The transformation of kaolinite into metakaolinite by thermal activation to obtain highly active aluminosilicate is commonly known. In addition to kaolin, the high content of kaolinite in coal mining waste is another potential source for obtaining an aluminosilicate precursor, thereby protecting the environment and adding value to industrial wastes. In this paper, the kaolinite-based high ash slime (KAS) was calcined at temperatures ranging from 400 °C to 1000 °C under air, N₂, and CO₂ atmospheres, respectively. The thermal behaviors and structural evolution of each component in KAS were analyzed by thermal analysis (TG-DSC), X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FTIR), and X-ray photoelectron spectroscopy (XPS). Moreover, the chemical reactivity of Al₂O₃ and SiO₂ in calcined KAS was evaluated by HCl and NaOH leaching methods. The results show that the applied KAS in this study primarily consisted of kaolinite and carbon, while the minor mineral phases included quartz, calcite, and pyrite. Additionally, the structural transformation of kaolinite during calcination included dehydroxylation, sintering, and the formation of mullite. Crystalline kaolinite completely decomposed into semicrystalline metakaolinite at 600–800 °C, accounting for the increase in chemical reactivity. The interlayer sintering of metakaolinite and the recrystallization of amorphous components led to the decrease in chemical reactivity after 800 °C. Furthermore, the thermal behaviors of carbon in KAS are greatly affected by the calcination atmosphere. The presence of carbon reduced the chemical reactivity of calcined KAS.

The cleaning process of coals is challenging due to the existence of clay minerals. The overall objective of this study is to investigate how the dewatering of coal slurry is impacted by the presence of clay minerals, i.e., kaolinite and montmorillonite. Filtration tests were first conducted to investigate the effect of kaolinite and montmorillonite on the dewatering efficiency of coal. Specifically, we measured the filtration velocity, moisture, average specific resistance, and porosity of filter cakes for six slurry samples, in which different amounts of kaolinite and montmorillonite were contained. Filtration tests show that a small amount of kaolinite and montmorillonite leads to a significant reduction in the filtration velocity and porosity, and a big increase in the average specific resistance and the moisture of the filter cake. We observe that most kaolinite existed in the top and middle layers of the filter cake, while most montmorillonite existed in the top layer; on the contrary, little montmorillonite is observed in the middle and bottom layers of the filter cake. Montmorillonite results in a much more deteriorative effect than kaolinite. Considering that the interactions between clay minerals and water may play a key role, we then further investigate the effect of such interactions using molecular simulations. Simulation results show that water molecules could hardly diffuse into kaolinite from the edge, while they could readily penetrate into the montmorillonite layers from the edge surface. This result can be explained by the hydrated cation in montmorillonite. The adsorption density of water on the octahedral surface of kaolinite is higher than that of water on the tetrahedral surface of kaolinite. Furthermore, the adsorption density of water on the double surfaces of kaolinite is higher than that of water on the montmorillonite surface. This research is expected to provide benefits or contributions to the dewatering of clay-rich coal tailings.

Montmorillonite is always a troublemaker for the dewatering in coal processing since its existence can decrease the rates of sedimentation and filtration of coal slurry. To eliminate the adverse effect of montmorillonite, adjusting the slurry pH and adding electrolytes are always the key methods. However, the underlying mechanism still needs to be further studied. The dewatering of Na-montmorillonite (Na-Mt) suspensions has been studied as a function of NaCl concentration (10⁻³, 10⁻², and 10⁻¹ M) at different pH values (6.0, 7.7, 8.1, 9.2). The point of zero charge of edge surface of Na-Mt (pH_PZC,edge) appeared at the pH value of 6.8. The sedimentation and rheology experiments described the coagulation and flow behaviors of Na-Mt suspensions, respectively. The Na-Mt suspension coagulated spontaneously at low salt concentration with the pH ~ 6.0. For the pH > pH_PZC,edge, the height of the sediment bed reduced and apparent viscosity increased with the increase of the electrolyte concentration. The filtration properties were evaluated on the basis of Darcy’s law. The obtained result clearly demonstrated that the filtration rate was accelerated with the increase of pH and electrolyte concentration. The modes of particle association and its effect on filtration performance were discussed. Moreover, a comparison with related results from the literature was performed. At pH ~ 6 and low electrolyte concentration, the positively charged Edge surfaces and negatively charged Face surfaces coagulate rapidly to form a sealed structure by electrostatic attraction. Furthermore, inside this sealed structure, the water molecules cannot be removed in the filtration process easily. However, by increasing the electrolyte concentration at pH > pH_PZC,edge, the gradually formed Face/Face structure increases the filtration rate sharply because of the inhibiting effect of the electric double layer (EDL) and the osmotic expansion. Therefore, adjusting solution conditions of the aqueous suspension to tune the particle coagulation behavior is one of the effective methods to solve the problem of montmorillonite dewatering.

