The characteristics of nonmetallic inclusions formed during steel production have a significant influence on steel performance. In this paper, studies on inclusions using confocal scanning laser microscopy (CSLM) are reviewed and summarized, particularly the collision of various inclusions, dissolution of inclusions in liquid slag, and reactions between inclusions and steel. Solid inclusions exhibited a high collision tendency, whereas pure liquid inclusions exhibited minimal collisions because of the small attraction force induced by their <90° contact angle with molten steel. The collision of complex inclusions in molten steel was not included in the scope of this study and should be evaluated in future studies. Higher CaO/Al₂O₃ and CaO/SiO₂ ratios in liquid slag promoted the dissolution of Al₂O₃-based inclusions. The formation of solid phases in the slag should be prevented to improve dissolution of inclusions. To accurately simulate the dissolution of inclusions in liquid slag, in-situ observation of the dissolution of inclusions at the steel–slag interface is necessary. Using a combination of CSLM and scanning electron microscopy–energy dispersive spectroscopy, the composition and morphological evolution of the inclusions during their modification by the dissolved elements in steel were observed and analyzed. Although the in-situ observation of MnS and TiN precipitations has been widely studied, the in-situ observation of the evolution of oxide inclusions in steel during solidification and heating processes has rarely been reported. The effects of temperature, heating and cooling rates, and inclusion characteristics on the formation of acicular ferrites (AFs) have been widely studied. At a cooling rate of 3–5 K/s, the order of AF growth rate induced by different inclusions, as reported in literature, is Ti–O < Ti–Ca–Zr–Al–O < Mg–O < Ti–Zr–Al–O < Mn–Ti–Al–O < Ti–Al–O < Zr–Ti–Al–O. Further comprehensive experiments are required to investigate the quantitative relationship between the formation of AFs and inclusions.

Electrochemical metallurgy at low temperature (<473 K) shows promise for the extraction and refinement of metals and alloys in a green and sustainable manner. However, the kinetics of the electrodeposition process is generally slow at low temperature, resulting in large overpotential and low current efficiency. Thus, the application of external physical fields has emerged as an effective strategy for improving the mass and charge transfer processes during electrochemical reactions. This review highlights the challenges associated with low-temperature electrochemical processes and briefly discusses recent achievements in optimizing electrodeposition processes through the use of external physical fields. The regulating effects on the optimization of the electrodeposition process and the strategies for selecting various external physical fields, including magnetic, supergravity, and ultrasonic fields are summarized from the perspectives of equipment and mechanisms. Finally, advanced methods for in-situ characterization of external physical field-assisted electrodeposition processes are reviewed to gain a deeper understanding of metallic electrodeposition. An in-depth exploration of the mechanism by which external physical fields affect the electrode process is essential for enhancing the efficiency of metal extraction at low temperatures.

Liquid metals (LMs), because of their ability to remain in a liquid state at room temperature, render them highly versatile for applications in electronics, energy storage, medicine, and robotics. Among various LMs, Ga-based LMs exhibit minimal cytotoxicity, low viscosity, high thermal and electrical conductivities, and excellent wettability. Therefore, Ga-based LM composites (LMCs) have emerged as a recent research focus. Recent advancements have focused on novel fabrication techniques and applications spanning energy storage, flexible electronics, and biomedical devices. Particularly noteworthy are the developments in wearable sensors and electronic skins, which hold promise for healthcare monitoring and human–machine interfaces. Despite their potential, challenges, such as oxidative susceptibility and biocompatibility, remain. Creating bio-based LMC materials is a promising approach to address these issues while exploring new avenues to optimize LMC performance and broaden its application domains. This review provides a concise overview of the recent trends in LMC research, highlights their transformative impacts, and outlines key directions for future investigation and development.

