This study uses density functional theory (DFT) to investigate the selective hydrogenation of acetylene (C2H2) on palladium-based catalysts with core@shell (M13@Pd42) and Crown-Jewel (CJ-M43Pd12) structures. The influence of Cu, Ag, and Au dopants are evaluated to guide the design of highly efficient Pd-based catalysts for converting acetylene to ethylene (C2H4). The calculation reveals that the Crown-Jewel structured Cu43Pd12 (CJ-Cu43Pd12) catalyst exhibits superior activity and selectivity for ethylene production compared to the core@shell structured Cu13@Pd42 and the pure Pd55 catalysts. Electronic structure analysis reveals that the Cu-Pd interaction and electron transfer from Cu to Pd enhance performance in the CJ-Cu43Pd12 catalyst. The findings highlight the significance of geometrical and electronic considerations in the design of catalytic systems for acetylene hydrogenation. These results establish an atomistic theoretical framework for Pd-efficient acetylene semihydrogenation catalysts, demonstrating that the Crown-Jewel geometry can integrate Pd-site isolation and Cu to Pd electronic modulation to balance C2H2 activation, C2H4 desorption, and Pd atom utilization efficiency.

Natural flake graphite exhibits superior oxidation and corrosion resistance among carbon sources, but its hydrophobicity and poor dispersion limit its use in refractory castables, increasing water demand and degrading high-temperature performance. In this study, AlOOH nanofiber-coated graphite (G@AlOOH) was prepared via a hydrothermal method to address these issues. Monte Carlo simulation was employed to reveal the growth mechanism of nanofibers on graphite surfaces. The uniform AlOOH coating creates a rough structure and introduces hydrophilic hydroxyl groups, reducing the water contact angle from 95.2° to 26.0°. Rheological and settling tests confirm improved dispersion and reduced viscosity. Consequently, Al2O3-SiC-C castables with G@AlOOH show lower water demand, reduced porosity, higher bulk density, and enhanced thermal shock resistance and slag corrosion resistance.

Hydrogen production via water electrolysis is a promising route toward sustainable and carbon-free energy. Transition metal dichalcogenide (TMD) nanosheets have emerged as efficient electrocatalysts for the hydrogen evolution reaction (HER), owing to their tuneable electronic properties and abundant active sites. In this study, we report the in-situ solvothermal synthesis of a compositionally tuneable library of molybdenum sulfoselenide (MoS2(1-x)Se2x) nanosheets uniformly anchored on reduced graphene oxide (rGO). The resulting MoS2(1-x)Se2x/rGO nanocomposites exhibit significantly enhanced HER activity, with the optimal MoS0.6Se1.4/rGO sample achieving a current density of 10 mA cm−2 at a low overpotential of 118 mV and a Tafel slope of 46.6 mV dec−1 in acidic media. The improved performance is attributed to the synergistic effects of sulfur and selenium incorporation, which modulate hydrogen adsorption energy, enhance orbital hybridization (Mo 4d, S 3p, Se 4p), and facilitate charge separation. Density functional theory (DFT) simulations further reveal that the Janus-type configuration enhances electronic conductivity and reactivity. The rGO substrate provides a conductive framework, promoting efficient charge transport and mechanical stability. These findings demonstrate that interface-engineered MoS2(1-x)Se2x/rGO hybrids are highly efficient and tunable HER catalysts, offering valuable insights for the design of advanced electrocatalytic materials.

Y2O3-enhanced MgO refractory crucibles were fabricated based on a novel design of Y2O3 crystal boundary-enhanced magnesia raw materials, and the interface reactions between the Y2O3-enhanced MgO refractory crucibles and Ni-TiAl superalloy were explored. Micro-CT analysis revealed no substantial infiltration or structural damage to the crucible after two cycles of melting. Y2O3 was found to uniformly distribute along MgO grain boundaries, forming a protective core-shell structure that effectively isolates MgO grains from direct contact with the alloy melt. This unique core-shell structure significantly enhanced the crucible's corrosion resistance. Furthermore, a dense MgCr2O4 spinel layer formed at the alloy-crucible interface, serving as a robust barrier against further refractory corrosion. The utilization of high-purity magnesia from Salt Lake resources not only minimized impurity-driven interfacial reactions but also endowed the crucible with superior performance.