This study investigates the interaction between montmorillonite and polyacrylamide (PAM) with different ionic types using quartz crystal microbalance with dissipation monitoring (QCM-D) and molecular dynamics (MD) simulations. The goal was to understand the effect of ionicity and ionic type on polymer deposition on montmorillonite surfaces. The results of the QCM-D analysis showed that a decrease in pH led to an increase in the adsorption of montmorillonite on the alumina surface. The ranking of adsorption mass on alumina and pre-adsorbed montmorillonite alumina surfaces was found to be cationic polyacrylamide (CPAM) > polyacrylamide (NPAM) > anionic polyacrylamide (APAM). The study also found that CPAM had the strongest bridging effect on montmorillonite nanoparticles, followed by NPAM, while APAM had a negligible bridging effect. The MD simulations showed that ionicity had a significant influence on the adsorption of polyacrylamides. The cationic functional group N(CH₃)³⁺ had the strongest attraction interaction with the montmorillonite surface, followed by the hydrogen bonding interaction of the amide functional group CONH₂, and the anionic functional group COO- had a repulsive interaction. The results suggest that at high ionicity levels, CPAM can be adsorbed on the montmorillonite surface, while at low ionicity levels, APAM may still be adsorbed with a strong coordination trend.

High-ash coal, also known as low-grade coal, has becomes a viable alternative in recent years to high-quality coal because available resources have become increasingly scarce due to extensive mining activity. This work aims to provide a comprehensive understanding of the structural characteristics of high-ash coal and construct a plausible molecular structure to elucidate its chemical reactivity in future applications. Its properties were investigated using Solid-state ¹³C nuclear magnetic resonance (¹³C NMR), X-ray photoelectron spectroscopy analysis (XPS), X-ray diffraction (XRD), and Fourier transform infrared spectroscopy (FT-IR). The molecular structure was constructed and validated using Material Studio, LAMMPS Software Package, and MATLAB program. The characterization results revealed that high-ash coal contains 72.15% aromatic carbon, significantly surpassing the percentage of aliphatic carbon (27.85%). The ratio of bridgehead carbon to peripheral aromatic carbon was calculated as 0.67, indicating that the pentacene is the main carbon skeleton form in the high-ash coal structure. Furthermore, oxygen-containing functional groups presented as C=O/O–C–O, C–O, and COO– within the structure along with pyridine and pyrrolic structures. Consequently, the molecular structure comprises pentacene with aliphatic carbon chains, such as methylene, that connect the benzene rings and form a three-dimensional network. The results of a simulated IR spectrum and contact angle simulation aligned with the experimental results, validating the molecular structure of high-ash coal. The chemical formula for the high-ash coal model was determined as C₂₀₃H₁₈₉N₇O₆₁S with a molecular weight of 3734.79.

It is important to identify an environmentally friendly and efficient flocculant that can replace polyacrylamide for the solid–liquid separation of coal wastewater. In this study, to explore whether chitosan can be used as an environmentally friendly and efficient flocculant for the solid–liquid separation of coal wastewater, AlCl₃–chitosan was used to conduct flocculation–sedimentation and dewatering tests under different chitosan dosages and shear-strength conditions for the prepared coal wastewater. Focused beam reflectance was measured to dynamically monitor the number of refractory fine particles, and the settled flocs were photographed and analyzed with microscopy to explore the effect of AlCl₃–chitosan on the flocculation settlement effect and floc characteristics. The synergistic mechanisms of AlCl₃ and chitosan were investigated using quartz crystal dissipative microbalance and zeta potential measurement. The results showed that the addition of chitosan can significantly improve the flocculation–sedimentation and dewatering effects of coal wastewater. A reasonable dosage under a certain shear strength is conducive to the reduction of fine slime particles, which results in a compact floc structure, increases the floc size, and improves the settling effect. The synergistic effect of AlCl₃–chitosan improved the electric neutralization and adsorption bridging abilities of the chitosan, and the mixed solution of AlCl₃ and chitosan had stronger adsorption on the carbon surface. This study provides a new approach to the selection of flocculants for coal wastewater treatment.