The DOI matches its Crossref record; 235 of the 235 references it cites were found in a registry or an index; 19 of the 94 sources its claims cite were checked for support.
Molecular-scale mechanisms of CO2 mineralization in nanoscale interfacial water films
Open accessAbstract
The calamitous impacts of unabated carbon emission from fossil-fuel-burning energy infrastructure call for accelerated development of large-scale CO 2 capture, utilization and storage technologies that are underpinned by a fundamental understanding of the chemical processes at a molecular level. In the subsurface, rocks rich in divalent metals can react with CO 2, permanently sequestering it in the form of stable metal carbonate minerals, with the CO 2-H 2 O composition of the post-injection pore fluid acting as a primary control variable. In this Review, we discuss mechanistic reaction pathways for aqueous-mediated carbonation with carbon mineralization occurring in nanoscale adsorbed water films. In the extreme of pores filled with a CO 2-dominant fluid, carbonation reactions are confined to angstrom to nanometre-thick water films coating mineral surfaces, which enable metal cation release, transport, nucleation and crystallization of metal carbonate minerals. Although seemingly counterintuitive, laboratory studies have demonstrated facile carbonation rates in these low-water environments, for which a better mechanistic understanding has come to light in recent years. The overarching objective of this Review is to delineate the unique underlying molecular-scale reaction mechanisms that govern CO 2 mineralization in these reactive and dynamic quasi-2D interfaces. We highlight the importance of understanding unique properties in thin water films, such as how water dielectric properties, and consequently ion solvation and hydration behaviour, can change under nanoconfinement. We conclude by identifying important frontiers for future work and opportunities to exploit these fundamental chemical insights for decarbonization technologies in the twenty-first century.
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Claims the paper makes
25 No full text of the sources · 25 Own interpretation · 18 No basis given · 9 Partly supported · 5 Not checked yet · 4 Sources not found · 3 Supported so far · 1 Supported · 1 Couldn’t confirm · accuracy not yet measured
The cited sources support only part of this claim — read each source’s verdict below.
In the paper
“Magnesite formation has been reported at only 25-35 °C and 90 bar 60 49 61 , compared to ~65 °C necessary for uncatalyzed formation in bulk water environments, a barrier attributed to notoriously sluggish Mg 2+ water exchange kinetics.49,62,63”
§ Molecular-Scale Mechanisms of CO 2 Mineralization in Nanoscale Interfacial Water Films > Humidified CO 2
What the sources say
- Not checked — no full text of the sourcecites [60] Qafoku, O. et al. Formation of submicron magnesite during reaction of natural forsterite in H2O-saturated supercritical CO2. Geochim. Cosmochim. Acta 134, 197–209 (2014). source
- Not checked — no full text of the sourcecites [49] Felmy, A. R. et al. Reaction of water-saturated supercritical CO2 with forsterite: evidence for magnesite formation at low temperatures. Geochim. Cosmochim. Acta 91, 271–282 (2012). source
- Partly supportedcites [61] Mergelsberg, S. T. et al. Low temperature and limited water activity reveal a pathway to magnesite via amorphous magnesium carbonate. Chem. Commun. 56, 12154–12157 (2020). This study expanded the temperature of abiotic magnesite precipitation in thin water films down to ambient temperature while hinting at amorphous carbonate phase stabilization in low water activity interfaces. sourceExperimental — accuracy not yet measured
The Figure 2 caption reports magnesite formation at 25 °C and 90 bar, and the introduction describes earlier formation at 35 °C in thin water films. The introduction says magnesite is rarely observed below 60 °C in aqueous solution, likely because of slow Mg²⁺ water exchange; it does not establish that ~65 °C is necessary for uncatalyzed formation in bulk water or give 90 bar for the 35 °C result. (LLM, conf=0.86)
plain- Asserted: passes — The authors put it forward as true.
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In the paper
“Conversely, the dissolution of quartz (SiO2), the structure of which is based entirely on Si-O-Si bridges, increases with increasing pH 117 because Si-O-Si bond breakage is facilitated by hydroxyls.118,119”
§ Molecular-Scale Mechanisms of CO 2 Mineralization in Nanoscale Interfacial Water Films > Humidified CO 2
What the sources say
- Not checked — no full text of the sourcecites [117] Palandri, J. L. & Kharaka, Y. K. A compilation of rate parameters of water–mineral interaction kinetics for application to geochemical modeling. DTIC https://apps.dtic.mil/docs/citations/ADA440035 (2004). source
- Not checked — no full text of the sourcecites [118] Dove, P. M. & Crerar, D. A. Kinetics of quartz dissolution in electrolyte solutions using a hydrothermal mixed flow reactor. Geochim. Cosmochim. Acta 54, 955–969 (1990). source
- Could not verifycites [119] Dove, P. M., Han, N. & Yoreo, J. J. D. Mechanisms of classical crystal growth theory explain quartz and silicate dissolution behavior. Proc. Natl Acad. Sci. USA 102, 15357–15362 (2005). sourceExperimental — accuracy not yet measured
The Methods report that the quartz experiments used input solutions at circumneutral pH, while the Results examine saturation state and added salts—not increasing pH. A separate passage says pH strongly controls silicate dissolution rates, but gives no direction for quartz. The hydroxyl-mediated bond-breakage explanation is attached to other citations in the citing sentence. (LLM, conf=0.74)
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The cited sources support only part of this claim — read each source’s verdict below.
In the paper
“Miller et al. 46,137 measured time-dependent forsterite to magnesite carbonation at different temperatures, and determined apparent activation energies of 34±7 kJ/mol at 100% RH and 83±17 kJ/mol at 85% RH, Figure 7.”
