Versatile Surface Modification of Ceramsite Via Honeycomb Calcium-aluminum-silicate-hydrate and Its Functionalization by 3-thiocyanatopropyltriethoxysilane for Enhanced Cadmium(II) Removal

Abstract

A low-cost and efficient filter medium for Cd(II) removal was prepared by anchoring -SCN functional groups (by 3-thiocyanatopropyltriethoxysilane, TCPS) on ceramsite via the approach of synthesizing a honeycomb calciumaluminum-silicate-hydrate (C-A-S-H) layer as intermediate. The specific surface area of ceramsite was increased enormously by more than 50 times because of the modification of honeycomb layer. Moreover, the abundant Si-OH bonds existing in the structure of CAS-H can serve as active sites for TCPS. The combined effects ensure that the hybrid filter medium (named ceramsite/C-A-S-H/TCPS) demonstrated a high Cd(II) adsorption capacity of 18.27 mg·g¹ for particle size of 0.1-0.6 mm, 12.63 mg·g⁻¹ for 0.6-1.25 mm and 8.64 mg g⁻¹ for 1.25-2.35 mm. The Cd(II) adsorption capacity per unit area of ceramsite/C-A-S-H/TCPS (0.1-0.6 mm) is up to 4.07 mg·m⁻², which is much higher than that of many nano-adsorbents. In addition, ceramsite/C-AS- H/TCPS could maintain a high removal efficiency (> 85%) in a wide range of pH 3-11 and showed excellent selectivity in the presence of competing ions. Furthermore, Cd(II) could be desorbed from ceramsite/C-A-S-H/TCPS composites with nearly 100%, suggesting the potential application in recycling of heavy metal ions.

Keywords

honeycomb C-A-S-H / 3-thiocyanatopropyltriethoxysilane / ceramsite / amorphous silica / Cd(II) removal

References

[1] Su Y, Adeleye AS, Huang Y, et al. Simultaneous Removal of Cadmium and Nitrate in Aqueous Media by Nanoscale Zerovalent Iron (nZVI) and Au Doped nZVI Particles[J]. Water Res., 2014, 63: 102-111.

[2] Ma L, Wang Q, Islam SM, et al. Highly Selective and Efficient Removal of Heavy Metals by Layered Double Hydroxide Intercalated with the MoS4^2- Ion[J]. J. Am. Chem. Soc., 2016, 138: 2858-2866.

[3] Ge F, Li MM, Ye H, et al. Effective Removal of Heavy Metal Ions Cd²⁺, Zn²⁺, Pb²⁺, Cu²⁺ from Aqueous Solution by Polymer-modified Magnetic Nanoparticles[J]. J. Hazard. Mater., 2012, 211-212: 366-372.

[4] Lai YC, Chang YR, Chen ML, et al. Poly(vinyl alcohol) and Alginate Cross-linked Matrix with Immobilized Prussian Blue and Ion Exchange Resin for Cesium Removal from Waters[J]. Bioresour. Technol., 2016, 214: 192-198.

[5] Luo C, Wei R, Guo D, et al. Adsorption Behavior of MnO₂ Functionalized Multi-walled Carbon Nanotubes for the Removal of Cadmium from Aqueous Solutions[J]. Chem. Eng. J., 2013, 225: 406-415.

[6] Sun Y, Lou Z, Yu J, et al. Immobilization of Mercury (II) from Aqueous Solution using Al₂O₃-supported Nanoscale FeS[J]. Chem. Eng. J., 2017, 323: 483-491.

[7] Takaesu H, Matsui Y, Nishimura Y, et al. Micro-milling Super-fine Powdered Activated Carbon Decreases Adsorption Capacity by Introducing Oxygen/hydrogen-containing Functional Groups on Carbon Surface from Water[J]. Water Res., 2019, 155: 66-75.

[8] Zhou G, Luo J, Liu C, et al. Efficient Heavy Metal Removal from Industrial Melting Effluent using Fixed-bed Process Based on Porous Hydrogel Adsorbents[J]. Water Res., 2018, 131: 246-254.

[9] Zhao D, Wang F L P L, et al. Preparation, Physicochemical Properties, and Long-Term Performance of Photocatalytic Ceramsite Sand in Cementitious Materials[J]. Applied Sciences, 2017, 7: 828.