Bioleaching is confronted with problems, such as low efficiency, long production cycle length, and vegetation destruction. In order to solve problems above, fly ash and low-grade copper sulfide ores were used to investigate bioleaching behaviors and bacterial community succession. Results showed that copper recovery, bacterial concentration, total proportion of main leaching bacteria including Acidithiobacillus ferrooxidans, Acidibacillus ferrooxidans, and Leptospirillum ferriphilum, were improved through using appropriate dosage of fly ash. The maximum copper recovery of 79.87% and bacterial concentration of 7.08 × 10⁷ cells·mL⁻¹ were obtained after using 0.8 g·L⁻¹ fly ash. Exclusive precipitation including Zn(Fe₃(SO₄)₂(OH)₆)₂ and Mg(Fe₃(SO₄)₂(OH)₆)₂ was found in sample added 0.8 g·L⁻¹ fly ash, which reduced the effect of hazardous ions on bacteria and thus contributing to bacterial proliferation. Bacterial community structure was differentiated, which indicated difference between original inoculation and sample used 0.8 g·L⁻¹ fly ash was less than others. Total proportion of the three microorganism above accounted for more than 95% in all tests, especially in sample with 0.8 g·L⁻¹ fly ash up to 99.81%. Cl⁻ and Ag⁺ contained in fly ash can act as catalytic agent, which contributed to conversion from smooth and dense passivation layer to sparse and scattered one, and therefore improving contact between ores, lixiviant, and bacteria. Using appropriate dosage of fly ash showed prospects in bioleaching.

This study investigated the effect of konjac glucomannan (KGM) on the flotation separation of calcite and scheelite. Microflotation tests showed that under the action of 50 mg/L KGM, the floatability of calcite notably decreased, while the impact on scheelite was negligible, resulting in a recovery difference of 82.53%. Fourier transform infrared (FTIR) spectroscopy and atomic force microscopy (AFM) analyses indicated the selective adsorption of KGM on the calcite surface. Test results of the zeta potential and UV-visible absorption spectroscopy revealed that KGM prevented the adsorption of sodium oleate on the calcite surface. X-ray photoelectron spectroscopy (XPS) analysis further confirmed the chemical adsorption of KGM on the calcite surface and the formation of Ca(OH)₂. The density functional theory (DFT) simulation results were consistent with the flotation tests, demonstrating the strong adsorption performance of KGM on the calcite surface. This study offers a pathway for highly sustainable and cost-effective mineral processing by utilizing the unique properties of biopolymers such as KGM to separate valuable minerals from gangue minerals.

The high-temperature properties of the Al₂O₃–CaO–SiO₂–Fe₂O₃ basic slag had significant influences on steelmaking operations and waste slag utilization. To further clarify the structural characteristics and properties of Al₂O₃–CaO–SiO₂–Fe₂O₃ slags, the structures and viscosities of the slags were researched. The slag liquidus temperature was determined, which decreased from 1365 to 1287°C after 4.16wt%–8.52wt% Al₂O₃ was added to the slags and then increased to 1356°C after 17.07wt% Al₂O₃ was added. Structure analysis indicated that increasing temperature depolymerized the structure of the 4.16wt%Al₂O₃–CaO–SiO₂–Fe₂O₃ slag by decreasing the amount of complex AlO₄ units and promoting the formation of simplified silicate monomers. The addition of Al₂O₃ to slags could promote the polymerization of the slag structure by increasing the quantities of complex AlO₄ tetrahedral and complicated Si–O units. Variations in the degree of structure polymerization showed similar trends at the same superheat degree and the same quenching temperature, and both samples could be used for analyzing the impact of Al₂O₃ on slag structures. Finally, the viscous behavior of the present slag system was evaluated. Increasing Al₂O₃ content could increase slag viscosity, and the apparent activation energy increased from 132.13 to 174.83 kJ/mol as the content of Al₂O₃ increased from 4.16wt% to 17.07wt%.