This study investigated the high brittleness and inadequate thermal shock resistance of conventional conventional Al2O3-MgO refractory castables by incorporating aluminosilicate fibers. The interfacial evolution between the fibers and the matrix, along with the subsequent toughening mechanisms, were systematically characterized. Experimental results demonstrated that the 0.02 wt%-adding aluminosilicate fibers significantly enhanced the thermal shock resistance by 19%. SEM results indicated that the performance enhancement was primarily attributed to the in-situ formation of calcium hexaluminate (CA6) coatings on the fiber surfaces. This reaction-bonded interface strengthens the adhesion between the fibers and the matrix, leading to a synergistic improvement in both fracture toughness and thermal shock resistance. Furthermore, wedge splitting tests coupled with digital image correlation revealed significant fiber bridging, pull-out, and interlocking behaviors during crack propagation, which effectively reduced the material's brittleness.

The application of graphene nanosheets (GNs) in low-carbon refractories is hindered by their poor dispersibility and weak interfacial bonding with the matrix of the latter. In this work, we developed a phenolic resin (PF) assisted ball milling exfoliation strategy using flake graphite (FG) as the raw material to prepare a homogeneous GNs/PF slurry, this approach enables the in-situ exfoliation of FG into well-dispersed GNs. When incorporated into MgAl2O4-C refractories, the GNs/PF slurry significantly improved the homogeneous dispersion and interfacial bonding of the GNs with MgAl2O4. Compared to the control samples with and without FG, the counterpart containing GNs exhibited superior high-temperature performances, including an increase of up to 60 % in oxidation resistance, an 18.7 % improvement in thermal shock resistance, and a significant reduction in slag penetration depth from 1095 mu m to 590 mu m. This work establishes an economically feasible route for the largescale production of high-performance GNs-reinforced low-carbon refractories.

Sodium-ion batteries are promising candidates for large-scale energy storage because of the abundance and low cost. However, cathode development remains a major bottleneck. O3-type layered oxides exhibit high theoretical capacities, yet their polycrystalline nature causes renders them susceptible to grain-boundary fracture during cycling, resulting in capacity degradation. By contrast, single-crystal structures offer superior structural robustness and electrochemical stability but face challenges in synthesis due to their intrinsic sensitivity to air and moisture. Herein, we report a NaBr-assisted molten-salt route to fabricate large-sized O3-type NaCu0.1Fe0.42Mn0.48O2 single-crystals with large lateral size up to 27.3 μm. The cathode delivers an initial discharge capacity of 126 mAh g-1 within 2.0-4.2 V. After 100 cycles at 0.5 C, the cathode retains 70% of its initial capacity. Structural characterization confirms excellent lattice integrity and interfacial stability during cycling. This work provides a valuable strategy for O3-type layered oxides and the development of sodium-ion batteries.

Electrochemical CO2 reduction to formate is attractive for sustainable chemical production, but further progress is limited by the difficulty of simultaneously regulating selectivity, interfacial transport, and catalyst stability in Cu-based systems. Herein, we report a boron-modified dual-layer hollow CuInCeOx nanotube catalyst (B(CuInCe)Ox-DNTs), which can serve as a multicomponent oxide platform for facilitating the electroreduction of CO2 to formate. Boron incorporation is used to regulate the local electronic/defect environment, while the dual-layer hollow nanotube architecture improves interfacial accessibility and gas/electrolyte transport. The optimized catalyst delivers a formate Faradaic efficiency of 74.87% at −1.0 V vs. RHE with a partial current density of 21.12 mA cm−2 in an H-type cell. Structural and spectroscopic analyses reveal that boron incorporation suppresses CuO crystallization, increases oxygen-deficient species, and stabilizes low-valent Cu/Ce surface states. In-situ spectroscopic studies and theoretical calculations further indicate that boron incorporation strengthens CO2 adsorption and lowers the free-energy barrier of the key *OCHO → *HCOOH protonation step, thereby shifting the reaction competition toward the formate pathway. This work provides a multicomponent oxide design strategy for understanding and regulating the interfacial behavior of Cu-based catalysts in formate-selective CO2RR.

