Search Results (2,604)

A novel K-resistant CeSbTi mixed oxide catalyst was prepared by co-precipitation method for ammonia selective catalytic reduction (NH₃-SCR) of NO_x. The experimental results show that the introduction of Sb₂O₅ can significantly improve the catalytic activity of the CeTi catalyst. The modulated CeSbTi catalyst has good resistance to K, and the NO_x conversion rate was as high as 95% after K poisoning. Its superior catalytic activity could be ascribed to the large specific surface area with increased acid sites and more oxygen defects and Ce³⁺ species after the introduction of Sb₂O₅, which prompt NH₃ adsorption and activation. In addition, NH₃-SCR reaction over CeSbTi and K/CeSbTi catalysts follows the E-R mechanism. The introduced Sb-O bond as the base capture site preferentially binds to potassium and releases part of the active Ce sites, thus retaining more acid sites and oxygen defects to a certain extent. Full article

An efficient catalyst for the reaction of ethanol–acetaldehyde into 1,3-butadiene (EATB) is prepared through the grafting of zirconia into a zeolite Beta lattice. The grafting is achieved through the dealumination of a zeolite framework by acid treatment followed by zirconia impregnation, leading to the substitution of aluminum in the zeolite framework by zirconia. The catalyst with zirconia grafted into the zeolite framework promotes desirable catalyst properties like high zirconium dispersion, stability, and the close proximity of Lewis acid, Bronsted acid, and medium basic sites. The phase, the coordination of zirconia, the location of the active center and the cooperative synergism were elucidated through various characterization techniques, including X-ray diffraction, Raman spectroscopy, N₂ adsorption, UV–vis spectroscopy, XPS, ²⁹Si MAS NMR, NH₃-TPD, Py-IR, CO-IR and CO₂-TPD. The catalytic results show that a suitable phase and content of zirconia were needed to improve the ethanol–acetaldehyde conversion, butadiene selectivity and catalyst stability. Among the catalysts, m+t-ZrO_x-Beta-H₂O-9020 (m = monoclinic, t = tetragonal ZrO₂ phase) achieved the best butadiene selectivity of 82–73% at the conversion of 100–66%, run over 200 h. The results allow us to propose a Lewis acid–medium basic pairing for the Si–O–Zr–O–Si group, where the adjacent Si-OH is the active center for reactions. Full article

Petroleum hydrocarbons contamination in soil is difficult to remediate due to strong adsorption and limited bioavailability. This study investigated the coupled remediation of diesel contamination in an alkaline kaolin-based model substrate using a silica gel-loaded, iron-catalyzed sodium percarbonate composite (SPC^SF) and Bacillus subtilis. The alkaline model substrate was used as a simplified representation of difficult-to-reclaim hydrocarbon- and reagent-impacted matrices that may occur at oil drilling or production sites. In this study, a combined remediation strategy integrating a silica gel-loaded, iron-catalyzed sodium percarbonate composite (SPC^SF) with Bacillus subtilis ATCC 11774 was developed for diesel-contaminated soil. The remediation performance of chemical oxidation, microbial remediation, and their combined application was systematically evaluated. The simultaneous SPC^SF–microbial treatment achieved the highest removal efficiency, reaching 65.1% after 31 d, which was markedly higher than that of chemical oxidation (22.5%) or microbial remediation alone (31.1%). Within the mineral model substrate used in this study, SPC^SF effectively regulated pH and oxidation–reduction potential, creating conditions more favorable for microbial activity. Spectroscopic analyses (three-dimensional fluorescence spectrum, Fourier transform infrared spectroscopy, and X-ray photoelectron spectroscopy) indicated that SPC^SF promoted the transformation of diesel hydrocarbons into bioavailable intermediates, which were further converted by microorganisms into carboxyl-rich organic matter. Bacillus subtilis was associated with a higher Fe(II) proportion in the coupled system, which may have favored maintenance of Fe redox activity and sustained Fenton-like reactivity. However, direct measurements of reactive oxygen species and Fe(II)/Fe(III) dynamics were not performed; therefore, this interpretation should be regarded as a plausible hypothesis based on indirect evidence. The specific microbial contribution to Fe redox transformation was inferred from indirect evidence and may also have been influenced by medium-derived components or microbial metabolites. This study presents a coupled supported sodium percarbonate and microbial remediation strategy providing mechanistic evidence for the compatibility of supported chemical oxidation and microbial degradation in diesel-contaminated soil. Full article

