the release of silica - Tom pointed out it would increase productivity, but I’m wondering if/when it would be too much of a good thing given the massive discharge envisioned here

In contrast, I think that carbonates would be more compatible with this scenario, as we’d just be increasing Ca2+ and DIC.

If I have this right, I think that 1 mol of CaCO3 can neutralize 1 mol of HCl, supporting the generation of 1 mol of alkalinity:

CaCO3 + 2HCl → Ca2+ + 2Cl- + H2CO3

but then:

CaCO3 + H2CO3 → Ca2+ + 2HCO3-

while silicates like MgSiO3 could neutralize 2 mol HCl per mol rock (other silicates less). So unfortunately more carbonate rock would need to be mined and transported than if silicates were dissolved. But my thinking is carbonates could enable this model, and happily they are already mined more.

Thoughts? Especially any concerns about the massive localized discharge of dissolved limestone?

-Josh

[Anton Alferness]

Josh - 

Another consideration (you ask at the end) is the size or volume of effluent release in any one area in a given time frame. My intuition says you would have marine biologists, environmentalists and some regulators displeased with the notion of releasing large amounts of mineral alkalinity effluent. Are you limited to a single location for outflow? Could you expand the release or in some way develop (clever/cheap or expensive/infrastructure) piping extensions? Could you employ some form of transport for some portion of the alkalinity for release? Can the amount of alkaline outflow be reduced to levels below harm thresholds or tested to prove out harm thresholds are higher than those opposing intuitively think? 

My intuition says single point large volume (maybe we need to define large...) is going to be viewed as problematic, so thinking through ways to increase spatial release and decrease concentration would be a good engineering exercise. And I think this would be regardless of what mineral you use. 

This issue of OAE dispersal area and volume in a given time frame is being worked on right now by multiple entities. Another person to maybe reach out to is Antonius Gagern at Additional Ventures as he is heading up a large effort to get answers to the remaining OAE questions so it can (presumably) scale. 

-Anton 

To view this discussion on the web visit https://groups.google.com/d/msgid/CarbonDioxideRemoval/CA%2BL%3DET1C1cZWVs%2B9M0RcHAxmcNCQbj2Dc9oM08tn09TRKRp-_g%40mail.gmail.com.

[Michael Tyka]

I think it’s clear that alkalinity in the ocean can be generated by removing acidity. I realize there’s a market for HCl but I am thinking about the long-term where there is way more need for CDR than HCl.

I totally agree that the market for dilute, seasalt-contaminated acid (from electrochemical seawater splitting) is not going to scale to large CDR, so this is only an option for very small operations.

 

This leads to my concerns about silicates (and I am new at this so again please correct any mis-assumptions):

Yes, one of the potential advantages of electrochemical OAE over just adding silicates directly to the ocean is that those co-disolution products don't end up in the ocean. Discharging the HCl-dissolved olivine into the sea defeats that. The effect of co-dissolving ions has been studied recently in a number of papers, e.g.: Bach et al, 2019, Ferderer et al, 2022, Guo et al. 2022

In that sense CaCO3 is an excellent source of alkalinity, as it tends to have many fewer exogenous contaminants (originating ultimately from sea itself).

However as previously noted, because it is a carbonate rock its co-dissolving bicarbonate has to be subtracted from the CO2 absorbtion capacity. Overall (inc. the electrochem) you can consider the process as:

CaCO3 + H2O → Ca2+ + CO2(g) + 2OH-

I.e. 2 mols of alkalinity, which affords 1.4-1.6 mols of CO2 uptake capacitiy (the ocean's mol/mol efficiency is ~0.7-0.8) but you also get 1 mol of CO2. So the net absorbtion of atmospheric CO2 per mol CaCO3 is only 0.4-0.6.