[10] Zhao D, Gao Y, Nie S, et al. Self-assembly of Honeycomb-like Calcium-aluminum-silicate-hydrate (C-A-S-H) on Ceramsite Sand and Its Application in Photocatalysis[J]. Chem. Eng. J., 2018, 344: 583-593.

[11] Wang Y, Ye G, Chen H, et al. Functionalized Metal–organic Framework as a New Platform for Efficient and Selective Removal of Cadmium( II) from Aqueous Solution[J]. J. Mater. Chem. A, 2015, 3: 15292-15298.

[12] Zhang H, Dang Q, Liu C, et al. Uptake of Pb(II) and Cd(II) on Chitosan Microsphere Surface Successively Grafted by Methyl Acrylate and Diethylenetriamine[J]. ACS Appl. Mater. Inter., 2017, 9: 11144-11155.

[13] Wang D, Zhang G, Dai Z, et al. Sandwich-like Nanosystem for Simultaneous Removal of Cr(VI) and Cd(II) from Water and Soil[J]. ACS Appl. Mater. Inter., 2018, 10: 18316-18326.

[14] Jin F, Gu K, Al-Tabbaa A. Strength and Drying Shrinkage of Reactive MgO Modified Alkali-activated Slag Paste[J]. Constr. Build. Mater., 2014, 51: 395-404.

[15] Wu J, Zhu YJ, Chen F. Ultrathin Calcium Silicate Hydrate Nanosheets with Large Specific Surface Areas: Synthesis, Crystallization, Layered Self-assembly and Applications as Excellent Adsorbents for Drug, Protein, and Metal Ions[J]. Small, 2013, 9: 2911-2925.

[16] Liu P, Gao Y, Wang F, et al. Preparation of Pervious Concrete with 3-thiocyanatopropyltriethoxysilane Modified Fly Ash and Its Use in Cd (II) Sequestration[J]. J. Clean. Prod., 2019, 212: 1-7.

[17] Yasutaka K, Takato Y, Takashi K, et al. Enhancement in Adsorption 80 Vol.35 No.1 ZHAO Du et al: Versatile Surface Modification of Ceramsite Via Honeycomb… and Catalytic Activity of Enzymes Immobilized on Phosphorus- and Calcium-modified MCM-41[J]. J. Phys. Chem. B, 2011, 115: 10335-10345.

[18] Kuwahara Y, Tamagawa S, Fujitani T, et al. A Novel Conversion Process for Waste Slag: Synthesis of Calcium Silicate Hydrate from Blast Furnace Slag and its Application as a Versatile Adsorbent for Water Purification[J]. J. Mater. Chem. A, 2013, 1: 7199.

[19] Meiszterics A, Rosta L, Peterlik H, et al. Structural Characterization of Gel-Derived Calcium Silicate Systems[J]. J. Phys. Chem. A, 2010, 114: 10403-10411.

[20] Koley P, Sakurai M, Aono M. Controlled Fabrication of Silk Protein Sericin Mediated Hierarchical Hybrid Flowers and Their Excellent Adsorption Capability of Heavy Metal Ions of Pb(II), Cd(II) and Hg(II) [J]. ACS Appl. Mater. Inter., 2016, 8: 2380-2392.

[21] Li Y, He J, Zhang K, et al. Super Rapid Removal of Copper, Cadmium and Lead Ions from Water by NTA-silica Gel[J]. RSC Advances, 2019, 9: 397-407.

[22] Wang K, Gu J, Yin N. Efficient Removal of Pb(II) and Cd(II) Using NH₂-Functionalized Zr-MOFs via Rapid Microwave-Promoted Synthesis[J]. Ind. Eng. Chem. Res., 2017, 56: 1880-1887.

[23] Tang J, Mu B, Zheng M, et al. One-Step Calcination of the Spent Bleaching Earth for the Efficient Removal of Heavy Metal Ions[J]. ACS Sustain. Chem. Eng., 2015, 3: 1125-1135.

[24] Liang J, Li X, Yu Z, et al. Amorphous MnO₂ Modified Biochar Derived from Aerobically Composted Swine Manure for Adsorption of Pb(II) and Cd(II)[J]. ACS Sustain. Chem. Eng., 2017, 5: 5049-5058.