Secondary aluminum dross (SAD) is a rich source of recyclable aluminum but poses considerable risk due to its high AlN content. Therefore, thoroughly removing AlN is essential, but intricate aluminum components and expensive additives pose challenges to the process. In this study, waste sodium acetate is proposed as an environmentally friendly additive for completely removing AlN and enhancing the extraction of aluminum from SAD. Through the exothermic decomposition of NaAc, reactions can occur at 850°C. AlN removal efficiency reached 93.19% after sintering, whereas Al leaching efficiency in the subsequent leaching process reached 90.49%, which were 37.86% and 375.26% higher than the removal efficiency of the control, respectively. These favorable results were attributed to the comprehensive transformation of aluminum species. The formation of soluble phase Na_1.95Al_1.95Si_0.05O₄ occurred during the destruction of the Al₂O₃ layer surrounding AlN and the transformation of other aluminum components. AlN decomposed upon contact with NaAc. Therefore, this study utilizes the decomposition properties of NaAc to provide an efficient and environmentally friendly route for removing AlN and extracting Al from SAD.

Replacing solid carbon with hydrogen gas in ferromanganese production presents a forward-thinking, sustainable solution to reducing the ferro-alloy industry’s carbon emissions. The HAlMan process, a groundbreaking and eco-friendly method, has been meticulously researched and scaled up from laboratory experiments to pilot tests, aiming to drastically cut CO₂ emissions associated with ferromanganese production. This innovative process could potentially reduce CO₂ emissions by about 1.5 tonnes for every tonne of ferromanganese produced. In this study, a lab-scale vertical thermogravimetric furnace was used to carry out the pre-reduction of Nchwaning manganese ore, where direct reduction occurred with H₂ gas under controlled isothermal conditions at 700, 800, and 900°C. The results indicated that higher pre-reduction temperatures (800 and 900°C) effectively converted Fe₂O₃ to metallic iron and Mn₂O₃ to MnO. By continuously monitoring the mass changes during the reduction, both the rate and extent of reduction were assessed. A second-order reaction model was applied to validate the experimental outcomes of H₂ reduction at various temperatures, showing apparent activation energies of 29.79 kJ/mol for dried ore and 61.71 kJ/mol for pre-calcined ore. The reduction kinetics displayed a strong dependence on temperature, with higher temperatures leading to quicker and more complete reductions. The kinetics analysis suggested that the chemical reaction at the gas–solid interface between hydrogen and the manganese ore is likely the rate-limiting step in this process.

The enrichment of chromium in the magnetic iron chromite (Fe(Cr_xFe_1−x)₂O₄) phase is crucial for the recovery and recycling of chromium in stainless-steel pickling sludge. The kinetics and reaction mechanism of the solid-phase reaction between Fe₃O₄ and Cr₂O₃ were investigated using the diffusion couple method at 1473 K. Not only the diffusion behavior of Fe²⁺ ions and Cr³⁺ ions was elucidated, but also the solid solution behavior of Fe³⁺ ions was discussed clearly. The microscopic morphology of the diffusion couple and the change in the concentrations of Fe and Cr cations across the diffusion layers were analyzed using scanning electron microscopy and energy dispersive spectroscopy. The self-diffusion coefficients of cations were calculated based on the concentration profiles of Fe and Cr, with the results indicating that the self-diffusion coefficient of the Fe ions was consistently higher than that of the Cr ions. Additionally, a mixture of Fe₃O₄ and Cr₂O₃ was annealed at 1373–1473 K for 1–5 h, and the kinetic parameters were calculated by studying the phase content of the product. The phase content of Fe(Cr_xFe_1−x)₂O₄ in the product was determined by Rietveld refinement of X-ray diffraction data, revealing that an activation energy (E) of 177.20 kJ·mol⁻¹ and a pre-exponential factor (B) of 610.78 min⁻¹ of the solid-phase reaction that produced the Fe(Cr_xFe_1−x)₂O₄ spinel.