§ Molecular-Scale Mechanisms of CO 2 Mineralization in Nanoscale Interfacial Water Films > [H2] Surface Speciation and Proton Transfer
What the sources say
- Partly supportedcites [46] Miller, Q. R. S. et al. Anomalously low activation energy of nanoconfined MgCO3 precipitation. Chem. Commun. 55, 6835–6837 (2019). The first study to quantify carbonation kinetics in thin water films, and the temperature dependence of the reaction rate suggested that the nanoconfined Mg2+ hydration configuration is responsible for facile magnesite precipitation in thin water films relative to the bulk. sourceExperimental — accuracy not yet measured
The results section reports an apparent activation energy of 36±6 kJ/mol for magnesite precipitation in ~1 nm water films from 50–90 °C, using forsterite reacted with water-saturated CO₂. That supports the general measurement described, but not the quoted 34±7 kJ/mol value; our copy also does not report an 85% RH measurement or 83±17 kJ/mol. (LLM, conf=0.86)
- Supportedcites [137] Miller, Q. R. S. et al. Emerging investigator series: ion diffusivities in nanoconfined interfacial water films contribute to mineral carbonation thresholds. Environ. Sci. Nano 7, 1068–1081 (2020). This is the first study of carbonation activation energy as a function of water film thickness, in conjunction with molecular simulation, and revealed that ion diffusion controls carbonation reactivity thresholds. source
Section 3.3 reports apparent forsterite carbonation activation energies of 34±7 kJ/mol at 100% RH and 83±17 kJ/mol at 85% RH. Section 2.4 explains that these values were calculated from experimental rate constants. (LLM, conf=0.95)
plain- Asserted: passes — The authors put it forward as true.
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- Partly supported
The sources with a verdict support this claim; the rest weren’t checked yet, have no full text we could read, or their verdicts aren’t rated yet.
In the paper
“Forsterite dissolution increases monotonically with decreasing pH.111,112”
§ Molecular-Scale Mechanisms of CO 2 Mineralization in Nanoscale Interfacial Water Films > Humidified CO 2
What the sources say
- Not checked — no full text of the sourcecites [111] Rimstidt, J. D., Brantley, S. L. & Olsen, A. A. Systematic review of forsterite dissolution rate data. Geochim. Cosmochim. Acta 99, 159–178 (2012). source
- Supportedcites [112] Oelkers, E. H., Declercq, J., Saldi, G. D., Gislason, S. R. & Schott, J. Olivine dissolution rates: a critical review. Chem. Geol. 500, 1–19 (2018). source
Section 3.3 states that forsterite dissolution rates appear to decrease monotonically with increasing pH—the equivalent of increasing monotonically as pH decreases. The statement concerns the aqueous inorganic systems reviewed there. (LLM, conf=0.93)
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Every source the paper cites for this claim was checked and supports it.
In the paper
“For example, the ~67 kJ/mol reduction of the energy barrier is much larger than the ~16 kJ/mol 131 difference between the Mg 2+ and Ca 2+ transition energy barriers from solvent-separated to monodentate contact ion-pair states.”
§ Molecular-Scale Mechanisms of CO 2 Mineralization in Nanoscale Interfacial Water Films > [H2] Surface Speciation and Proton Transfer
What the sources say
- Supportedcites [131] Raiteri, P., Demichelis, R. & Gale, J. D. Thermodynamically consistent force field for molecular dynamics simulations of alkaline-earth carbonates and their aqueous speciation. J. Phys. Chem. C 119, 24447–24458 (2015). source
The Solution Properties of Individual Ions section (page unavailable) reports an approximately 25 kJ/mol barrier for Mg²⁺ between solvent-shared and contact ion-pair states, and a barrier below 8 kJ/mol for the other cations, including Ca²⁺. That supports the cited approximate Mg²⁺–Ca²⁺ difference; the ~67 kJ/mol reduction is the citing authors’ comparison, not a value attributed to this source. (LLM, conf=0.83)
plain- Asserted: passes — The authors put it forward as true.
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In the paper
“A salient investigation by Min et al. 202 revealed that interfacial silica-rich layers that form during dissolution in interfacial water films are different from those that repolymerize in a bulk aqueous environment.”
§ Molecular-Scale Mechanisms of CO 2 Mineralization in Nanoscale Interfacial Water Films > [H2] Surface Speciation and Proton Transfer
What the sources say
- Partly supportedcites [202] Min, Y., Li, Q., Voltolini, M., Kneafsey, T. & Jun, Y.-S. Wollastonite carbonation in water-bearing supercritical CO2: effects of particle size. Environ. Sci. Technol. 51, 13044–13053 (2017). sourceExperimental — accuracy not yet measured
The Environmental Implications section reports that silica layers formed in water-bearing supercritical CO₂ and aqueous solutions have different morphologies; the diffusion-barrier section also finds different porosities. The copy does not establish that the layers formed in bulk aqueous solution do so by repolymerization. (LLM, conf=0.82)
plain- Asserted: passes — The authors put it forward as true.
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The sources with a verdict support this claim; the rest weren’t checked yet, have no full text we could read, or their verdicts aren’t rated yet.
In the paper
“After the presence of amorphous carbonates were deduced from infrared spectroscopic and thermogravimetric-mass spectrometry [G] measurements, 50,53 Mergelsberg et al. 61 definitively showed that amorphous magnesium carbonate plays a key role in the nucleation and growth of carbonates in nanoscale water film, especially at low temperature.”
§ Molecular-Scale Mechanisms of CO 2 Mineralization in Nanoscale Interfacial Water Films > [H2] Amorphous Phase Stabilization
What the sources say
- Not checked — no full text of the sourcecites [50] Schaef, H. T. et al. Forsterite [Mg2SiO4)] carbonation in wet supercritical CO2: an in situ high-pressure X-ray diffraction study. Environ. Sci. Technol. 47, 174–181 (2013). source
- Not checked — no full text of the sourcecites [53] Miller, Q. R. S. et al. Insights into silicate carbonation processes in water-bearing supercritical CO2 fluids. Int. J. Greenh. Gas Control 15, 104–118 (2013). source
- Supportedcites [61] Mergelsberg, S. T. et al. Low temperature and limited water activity reveal a pathway to magnesite via amorphous magnesium carbonate. Chem. Commun. 56, 12154–12157 (2020). This study expanded the temperature of abiotic magnesite precipitation in thin water films down to ambient temperature while hinting at amorphous carbonate phase stabilization in low water activity interfaces. source
The paper reports that, at 25 °C, forsterite carbonated in thin water films to magnesite through an amorphous magnesium carbonate (AMC) precursor (Abstract; page not provided). It further reports that AMC grew for more than 120 hours before magnesite nucleated and subsequently transformed to magnesite (main text, section labeled “This journal is © The Royal Society of Chemistry 20xx”; page not provided). (LLM, conf=0.91)
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In the paper
“Compiled literature results for the dielectric permittivity constants of confined water as a function of pore size136- 140 .”
§ Molecular-Scale Mechanisms of CO 2 Mineralization in Nanoscale Interfacial Water Films > Chem. Commun. 55, 6835-6837 (2019).
