Abstract
Limestone calcined clay cement (LC3) is an environment-friendly and sustainable cementitious material. It has recently gained considerable attention for the stabilization/solidification (S/S) of soils contaminated by heavy metals. However, the existing studies on S/S of Zn-contaminated soils using LC3 in terms of hydraulic conductivity and microstructural properties as compared to ordinary Portland cement (OPC) are limited. This study focuses on the evaluation of the mechanical, leaching, and microstructural characteristics of Zn-contaminated soils treated with different contents (0%, 4%, 6%, 8%, and 10%) of low-carbon LC3. The engineering performance of the treated Zn-contaminated soils is assessed over time using unconfined compressive strength (UCS), hydraulic conductivity (k), toxicity characteristic leaching procedure (TCLP), and synthetic precipitation leaching procedure (SPLP) tests. Experimental results show that the UCS of Zn-contaminated soils treated with LC3 ranged from 1.47 to 2.49 MPa, which is higher than 1.63%–13.07% for those treated with OPC. The k of Zn-contaminated soils treated with LC3 ranged from 1.16×10−8 to 5.18×10−8 cm/s as compared to the OPC treated samples. For the leaching properties, the leached Zn from TCLP and SPLP is 1.58–321.10 mg/L and 0.52–284.65 mg/L as the LC3 contents ranged from 4% to 10%. Further, the corresponding pH modeling results indicate that LC3 promotes a relatively suitable dynamic equilibrium condition to immobilize the higher-level Zn contamination. In addition, microscopic analyses demonstrate that the formations of hydration products, i.e., Zn(OH)2, Zn2SiO4, calcium silicate hydrate (C–S–H), calcium silicate aluminate hydrate (C–A–S–H) gel, ettringite, and CaZn(SiO4)(H2O), are the primary mechanisms for the immobilization of Zn. This study also provides an empirical formula between the UCS and k to support the application of LC3-solidified Zn-contaminated soils in practical engineering in the field.
概要
目的
传统水泥材料普通硅酸盐水泥(OPC)处置总金属污染土面临高碳排及长期环境安全性的问题。本文旨在利用新型低碳探讨多尺度的形式获取新型绿色低碳固化剂石灰石煅烧粘土水泥(LC3)修复锌污染土的关键环境岩土工程参数,揭示LC3固化稳定化锌污染土的微观机理。
创新点
1. 探明LC3固化多浓度梯度Zn污染土的物理化学特性、力学强度和环境安全性特征规律;2. 揭示LC3固化土重金属固定及强度增长的关键机理。
方法
1. 通过无侧限抗压强度(UCS)和渗透试验,获取LC3固化多浓度梯度Zn污染土的力学参数发展规律(图3);2. 通过毒性特征浸出试验(TCLP)和合成沉降浸出试验(SPLP),得到LC3固化剂符合毒性浸出安全指标的浓度(图6);3. 采用X射线衍射(XRD)、扫描电子显微镜-能谱仪(SEM-EDS)等微观测试技术,明确LC3固化Zn污染土的微观机理(图7和8)。
结论
1. 证明了LC3替代OPC处理锌污染土壤的可行性;2. LC3和OPC固化污染土的UCS和渗透率k之间为负增长关系;3. LC3固化土壤中的锌离子及提高污染土强度的主要取决于水化产物的形成。
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References
Albino V, Cioffi R, Marroccoli M, et al., 1996. Potential application of ettringite generating systems for hazardous waste stabilization. Journal of Hazardous Materials, 51(1–3): 241–252. https://doi.org/10.1016/S0304-3894(96)01828-6
Avet F, Snellings R, Diaz AA, et al., 2016. Development of a new rapid, relevant and reliable (R3) test method to evaluate the pozzolanic reactivity of calcined kaolinitic clays. Cement and Concrete Research, 85:1–11. https://doi.org/10.1016/j.cemconres.2016.02.015
Bakera AT, Alexander MG, 2019. Use of metakaolin as supplementary cementitious material in concrete, with focus on durability properties. RILEM Technical Letters, 4:89–102. https://doi.org/10.21809/rilemtechlett.2019.94
Beaudoin J, Odler I, 2019. Hydration, setting and hardening of Portland cement. In: Hewlett PC, Liska M (Eds.), Lea’s Chemistry of Cement and Concrete, 5th Edition. Butterworth-Heinemann, Cambridge, UK, p.157–250. https://doi.org/10.1016/B978-0-08-100773-0.00005-8