The application of liquid core reduction (LCR) technology in thin slab continuous casting can refine the internal microstructures of slabs and improve their production efficiency. To avoid crack risks caused by large deformation during the LCR process and to minimize the thickness of the slab in bending segments, the maximum theoretical reduction amount and the corresponding reduction scheme for the LCR process must be determined. With SPA-H weathering steel as a specific research steel grade, the distributions of temperature and deformation fields of a slab with the LCR process were analyzed using a three-dimensional thermal-mechanical finite element model. High-temperature tensile tests were designed to determine the critical strain of corner crack propagation and intermediate crack initiation with various strain rates and temperatures, and a prediction model of the critical strain for two typical cracks, combining the effects of strain rate and temperature, was proposed by incorporating the Zener–Hollomon parameter. The crack risks with different LCR schemes were calculated using the crack risk prediction model, and the maximum theoretical reduction amount for the SPA-H slab with a transverse section of 145 mm × 1600 mm was 41.8 mm, with corresponding reduction amounts for Segment 0 to Segment 4 of 15.8, 7.3, 6.5, 6.4, and 5.8 mm, respectively.

The demand for oil casing steel with ultra-high strength and excellent impact toughness for safe application in ultra-deep wells is pressing. In improving the combination of strength, ductility, and impact toughness, the designed Cr–Mo–V micro-alloyed oil casing steel was quenched at 800, 900, and 1000°C, followed by tempering at 600, 680, and 760°C, respectively, to obtain distinct microstructures. The results showed that the microstructure of the samples quenched at 800°C followed by tempering comprised untransformed ferrite and large undissolved carbides, which considerably deteriorated tensile strength and impact toughness. For other conditions, the nucleated carbides and the boundaries are key factors that balance the tensile strength from 1226 to 971 MPa and the impact toughness from 65 to 236 J. From the perspective of carbide, optimal precipitation strengthening is achieved with a smaller carbide size obtained by a low tempering temperature of 600°C, while larger-sized carbides would remarkably soften the matrix to improve the toughness but deteriorate the tensile strength. Additionally, an increase in prior austenite grain size with the corresponding enlarged sub-boundaries obtained by high quenching temperatures substantially diminishes grain refinement strengthening, dislocation strengthening, and the energy absorbed in the crack propagation process, which is unfavorable to strength and toughness.

Weathering steel exhibits excellent corrosion resistance and is widely used in bridges, towers, railways, highways, and other engineering projects that are exposed to the atmosphere for long periods of time. However, before the formation of stable rust layers, weathering steel is prone to liquid rust sagging and spattering, leading to environmental pollution and city appearance concerns. These factors limit the application and development of weathering steel. In this study, a rapid and environmentally friendly method was developed by introducing alloying elements, specifically investigating the role of Sn in the rapid stabilization of rust layers in marine atmospheric environments. The rust layer formed on weathering low-alloy steel exposed to prolonged outdoor conditions and laboratory immersion experiments was explored using electron probe micro-analyzer (EPMA), micro-Raman, X-ray photoelectron spectroscopy (XPS), and electrochemical measurements. Results showed an optimal synergistic effect between Sn and Cr, which facilitated the accelerated densification of the rust layer. This beneficial effect enhanced the capability of the rust layer to resist Cl⁻ erosion and improved the protection performance of the rust layer.

The corrosion degradation of organic coatings in tropical marine atmospheric environments results in substantial economic losses across various industries. The complexity of a dynamic environment, combined with high costs, extended experimental periods, and limited data, places a limit on the comprehension of this process. This study addresses this challenge by investigating the corrosion degradation of damaged organic coatings in a tropical marine environment using an atmospheric corrosion monitoring sensor and a random forest (RF) model. For damage simulation, a polyurethane coating applied to a Fe/graphite corrosion sensor was intentionally scratched and exposed to the marine atmosphere for over one year. Pearson correlation analysis was performed for the collection and filtering of environmental and corrosion current data. According to the RF model, the following specific conditions contributed to accelerated degradation: relative humidity (RH) above 80% and temperatures below 22.5°C, with the risk increasing significantly when RH exceeded 90%. High RH and temperature exhibited a cumulative effect on coating degradation. A high risk of corrosion occurred in the nighttime. The RF model was also used to predict the coating degradation process using environmental data as input parameters, with the accuracy showing improvement when the duration of influential environmental ranges was considered.