What the sources say
- Not checked — no full text of the sourcecites [136] Faucher, S. et al. Critical knowledge gaps in mass transport through single-digit nanopores: a review and perspective. J. Phys. Chem. C 123, 21309–21326 (2019). source
- Partly supportedcites [137] Miller, Q. R. S. et al. Emerging investigator series: ion diffusivities in nanoconfined interfacial water films contribute to mineral carbonation thresholds. Environ. Sci. Nano 7, 1068–1081 (2020). This is the first study of carbonation activation energy as a function of water film thickness, in conjunction with molecular simulation, and revealed that ion diffusion controls carbonation reactivity thresholds. sourceExperimental — accuracy not yet measured
The Introduction states that interfacial water has a significantly lower dielectric constant than bulk water. It does not establish that permittivity decreases as pore size decreases or compile dielectric-permittivity results by pore size. (LLM, conf=0.83)
- Not checked — no full text of the sourcecites [138] Masoumi, S., Zare, S., Valipour, H. & Abdolhosseini Qomi, M. J. Effective interactions between calcium-silicate-hydrate nanolayers. J. Phys. Chem. C 123, 4755–4766 (2019). source
- Not checked — no full text of the sourcecites [139] Teschke, O., Ceotto, G. & de Souza, E. F. Interfacial water dielectric-permittivity-profile measurements using atomic force microscopy. Phys. Rev. E 64, 011605 (2001). source
- Supportedcites [140] Fumagalli, L. et al. Anomalously low dielectric constant of confined water. Science 360, 1339–1342 (2018). Validated predictions of significant dielectric constant decrease for interfacial water relative to bulk value. source
Page 3 reports that the measured out-of-plane dielectric constant decreases as the water-filled channel height decreases, approaching 2.1 below 2 nm. The paper therefore supports the size-dependent trend, specifically for water confined in slit-like channels. (LLM, conf=0.93)
plaindirect- Asserted: passes — The authors put it forward as true.
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In the paper
“As confined environments lead to amorphous phase stabilization [207][208][209][210][211] and accessing of unique crystallization pathways 212,213 , the roles of amorphous carbonates have potential to be more prominent in thin water film environments than in bulk aqueous conditions.”
§ Molecular-Scale Mechanisms of CO 2 Mineralization in Nanoscale Interfacial Water Films > [H2] Amorphous Phase Stabilization
What the sources say
- Not matchedcites [207][208][209][210][211]
Couldn’t be matched to a paper in Crossref, so it can’t be checked.
- Partly supportedcites [212] Anduix-Canto, C. et al. Effect of nanoscale confinement on the crystallization of potassium ferrocyanide. Cryst. Growth Des. 16, 5403–5411 (2016). sourceExperimental — accuracy not yet measured
The Introduction (p. 4) reports a crystallization pathway in confined pores that differs from bulk solution, supporting the point about distinct pathways. The Discussion (pp. 15–16) reports longer-lived metastable crystalline polymorphs and mentions amorphous calcium carbonate in other confinement studies, but this paper does not demonstrate stabilization of an amorphous carbonate phase. The statement about its potential role in thin water films is the citing authors’ inference, not a finding of this source. (LLM, conf=0.86)
- Not checked — no full text of the sourcecites [213] Sinnwell, M. A. et al. Molecular intermediate in the directed formation of a zeolitic metal–organic framework. J. Am. Chem. Soc. 142, 17598–17606 (2020). source
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The paper states this without a source or data behind it here, so there is nothing to check it against. The quote shows it is in the paper.
In the paper
“At higher temperatures and pressures, the carbonation significantly slows down due to the competitive serpentinization reactions that produce H2 and CH4.”
§ Molecular-Scale Mechanisms of CO 2 Mineralization in Nanoscale Interfacial Water Films > Humidified CO 2
plaindirect- Asserted: passes — The authors put it forward as true.
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- It may state two separate claims as one. 29
- Probably not a substantial claim. 13
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In the paper
“Although structurally and dimensionally highly-constrained, adsorbed water nanofilms can readily mediate the nucleation and growth of metastable intermediates, including nesquehonite (MgCO3•3H2O) 55 , hydromagnesite [Mg5(CO3)4(OH)2•4H2O] 50 , aragonite (CaCO3) 56 , and amorphous Mg/Ca carbonates, 53,57 as well as facilitate transformations of carbonate minerals, including dolomite [CaMg(CO3)2] rec”
§ Molecular-Scale Mechanisms of CO 2 Mineralization in Nanoscale Interfacial Water Films > Humidified CO 2
What the sources say
- Partly supportedcites [55] Miller, Q. R. S. et al. Tunable manipulation of mineral carbonation kinetics in nanoscale water films via citrate additives. Environ. Sci. Technol. 52, 7138–7148 (2018). sourceExperimental — accuracy not yet measured
Split into 2 atoms — 0 confirmed, 2 partially supported, 0 disputed, 0 misattributed, 0 unverifiable. Expand the claim to see per-atom verdicts.
- Not checked — no full text of the sourcecites [50] Schaef, H. T. et al. Forsterite [Mg2SiO4)] carbonation in wet supercritical CO2: an in situ high-pressure X-ray diffraction study. Environ. Sci. Technol. 47, 174–181 (2013). source
- Partly supportedcites [56] Chai, Y. E. et al. Pressurized in situ X-ray diffraction insights into super/subcritical carbonation reaction pathways of steelmaking slags and constituent silicate minerals. J. Supercrit. Fluids 171, 105191 (2021). sourceExperimental — accuracy not yet measured
Split into 2 atoms — 0 confirmed, 1 partially supported, 0 disputed, 0 misattributed, 1 unverifiable. Expand the claim to see per-atom verdicts.
plaindirect- Asserted: passes — The authors put it forward as true.
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It may state two separate claims as one.
- Partly supported
The sources with a verdict support this claim; the rest weren’t checked yet, have no full text we could read, or their verdicts aren’t rated yet.
In the paper
“Two years after injections, the Wallula pilot project and the Carbfix project have reported 60% (293 tonnes/year) 33 and between 72-95% (57-75 tonnes/year) 4,34 mineralization of injected CO2, respectively.”