Bucher R, Diederich P, Escadeillas G, et al., 2017. Service life of metakaolin-based concrete exposed to carbonation: comparison with blended cement containing fly ash, blast furnace slag and limestone filler. Cement and Concrete Research, 99:18–29. https://doi.org/10.1016/j.cemconres.2017.04.013
Buj I, Torras J, Rovira M, et al., 2010. Leaching behaviour of magnesium phosphate cements containing high quantities of heavy metals. Journal of Hazardous Materials, 175(1–3):789–794. https://doi.org/10.1016/johazmat2009.10.077
Capasso I, Lirer S, Flora A, et al., 2019. Reuse of mining waste as aggregates in fly ash-based geopolymers. Journal of Cleaner Production, 220:65–73. https://doi.org/10.1016/j.jclepro.2019.02.164
Chen J, Chen JZ, Tan MZ, et al., 2002. Soil degradation: a global problem endangering sustainable development. Journal of Geographical Sciences, 12(2):243–252. https://doi.org/10.1007/BF02837480
Chen L, Wang L, Cho DW, et al., 2019. Sustainable stabilization/solidification of municipal solid waste incinerator fly ash by incorporation of green materials. Journal of Cleaner Production, 222:335–343. https://doi.org/10.1016/j.jclepro.2019.03.057
Choi YC, Park B, 2020. Effects of high-temperature exposure on fractal dimension of fly-ash-based geopolymer composites. Journal of Materials Research and Technology, 9(4):7655–7668. https://doi.org/10.1016/jomrt2020.05.034
Cuisinier O, Le Borgne T, Deneele D, et al., 2011. Quantification of the effects of nitrates, phosphates and chlorides on soil stabilization with lime and cement. Engineering Geology, 117(3–4):229–235. https://doi.org/10.1016/j.enggeo.2010.11.002
de Andrade Lima LRP, Bernardez LA, 2013. Evaluation of the chemical stability of a landfilled primary lead smelting slag. Environmental Earth Sciences, 68(4):1033–1040. https://doi.org/10.1007/s12665-012-1805-x
Deng L, Shi Z, 2015. Synthesis and characterization of a novel Mg-Al hydrotalcite-loaded kaolin clay and its adsorption properties for phosphate in aqueous solution. Journal of Alloys and Compounds, 637:188–196. https://doi.org/10.1016/j.jallcom.2015.03.022
Dixit A, Du HJ, Pang SD, 2021. Performance of mortar incorporating calcined marine clays with varying kaolinite content. Journal of Cleaner Production, 282:124513. https://doi.org/10.1016/j.jclepro.2020.124513
Drissi S, Shi CJ, Li N, et al., 2021. Relationship between the composition and hydration-microstructure-mechanical properties of cement-metakaolin-limestone ternary system. Construction and Building Materials, 302:124175. https://doi.org/10.1016/j.conbuildmat.2021.124175
Du YJ, Jiang NJ, Liu SY, et al., 2014. Engineering properties and microstructural characteristics of cement-stabilized zinc-contaminated kaolin. Canadian Geotechnical Journal, 51(3):289–302. https://doi.org/10.1139/cgj-2013-0177
Elbltagy HM, Elbasiouny H, Almuhamady A, et al., 2021. Low cost and eco-friendly removal of toxic heavy metal from industrial wastewater. Egyptian Journal of Soil Science, 61(2):219–229. https://doi.org/10.21608/ejss.2021.75492.1444
Garcia-Lodeiro I, Palomo A, Fernández-Jiménez A, et al., 2011. Compatibility studies between N-A-S-H and C-A-S-H gels. Study in the ternary diagram Na2O–CaO–Al2O3–SiO2–H2O. Cement and Concrete Research, 41(9):923–931. https://doi.org/10.1016/j.cemconres.2011.05.006