The dynamic recrystallization (DRX) and dynamic precipitation of Mg–5Gd–3Sm(–1Zn)–0.5Zr alloys after hot compression deformation were analyzed by electron backscatter diffraction (EBSD) and transmission electron microscopy (TEM) techniques. Furthermore, the DRX mechanisms were investigated by calculating the deformation activation energy, establishing the constitutive equation, and creating a critical strain model. The results indicate that the presence of Zn element enhanced the production of DRX, considerably reduced the strength of {0001} plane texture, and boosted the Schmidt factor of nonbasal plane slip. The Mg–5Gd–3Sm–0.5Zr alloy had a low degree of DRX, manifested as a monolayer of DRX grains at the grain boundaries, and dominated by the discontinuous DRX mechanism. However, the Mg–5Gd–3Sm–1Zn–0.5Zr alloy had a high degree of DRX, which occurred in the form of multilayered DRX grains by the main mechanism of continuous DRX. Compared with the Mg–5Gd–3Sm–0.5Zr alloy, in addition to the Mg₅(Gd,Sm) phase, the Mg–5Gd–3Sm–1Zn–0.5Zr alloy also introduced a new dynamic precipitation phase called (Mg,Zn)₃(Gd,Sm) phase. The dynamic precipitation phase prevented grain boundary migration and dislocation motion, which promoted DRX nucleation and prevented the growth of recrystallized grains.

7039 Al alloys are widely used in armor vehicles, given the material’s high specific strength and fracture toughness. However, laminar tearing in the thickness plane of the base metal (BM), specifically in the normal direction (ND) and rolling direction (RD) plane, was occasionally observed after the welding of thick plates, resulting in premature material failure. A vertically metal-inert gas (MIG)-welded laminar tearing component of a 30 mm thick plate was analyzed to determine the factors associated with this phenomenon. The texture, residual stress, microhardness, and tensile properties were also investigated. The results indicated that the crack extended along the RD as a transcrystalline fracture and terminated at the BM. The grains near the crack grew preferentially in the (001) crystal direction. Furthermore, the tensile strength (83 MPa) and elongation (6.8%) in the RD were relatively higher than those in the ND. In particular, the primary factors for crack initiation include stronger texture, higher dislocation density, increased Al₇Cu₂Fe phases, lower proportion of small-angle grain boundaries, and varying grain sizes in different regions, leading to the fragile microstructure. The higher residual stress of the BM promotes the formation and extension of cracks. The restraining force due to fixation and welding shrinkage force transformed the crack into laminar tearing. Preventive measures of laminar tearing were also proposed.

The binder phase performs critically on the comprehensive properties of cemented carbides, especially the hardness (HV) and fracture toughness (K_IC) relationship. There are strong motivations in both research community and industry for developing alternative binders to Co in cemented carbide system, due to the reasons such as price instability, property degeneration, and toxicity. Herein, six kinds of high entropy alloys (HEA) including CoCrFeNiMn, CoCrFeMnAl, CoCrFeNiAl, CoCrNiMnAl, CoFeNiMnAl, and CrFeNiMnAl were employed as the alternative binder for the preparation of WC–HEA cemented carbides through mechanical alloying and two-step spark plasma sintering. The impacts of HEA on the microstructures, mechanical properties, and thermal conductivity of WC–HEA hardmetals were determined and discussed. WC–HEA hardmetals exhibited both superior HV and K_IC to WC–metal or WC–intermetallic cemented carbides, indicating that HEA alloys were not only harder but also tougher in comparison with traditional metal or intermetallic binders. The HEA bonded hardmetals yielded thermal conductivities much lower than that of traditional WC–Co cemented carbide. The excellent HV–K_IC relationship of WC–HEA facilitated the potential engineering structural application of cemented carbides.