The purpose of this study was to investigate the effectiveness and mechanism of iron-based catalysts in the treatment of phenolic wastewater by catalyzing ozone oxidation. The removal rates of phenolics and COD were systematically examined using simulation experiments with water and actual wastewater, which involved analyzing the effects of reaction time, pH, ozone dosage, catalyst dosage, and initial concentration. The phenol and COD removal rates in the simulated wastewater were 95.9% and 93.5%, respectively, respectively, while the ozone dosage was 16 mg/L/min, pH was 6.7–6.8, and catalyst dosage was 0.3 g/L. The phenol and COD removal rates in the actual wastewater were 68.6% and 68.0%, respectively. The reaction time was 30 min. The system’s efficient removal ability for phenolic compounds, polycyclic aromatic hydrocarbons, and others was confirmed through three-dimensional fluorescence and ultraviolet spectroscopy. The iron-based catalyst generates ·OH through three pathways: adsorption of activated ozone on surface active sites, continuous production of free radicals by Fe²⁺/Fe³⁺ cycling, and direct activation of ozone by Fe²⁺. This mechanism analysis showed that the catalyst generates ·OH. These pathways convert pollutants into small molecules or mineralized by attacking the aromatic rings and conjugated structures of pollutants. Technical references for the deep treatment of phenol-containing wastewater are provided in this study. Full article

In this study, activated biochars derived from spent coffee grounds (CAC-600) and lemon pomace (LAC-600) were prepared through pyrolysis with FeCl₃ activation and evaluated for the selective adsorption of Acid Blue 74 (AB74), a dye widely used in the denim textile industry. FeCl₃ activation significantly increased the surface area and pore development relative to the pristine biochars, while also promoting the formation of Fe₂O₃ phases on the activated biochars surfaces. The activated biochars exhibited comparable adsorption capacities of 39.44 and 37.16 mg·g⁻¹ for CAC-600 and LAC-600, respectively, indicating that adsorption performance was governed mainly by the activation process rather than by the precursor biomass. Isotherm and kinetic models revealed heterogeneous adsorption behavior involving surface interactions combined with internal diffusion. The materials showed stable adsorption performance within a pH range of 4–10. Competitive adsorption experiments demonstrated preferential adsorption of AB74 over Acid Red 1 (AR1), confirming the selectivity of LAC-600 and CAC-600. Density Functional Theory (DFT) calculations revealed a cooperative adsorption mechanism combining π-surface interactions with localized Fe-oxide anchoring sites on the graphene-based model, increasing the adsorption energy by approximately 24 kcal·mol⁻¹ relative to carbon-only systems. These findings demonstrate the potential of Fe-activated agro-industrial biochars as adsorbents for dye removal from aqueous media. Full article

The presence of residual moisture in tetrahydrofuran (THF) greatly limits its suitability for moisture-sensitive processes, including polymerization, Grignard chemistry, and fine-chemical production, where the allowable water concentration is generally lower than 10 mg/kg. Here, a hierarchical microporous/mesoporous composite adsorbent was prepared via extrusion molding, combining an LTA-type zeolite microporous framework with an amorphous mesoporous matrix. Characterization by XRD, FTIR, SEM, and pore analysis confirmed that the LTA crystal structure was retained while mesopores provided channels for mass transport. Static dehydration tests showed that the composite reduced THF water content from 70 mg/kg to 8.3 mg/kg, compared to 23.4 mg/kg for commercial 3A molecular sieves. The enhanced performance arises from micropores supplying uniform adsorption sites for deep dehydration and mesopores accelerating diffusion. Water vapor adsorption, kinetic and isotherm analyzes, regeneration, and competitive adsorption experiments indicated improved water accessibility and high selectivity, with kinetics described by a double-exponential model. The adsorbent remained stable over six adsorption–regeneration cycles. These results demonstrate that hierarchical microporous/mesoporous structures effectively achieve deep THF dehydration. Full article