§ Molecular-Scale Mechanisms of CO 2 Mineralization in Nanoscale Interfacial Water Films > [H1] Introduction and Motivation
What the sources say
- Supportedcites [33] Pogge von Strandmann, P. A. E. et al. Rapid CO2 mineralisation into calcite at the CarbFix storage site quantified using calcium isotopes. Nat. Commun. 10, 1983 (2019). source
The Results (‘The CarbFix site’) report that approximately 95% of injected carbon was mineralised within two years. The Discussion reports a 72 ± 5% estimate for CO2 precipitated into calcite and explains that the higher estimate comes from carbon tracers. The Wallula figure has a separate citation in the citing sentence and is not attributed to this source. (LLM, conf=0.91)
- Not checked — no full text of the sourcecites [4] Matter, J. M. et al. Rapid carbon mineralization for permanent disposal of anthropogenic carbon dioxide emissions. Science 352, 1312–1314 (2016). source
- Supportedcites [34] White, S. K. et al. Quantification of CO2 mineralization at the Wallula Basalt Pilot Project. Environ. Sci. Technol. 54, 14609–14616 (2020). source
The Abstract reports that modeling indicated approximately 60% of injected CO₂ at Wallula was mineralized within two years. The Carbfix percentage has separate citations in the citing sentence and is not attributed to this source. (LLM, conf=0.92)
plain- Asserted: passes — The authors put it forward as true.
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It may state two separate claims as one.
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In the paper
“Among various important nanoscale processes affecting carbon storage reservoirs 41,42 , reactivity hosted in thin water films have been demonstrated to alter geomechanical properties 43 and subsurface porosity 44 of reservoir rocks.”
§ Molecular-Scale Mechanisms of CO 2 Mineralization in Nanoscale Interfacial Water Films > [H2] CO 2 Mineralization in Water Films
What the sources say
- Supportedcites [41] Bourg, I. C., Beckingham, L. E. & DePaolo, D. J. The nanoscale basis of CO2 trapping for geologic storage. Environ. Sci. Technol. 49, 10265–10284 (2015). source
The Summary and Conclusions (page unavailable) state that long-term CO₂ storage depends on properties with a nanoscale basis, including properties of reservoir rocks. In the citing sentence, this source is cited for that broad background point; the specific claim about thin-water-film reactivity altering geomechanical properties and porosity is assigned to citations 43 and 44, not to this paper. (LLM, conf=0.91)
- Not checked — no full text of the sourcecites [42] Jun, Y.-S., Zhang, L., Min, Y. & Li, Q. Nanoscale chemical processes affecting storage capacities and seals during geologic CO2 sequestration. Acc. Chem. Res. 50, 1521–1529 (2017). source
- Not checked — no full text of the sourcecites [43] Choens, R. C. et al. Impacts on mechanical strength of chemical reactions induced by hydrous supercritical CO2 in Boise Sandstone. Int. J. Greenh. Gas Control 95, 102982 (2020). source
- Partly supportedcites [44] Rimmelé, G., Barlet-Gouédard, V. & Renard, F. Evolution of the petrophysical and mineralogical properties of two reservoir rocks under thermodynamic conditions relevant for CO2 geological storage at 3 km depth. Oil Gas. Sci. Technol. 65, 565–580 (2010). sourceExperimental — accuracy not yet measured
The Conclusions report increased porosity in both reservoir rocks after exposure to wet supercritical CO₂ or CO₂-saturated water, supporting the part attributed to citation 44. The paper does not identify reactivity in thin water films as the demonstrated mechanism; its experiments used those two fluid-exposure conditions. (LLM, conf=0.84)
boosteddirect- Asserted: passes — The authors put it forward as true.
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It may state two separate claims as one.
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In the paper
“This is consistent with the prospect of synergistic effects arising from carbonate anions that can catalyse the water exchange reaction around Mg 2+ in the solvent-separated ion-pair state.131”
§ Molecular-Scale Mechanisms of CO 2 Mineralization in Nanoscale Interfacial Water Films > [H2] Surface Speciation and Proton Transfer
What the sources say
- Partly supportedcites [131] Raiteri, P., Demichelis, R. & Gale, J. D. Thermodynamically consistent force field for molecular dynamics simulations of alkaline-earth carbonates and their aqueous speciation. J. Phys. Chem. C 119, 24447–24458 (2015). sourceExperimental — accuracy not yet measured
In “Solution Properties of Individual Ions” (page unavailable), the paper says water exchange around Mg²⁺ might be faster when Mg²⁺ is bound to carbonate, but reports no exchange during a 50 ns simulation. That possibility concerns carbonate-bound Mg²⁺, not the solvent-separated ion-pair state specified in the claim; the paper does not establish catalysis in that state. (LLM, conf=0.87)
hedgeddirect- Asserted: passes — The authors put it forward as true.
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Probably not a substantial claim. The paper’s conclusions may not depend on it.
- Partly supported
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In the paper
“Specifically, amorphous silica formed during wollastonite [CaSiO3] in wet scCO2 is not porous and was implicated as a diffusion barrier, contributing to fundamentally unique solute transport properties associated with thin water films.202”
§ Molecular-Scale Mechanisms of CO 2 Mineralization in Nanoscale Interfacial Water Films > [H2] Surface Speciation and Proton Transfer
What the sources say
- Partly supportedcites [202] Min, Y., Li, Q., Voltolini, M., Kneafsey, T. & Jun, Y.-S. Wollastonite carbonation in water-bearing supercritical CO2: effects of particle size. Environ. Sci. Technol. 51, 13044–13053 (2017). sourceExperimental — accuracy not yet measured
The section “Amorphous silica acts as a diffusion barrier for water-bearing scCO2” (page unavailable) describes the silica layer as low-porosity and says it can act as a diffusion barrier; it links the porosity difference to chemistry in thin water films. It does not say the layer is nonporous or establish fundamentally unique solute-transport properties. (LLM, conf=0.86)
hedgeddirect- Asserted: passes — The authors put it forward as true.
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It may state two separate claims as one.
- Partly supported
The paper states this without a source or data behind it here, so there is nothing to check it against. The quote shows it is in the paper.
In the paper
“As shown in Figure 3.b, the required reaction time to achieve 50% conversion (t50%) varies significantly and is optimized around 180 °C and 140 bar.”
§ Molecular-Scale Mechanisms of CO 2 Mineralization in Nanoscale Interfacial Water Films > Humidified CO 2
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The paper states this without a source or data behind it here, so there is nothing to check it against. The quote shows it is in the paper.