Ammonia production remains energy-intensive and high carbon emission through conventional processes, making the conversion of aqueous nitrate pollutants into ammonia a "waste-to-wealth" strategy. Current nitrate treating methods including photocatalysis and electrocatalysis are respectively limitted by light shielding effect and complex electrode fabrication. Here we propose a novel and efficient microwave catalytic approach for nitrate to ammonia conversion using a Pd-dispersed fiber-structured ZnFe2O4@Carbon@MoS2 (Pd-FCM) catalyst, demonstrating remarkable efficiency even with a household-microwave-oven. This approach achieves an exceptional ammonia yield rate of 20.04 mmol h- 1 L- 1 and a total ammonia yield of 5.52 mmol, outperforming most photocatalytic and electrocatalytic approaches. This exceptional catalytic performance stems from the synergistic effects of ZnFe2O4@Carbon's microwave absorption, MoS2's nitrate adsorption, and the activation energy reduction by Pd nanoclusters. Our work advances sustainable nitrogen management by integrating wastewater denitrification with green ammonia synthesis, contributing to the circular nitrogen economy and sustainable development goals.

The electrochemical nitrate reduction reaction (e-NO3RR) is a green pathway for ammonia synthesis with subsequent recovery of the nitrogen cycle. However, kinetics under neutral pH conditions is challenging since water dissociation becomes slow and inadequate active hydrogen (*H) species to participate. The study systematically designs an atomically precise dual-site catalyst by engineering Ru single atoms supported on ultrathin nanosheets of cobalt-based metal-organic frameworks (MOFs). According to kinetic isotope effects (KIEs) evaluation, hard-soft acid-based (HSAB) poisoning tests, and in situ spectroscopic analysis, Ru single atom sites serve as efficient proton pumps lowering significantly the barrier for water dissociation. The produced *H species are transferred to adjacent oxygen-bridged cobalt sites, facilitating the hydrogenation as well as deoxygenation processes of N & horbar;O. The proximity of these atoms has a combined effect that reduces the gap in rate between nitrate reduction and proton supply, yielding a faradaic efficiency of ca. 97% and an ammonia production rate of 562.44 & micro;mol h-1 cm-2. This study not only fixes the age-old "hydrogen lack" problem in neutral e-NO3RR but also gives an atom-level view into the two-site electron-proton transfer link, thus setting up a general design model for working active sites in complex many-electron electrocatalytic steps.

This study investigated the effect of mullite-corundum fibers on the brittleness and thermal shock resistance of conventional Al2O3-MgAl2O4 refractory castables. The interfacial evolution between the fibers-adding and the matrix, along with the subsequent toughening mechanisms, were systematically discussed. The results demonstrated that the 0.2 wt%-adding mullite-corundum fibers significantly enhanced the thermal shock resistance, with the residual strength retention rate increasing from 31% to 37%. SEM revealed that this was primarily attributed to the strong bonding between the fiber interface and the matrix, which resulted from the in-situ formation of CA6 and interface roughening due to fiber recrystallization. Furthermore, these interfacial modifications significantly affected the fracture behavior. The wedge splitting tests combined with digital image correlation (DIC) confirmed that the fibers-adding successfully facilitated a transition from brittle to quasi-ductile fracture in the conventional castables. This transition was attributed to effective energy dissipation through fiber bridging and the increased tortuosity of crack propagation paths.

The catalytic conversion of polysulfides remains a critical bottleneck in the development of high-performance lithium-sulfur batteries (LSBs). Despite extensive efforts to engineer carbon-based materials for LSBs, such as nitrogen (N)-doped graphene, the intrinsic limitations of conventional N-doped configurations have hindered catalytic effectiveness. Here, we reveal how the curvature-rich structure of N-doped graphene (N-CR-G) regulates catalytic properties to promote the sulfur reduction reaction (SRR). This architecture induces a diversity of active N configurations and optimizes the local electronic structure, directly accelerating the polysulfide redox kinetics. Unlike conventional carbon-based materials, the main N-doped configuration of N-CR-G catalyzes an uncommon asymmetric reaction pathway involving the rapid generation of soluble S3 & sdot;- radicals, effectively suppressing the accumulation of insoluble Li2S2 intermediates and enhancing sulfur utilization. While the curvature structure also facilitates carbon vacancy formation and enables room-temperature N doping, its primary contribution lies in tailoring the catalytic landscape of graphene. This work underscores the significance of curvature engineering for activating and regulating electrocatalytic behavior, offering a powerful strategy to design advanced cathode materials for highly promising LSBs.