Inorganic mercury ions (Hg²⁺) are highly toxic, posing a threat to aquatic ecosystems and human health. In this study, iron phthalocyanine (FePc) was anchored onto the surface of MXene via a self-assembly strategy to construct an FePc/MXene-x (F/M-x) heterostructure. Characterization by scanning electron microscopy (SEM), transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS), and nitrogen adsorption–desorption (BET) confirmed that the high specific surface area and good conductivity of MXene effectively inhibited FePc aggregation and increased the exposure of active sites. The F/M-x composite was then modified onto a glassy carbon electrode (GCE) to fabricate an electrochemical sensor, and the detection performance for Hg²⁺ was evaluated using square-wave anodic stripping voltammetry (SWASV). Under optimized conditions (pH = 5.0, accumulation at −1.2 V for 180 s), the F/M-100/GCE exhibited a linear range of 0.1–1.0 μM, a sensitivity of 19.02 μA/μM, and a detection limit of 5.9 nM. The sensor showed good anti-interference ability against coexisting metal ions such as Cd²⁺, Cu²⁺, and Pb²⁺, with a batch-to-batch RSD of 2.03% and a long-term stability RSD of 2.49%. Spike recovery experiments in real water samples (lake water and groundwater) verified the accuracy of the method. This study provides a new electrochemical platform for the rapid detection of trace Hg²⁺ in water environments. Full article

In nitrate electrochemical reduction reaction (NO₃RR), competing side reactions like hydrogen evolution often lead to poor selectivity and subpar kinetics, limiting practical use. Herein, using iron oxyhydroxide nanoarrays grown on a titanium mesh as the substrate, silver nanoparticles were introduced onto the tips of the iron oxyhydroxide nanowires via electrochemical deposition, thereby forming an Ag/FeOOH heterojunction electrocatalyst. At −0.85 V, Ag/FeOOH demonstrates excellent performance, with 97.56% ammonium selectivity, 92.45% nitrate conversion rate, and an ammonium yield of 3.21 mg h⁻¹ cm⁻². Furthermore, the Zn-NO₃⁻ battery exhibited a power density of 1.28 mW cm⁻². Ag/FeOOH’s structure enhances interfacial nitrate adsorption and reduces NO₃RR energy barriers, accelerating reaction kinetics. It promotes NO₃⁻-to-NO₂⁻ conversion via dual-site synergy, boosting NH₄⁺ yield and advancing electrocatalyst design. Full article

Zeolites, both natural (e.g., clinoptilolite) and synthetic (e.g., FAU, ZSM-5), provide robust, tunable platforms for the removal of air pollutants and process-stream contaminants via adsorption and catalysis. This author-led article integrates experimental and theoretical insights on the adsorption of odorous compounds and ammonia (NH₃) and the catalytic abatement of nitrogen oxides (NOx) and nitrous oxide (N₂O), highlighting how topology, acidity, and metal speciation jointly control performance. Representative theoretical results show that adsorption on Brønsted acid sites is significantly more favorable (≈−1.1 eV for NH₃ and −0.37 eV for acetaldehyde) than on Na⁺ sites (≈0.02 eV and 1.22 eV, respectively), demonstrating the critical role of acid site distribution in adsorption selectivity. We dissect structure–function relationships encompassing pore size and connectivity, Si/Al ratio, Brønsted/Lewis site distribution, hydrophilicity/hydrophobicity, and the role of water, with emphasis on hierarchical porosity to alleviate transport limitations. Metal exchange and surface functionalization are discussed as levers to tailor adsorption strength and redox activity, supported by density functional theory (DFT) analyses and reaction pathways. We propose practical design descriptors (acid strength metrics, metal nuclearity, and confinement factors) that enable faster iteration of zeolite architecture for targeted separations and reactions. Sustainability considerations include the use of abundant natural zeolites, low-energy regeneration, stability under humid, mixed-stream conditions that minimize pressure drop and waste. The article closes with a forward look at data-guided optimization to accelerate “engineering zeolites” for durable, selective, and energy-efficient clean-air and process-intensification applications. Full article