If I have this right, I think that 1 mol of CaCO3 can neutralize 1 mol of HCl, supporting the generation of 1 mol of alkalinity:

If you already have HCl and pure CaCO3 at hand, why not capture the CO2 first and significantly increase the overall CO2 capturing capacity (back to 1.4-1.6 mol CO2 per mol CaCO3):

CaCO3 + 2HCl → CaCl2(aq) + CO2(g) + H2O

(Now it's two mol HCl per mol CaCO3 and you're not releasing any bicarbonate to the ocean, only calcium chloride which is already abundant in the ocean).  Yes, you then need to dispose of the CO2 but my understanding is that underground disposal of pure CO2 is relatively cheap and storage durability is long and secure.

while silicates like MgSiO3 could neutralize 2 mol HCl per mol rock (other silicates less).

Olivine (Mg2SiO4) will neutralize 4mol of HCl per mol rock.

 

Anyone know what the worldwide abundance of CaCO3 deposits is, compared to mafic rocks (of which there are more than enough). Are those deposits in suitable, near-cost locations ?

Mike

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[Josh Perfetto]

HI Anton,

Yes certainly the alkalinity would need to be dispersed. However the alkalinity is in the base stream that was created alongside the HCl stream. That's a lower-volume stream, so it could be more easily dispersed using pipes or whatnot as you suggest.

The rock dissolution effluent stream would necessarily be a much higher volume stream because it needs to be below CaCO3 saturation and prevent its re-formation. So I was hoping to not have to dilute/disperse that stream beyond what was necessary to dissolve the rock, and thinking that that might be ok because this stream would just contain dissolved Ca+ and carbonates.

But I agree that there must be engineering and environmental limiting factors that would bound the maximum release per location. I'm just not sure what the environmental factors would be yet. Perhaps some contaminants in the rock?

Thanks for the pointer on Antonius and I'll reach out to him.

-Josh

[Josh Perfetto]

On Tue, Jun 6, 2023 at 9:25 AM Michael Tyka <mike...@gmail.com> wrote:

Yes, one of the potential advantages of electrochemical OAE over just adding silicates directly to the ocean is that those co-disolution products don't end up in the ocean. Discharging the HCl-dissolved olivine into the sea defeats that. The effect of co-dissolving ions has been studied recently in a number of papers, e.g.: Bach et al, 2019, Ferderer et al, 2022, Guo et al. 2022

In that sense CaCO3 is an excellent source of alkalinity, as it tends to have many fewer exogenous contaminants (originating ultimately from sea itself).

However as previously noted, because it is a carbonate rock its co-dissolving bicarbonate has to be subtracted from the CO2 absorbtion capacity. Overall (inc. the electrochem) you can consider the process as:

CaCO3 + H2O → Ca2+ + CO2(g) + 2OH-

I.e. 2 mols of alkalinity, which affords 1.4-1.6 mols of CO2 uptake capacitiy (the ocean's mol/mol efficiency is ~0.7-0.8) but you also get 1 mol of CO2. So the net absorbtion of atmospheric CO2 per mol CaCO3 is only 0.4-0.6.

I agree on the math and thanks for those excellent papers.

If you already have HCl and pure CaCO3 at hand, why not capture the CO2 first and significantly increase the overall CO2 capturing capacity (back to 1.4-1.6 mol CO2 per mol CaCO3):

CaCO3 + 2HCl → CaCl2(aq) + CO2(g) + H2O

(Now it's two mol HCl per mol CaCO3 and you're not releasing any bicarbonate to the ocean, only calcium chloride which is already abundant in the ocean).  Yes, you then need to dispose of the CO2 but my understanding is that underground disposal of pure CO2 is relatively cheap and storage durability is long and secure.

I was thinking about that but it complicates siting, as you now need not only upwelling, energy, and rock, but also geological storage. It's also not as free as it sounds, because as you point out it now needs 2 mol HCl per CaCO3, so now it needs twice the energy to get twice the amount of storage per mol rock compared to what we had before. So really we are just reducing rock requirements by half but introducing a whole geological storage component.

I was thinking that if you had upwelling, energy, and geological storage, it might be best to eliminate the rock part and just use the acid/base to degas CO2 from the sea and sequester that.

It's a tempting idea though and I could see it being ideal for sites where it worked once we're really talking megaton facilities.