The functionalization of refractories, which means refractory lining adsorbs exogenous inclusions and improves the cleanliness of steel, is always desired and pursued. This study investigated corrosion mechanism of MgO-C refractory at the bottom of a converter utilizing submerged O2-lime powder injection. X-ray Computed Tomography (CT) and SEM characterizations revealed the presence of a thin adherence slag layer on the refractory surface, comprising spalled MgO aggregates and an FeOt-rich phase-a phenomenon driven by the enhanced oxidation during O2 blowing. It was confirmed that the fine Ca2SiO4-Ca3P2O8 solid solutions particles were generated and embedded within the degraded layer of the refractory lining. It provided direct empirical evidence of the deteriorated layer's capacity to adsorb exogenous inclusions. Furthermore, the role of the bottom-blowing O2/CaO operation in facilitating the inclusion-removal function, mediated by the liquid-phase isolation layer, was systematically analyzed. Microstructural analysis further elucidated that the MgO aggregates at the corroded interface underwent two distinct degradation pathways: intergranular corrosion and a direct solid-liquid diffusion reaction.

Low-carbon MgO-CaO-C refractories are promising for clean steel refining, but their application is limited by CaO hydration and the deterioration of high-temperature performance caused by reduced carbon content. In this work, a CNTs/CaCO3 co-coated MgO-CaO powder (CC-MCP) was successfully fabricated via a densified microzone deposition process employing MgO-CaO particles, polyethylene powder, and starch as raw materials. The as-prepared CC-MCP was incorporated into low-carbon MgO-CaO-C refractories to achieve a "two birds with one stone" effect, simultaneously enhancing both hydration resistance and high-temperature service performance. Compared to the control sample prepared with flake graphite as the carbon source, the counterpart containing CC-MCP exhibited superior hydration resistance and high-temperature performances, including a 286% improvement in water vapor resistance, an increase of up to 209% in oxidation resistance, a 36% improvement in thermal shock resistance, and a reduction in slag penetration depth from 654 mu m to 435 mu m. This "two birds with one stone" strategy provides an effective and scalable route for developing high-performance ultralow -carbon MgO-CaO-C refractories for clean steel production, while simultaneously offering a practical solution to the hydration challenges faced by CaO-containing refractories under harsh storage and service conditions.

Flake graphite (FG) limits the development of high-performance carbon-containing castables due to its inherent hydrophobicity. In this study, a graphene nanosheet/nano-MgAl hydrotalcite (GN/MAH) composite powder was successfully synthesized via a hydrothermal method. Under optimal conditions, the water contact angle of the composite powder was reduced from 103.6 degrees for GNs to 44.6 degrees, indicating significantly improved hydrophilicity. The incorporation of the GN/MAH composite powder markedly enhanced the mechanical performance of the castables after heat treatment at 1600 degrees C. Compared with the reference sample (0#), the cold modulus of rupture and hot modulus of rupture increased by 77.22 % and 54.91 %, respectively. Furthermore, the uniform dispersion of GNs within the castable matrix facilitated the maintenance of superior high-temperature performance even with a reduced carbon content of similar to 0.15 wt%. As a result, the residual strength ratio of the castable after thermal shock increased by 13.69 %, while the slag corrosion index decreased by 43.26 %.

Catalyst microstructure and defect engineering are key strategies for boosting photocatalytic activity. In this study, Cu-doped hollow spherical g-C3N4 (Cu/HSCN) were fabricated using an in-situ chemical vapor deposition method. In contrast to bulk g-C3N4, the as-prepared HSCN exhibited a significantly enlarged surface area and mesoporosity, enabling improved light harvesting and mass transport. Moderate copper incorporation not only regulated nitrogen vacancy concentrations but also introduced sub-bandgap defect states. This defect engineering led to enhanced visible-light absorption and suppressed charge recombination. Band structure analysis revealed that Cu doping induced a downshift in the valence band and a reduction in the conduction band energy level, thereby enhancing the redox capacity of photogenerated carriers. Among the samples, the one with a copper loading of 0.18 % achieved the highest photocatalytic performance toward ketoprofen (KP) degradation, reaching a 99.9 % removal rate and a pseudo-first-order kinetic constant of 0.036 min(-1), nearly six times greater than that of bulk g-C3N4. Radical trapping and EPR experiments determined center dot OH and center dot O-2(-) to be the primary reactive species, while LC-MS and TOC analyses confirmed stepwise oxidative degradation and near-complete mineralization. The present work offers a comprehensive strategy combining structural design and electronic modulation for developing high-performance photocatalysts for pharmaceutical pollutant remediation.