In the paper
“We also note that t50% in wet scCO2 at lower temperatures and pressures is relatively fast, signalling an enhanced reactivity.”
§ Molecular-Scale Mechanisms of CO 2 Mineralization in Nanoscale Interfacial Water Films > Humidified CO 2
plaindirect- Asserted: passes — The authors put it forward as true.
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In the paper
“At depths relevant to geologic storage the wet scCO2 phase is buoyant relative to H2O-rich fluids and thus will tend to displace formation water beneath the caprock and comprise a multiphase fluid at least for decadal time scales.[37][38][39]”
§ Molecular-Scale Mechanisms of CO 2 Mineralization in Nanoscale Interfacial Water Films > [H2] CO 2 Mineralization in Water Films
What the sources say
- Not matchedcites [37][38][39]
Couldn’t be matched to a paper in Crossref, so it can’t be checked.
plaindirect- Asserted: passes — The authors put it forward as true.
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- Not matched
The paper states this without a source or data behind it here, so there is nothing to check it against. The quote shows it is in the paper.
In the paper
“Surprising carbonation reactivity can occur in these quasi-2D thin water film environments, including the emergence of phases not typically observed during carbonation in bulk aqueous solution, or the emergence of phases at conditions different than those expected.”
§ Molecular-Scale Mechanisms of CO 2 Mineralization in Nanoscale Interfacial Water Films > Humidified CO 2
plainconditional- Asserted: passes — The authors put it forward as true.
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In the paper
“However, in practice water consumption and production plays an important role, particularly in low-water CO2-rich fluids, due to the potential involvement of water cycling via hydrous transient phases in the carbonation pathway.”
§ Molecular-Scale Mechanisms of CO 2 Mineralization in Nanoscale Interfacial Water Films > Humidified CO 2
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In the paper
“In the subsurface, rocks rich in divalent metals can react with CO2, permanently sequestering it in the form of stable metal carbonate minerals, with the CO2-H2O composition of the post-injection pore fluid acting as a primary control variable.”
§ Molecular-Scale Mechanisms of CO 2 Mineralization in Nanoscale Interfacial Water Films > Abstract
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In the paper
“Overall, the net water consumption in the reactions formulated by Equations (1-3) is zero, meaning water behaves akin to a catalyzer in the carbonation process.”
§ Molecular-Scale Mechanisms of CO 2 Mineralization in Nanoscale Interfacial Water Films > Humidified CO 2
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In the paper
“These pH-dependent speciation reactions favor carbonic acid and carbonate in acidic and basic conditions, respectively.”
§ Molecular-Scale Mechanisms of CO 2 Mineralization in Nanoscale Interfacial Water Films > Humidified CO 2
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In the paper
“Over time, the silicic acid can polymerize to form an amorphous secondary passivation layer that limits the reaction kinetics while producing water, Equation (3).”
§ Molecular-Scale Mechanisms of CO 2 Mineralization in Nanoscale Interfacial Water Films > Humidified CO 2
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In the paper
“These rapid mineralization reactions are particularly significant in light of the expectation that only Å-to nmthick (single-digit nm or less) interfacial water films 38,45,50,53,54 separate wet scCO2 from reactive surfaces, and serve as the principal medium for the needed dissolution-precipitation processes.”
§ Molecular-Scale Mechanisms of CO 2 Mineralization in Nanoscale Interfacial Water Films > Humidified CO 2
What the sources say
- Not checked — no full text of the sourcecites [38] Loring, J. S., Miller, Q. R. S., Thompson, C. J. & Schaef, H. T. in Science of Carbon Storage in Deep Saline Formations (eds Newell, P. & Ilgen, A. G.) 63–88 (Elsevier, 2019). source
- Not checked — no full text of the sourcecites [45] Loring, J. S. et al. In situ infrared spectroscopic study of forsterite carbonation in wet supercritical CO2. Environ. Sci. Technol. 45, 6204–6210 (2011). The first direct observation of reactive thin water film development on mineral surfaces exposed to wet scCO2. source
- Not checked — no full text of the sourcecites [50] Schaef, H. T. et al. Forsterite [Mg2SiO4)] carbonation in wet supercritical CO2: an in situ high-pressure X-ray diffraction study. Environ. Sci. Technol. 47, 174–181 (2013). source
- Not checked — no full text of the sourcecites [53] Miller, Q. R. S. et al. Insights into silicate carbonation processes in water-bearing supercritical CO2 fluids. Int. J. Greenh. Gas Control 15, 104–118 (2013). source
- Not checked — no full text of the sourcecites [54] Placencia-Gómez, E. et al. Critical water coverage during forsterite carbonation in thin water films: activating dissolution and mass transport. Environ. Sci. Technol. 54, 6888–6899 (2020). source
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In the paper
“Key uncertainties obtained from the generally unknown structure and distribution of the thin water film, which controls dielectric permittivity, viscosity and, in turn, surface speciation and charge, ion speciation and solubilities, pH, ion diffusivities, and percolation pathways.”
§ Molecular-Scale Mechanisms of CO 2 Mineralization in Nanoscale Interfacial Water Films > Humidified CO 2
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In the paper
“At a given temperature and pressure, the speciation depends strongly on pH, with carbonic acid dominant in acidic and carbonate in basic conditions.”
§ Molecular-Scale Mechanisms of CO 2 Mineralization in Nanoscale Interfacial Water Films > Humidified CO 2
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In the paper
“For forsterite carbonation this could imply more facile Mg 2+ dehydration or Mg-CO3 interfacial contact ion-pair formation in thin films, energetically akin to that of Ca 2+ ions.”
§ Molecular-Scale Mechanisms of CO 2 Mineralization in Nanoscale Interfacial Water Films > [H2] Surface Speciation and Proton Transfer
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A conclusion the paper draws from its own results — it cites no other source for it, so there is none to check. The quote shows it is in the paper.
In the paper
“On the one hand, adsorbed water molecules exhibit increased hydrogen bond strength, 143-145 hindered rotational degrees of freedom, 145,146 and decreased selfdiffusivity [147][148][149][150][151] , which entails a lower apparent viscosity and consequently slower reaction rates.”
§ Molecular-Scale Mechanisms of CO 2 Mineralization in Nanoscale Interfacial Water Films > Humidified CO 2
plaindirect- Asserted: passes — The authors put it forward as true.
