CO₂ adsorption behaviour on β-C₂S(111) and (100) surfaces: Implications for carbon sequestration in cementitious materials

Abstract

Understanding the differences in CO₂ adsorption in cementitious material is critical in mitigating the carbon footprint of the construction industry. This study chose the most common β-C₂S phase in the industry as the cementitious material, selecting the β-C₂S(111) and β-C₂S(100) surfaces for CO₂ adsorption. First-principles calculations were employed to systematically compare the CO₂ adsorption behaviors on both surfaces focusing on adsorption energy, adsorption configurations, and surface reconstruction. The comparison of CO₂ and H₂O adsorption behaviors on the β-C₂S(111) surface was also conducted to shed light on the influence of CO₂ on cement hydration. The adsorption energies of CO₂ on the β-C₂S(111) and β-C₂S(100) surfaces were determined as −0.647 and −0.423 eV, respectively, suggesting that CO₂ adsorption is more energetically favorable on the β-C₂S(111) surface than on the β-C₂S(100) surface. The adsorption energy of H₂O on the β-C₂S(111) surface was −1.588 eV, which is 0.941 eV more negative than that of CO₂, implying that β-C₂S tends to become hydrated before reacting with CO₂. Bader charges, charge density differences, and the partial density of states were applied to characterize the electronic properties of CO₂ and H₂O molecules and those of the surface atoms. The initial Ca/O sites on the β-C₂S(111) surface exhibited higher chemical reactivity due to the greater change in the average number of valence electrons in the CO₂ adsorption. Specifically, after CO₂ adsorption, the average number of valence electrons for both the Ca and O atoms increased by 0.002 on the β-C₂S(111) surface, while both decreased by 0.001 on the β-C₂S(100) surface. In addition, due to the lower valence electron number of O atoms, the chemical reactivity of O atoms on the β-C₂S(111) surface after H₂O adsorption was higher than the case of CO₂ adsorption, which favors the occurrence of further reactions. Overall, this work assessed the adsorption capacity of the β-C₂S surface for CO₂ molecules, offering a strong theoretical foundation for the design of novel cementitious materials for CO₂ capture and storage.

Keywords

CO₂ adsorption / cementitious materials / first-principles calculations / carbon sequestration

References

[1] WaheedR, ChangDF, SarwarS, ChenW. Forest, agriculture, renewable energy, and CO₂ emission. J. Cleaner Prod., 2018, 1724231.

[2] LiuDN, GuoXD, XiaoBW. What causes growth of global greenhouse gas emissions? Evidence from 40 countries. Sci. Total Environ., 2019, 661750.

[3] IwataH, OkadaK. Greenhouse gas emissions and the role of the Kyoto protocol. Environ. Econ. Policy Stud., 2014, 164325.

[4] FriedlingsteinP, O’sullivanM, JonesMW, et al.. Global carbon budget 2022. Earth Syst. Sci. Data, 2022, 14114811.

[5] LvY, MaYC, LiHY, DingYH, MengQ H, GuoJ. Analysis of spatiotemporal patterns of atmospheric CO₂ concentration in the Yellow River Basin over the past decade based on time-series remote sensing data. Environ. Sci. Pollut. Res., 2023, 30115745.

[6] QianCG, LiCQ, HuangP, et al.. Research progress of CO₂ capture and mineralization based on natural minerals. Int. J. Miner. Metall. Mater., 2024, 3161208.

[7] L. Cao, H. Zhang, M.D. Zheng, and S.J. Wang, Response of ocean acidification to a gradual increase and decrease of atmospheric CO₂, Environ. Res. Lett., 9(2014), No. 2, art. No. 024012.

[8] JoosF, SarmientoJL, SiegenthalerU. Estimates of the effect of Southern Ocean iron fertilization on atmospheric CO₂ concentrations. Nature, 1991, 3496312772.

[9] RehmanA, MaH, IrfanM, AhmadM. Does carbon dioxide, methane, nitrous oxide, and GHG emissions influence the agriculture? Evidence from China. Environ. Sci. Pollut. Res. Int., 2020, 272328768.

[10] MallRK, GuptaA, SonkarGLarrocheC, SanrománM, DuGC, PandeyA. Effect of climate change on agricultural crops. Current Developments in Biotechnology and Bioengineering, 2017, Amsterdam. Elsevier. 23.