FeCoCrMnNiN_x high entropy nitride ceramics thin films were prepared using the magnetron sputtering method, and the effects of nitrogen content on the thin films’ properties were later examined. The addition of N₂ affected the microstructures of the thin films and their mechanical and corrosion properties. Compared with the FeCoCrMnNi thin films with 1-sccm N₂, the addition of 2 and 3 sccm of N₂ by as much as 5.45at% and 6.34at% changed the solid solution’s crystalline structure into an amorphous structure. The addition of nitrogen caused drastic changes to the surface morphology, creating a smoother and more uniform surface without cauliflower units. The atomic force microscopy image analysis indicated that the addition of nitrogen reduced the surface roughness from 5.58 to 1.82 nm. Adding N₂ to the CoCrFeMnNi thin film helped increase its mechanical properties, such as hardness and strength, while the Young’s modulus decreased. The hardness of (8.75 ± 0.5) GPa and the reduced Young’s modulus of (257.37 ± 11.4) GPa of the FeCoCrMnNi thin film reached (12.67 ± 1.2) and (194.39 ± 12.4) GPa, respectively, with 1 sccm N₂. The applied coating of the CoCrFeMnNi thin film on 304SUS increased the corrosion resistance, whereas the addition of nitrogen to the CoCrFeMnNi thin film also improved its corrosion resistance compared with that of the CoCrFeMnNi thin film without nitrogen.

High-purity SiO₂ nanoparticles (SNPs) play a crucial role in various electronic applications, such as semiconductors, solar cells, optical fibers, lenses, and insulating layers, given their purity and particle size, which significantly impact device efficiency. This study focuses on the synthesis and characterization of pure SNPs through the chemical etching of greater club rush. White powder SNPs were prepared using HCl etching, and their thermal behaviors were analyzed via thermogravimetric analysis/differential scanning calorimetry. Structural properties were investigated using X-ray fluorescence, scanning electron microscopy, and transmission electron microscopy. X-ray absorption near-edge structure was employed to assess the oxidation state of the SNPs. The morphology of the SNPs after the first etching was amorphous, with sizes ranging from 50 to 100 nm, which increased to 50–200 nm after the second etching. Despite this size variation, the SNPs maintained a high purity level of 99.8wt% SiO₂, comparable with industry standards. Notably, the second etching with 0.1-M HCl significantly enhanced the purity level, achieving 99.8wt% SiO₂ mass. Furthermore, HCl etching facilitated the formation of SiO₂ in the Si⁴⁺ oxidation state, akin to industrial SNPs. These findings underscore the critical role of HCl etching in synthesizing high-purity SNPs, with potential applications in advanced electronic devices.

Nanoferrites of the CoMn_xFe(_2−x)O₄ series (x = 0.00, 0.05, 0.10, 0.15, 0.20) were synthesized in this study using the sol–gel auto-combustion approach. The lattice constants were computed within the range of 8.312–8.406 Å, while crystallite sizes were estimated to range between 55.20 and 31.40 nm using the Scherrer method. The different functional groups were found to correlate with various absorption bands using Fourier transform infrared (FTIR) spectroscopy. Five active modes were identified by Raman spectroscopy, revealing vibration modes of O²⁻ ions at tetrahedral and octahedral locations. The ferromagnetic hysteresis loop was observed in all the synthesized samples, which can be explained by Neel’s model. The results showed that AC conductivity decreased with increasing Mn²⁺ content at the Fe²⁺ site, while the dielectric constant and dielectric loss increased with increasing frequency. Furthermore, the saturation magnetization (M_s), remnant magnetization (M_r), and coercivity (H_c) all showed declining trends with the increase in Mn²⁺ doping. Finally, the CoMn_0.20Fe_1.8O₄ samples showed M_s and M_r values ranging from 73.12 to 66.84 emu/g and from 37.77 to 51.89 emu/g, respectively, while H_c values ranged from 1939 to 1312 Oe, after which coercivity increased. Thus, the CoMn_0.20Fe_1.8O₄ sample can be considered a promising candidate for magnetic applications.