Pd-decorated Janus ZrSSe monolayers provide a promising platform for adsorption-coupled electronic modulation in two-dimensional materials. Using first-principles density functional theory, we systematically investigate the structural stability, electronic properties, and adsorbate-induced electronic response of Pd-modified Janus ZrSSe. The results show that Pd is most stably anchored at the hollow site on the S-terminated surface, with a formation energy of $-1.45$ eV, while substitutional incorporation remains energetically unfavorable even after HSE06 refinement. Compared with pristine ZrSSe, Pd decoration markedly strengthens the interaction with adsorbates, leading to strong chemisorption for CO ($-1.026$ eV) and C₂H₂ ($-0.748$ eV), whereas H₂ remains comparatively weakly bound ($-0.258$ eV). Electronic-structure analysis reveals that CO induces the most pronounced perturbation because of strong orbital hybridization between Pd 4d states and C/O 2p states, resulting in the largest band-edge modulation among the three adsorbates. More importantly, biaxial strain provides an effective external degree of freedom for continuously tuning the electronic structure: tensile strain widens the band gap, whereas compressive strain systematically narrows it and ultimately drives a semiconductor-to-metal transition at sufficiently large compression. These findings establish Pd-decorated Janus ZrSSe as a strain-tunable electronic material in which adsorption, orbital hybridization, and band-edge evolution are intimately coupled, offering fundamental insights into controllable electronic modulation in polar two-dimensional systems. Full article

Sodium caseinate (SC)-stabilized emulsions are highly susceptible to flocculation and phase separation near the protein isoelectric point (pI), limiting their application in acidified food systems. In this study, high acyl gellan gum (HA) was introduced to construct pH-responsive protein–polysaccharide complexes to modulate the interfacial assembly and stability of SC emulsions. Results demonstrated that HA interacts with SC primarily through electrostatic attraction and multi-site hydrogen bonding. This interaction induces protein conformational rearrangement and, as evidenced by combined structural and computational analyses, facilitates the assembly of a denser, interconnected composite network. The formation of HA–SC complexes significantly enhanced interfacial adsorption, reduced oil–water interfacial tension. Rheological and microrheological analyses revealed the composite system formed an elasticity-dominated weak gel network, restricting droplet mobility and suppressing aggregation. Consequently, HA–SC emulsions exhibited markedly improved pH tolerance and physical stability compared to SC-only emulsions, particularly near the pI, evidenced by reduced droplet size, lower Turbiscan stability indices, and more homogeneous microstructures. Crucially, utilizing a well-defined mechanistic model of fixed HA and SC concentrations, this study quantitatively links molecular interactions, interfacial network reconstruction, and macroscopic emulsion stability across a broad pH continuum. Rank-correlation analysis of pH-resolved descriptors shows the molecular charge state co-varies monotonically with the interfacial network and macroscopic stability, and is inversely coupled to droplet mobility. These findings provide new insights into protein–polysaccharide interfacial engineering, establishing the essential physical-stability foundation for the future rational design of acid-tolerant food emulsions and functional delivery systems. Full article

The hydrogen evolution reaction (HER) plays a pivotal role in electrochemical water splitting for sustainable hydrogen production. However, its practical implementation is hindered by sluggish kinetics and the reliance on costly noble-metal catalysts. In this work, a conductive polymer-inorganic hybrid electrode based on vanadium pentoxide (V₂O₅) and polyaniline (PANI) is rationally designed and fabricated on carbon cloth via a combined hydrothermal synthesis and electropolymerization strategy. Initially, hierarchical V₂O₅ nanoflowers were synthesized, followed by controlled PANI deposition through cyclic voltammetry at varying cycle numbers to tailor the interfacial architecture and electronic properties. Morphological and structural analyses reveal the formation of well-defined V₂O₅ nanoflowers uniformly decorated with PANI nanorods, establishing an interconnected conductive network. Among the prepared samples, the optimized V₂O₅-PANI-2 electrode exhibits superior interfacial integration and structural homogeneity. Electrochemical evaluation in 1.0 M KOH demonstrates that V₂O₅-PANI-2 achieves a low overpotential of 79.9 mV at −10 mA cm⁻², accompanied by a small Tafel slope of 46.6 mV dec⁻¹, indicating accelerated HER kinetics. Furthermore, the electrode shows reduced charge-transfer resistance and an enhanced electrochemically active surface area (ECSA), facilitating efficient charge transport and abundant active site exposure. The catalyst also delivers excellent durability, maintaining stable performance over 5000 CV cycles and prolonged 24 h operation. The enhanced HER performance is attributed to the synergistic interaction between V₂O₅ and the conductive PANI matrix, which promotes charge redistribution, improves electrical conductivity, and optimizes the adsorption/desorption energetics of hydrogen intermediates. Full article