Utilization of iron tailings to fabricate foam ceramics is of significant research value in both recycling of waste resources and meeting the demand for high-performance building insulation materials. In this work, foam ceramics were successfully fabricated using iron tailings via a foaming gel-casting method. Precise control of the foaming time could enable an effective tuning of the pore structure in foam ceramics. As-prepared foam ceramics showed a hierarchical porous structure with porosities of 61.82 %-80.07 %, compressive strengths of 3.08-13.02 MPa, and thermal conductivities of 0.184-0.351 W m(-1) K-1. After re-heating at 1150 degrees C for 10 h, the foam ceramics retained their original microstructure with a line shrinkage of 0.96 %. When they were further fired under an alcohol blowtorch at similar to 1105.7 degrees C for 40 min, the backside temperature of the foam ceramic was only 205.6 degrees C. These comprehensive properties make this tailings-based foam ceramic a promising lightweight material for fire-resistant and thermal insulation in construction and industry.

Conventional plasma-based advanced oxidation processes for wastewater treatment are often limited by the use of metal electrodes, which are susceptible to corrosion, secondary contamination, and poor scalability. To overcome these challenges, a novel metal-free microwave-induced carbon cloth discharge technology was developed in this study. The flexible and conductive carbon cloth acts as an efficient plasma-generation medium. Under microwave irradiation, intense localized electric fields are generated at the fiber tips, inducing dielectric breakdown at the gas-liquid interface and thereby initiating a stable plasma discharge. This process generates abundant reactive oxygen species (e.g., ·O2- and ·OH) that efficiently degrade Rhodamine B (RhB). Under optimal conditions (700 W microwave power, 3 g/L carbon cloth, pH 7, and Ar atmosphere), the microwave-induced carbon cloth discharge system achieves a high RhB removal efficiency of 98.42% and a significant mineralization rate (76.6% TOC removal) within 90 min. The system also demonstrates robust performance across a range of RhB concentrations, exceptional stability over multiple reuse cycles (∼95% removal efficiency after 8 cycles), and effective detoxification of the treated solution. Overall, this work presents a cost-effective, corrosion-resistant, and scalable plasma technology, offering a promising green strategy for the treatment of refractory organic wastewater.

MgO-based refractories, known for their high refractoriness, strong resistance to basic slags, and excellent thermal stability, are widely used as lining materials in the metallurgical industry, particularly in steelmaking. However, the interaction mechanisms between CaO-MgO-Al2O3-SiO2 (CMAS) slag and MgO at high temperature remain complex and are not fully understood. In this study, ab initio molecular dynamics (AIMD) simulations were employed to investigate the atomic-scale interaction mechanisms between CMAS slag and MgO surfaces with different crystallographic orientations. The results reveal that while MgO(100) and MgO(110) surfaces exhibit weak interfacial bonding and limited atomic diffusion, the MgO(111) surface undergoes pronounced atomic interdiffusion and bidirectional charge transfer, resulting in the highest interfacial interaction energy (8.67 J & centerdot;m- 2). The dynamic balance between the stabilizing covalent network of Al-O bonds (which inhibits diffusion) and the ionic redistribution of Ca/Mg (which promotes melting) is the critical factor determining the material's corrosion resistance. The findings provide a theoretical basis for optimizing the CMAS/MgO interfacial stability, thus providing guidance for improving the high-temperature performance and corrosion resistance of MgO-based refractories.

Developing efficient electrocatalysts for the oxygen evolution reaction (OER) is crucial for advancing renewable energy conversion technologies. Herein, phosphorus- engineered high-entropy oxide hollow nanofibers (HEPi-HNFs) with a crystalline-amorphous hybrid structure are rationally designed via electrospinning followed by controlled phosphorization. The optimized HEPi-HNFs catalyst consists of spinel (FeCoNiCrMn)3O4 nanocrystals uniformly embedded within an amorphous phosphate matrix, generating abundant oxygen vacancies and interfacial active sites. Benefiting from the synergistic effects of multimetal active centers, electronic modulation induced by phosphate groups, and enhanced mass transport in the hollow porous architecture, the optimal HEPi-HNFs exhibits outstanding OER activity with a low overpotential of 237 mV at 10 mA cm-2 and excellent stability over 120 h. Mechanistic studies and density functional theory calculations reveal that phosphorus incorporation activates lattice oxygen and shifts the OER pathway from the conventional adsorbate evolution mechanism to the lattice oxygen-mediated mechanism.