Three sets of MXene (Ti₃C₂T_x)@nano-Fe₁Co_0.8Ni₁ composites with 15, 45, and 90 mg MXene were prepared by in-situ liquid-phase deposition to effectively investigate the impact of the relationship between MXene (Ti₃C₂T_x) and nano-Fe₁Co_0.8Ni₁ magnetic particles on the electromagnetic absorption properties of the composites. The microstructure, static magnetic properties, and electromagnetic absorption performance of these composites were studied. Results indicate that the MXene@nano-Fe₁Co_0.8Ni₁ composites were primarily composed of face-centered cubic crystal structure particles and MXene, with spherical Fe₁Co_0.8Ni₁ particles uniformly distributed on the surface of the multilayered MXene. The alloy particles had an average particle size of approximately 100 nm and exhibited good dispersion without noticeable particle aggregation. With the increase in MXene content, the specific saturation magnetic and coercivity of the composite initially decreased and then increased, displaying typical soft magnetic properties. Compared with those of the Fe₁Co_0.8Ni₁ magnetic alloy particles alone, MXene addition caused an increasing trend in the real and imaginary parts of the dielectric constant of the composite. Meanwhile, the real and imaginary parts of the magnetic permeability exhibit decreasing trend. With the increase in MXene addition, the material attenuation constant increased and the impedance matching decreased. The minimum reflection loss increased, and the maximum effective absorption bandwidth decreased. When the MXene addition was 90 mg, the composite exhibited a minimum reflection loss of −46.9 dB with a sample thickness of 1.1 mm and a maximum effective absorption bandwidth of 3.60 GHz with a sample thickness of 1.0 mm. The effective absorption bandwidth of the composites and their corresponding thicknesses showed a decreasing trend with the increase in MXene addition, reducing by 50% from 1.5 mm without MXene addition to 1 mm with 90 mg of MXene addition.

To address the limitations associated with conventional Fenton processes, which often exhibit a restricted pH range and present challenges in terms of catalyst recovery and second pollutant, magnetic heterogeneous halloysite (HNT)/MnFe₂O₄ catalysts were optimally synthesized, which could achieve 90% removal efficiency for 50 mg/L methylene blue (MB) at pH 4–10 and have high hydrogen peroxide (H₂O₂) utilization efficiencies. In addition, the catalysts could be easily separated from a solution through magnetic separation. The degradation efficiency of MB exhibited remarkable resilience against common aqueous interferents with anions (NO₃⁻, Cl⁻, SO₄²⁻) and humic acid, demonstrating negligible inhibitory effects. Notably, carbonate species (CO₃²⁻ and HCO₃⁻) even elicited a promotional effect on the catalytic process. Furthermore, the removal efficiency of MB only decreased by less than 10% in the fifth cycle compared with that of a fresh catalyst. Furthermore, the HNT/MnFe₂O₄ catalyst effectively degraded various organic pollutants, such as benzohydroxamic acid, xanthate, and eosin Y. The excellent catalytic performance of the catalysts was attributed to the synergistic effects between HNT and MnFe₂O₄. The electron paramagnetic resonance spectra and quenching experiments indicated that the main reactive oxygen species that participated in the degradation process were ·OH and ·O₂⁻. ·OH directly attacked MB molecules, and ·O₂⁻ accelerated the reduction of metal ions. Therefore, the catalysts showed considerable potential for organic pollutant degradation. This study provides valuable insights into the synthesis of novel catalysts and their practical applications in organic wastewater purification.