Geng GQ, Myers RJ, Li JQ, et al., 2017. Aluminum-induced dreierketten chain cross-links increase the mechanical properties of nanocrystalline calcium aluminosilicate hydrate. Scientific Reports, 7:44032. https://doi.org/10.1038/srep44032
Gu YC, Li JL, Peng JK, et al., 2020. Immobilization of hazardous ferronickel slag treated using ternary limestone calcined clay cement. Construction and Building Materials, 250:118837. https://doi.org/10.1016/j.conbuildmat.2020.118837
Halim CE, Amal R, Beydoun D, et al., 2003. Evaluating the applicability of a modified toxicity characteristic leaching procedure (TCLP) for the classification of cementitious wastes containing lead and cadmium. Journal of Hazardous Materials, 103 (1–2): 125–140. https://doi.org/10.1016/S0304-3894(03)00245-0
Han RR, Zhou BH, Huang YY, et al., 2020. Bibliometric overview of research trends on heavy metal health risks and impacts in 1989–2018. Journal of Cleaner Production, 276:123249. https://doi.org/10.1016/j.jclepro.2020.123249
Hosan A, Shaikh FUA, 2021. Compressive strength development and durability properties of high volume slag and slag-fly ash blended concretes containing nano-CaCO3. Journal of Materials Research and Technology, 10:1310–1322. https://doi.org/10.1016/j.jmrt.2021.01.001
Huang X, Huang T, Li S, et al., 2016. Immobilization of chromite ore processing residue with alkali-activated blast furnace slag-based geopolymer. Ceramics International, 42(8):9538–9549. https://doi.org/10.1016/j.ceramint.2016.03.033
Kapeluszna E, Kotwica Ł, Röżycka A, et al., 2017. Incorporation of Al in C-A-S-H gels with various Ca/Si and Al/Si ratio: microstructural and structural characteristics with DTA/TG, XRD, FTIR and TEM analysis. Construction and Building Materials, 155:643–653. https://doi.org/10.1016/j.conbuildmat.2017.08.091
Khalid S, Shahid M, Niazi NK, et al., 2017. A comparison of technologies for remediation of heavy metal contaminated soils. Journal of Geochemical Exploration, 182:247–268. https://doi.org/10.1016/j.gexplo.2016.11.021
Kogbara RB, Al-Tabbaa A, Yi YL, et al., 2012. pH-dependent leaching behaviour and other performance properties of cement-treated mixed contaminated soil. Journal of Environmental Sciences, 24(9):1630–1638. https://doi.org/10.1016/S1001-0742(11)60991-1
Kua TA, Arulrajah A, Horpibulsuk S, et al., 2016. Strength assessment of spent coffee grounds-geopolymer cement utilizing slag and fly ash precursors. Construction and Building Materials, 115:565–575. https://doi.org/10.1016/j.conbuildmat.2016.04.021
Liu XM, Zhao XB, Yin HF, et al., 2018. Intermediate-calcium based cementitious materials prepared by MSWI fly ash and other solid wastes: hydration characteristics and heavy metals solidification behavior. Journal of Hazardous Materials, 349:262–271. https://doi.org/10.1016/j.jhazmat.2017.12.072
MEP (Ministry of Environmental Protection of the People’s Republic of China), 2014. China Soil Pollution Survey Communique. MEP, Beijing, China (in Chinese).
Moghal AAB, Ashfaq M, Al-Shamrani MA, et al., 2020. Effect of heavy metal contamination on the compressibility and strength characteristics of chemically modified semiarid soils. Journal of Hazardous, Toxic, and Radioactive Waste, 24(4):04020029. https://doi.org/10.1061/(ASCE)HZ.2153-5515.0000527
MWR (Ministry of Water Resources of the People’s Republic of China), 2019. Standard for Geotechnical Testing Method, GB/T 50123—2019. National Standards of the People’s Republic of China (in Chinese).