-Josh

[Josh Perfetto]

On Tue, Jun 6, 2023 at 12:29 PM Josh Perfetto <jo...@snowrise.com> wrote:

If you already have HCl and pure CaCO3 at hand, why not capture the CO2 first and significantly increase the overall CO2 capturing capacity (back to 1.4-1.6 mol CO2 per mol CaCO3):

CaCO3 + 2HCl → CaCl2(aq) + CO2(g) + H2O

(Now it's two mol HCl per mol CaCO3 and you're not releasing any bicarbonate to the ocean, only calcium chloride which is already abundant in the ocean).  Yes, you then need to dispose of the CO2 but my understanding is that underground disposal of pure CO2 is relatively cheap and storage durability is long and secure.

I was thinking about that but it complicates siting, as you now need not only upwelling, energy, and rock, but also geological storage. It's also not as free as it sounds, because as you point out it now needs 2 mol HCl per CaCO3, so now it needs twice the energy to get twice the amount of storage per mol rock compared to what we had before. So really we are just reducing rock requirements by half but introducing a whole geological storage component.

I was thinking that if you had upwelling, energy, and geological storage, it might be best to eliminate the rock part and just use the acid/base to degas CO2 from the sea and sequester that.

It's a tempting idea though and I could see it being ideal for sites where it worked once we're really talking megaton facilities.

I'm sorry, I see your point now that it's more than twice.. That is very nice.

-Josh 

[Michael Tyka]

I was thinking about that but it complicates siting, as you now need not only upwelling,

Why do you need upwelling ? You can add alkalinity anywhere and you'll get CO2 uptake (or reduction in outgassing). Take a look at He at al. 2023 for spatial maps of limits and site-dependent CO2 uptake efficiency.

I was thinking that if you had upwelling, energy, and geological storage, it might be best to eliminate the rock part and just use the acid/base to degas CO2 from the sea and sequester that.

Well, the problem with any approach degassing CO2 from seawater is that DIC in seawater is just 2mM and so you need to process a great deal of seawater per tonne of CO2, which is expensive. The nice thing about OAE is that you can handle much more concentrated substances and thus much smaller volumes. If you degas CO2 from CaCO3, you likewise have a much more concentrated source of CO2.

 

[Bhaskar M V]

Josh

Ocean Fertilization is beneficial when it causes Diatom Algae to grow and it may or may not be beneficial when other types of algae grow / bloom.

You had asked the following:

"This leads to my concerns about silicates (and I am new at this so again please correct any mis-assumptions):
1. I’m worried Fe in silicates would cause massive ocean fertilization in this scenario, which is not agreed on as a good thing

2. Similarly I’m concerned that any trace metals would cause major concern in this scenario, given the concentrated point-source release of effluent

3. I’m unsure about the release of silica - Tom pointed out it would increase productivity, but I’m wondering if/when it would be too much of a good thing given the massive discharge envisioned here"

1. Fe is required to grow Diatoms, so this may be beneficial.

2. Diatoms also require more trace metals than other types of algae, so this too would be beneficial.

3. Only Diatoms require silica,  so silica will ensure that Diatoms grow and not other algae.  The max limit for Diatom production would depend on the zooplankton production and on depth of the ocean, etc. If most Diatoms are consumed by Zooplankton there would be no problems and if most of the Diatoms not consumed fall to ocean bed, it will help sequester carbon. Zooplankton and Fish too help sequester carbon.

Regards

Bhaskar

[Tom Goreau]

Bhaskar is right. Only diatoms benefit from silica, which they will completely consume, and diatoms are best for productive fisheries.

 

Promoting diatoms helps prevent harmful algae blooms (HABs) of dinoflagellates and cyanobacteria that release toxins causing mass fish and shellfish kills.

 

These are increasing in all coastal waters with excessive land-based nutrients from sewage and fertilizers.

 

Diatoms lead to rapid and effective biological carbon recycling, dinoflagellates and cyanobacteria lead to dead zones.

 

Many people miss the point that amorphous opaline silica is vastly more soluble than quartz or aluminosilicates, and there is plenty of it available, mostly of fossil biological origin.

 

Thomas J. F. Goreau, PhD
President, Global Coral Reef Alliance

Chief Scientist, Blue Regeneration SL
President, Biorock Technology Inc.