[11] JacobsonTA, KlerJS, HernkeMT, BraunRK, MeyerKC, FunkWE. Direct human health risks of increased atmospheric carbon dioxide. Nat. Sustain., 2019, 28691.

[12] GiorginiP, Di GiosiaP, PetrarcaM, LattanzioF, StamerraCA, FerriC. Climate changes and human health: A review of the effect of environmental stressors on cardiovascular diseases across epidemiology and biological mechanisms. Curr. Pharm. Des., 2017, 23223247.

[13] S.A.F. Al-Arkawazi, Measuring the influences and impacts of signalized intersection delay reduction on the fuel consumption, operation cost and exhaust emissions, Civ. Eng. J., 4(2018), No. 3, art. No. 552.

[14] L.J.R. Nunes, The rising threat of atmospheric CO₂: A review on the causes, impacts, and mitigation strategies, Environments, 10(2023), No. 4, art. No. 66.

[15] X.H. Xu, C.C. Qi, X.M. Aretxabaleta, C.D. Ma, D. Spagnoli, and H. Manzano, The initial stages of cement hydration at the molecular level, Nat. Commun., 15(2024), No. 1, art. No. 2731.

[16] H. Takayabu, S. Kagawa, H. Fujii, S. Managi, and S. Eguchi, Impacts of productive efficiency improvement in the global metal industry on CO₂ emissions, J. Environ. Manage., 248(2019), art. No. 109261.

[17] Ürge-VorsatzD, HarveyLDD, MirasgedisS, LevineMD. Mitigating CO₂ emissions from energy use in the world’s buildings. Build. Res. Inf., 2007, 354379.

[18] SolaymaniS, VillamorG, DunninghamA, HallP. The relationship between energy and non-energy factors and CO₂ emissions in New Zealand. Environ. Sci. Pollut. Res., 2023, 3047104270.

[19] EllabbanO, Abu-RubH, BlaabjergF. Renewable energy resources: Current status, future prospects and their enabling technology. Renewable Sustainable Energy Rev., 2014, 39748.

[20] SmitB. Carbon capture and storage: Introductory lecture. Faraday Discuss., 2016, 1929.

[21] ArningK, Offermann-van HeekJ, LinzenichA, et al.. Same or different? Insights on public perception and acceptance of carbon capture and storage or utilization in Germany. Energy Policy, 2019, 125235.

[22] Y.C. Hu, L.Y. Xiong, Y. Yan, and G.Q. Geng, Performance of limestone calcined clay cement (LC3) incorporating low-grade marine clay, Case Stud. Constr. Mater., 20(2024), art. No. e03283.

[23] ZhangYJ, LiuZ, QinCX, TanTD. The direct and indirect CO₂ rebound effect for private cars in China. Energy Policy, 2017, 100149.

[24] TurnerK. “Rebound” effects from increased energy efficiency: A time to pause and reflect. Energy J., 2013, 34425.

[25] ErdemZB. The contribution of renewable resources in meeting Turkey’s energy-related challenges. Renewable Sustainable Energy Rev., 2010, 1492710.

[26] de LucenaAFP, SzkloAS, SchaefferR, et al.. The vulnerability of renewable energy to climate change in Brazil. Energy Policy, 2009, 373879.

[27] Nguyen-TienV, ElliottRJR, StroblEA. Hydropower generation, flood control and dam cascades: A national assessment for Vietnam. J. Hydrol., 2018, 560109.

[28] PiresJCM, MartinsFG, Alvim-FerrazMCM, SimõesM. Recent developments on carbon capture and storage: An overview. Chem. Eng. Res. Des., 2011, 8991446.

[29] MarkussonN, KernF, WatsonJ, et al.. A socio-technical framework for assessing the viability of carbon capture and storage technology. Technol. Forecast. Soc. Change, 2012, 795903.

[30] S.Y. Chen, J.F. Liu, Q. Zhang, F. Teng, and B.C. McLellan, A critical review on deployment planning and risk analysis of carbon capture, utilization, and storage (CCUS) toward carbon neutrality, Renewable Sustainable Energy Rev., 167(2022), art. No. 112537.

[31] D. Snoeck, Autogenous healing in 10-years aged cementitious composites using microfibers and superabsorbent polymers, Infrastructures, 7(2022), No. 10, art. No. 129.