[25] Guo Z, Zhang X, Kang Y, et al. Biomass-Derived Carbon Sorbents for Cd(II) Removal: Activation and Adsorption Mechanism, ACS Sustain[J]. Chem. Eng., 2017, 5: 4103-4109.

[26] Ma L, Islam SM. Rapid Simultaneous Removal of Toxic Anions [HSeO₃]^-, [SeO₃]^2-, and [SeO₄]^2-, and Metals Hg²⁺, Cu²⁺, and Cd²⁺ by MoS4^2- Intercalated Layered Double Hydroxide[J]. J. Am. Chem. Soc., 2017, 139: 12745-12757.

[27] Zhang S, Zhang Y, Liu J, et al. Thiol Modified Fe₃O₄@SiO₂ as a Robust, High Effective, and Recycling Magnetic Sorbent for Mercury Removal[J]. Chem. Eng. J., 2013, 226: 30-38.

[28] Sun Y, Liu Y, Lou Z, et al. Enhanced Performance for Hg(II) Removal using Biomaterial (CMC/gelatin/starch) Stabilized FeS Nanoparticles: Stabilization Effects and Removal Mechanism[J]. Chem. Eng. J., 2018, 344: 616-624.

[29] Jeong HY, Klaue B, Blum JD, et al. Sorption of Mercuric Ion by Synthetic Nanocrystalline Mackinawite (FeS)[J]. Environ. Sci. Technol., 2007, 41: 7699-7705.

[30] Huang N, Zhai L, Xu H, et al. Stable Covalent Organic Frameworks for Exceptional Mercury Removal from Aqueous Solutions[J]. J. Am. Chem. Soc., 2017, 139: 2428-2434.

[31] Aguila B, Sun Q, Perman JA, et al. Efficient Mercury Capture Using Functionalized Porous Organic Polymer[J]. Adv. Mater., 2017, 29: 1700665.

[32] Yang GX, Jiang H. Amino Modification of Biochar for Enhanced Adsorption of Copper Ions from Synthetic Wastewater[J]. Water Res., 2014, 48: 396-405.

[33] Gong Y, Liu Y, Xiong Z, et al. Immobilization of Mercury by Carboxymethyl Cellulose Stabilized Iron Sulfide Nanoparticles: Reaction Mechanisms and Effects of Stabilizer and Water Chemistry[J]. Environ. Sci. Technol., 2014, 48: 3986-3994.

[34] Sun W, Pan W, Wang F, et al. Removal of Se(IV) and Se(VI) by MFe2O4 Nanoparticles from Aqueous Solution[J]. Chem. Eng. J., 2015, 273: 353-362.

[35] Fischer L, Falta T, Koellensperger G, et al. Ionic Liquids for Extraction of Metals and Metal Containing Compounds from Communal and Industrial Waste Water[J]. Water Res., 2011, 45: 4601-4614.

[36] You W, Weng Y, Wang X, et al. Synthesis and Adsorption Properties of Hierarchically Ordered Nanostructures Derived from Porous CaO Network[J]. ACS Appl. Mater. Inter., 2016, 8: 33656-33665.

[37] Qi G, Lei X, Li L, et al. Preparation and Evaluation of a Mesoporous Calcium-silicate Material (MCSM) from Coal Fly Ash for Removal of Co(II) from Wastewater[J]. Chem. Eng. J., 2015, 279: 777-787.

[38] Zhao J, Zhu YJ, Wu J, et al. Chitosan-coated Mesoporous Microspheres of Calcium Silicate Hydrate: Environmentally Friendly Synthesis and Application as a Highly Efficient Adsorbent for Heavy Metal Ions[J]. J. Colloid Interface Sci, 2014, 418: 208-215.

[39] Guo H, Sun P, Liang Y, et al. In-situ Fabrication of Polyelectrolyte-CSH Superhydrophilic Coatings via Layer-by-layer Assembly[J]. Chem. Eng. J., 2014, 253: 198-206.

[40] Pegado L, Labbez C, Churakov SV. Mechanism of Aluminium Incorporation into C-S-H from Ab Initio Calculations[J]. J. Mater. Chem. A., 2014, 2: 3477-3483.