Pandey B, Kinrade SD, Catalan LJJ, 2012. Effects of carbon-ation on the leachability and compressive strength of cement-solidified and geopolymer-solidified synthetic metal wastes. Journal of Environmental Management, 101:59–67. https://doi.org/10.1016/joenvman.2012.01.029
Pantazopoulou E, Ntinoudi E, Zouboulis AI, et al., 2020. Heavy metal stabilization of industrial solid wastes using low-grade magnesia, Portland and magnesia cements. Journal of Material Cycles and Waste Management, 22(4):975–985. https://doi.org/10.1007/s10163-020-00985-9
Paria S, Yuet PK, 2006. Solidification—stabilization of organic and inorganic contaminants using Portland cement: a literature review. Environmental Reviews, 14(4):217–255. https://doi.org/10.1139/a06-004
Parus A, Framski G, 2018. Impact of O-alkyl-pyridineamidoximes on the soil environment. Science of the Total Environment, 643:1278–1284. https://doi.org/10.1016/j.scitotenv.2018.06.266
Parus A, Idziak M, Jacewicz P, et al., 2021. Assessment of environmental risk caused by the presence of antibiotics. Environmental Nanotechnology, Monitoring & Management, 16:100533. https://doi.org/10.1016/j.enmm.2021.100533
Peng DD, Wang YG, Liu XM, et al., 2019. Preparation, characterization, and application of an eco-friendly sand-fixing material largely utilizing coal-based solid waste. Journal of Hazardous Materials, 373:294–302. https://doi.org/10.1016/j.jhazmat.2019.03.092
Qian GR, Sun DD, Tay JH, 2003. Immobilization of mercury and zinc in an alkali-activated slag matrix. Journal of Hazardous Materials, 101(1):65–77. https://doi.org/10.1016/S0304-3894(03)00143-2
Reddy VA, Solanki CH, Kumar S, et al., 2019. New ternary blend limestone calcined clay cement for solidification/ stabilization of zinc contaminated soil. Chemosphere, 235:308–315. https://doi.org/10.1016/j.chemosphere.2019.06.051
Reddy VA, Solanki CH, Kumar S, et al., 2020. Stabilization/ solidification of zinc- and lead-contaminated soil using limestone calcined clay cement (LC3): an environmentally friendly alternative. Sustainability, 12(9):3725. https://doi.org/10.3390/su12093725
Reddy VA, Solanki CH, Kumar S, et al., 2022. Comparison of limestone calcined clay cement and ordinary Portland cement for stabilization/solidification of Pb-Zn smelter residue. Environmental Science and Pollution Research, 29(8):11393–11404. https://doi.org/10.1007/s11356-021-16421-w
Scrivener KL, 2014. Options for the future of cement. The Indian Concrete Journal, 88(7): 11–21.
Senneca O, Cortese L, di Martino R, et al., 2020. Mechanisms affecting the delayed efficiency of cement based stabilization/ solidification processes. Journal of Cleaner Production, 261:121230. https://doi.org/10.1016/j.jclepro.2020.121230
Snehal K, Das B, 2022. Pozzolanic reactivity and drying shrinkage characteristics of optimized blended cementitious composites comprising of Nano-Silica particles. Construction and Building Materials, 316:125796. https://doi.org/10.1016/j.conbuildmat.2021.125796
SEPA (State Environmental Protection Administration), 2007. Identification Standards for Hazardous Wastes-Identification for Extraction Toxicity, GB 5085.3-2007. National Standards of the People’s Republic of China (in Chinese).
Tang J, Wei SF, Li WF, et al., 2019. Synergistic effect of metakaolin and limestone on the hydration properties of Portland cement. Construction and Building Materials, 223:177–184. https://doi.org/10.1016/j.conbuildmat.2019.06.059
USEPA (United States Environmental Protection Agency), 1992. SW-846 Test Method 1311: Toxicity Characteristic Leaching Procedure. USEPA, USA.