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In the paper
“However, in classical nucleation theory adapted to heterogeneous pathways, nucleation preferentially occurs on the existing mineral surface(s) with an effective interfacial free energy (γ′) defined as 𝛾 ′ = 𝛾 𝑙𝑐 -(𝛾 𝑙𝑠 -𝛾 𝑠𝑐 )/2, where l, c and s subscripts respectively denote liquid, crystal, and surface (step 5).133”
§ Molecular-Scale Mechanisms of CO 2 Mineralization in Nanoscale Interfacial Water Films > Humidified CO 2
What the sources say
- Not checked — no full text of the sourcecites [133] Kashchiev, D. Nucleation (Butterworth-Heinemann, 2000). source
plaindirect- Asserted: passes — The authors put it forward as true.
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In the paper
“Because cation dehydration is an integral part of forming the cation-carbonate bonds that comprise metal carbonates, one can frame these observations in terms of relative affinities of the cations for inner-sphere waters of hydration.”
§ Molecular-Scale Mechanisms of CO 2 Mineralization in Nanoscale Interfacial Water Films > [H2] Surface Speciation and Proton Transfer
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In the paper
“The crystallization process nominally proceeds by monomer addition unless the extent of supersaturation favors nucleation and self-assembly of particles, so-called particle-mediated crystallization pathways.134”
§ Molecular-Scale Mechanisms of CO 2 Mineralization in Nanoscale Interfacial Water Films > Humidified CO 2
What the sources say
- Not checked — no full text of the sourcecites [134] Yoreo, J. J. D. et al. Crystallization by particle attachment in synthetic, biogenic, and geologic environments. Science 349, aaa6760 (2015). source
plainconditional- Asserted: passes — The authors put it forward as true.
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A conclusion the paper draws from its own results — it cites no other source for it, so there is none to check. The quote shows it is in the paper.
In the paper
“Conceptually, a reduced dielectric constant and less effective charge screening may also contribute.”
§ Molecular-Scale Mechanisms of CO 2 Mineralization in Nanoscale Interfacial Water Films > [H2] Surface Speciation and Proton Transfer
hedgedconditional- Asserted: passes — The authors put it forward as true.
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Probably not a substantial claim. The paper’s conclusions may not depend on it. The paper may give no reason why it holds. It may state two separate claims as one.
A conclusion the paper draws from its own results — it cites no other source for it, so there is none to check. The quote shows it is in the paper.
In the paper
“On the other hand, adsorbed water nanofilms confine reactants to a smaller volume and increase the collision frequency at the mineral-H2O-CO2 interface, conceptually capable of promoting increased surface reactivity.”
§ Molecular-Scale Mechanisms of CO 2 Mineralization in Nanoscale Interfacial Water Films > Humidified CO 2
hedgeddirect- Asserted: passes — The authors put it forward as true.
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Probably not a substantial claim. The paper’s conclusions may not depend on it. The paper may give no reason why it holds. It may state two separate claims as one.
None of the sources cited for this claim have been checked yet.
In the paper
“On the one hand, adsorbed water molecules exhibit increased hydrogen bond strength, 143-145 hindered rotational degrees of freedom, 145,146 and decreased selfdiffusivity [147][148][149][150][151] , which entails a lower apparent viscosity and consequently slower reaction rates.”
§ Molecular-Scale Mechanisms of CO 2 Mineralization in Nanoscale Interfacial Water Films > Humidified CO 2
What the sources say
- Not checked — no full text of the sourcecites [143] Musat, R. et al. Finite size effects on hydrogen bonds in confined water. Angew. Chem. Int. Ed. 47, 8033–8035 (2008). source
- Not checked — no full text of the sourcecites [144] Le Caër, S. et al. Time-resolved studies of water dynamics and proton transfer at the alumina−air interface. J. Am. Chem. Soc. 129, 11720–11729 (2007). source
- Not checked — no full text of the sourcecites [145] Caër, S. L. et al. A trapped water network in nanoporous material: the role of interfaces. Phys. Chem. Chem. Phys. 13, 17658–17666 (2011). source
- Not checked — no full text of the sourcecites [146] Bonnaud, P. A., Coasne, B. & Pellenq, R. J.-M. Molecular simulation of water confined in nanoporous silica. J. Phys. Condens. Matter 22, 284110 (2010). source
- Not matchedcites [147][148][149][150][151]
Couldn’t be matched to a paper in Crossref, so it can’t be checked.
plaindirect- Asserted: passes — The authors put it forward as true.
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A claim is checked only against the cited paper’s full text, never its abstract, and none is available for its sources.
In the paper
“At low water-coverages, complexes 47,48 and limited nano-precipitates 47 are the dominant manifestations of reactivity, whereas magnesite formation is promoted in the thin water film above 1.5 ML.”
§ Molecular-Scale Mechanisms of CO 2 Mineralization in Nanoscale Interfacial Water Films > [H2] Surface Speciation and Proton Transfer
What the sources say
- Not checked — no full text of the sourcecites [47] Miller, Q. R. S. et al. Surface-catalyzed oxygen exchange during mineral carbonation in nanoscale water films. J. Phys. Chem. C 123, 12871–12885 (2019). source
- Not checked — no full text of the sourcecites [48] Loring, J. S. et al. Evidence for carbonate surface complexation during forsterite carbonation in wet supercritical carbon dioxide. Langmuir 31, 7533–7543 (2015). source
plaindirect- Asserted: passes — The authors put it forward as true.
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A claim is checked only against the cited paper’s full text, never its abstract, and none is available for its sources.
In the paper
“Bulk equilibrium thermodynamic calculations and experimental data indicate that these polymorphs may transform to magnesite above 60 °C, 73 which involves drying-shrinkage and dissolution-precipitation solvent-mediated mechanisms. 74”
§ Molecular-Scale Mechanisms of CO 2 Mineralization in Nanoscale Interfacial Water Films > Humidified CO 2
What the sources say
- Not checked — no full text of the sourcecites [73] Chaka, A. M. & Felmy, A. R. Ab initio thermodynamic model for magnesium carbonates and hydrates. J. Phys. Chem. A 118, 7469–7488 (2014). source
- Not checked — no full text of the sourcecites [74] Hänchen, M., Prigiobbe, V., Baciocchi, R. & Mazzotti, M. Precipitation in the Mg-carbonate system — effects of temperature and CO2 pressure. Chem. Eng. Sci. 63, 1012–1028 (2008). source
hedgedconditional- Asserted: passes — The authors put it forward as true.
