Cited by 127CO2 Sequestration and Geologic InteractionsCarbon Dioxide Capture TechnologiesCarbon dioxide utilization in catalysis

Integration of CO 2 Capture and Mineral Carbonation by Using Recyclable Ammonium Salts

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Wang, Xiaolong, Maroto‐Valer, M. Mercedes·2011·ChemSusChem

Abstract

A new approach to capture and store CO 2 by mineral carbonation using recyclable ammonium salts was studied. This process integrates CO 2 capture with mineral carbonation by employing NH 3 , NH 4 HSO 4 , and NH 4 HCO 3 in the capture, mineral dissolution, and carbonation steps, respectively. NH 4 HSO 4 and NH 3 can then be regenerated by thermal decomposition of (NH 4 ) 2 SO 4 . The use of NH 4 HCO 3 as the source of CO 2 can avoid desorption and compression of CO 2 . The mass ratio of Mg/NH 4 HCO 3 /NH 3 is the key factor controlling carbonation and the optimum ratio of 1:4:2 gives a conversion of Mg ions to hydromagnesite of 95.5 %. Thermogravimetric analysis studies indicated that the regeneration efficiency of NH 4 HSO 4 and NH 3 in this process is 95 %. The mass balance of the process shows that about 2.63 tonnes of serpentine, 0.12 tonnes of NH 4 HSO 4 , 7.48 tonnes of NH 4 HCO 3 , and 0.04 tonnes of NH 3 are required to sequester 1 tonne of CO 2 as hydromagnesite.

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Crossref · 10.1002/cssc.201000441

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  • For selective leaching, ammonium salts have performed better than sulfuric acid.

    “For selective leaching, ammonium salts have performed better than sulfuric acid [39].”

    From Integrated Mineral Carbonation of Ultramafic Mine Deposits—A Review (2018) · cites this paper as [39]

    The Results and Discussion section reports selective dissolution with NH4HSO4: 91% of magnesium but only 17% of silicon dissolved from serpentine in one experiment. The Introduction reports 70% serpentine dissolution using sulfuric acid, but gives no comparable measure of selective leaching. The paper therefore supports the ammonium-salt part of the claim, not the asserted superiority over sulfuric acid. (LLM, conf=0.82)

    Experimental — accuracy not yet measured
  • Indirect processes can generally separate silica, magnesium/calcium carbonate and iron hydroxides with purities as high as 90% by switching pH from acidic to basic.

    “t has been shown that indirect processes are generally able to separate silica, magnesium/calcium carbonate and iron hydroxides with purities as high as 90% by switching the pH of the solution from acidic to basic.10,72,200,202”

    From A review of mineral carbonation technologies to sequester CO <sub>2</sub> (2014) · cites this paper as [72]

    The Experimental Section describes raising the pH of an acidic serpentine solution to remove impurities before magnesium carbonation, and the Mass balance section reports silica in the dissolution residue and iron in the residue or pH-swing precipitate. But the paper does not establish that indirect processes generally separate all the named products at 90% purity: it reports 80% pure hydromagnesite in Precipitation studies, no calcium-carbonate product, and a byproduct with at most 27.5 wt% iron in the Conclusions. Its approximately 90% figure for that experiment is carbonation efficiency, not product purity; page numbers are unavailable in our copy. (LLM, conf=0.90)

    Experimental — accuracy not yet measured
  • Precipitated hydromagnesite with purity >93 wt% can be produced by indirect processes.

    “Precipitated hydromagnesite (Mg 5 (CO 3 ) 4 (OH) 2 4H 2 O) with purity 493 wt% can be produced by indirect processes.72,163,201”

    From A review of mineral carbonation technologies to sequester CO <sub>2</sub> (2014) · cites this paper as [72]

    The Experimental Section describes an indirect process that extracts magnesium from serpentine and precipitates hydromagnesite. But Results and Discussion > Precipitation studies reports 80% purity for the measured product in experiment 7, not >93 wt%. The Conclusions calls the product “pure” without establishing the claimed threshold; the reported 95.9% is carbonation efficiency, not purity. Page numbers are unavailable in our copy. (LLM, conf=0.88)

    Experimental — accuracy not yet measured
  • The lowest liquid-to-solid ratio in an autoclave reactor is 2 kg kg−1.