[32] JangJ, KimG, KimH, LeeH. Review on recent advances in CO₂ utilization and sequestration technologies in cement-based materials. Constr. Build. Mater., 2016, 127762.

[33] ZhangQ, LiuB, XiaoK, EkbergC, ZhangSG. Preparation and hydration of industrial solid waste: Cement blends: A review. Int. J. Miner. Metall. Mater., 2022, 29122106.

[34] HasanbeigiA, PriceL, LinE. Emerging energy-efficiency and CO₂ emission-reduction technologies for cement and concrete production: A technical review. Renewable Sustainable Energy Rev., 2012, 1686220.

[35] MadloolNA, SaidurR, RahimNA, IslamMR, HossianMS. An exergy analysis for cement industries: An overview. Renewable Sustainable Energy Rev., 2012, 161921.

[36] LiuYK, WangYM, ChenQS. Using cemented paste backfill to tackle the phosphogypsum stockpile in China: A down-to-earth technology with new vitalities in pollutant retention and CO₂ abatement. Int. J. Miner. Metall. Mater., 2024, 3171480.

[37] BenhelalE, ZahediG, ShamsaeiE, BahadoriA. Global strategies and potentials to curb CO₂ emissions in cement industry. J. Cleaner Prod., 2013, 51142.

[38] OstovariH, MüllerL, SkocekJ, BardowA. From unavoidable CO₂ source to CO₂ sink? A cement industry based on CO₂ mineralization. Environ. Sci. Technol., 2021, 5585212.

[39] XiFM, DavisSJ, CiaisP, et al.. Substantial global carbon uptake by cement carbonation. Nat. Geosci., 2016, 912880.

[40] D.C. Wang, J.Z. Xiao, and Z.H. Duan, Strategies to accelerate CO₂ sequestration of cement-based materials and their application prospects, Constr. Build. Mater., 314(2022), art. No. 125646.

[41] J. Chang, T. Jiang, and K. Cui, Influence on compressive strength and CO₂ capture after accelerated carbonation of combination β-C₂S with γ-C₂S, Constr. Build. Mater., 312(2021), art. No. 125359.

[42] WangD, FangYF, ZhangYY, ChangJ. Changes in mineral composition, growth of calcite crystal, and promotion of physico-chemical properties induced by carbonation of β-C₂S. J. CO2 Util., 2019, 34149.

[43] J. Zhao, B.W. Huang, W. Gao, L.M. Zheng, P.Z. Song, and M.C. He, Periodic DFT study on heavy metals Cu(II) and Pb(II) atoms adsorption on Na-montmorillonite (010) edge surface, Solid State Commun., 366–367(2023), art. No. 115171.

[44] J. Lehtomäki, I. Makkonen, M.A. Caro, A. Harju, and O. Lopez-Acevedo, Orbital-free density functional theory implementation with the projector augmented-wave method, J. Chem. Phys., 141(2014), art. No. 234102.

[45] FanYH, ZhangJY, QiuYZ, ZhuJ, ZhangYF, HuGL. A DFT study of transition metal (Fe, Co, Ni, Cu, Ag, Au, Rh, Pd, Pt and Ir)-embedded monolayer MoS₂ for gas adsorption. Comput. Mater. Sci., 2017, 138255.

[46] Y.C. Chen, A. Sihag, R. Sarkar, et al., Hydrogen adsorption, migration and desorption on amorphous carbon: A DFT and AIMD study, Mater. Chem. Phys., 325(2024), art. No. 129711.

[47] IzadifarM, KönigerF, GerdesA, WöllC, ThissenP. Correlation between composition and mechanical properties of calcium silicate hydrates identified by infrared spectroscopy and density functional theory. J. Phys. Chem. C, 2019, 1231710868.

[48] JostKH, ZiemerB, SeydelR. Redetermination of the structure of β-dicalcium silicate. Acta Crystallogr., Sect. B: Struct. Sci., 1977, 3361696.

[49] V. Timón, D. Torrens-Martin, L.J. Fernández-Carrasco, and S. Martínez-Ramírez, Infrared and Raman vibrational modelling of β-C₂S and C₃S compounds, Cem. Concr. Res., 169(2023), art. No. 107162.

[50] Q.Q. Wang, H. Manzano, I. López-Arbeloa, and X.D. Shen, Water adsorption on the β-dicalcium silicate surface from DFT simulations, Minerals, 8(2018), No. 9, art. No. 386.