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A conclusion the paper draws from its own results — it cites no other source for it, so there is none to check. The quote shows it is in the paper.
In the paper
“Since CO2 is displaced from the surface, carbonic acid and bicarbonate form either with hydroxyl groups at the water-solid interface (Step 2a) or adsorbed water molecules and catalysed by the dissolved metal ions (Step 2b).”
§ Molecular-Scale Mechanisms of CO 2 Mineralization in Nanoscale Interfacial Water Films > Chem. Commun. 55, 6835-6837 (2019).
plaindirect- Asserted: passes — The authors put it forward as true.
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It may state two separate claims as one.
- Rests on an assumption: CO2 is displaced from the mineral surface when wet CO2 contacts it.
A claim is checked only against the cited paper’s full text, never its abstract, and none is available for its sources.
In the paper
“The importance of waterbearing CO2 for the stability and carbonation of steel, steel slag, cement, and fly ash is well etablished.153,239- 244”
§ Molecular-Scale Mechanisms of CO 2 Mineralization in Nanoscale Interfacial Water Films > [H2] Amorphous Phase Stabilization
What the sources say
- Not checked — no full text of the sourcecites [153] Regnault, O., Lagneau, V. & Schneider, H. Experimental measurement of portlandite carbonation kinetics with supercritical CO2. Chem. Geol. 265, 113–121 (2009). source
- Not checked — no full text of the sourcecites [239] Barlet-Gouédard, V., Rimmelé, G., Porcherie, O., Quisel, N. & Desroches, J. A solution against well cement degradation under CO2 geological storage environment. Int. J. Greenh. Gas Control 3, 206–216 (2009). source
- Not checked — no full text of the sourcecites [240] Barlet-Gouédard, V., Rimmelé, G., Goffé, B. & Porcherie, O. Well technologies for CO2 geological storage: CO2-resistant cement. Oil Gas. Sci. Technol. 62, 325–334 (2007). source
- Not checked — no full text of the sourcecites [241] Hua, Y., Barker, R. & Neville, A. Comparison of corrosion behaviour for X-65 carbon steel in supercritical CO2-saturated water and water-saturated/unsaturated supercritical CO2. J. Supercrit. Fluids 97, 224–237 (2015). source
- Not checked — no full text of the sourcecites [242] Kutchko, B. G., Strazisar, B. R., Dzombak, D. A., Lowry, G. V. & Thaulow, N. Degradation of well cement by CO2 under geologic sequestration conditions. Environ. Sci. Technol. 41, 4787–4792 (2007). source
- Not checked — no full text of the sourcecites [243] Rimmelé, G., Barlet-Gouédard, V., Porcherie, O., Goffé, B. & Brunet, F. Heterogeneous porosity distribution in Portland cement exposed to CO2-rich fluids. Cem. Concr. Res. 38, 1038–1048 (2008). source
- Not checked — no full text of the sourcecites [244] Santos, R. M. et al. Accelerated mineral carbonation of stainless steel slags for CO2 storage and waste valorization: effect of process parameters on geochemical properties. Int. J. Greenh. Gas Control 17, 32–45 (2013). source
boostedcorrelational- Asserted: passes — The authors put it forward as true.
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Probably not a substantial claim. The paper’s conclusions may not depend on it.
A conclusion the paper draws from its own results — it cites no other source for it, so there is none to check. The quote shows it is in the paper.
In the paper
“The carbonic acid and bicarbonate deprotonate to form carbonate anions that may chemisorb on the surface to produce a metal-carbonate surface complex (Step 2c).”
§ Molecular-Scale Mechanisms of CO 2 Mineralization in Nanoscale Interfacial Water Films > Chem. Commun. 55, 6835-6837 (2019).
hedgedconditional- Asserted: passes — The authors put it forward as true.
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A claim is checked only against the cited paper’s full text, never its abstract, and none is available for its sources.
In the paper
“The emergence of silica-rich 'leached layers' during metal silicate mineral dissolution in contact with bulk aqueous solution that can act as passivating layers is a well-known phenomenon, though debate continues regarding the deposition and polymerization mechanism.200,201”
§ Molecular-Scale Mechanisms of CO 2 Mineralization in Nanoscale Interfacial Water Films > [H2] Surface Speciation and Proton Transfer
What the sources say
- Not checked — no full text of the sourcecites [200] Hellmann, R. et al. Nanometre-scale evidence for interfacial dissolution–reprecipitation control of silicate glass corrosion. Nat. Mater. 14, 307–311 (2015). source
- Not checked — no full text of the sourcecites [201] Hellmann, R. et al. Unifying natural and laboratory chemical weathering with interfacial dissolution–reprecipitation: a study based on the nanometer-scale chemistry of fluid–silicate interfaces. Chem. Geol. 294–295, 203–216 (2012). source
boosteddirect- Asserted: passes — The authors put it forward as true.
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Probably not a substantial claim. The paper’s conclusions may not depend on it. It may state two separate claims as one.
In the paper
“These topics are pressing, given that different mineral facets can have distinct dissolution rates, hydrophilicities, and silicalayer development.[216][217][218][219][220]”
§ Molecular-Scale Mechanisms of CO 2 Mineralization in Nanoscale Interfacial Water Films > [H2] Amorphous Phase Stabilization
What the sources say
- Not matchedcites [216][217][218][219][220]
Couldn’t be matched to a paper in Crossref, so it can’t be checked.
plaincorrelational- Asserted: passes — The authors put it forward as true.
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- Not matched
In the paper
“That group also deduced that the temperature history of partial wollastonite carbonation influences the reaction extent of followup experiments.203”
§ Molecular-Scale Mechanisms of CO 2 Mineralization in Nanoscale Interfacial Water Films > [H2] Surface Speciation and Proton Transfer
What the sources say
- Not checked — no full text of the sourcecites [203] Min, Y. & Jun, Y.-S. Wollastonite carbonation in water-bearing supercritical CO2: effects of water saturation conditions, temperature, and pressure. Chem. Geol. 483, 239–246 (2018). source
plaindirect- Asserted: passes — The authors put it forward as true.
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Probably not a substantial claim. The paper’s conclusions may not depend on it.
A conclusion the paper draws from its own results — it cites no other source for it, so there is none to check. The quote shows it is in the paper.