Technical Advisor, Blue Guardians Programme, SIDS DOCK

37 Pleasant Street, Cambridge, MA 02139

gor...@globalcoral.org
www.globalcoral.org
Skype: tomgoreau
Tel: (1) 617-864-4226 (leave message)

 

Books:

Geotherapy: Innovative Methods of Soil Fertility Restoration, Carbon Sequestration, and Reversing CO2 Increase

http://www.crcpress.com/product/isbn/9781466595392

 

Innovative Methods of Marine Ecosystem Restoration

http://www.crcpress.com/product/isbn/9781466557734

 

No one can change the past, everybody can change the future

 

It’s much later than we think, especially if we don’t think

 

Those with their heads in the sand will see the light when global warming and sea level rise wash the beach away

 

Geotherapy: Regenerating ecosystem services to reverse climate change

 

 

 

From: <carbondiox...@googlegroups.com> on behalf of Bhaskar M V <bhaska...@gmail.com>
Date: Wednesday, June 7, 2023 at 3:21 AM
To: Carbon Dioxide Removal <carbondiox...@googlegroups.com>
Subject: Re: [CDR] Dissolving Carbonate Rocks

 

Josh

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[Josh Perfetto]

Hi Michael,

Thank you for pointing out the storage benefit that would result from capturing the CO2, leading to decreased capital and energy costs per CO2 stored. I now think it wouldn't make sense to do this with carbonate rocks without capturing the CO2. I'm still reading through your paper, but I should have said something like "efficient and easier to verify alkalinity addition site" rather than upwelling.

My main concern though is the additional complexity geologic sequestration would bring to an already complex project, which I think would limit the ability to deploy and scale this in the near term. I mean I was already contemplating marine engineering, social license and governance issues with OAE, and complex MRV. And now there is a new type of geological storage :) Solid Carbon is one project attempting to demonstrate mineralization in seafloor basalts which I think would be very promising for this in the long-run. Saline aquifers might be a more similar technology, but to my knowledge no one has sequestered CO2 in one at sea yet.

I explored another idea earlier, to electrochemically generate slaked lime Ca(OH)2 from CaCO3 on land with CO2 sequestration, and then deploy that for ocean liming (or maybe sell for cement or other peoples' OAE projects too).

One thing I got hung up on was the existence of Heirloom Carbon - they do the same thing with an electric kiln, and then set it out on trays locally in an automated manner to absorb CO2 for DAC, and then do looping. I think you could also do a similar but larger loop using seawater to regenerate the CaCO3. Seabound is a company doing an even larger loop across a ship's voyage to capture exhaust emissions.

So this directly raises the question: if you have a way to calcine CaCO3 with CCS, is it better to do looping or consume rock for OAE?

-Josh

[Stefano Caserini]

 

@ Anyone know what the worldwide abundance of CaCO3 deposits is, compared to mafic rocks (of which there are more than enough). Are those deposits in suitable, near-cost locations ?

 

Here https://agupubs.onlinelibrary.wiley.com/doi/10.1029/2021GB007246, we made some evaluation on the availability and localizations of different raw materials suitable for ocean alkalinity enhancement, at different distances from the coastline.

Main conclusions:

• Pure carbonate potential resources are several trillion tons and are not a constraint for the development of global-scale OAE.
• A large part of pure limestone resources is located nearby the coastline, in area with no to low vegetation cover, mainly in North Africa and Iran
• The global limestone yearly production is similar to that of coal, thus the needed upscale is far lower than for olivine, magnesite and brucite

 

Best regards,

Stefano

 

 

 

 

Da: carbondiox...@googlegroups.com <carbondiox...@googlegroups.com> Per conto di Josh Perfetto
Inviato: martedì 6 giugno 2023 21:29
A: Michael Tyka <mike...@gmail.com>
Cc: Carbon Dioxide Removal <carbondiox...@googlegroups.com>
Oggetto: Re: [CDR] Dissolving Carbonate Rocks

To view this discussion on the web visit https://groups.google.com/d/msgid/CarbonDioxideRemoval/CA%2BL%3DET20HZbAYRgQN1xNZFiDTgoueHdDurTd9VVW32fAkopY-w%40mail.gmail.com.