[51] ChiL, ZhangAL, QiuZD, et al.. Hydration activity, crystal structural, and electronic properties studies of Ba-doped dicalcium silicate. Nanotechnol. Rev., 2020, 911027.

[52] Y. Sun, X. Li, T. Iitaka, H.Y. Liu, and Y. Xie, Crystal structures and superconductivity of carbonaceous sulfur hydrides at pressures up to 300 GPa, Phys. Rev. B, 105(2022), No. 13, art. No. 134501.

[53] Y. Xie and P. Kent, Hybrid density functional study of structural and electronic properties of functionalized Ti_n+1X_n (X = C, N) monolayers, Phys. Rev. B, 87(2013), No. 23, art. No. 235441.

[54] S.P. Ramkumar and E.A. Nowadnick, Octahedral rotations in Ruddlesden-popper layered oxides under pressure from first principles, Phys. Rev. B, 104(2021), No. 14, art. No. 144105.

[55] QiCC, XuXH, ChenQS. Hydration reactivity difference between dicalcium silicate and tricalcium silicate revealed from structural and Bader charge analysis. Int. J. Miner. Metall. Mater., 2022, 292335.

[56] YangLF, MiWB, WangXC. Tailoring magnetism of black phosphorene doped with B, C, N, O, F, S and Se atom: A DFT calculation. J. Alloy. Compd., 2016, 662528.

[57] Y.F. Wang, M.J. He, W.H. He, Y. Niu, and Z.B. Lu, The influences of atom relaxation on the DFT-calculated friction properties of the h-BN/h-BN and Gr/Gr interfaces, Tribol. Int., 173(2022), art. No. 107586.

[58] VenerMV, EgorovaAN, ChurakovAV, TsirelsonVG. Intermolecular hydrogen bond energies in crystals evaluated using electron density properties: DFT computations with periodic boundary conditions. J. Comput. Chem., 2012, 33292303.

[59] C.C. Qi, D. Spagnoli, and A. Fourie, DFT-D study of single water adsorption on low-index surfaces of calcium silicate phases in cement, Appl. Surf. Sci., 518(2020), art. No. 146255.

[60] LiHS, WangSS, SawadaH, et al.. Atomic structure and dynamics of single platinum atom interactions with monolayer MoS₂. ACS Nano, 2017, 1133392.

[61] C.R. Wang, Y.H. Fang, H.M. Duan, et al., DFT study of CO₂ adsorption properties on pristine, vacancy and doped graphenes, Solid State Commun., 337(2021), art. No. 114436.

[62] C.C. Qi, L. Liu, J.Y. He, Q.S. Chen, L.J. Yu, and P.F. Liu, Understanding cement hydration of cemented paste backfill: DFT study of water adsorption on tricalcium silicate (111) surface, Minerals, 9(2019), No. 4, art. No. 202.

[63] RasiNM, PonnurangamS, MahinpeyN. First-principles investigations into the effect of oxygen vacancies on the enhanced reactivity of NiO via Bader charge and density of states analysis. Catal. Today, 2023, 407172.

[64] KosaM, MajorDT. Structural trends in hybrid perovskites [Me₂NH₂]M[HCOO]₃ (M = Mn, Fe, Co, Ni, Zn): Computational assessment based on Bader charge analysis. CrystEngComm, 2015, 172295.

[65] Carballo-CórdovaDA, Ochoa-LaraMT, Olive-MéndezSF, Espinosa-MagañaF. First-principles calculations and Bader analysis of oxygen-deficient induced magnetism in cubic BaTiO_3−x and SrTiO_3−x. Philos. Mag., 2019, 992181.

[66] BaderRFW. Atoms in molecules. Acc. Chem. Res., 1985, 1819.

[67] SaoudFS, PlenetJC, HeniniM. Band gap and partial density of states for ZnO: Under high pressure. J. Alloy. Compd., 2015, 619812.

[68] SinghaB, RayK. Density functional theory insights on photocatalytic ability of CuO/TiO₂ and CuO/ZnO. Mater. Today Proc., 2023, 72451.

[69] C.C. Qi, X.H. Xu, J. Chen, L. Guo, and Q.S. Chen, Ab initio calculations of CO₂ adsorption on β-C₂S(100) and M3-C₃S(001) surfaces: An exploration of early CO₂ sequestration pathways, Environ. Res., 215(2022), art. No. 114412.

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