In the paper
“Though seemingly counterintuitive, laboratory studies have demonstrated facile reactivity in thin water film environments, here exemplified in the context of carbonation processes of metal silicate minerals relevant to permanent safe storage of CO2.”
§ Molecular-Scale Mechanisms of CO 2 Mineralization in Nanoscale Interfacial Water Films > [H2] Amorphous Phase Stabilization
boosteddirect- Asserted: passes — The authors put it forward as true.
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Probably not a substantial claim. The paper may give no reason why it holds.
A conclusion the paper draws from its own results — it cites no other source for it, so there is none to check. The quote shows it is in the paper.
In the paper
“The dissolved ions and ion-pairs are transported diffusively through the adsorbed water nanofilm (Step 5) and reach nucleation and growth sites fueling a nanofilm-mediated monomer-by-monomer addition mechanism (Step 6).”
§ Molecular-Scale Mechanisms of CO 2 Mineralization in Nanoscale Interfacial Water Films > Chem. Commun. 55, 6835-6837 (2019).
plaindirect- Asserted: passes — The authors put it forward as true.
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A conclusion the paper draws from its own results — it cites no other source for it, so there is none to check. The quote shows it is in the paper.
In the paper
“The deportation process can involve a longrange proton transport to the surface that accelerates the dissolution process via a proton-promoted mechanism (Step 3a) and/or a ligand-enhanced dissolution (Step 3b) leveraging the produced carbonate anions in the process.”
§ Molecular-Scale Mechanisms of CO 2 Mineralization in Nanoscale Interfacial Water Films > Chem. Commun. 55, 6835-6837 (2019).
plaindirect- Asserted: passes — The authors put it forward as true.
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It may state two separate claims as one.
The authors state this as an assumption.
The water nanofilm adsorbed on forsterite has a pH of ~3-6.
“If a pH of ~3-6 is assumed for the water nanofilm adsorbed on forsterite 60,177 , the effective energy barrier to dissolution can be estimated to fall below 36 kJ/mol.”
The paper relies on this without support.
Mineral surfaces often tend to be hydrophilic.
“Notably, because mineral surfaces often tend to be hydrophilic, H2Obearing CO2 leads to the formation of nominally Å-to nm-scale adsorbed H2O that hosts CO2 dissolution and HxCO3(2-x)- formation.”
The paper relies on this without support.
The adsorbed water nanofilm is physiochemically distinct from bulk CO2-rich and H2O phases, with properties tied to surface properties and water activity of the CO2.
“This nanofilm is physiochemically distinct from bulk CO2-rich and H2O phases, with properties intimately tied to the surface properties and the water activity of the CO2.”
The paper relies on this without support.
CO2 is displaced from the mineral surface when wet CO2 contacts it.
“Since CO2 is displaced from the surface, carbonic acid and bicarbonate form either with hydroxyl groups at the water-solid interface (Step 2a) or adsorbed water molecules and catalysed by the dissolved metal ions (Step 2b).”
Citations
Cites
Items 201–235 of 235
Mergelsberg, S. T., Kerisit, S. N., Ilton, E. S., Qafoku, O., Thompson, C. J., & Loring, J. S. (2020) · Chemical Communications · doi:10.1039/d0cc04907g · Cited by 35
Thin Water Films at Multifaceted Hematite Particle Surfaces
Boily, J.-F., Yeşilbaş, M., Md. Musleh Uddin, M., Baiqing, L., Trushkina, Y., & Salazar-Alvarez, G. (2015) · Langmuir · doi:10.1021/acs.langmuir.5b03167 · Cited by 34
Early Stage Hydration of Wollastonite: Kinetic Aspects of the Metal-Proton Exchange Reaction
Giraudo, N., Krolla-Sidenstein, P., Bergdolt, S., Heinle, M., Gliemann, H., Messerschmidt, F., Brüner, P., & Thissen, P. (2015) · The Journal of Physical Chemistry C · doi:10.1021/acs.jpcc.5b02327 · Cited by 34
Confinement Effects on Carbon Dioxide Methanation: A Novel Mechanism for Abiotic Methane Formation
Le, T., Striolo, A., Turner, C. H., & Cole, D. R. (2017) · Scientific Reports · doi:10.1038/s41598-017-09445-1 · Cited by 33
Structural Basis for Metastability in Amorphous Calcium Barium Carbonate (ACBC)
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“This energy barrier, intricately related to interfacial energy and affinity, serves as a pivotal determinant governing both the quantity and attributes of resultant particles (Abdolhosseini Qomi et al. 2022; Wallace et al. 2013).”
InfluentialChemistry advances driving industrial carbon capture technologies
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Metadata
- Authors
- Abdolhosseini Qomi, M. J., Miller, Q. R. S., Zare, S., Schaef, H. T., Kaszuba, J. P., & Rosso, K. M.
- Affiliations
- Pacific Northwest National Laboratory (US)
- University of California, Irvine (US)
- University of Wyoming (US)
- Corresponding author
- Miller, Q. R. S.
- Venue
- Nature Reviews Chemistry
- Published
- 2022-08-30
- Volume
- 6
- Issue
- 9
- Pages
- 598-613
- ISSN
- 2397-3358 (ISSN-L)
- OpenAlex
- W4293567442
- Cited by
- 147
- References
- 234
- Citations by year
- 2026: 54 · 2025: 41 · 2024: 35 · 2023: 13 · 2022: 4
- FWCI
- 2.14
- Type
- journal article
- Language
- en
- Open access
- green
- www.osti.gov
- Locations
- Nature Reviews Chemistry (publishedVersion)
- PubMed (publishedVersion)
- OSTI OAI (U.S. Department of Energy Office of Scientific and Technical Information) (submittedVersion)
- Funders
- U.S. Department of Energy (DESC0022301)
- Office of Science
- University of California, Irvine
- Basic Energy Sciences (DE-SC0022301)
- Chemical Sciences, Geosciences, and Biosciences Division
- Pacific Northwest National Laboratory
- Topics
- Physical Sciences › Environmental Science › Environmental Engineering › CO2 Sequestration and Geologic Interactions
- Physical Sciences › Materials Science › Biomaterials › Calcium Carbonate Crystallization and Inhibition
- Physical Sciences › Engineering › Biomedical Engineering › Nanopore and Nanochannel Transport Studies
- Keywords
- CO2 mineralization, nanoconfinement, ion solvation, hydration, decarbonization
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