    “Therefore, the lowest liquid-to-solid ratio in an autoclave reactor is 2 kg kg À1 , although the majority of aqueous carbonation experiments are carried out at a higher L/S-ratio to enhance the conversion efficiency.72”

    From A review of mineral carbonation technologies to sequester CO <sub>2</sub> (2014) · cites this paper as [72]

    The Introduction mentions a batch autoclave used in another study but gives no liquid-to-solid ratio. The Results and Discussion section reports a 1:2 mass ratio of Mg to NH4HCO3, which is not a liquid-to-solid ratio. Searches for “autoclave,” “liquid-to-solid,” and related terms found no statement that the lowest autoclave L/S ratio is 2 kg kg−1; page numbers were unavailable in our copy. (LLM, conf=0.76)

    Experimental — accuracy not yet measured
  • L/S-ratios lower than 2 cannot be stirred sufficiently in an autoclave reactor and may result in poor CO2 gas-liquid and solid-liquid mass transfer rates.

    “L/S-ratios lower than 2 cannot be stirred sufficiently in an autoclave reactor and may result in poor CO 2 gas-liquid and solid-liquid mass transfer rates.”

    From A review of mineral carbonation technologies to sequester CO <sub>2</sub> (2014) · cites this paper as [72]

    The Introduction (page unavailable) mentions a batch autoclave only when describing another study. The Results and Discussion section on carbonation ratios (page unavailable) examines Mg/NH4HCO3/NH3 ratios, not liquid-to-solid ratios. Searches for L/S ratios below 2, inadequate stirring, and gas–liquid or solid–liquid mass transfer found no passage addressing the claim. (LLM, conf=0.76)

    Experimental — accuracy not yet measured

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Cites

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Research works printed but not linked: 5

  1. [1]Working Group III of the Intergovernmental Panel on Climate Change Metz B Davidson HCdCO Loos M Meyer LA IPCC Special Report on Carbon Dioxide Capture and Storage 2005 Cambridge Cambridge University Press
  2. [8]Gerdemann SJ O’Connor WK Dahlin DC Penner LR Rush H Environ. Sci. Technol. 2007 41 2587 2593 17438820
  3. [13]Nduagu E Zevenhoven R 2010 Production of Magnesium Hydroxide from Magnesium Silicate for the Purpose of CO2 Mineralisation and Increasing Ocean Alkalinity: Effect of Reaction Parameters, in ACEME 10, Proceedings 31–40, Turku
  4. [14]Zevenhoven R Björklöf T Fagerlund J Romao I Highfield J Jie B 2011 Assessment & Improvement of a Stepwise Magnesium Silicate Carbonation Route via MgSO4 & Mg(OH)2, in ACEME 10, Proceedings 41–50, Turku
  5. [19]Zhang Y Li Z-z Li X Dong J-x Wang Y Smouse SM Ekmann JM 2003 Second Annual Conference on Carbon Sequestration, Alexandria, VA (USA)

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Authors
Wang, X., & Maroto‐Valer, M. M.
Affiliations
University of Nottingham (GB)
Corresponding author
Maroto‐Valer, M. Mercedes
Venue
ChemSusChem
Publisher
Wiley
Published
2011-07-05
Volume
4
Issue
9
Pages
1291-1300
ISSN
  • 1864-5631 (ISSN-L)
  • 1864-564X
OpenAlex
W2152712954
Cited by
127
References
0
Citations by year
2026: 8 · 2025: 12 · 2024: 5 · 2023: 10 · 2022: 12 · 2021: 6 · 2020: 8 · 2019: 4 · 2018: 12 · 2017: 4 · 2016: 10 · 2015: 8 · 2014: 15 · 2013: 10 · 2012: 3
FWCI
7.96
Type
journal article
Language
en
Open access
Locations
  • ChemSusChem (publishedVersion)
  • PubMed Central (publishedVersion, cc-by)
  • PubMed (publishedVersion)
Funders
Engineering and Physical Sciences Research Council (EP/F012098/1, grant EP/F012098/1)
Topics
  • Physical Sciences › Environmental Science › Environmental Engineering › CO2 Sequestration and Geologic Interactions
  • Physical Sciences › Engineering › Mechanical Engineering › Carbon Dioxide Capture Technologies
  • Physical Sciences › Chemical Engineering › Process Chemistry and Technology › Carbon dioxide utilization in catalysis
Keywords
CO2 capture, CO2 mineralization, ammonium salts, ammonium bisulfate, ammonium bicarbonate, ammonia regeneration, hydromagnesite, serpentine, thermal decomposition, CO2 sequestration, process integration
MeSH terms
Ammonia, Ammonium Sulfate, Carbon Dioxide, Carbonates, Hydrogen-Ion Concentration, Magnesium, Minerals, Chemical Precipitation, Temperature, Carbon Sequestration, Recycling

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