USEPA (United States Environmental Protection Agency), 1994. SW-846 Test Method 1312: Synthetic Precipitation Leaching Procedure. USEPA, USA.
Wang H, Hou PK, Li QF, et al., 2021. Synergistic effects of supplementary cementitious materials in limestone and calcined clay-replaced slag cement. Construction and Building Materials, 282:122648. https://doi.org/10.1016/j.conbuildmat.2021.122648
Wang L, Chen L, Tsang DCW, et al., 2018. Green remediation of contaminated sediment by stabilization/solidification with industrial by-products and CO2 utilization. Science of the Total Environment, 631–632:1321–1327. https://doi.org/10.1016/j.scitotenv.2018.03.103
Wang L, Cho DW, Tsang DCW, et al., 2019. Green remediation of As and Pb contaminated soil using cement-free clay-based stabilization/solidification. Environment International, 126:336–345. https://doi.org/10.1016/j.envint.2019.02.057
Wang L, Geddes DA, Walkley B, et al., 2020. The role of zinc in metakaolin-based geopolymers. Cement and Concrete Research, 136:106194. https://doi.org/10.1016/j.cemconres.2020.106194
Wu HL, Jin F, Bo YL, et al., 2018. Leaching and microstructural properties of lead contaminated kaolin stabilized by GGBS-MgO in semi-dynamic leaching tests. Construction and Building Materials, 172:626–634. https://doi.org/10.1016/j.conbuildmat.2018.03.164
Xue ST, 2018. Study on the Effect and Mechanism of Zinc Compounds on the Properties of Cement-Based Materials. MS Thesis, Zhejiang University of Technology, Hangzhou, China (in Chinese).
Yadav AL, Sairam V, Muruganandam L, et al., 2020. An overview of the influences of mechanical and chemical processing on sugarcane bagasse ash characterisation as a supplementary cementitious material. Journal of Cleaner Production, 245:118854. https://doi.org/10.1016/j.jclepro.2019.118854
Yu J, Wu HL, Mishra DK, et al., 2021. Compressive strength and environmental impact of sustainable blended cement with high-dosage limestone and calcined clay (LC2). Journal of Cleaner Production, 278:123616. https://doi.org/10.1016/j.jclepro.2020.123616
Zhang YL, Liu XM, Xu YT, et al., 2020. Preparation of road base material by utilizing electrolytic manganese residue based on Si-Al structure: mechanical properties and Mn21 stabilization/solidification characterization. Journal of Hazardous Materials, 390:122188. https://doi.org/10.1016/j.jhazmat.2020.122188
Zhang YY, Wang L, Chen L, et al., 2021. Treatment of municipal solid waste incineration fly ash: state-of-the-art technologies and future perspectives. Journal of Hazardous Materials, 411:125132. https://doi.org/10.1016/j.jhazmat.2021.125132
Acknowledgments
This work is supported by the Scientific Research Foundation from Sun Yat-sen University and the Guangdong Basic and Applied Basic Research Foundation of China (No. 2022A1515110443).
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Haoliang WU processed the corresponding data and organized the manuscript. Heng SONG wrote the first draft of the manuscript. Xinpo SUN, Yuzhang BI, Shenjing FU, and Ning YANG helped to conduct experiments. Haoliang WU designed the research and revised and edited the final version.
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Haoliang WU, Heng SONG, Xinpo SUN, Yuzhang BI, Shenjing FU, and Ning YANG declare that they have no conflict of interest.
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Wu, H., Song, H., Sun, X. et al. Geo-environmental properties and microstructural characteristics of sustainable limestone calcined clay cement (LC3) binder treated Zn-contaminated soils. J. Zhejiang Univ. Sci. A 24, 898–911 (2023). https://doi.org/10.1631/jzus.A2200531
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DOI: https://doi.org/10.1631/jzus.A2200531
Key words
- Limestone calcined clay cement (LC3)
- Stabilization/solidification (S/S)
- Zn-contaminated soils
- Microstructural characteristics