Driven by the “Dual Carbon” goals, supercapacitors have become critical energy storage devices for new energy electric vehicles. In this paper, a ZnFe₂O₄@ZnCo₂O₄ core–shell cathode was prepared by a hydrothermal method followed by high-temperature annealing, and an AC@PANI composite anode was synthesized through in situ polymerization. The materials were characterized by SEM, TEM, XRD, XPS, nitrogen adsorption–desorption and electrochemical tests. The ZnFe₂O₄ rod-like core provides mechanical stability, whereas the ZnCo₂O₄ nanosheet shell increases the specific surface area and exposes more active sites. The cathode delivers 2133 F/g at 1 A/g with 94.4% retention after 10,000 cycles. The anode reaches 398 F/g at 1 A/g. The cathode delivers 2133 F/g at 1 A/g with 94.4% retention after 10,000 cycles. The anode reaches 398 F/g at 1 A/g. The assembled ZnFe₂O₄@ZnCo₂O₄//AC@PANI hybrid supercapacitor works in a wide voltage range of 0–1.6 V. It exhibits a specific capacitance of 157 F/g at 1 A/g and a high energy density of 54.7 Wh/kg at a power density of 1600 W/kg. The device retains 91.4% of its initial capacity after 10,000 charge–discharge cycles. This study offers a promising strategy for high-performance automotive supercapacitors. Full article

For the removal of hexavalent chromium [Cr(VI)] from drinking water, a hybrid biosorbent designated chitosan–natural diatomaceous earth (CNDE) was developed and thoroughly characterized. The material couples the ion-exchange and chelating capacity of chitosan—applied at an 85% degree of deacetylation—with the high-surface-area mineral framework of natural diatomaceous earth, onto which the polymer was deposited as a conformal coating. Surface morphology and internal microstructure were examined by scanning and transmission electron microscopy (SEM/TEM), while elemental composition across the hybrid matrix was resolved by energy-dispersive X-ray spectroscopy (EDX). Fourier transform infrared (FTIR) spectroscopy was employed to identify the surface functional groups responsible for chromate binding, and streaming current measurements established the pH of zero charge (pH_pzc), which governs the electrostatic environment at the sorbent–solution interface. Specific surface area was quantified by the Brunauer–Emmett–Teller (BET) method, and the balance of surface acidic and basic sites was determined through titrimetric analysis of total acidity and alkalinity. Thermogravimetric analysis (TGA) was conducted to assess thermal stability. Batch equilibrium isotherm experiments were performed to evaluate Cr(VI) uptake from model drinking water prepared using dilute potassium dichromate solutions adjusted to target pH levels. The effects of solution pH and competing anions (chloride and sulfate) were also investigated. Kinetic studies were conducted to determine the rate of Cr(VI) adsorption, and residual metal concentrations were measured using inductively coupled plasma mass spectrometry (ICP-MS). Results indicated that CNDE containing 30% chitosan (CNDE30) achieved effective Cr(VI) removal at pH 5. Adsorption was strongly pH-dependent, decreasing as pH increased from 5 to 8. Equilibrium data were well described by both Langmuir and Freundlich isotherm models, while kinetic data followed a pseudo-second-order model. The presence of chloride ions (15 mg/L) reduced adsorption capacity by approximately one-third, whereas sulfate at the same concentration significantly inhibited Cr(VI) removal. Overall, the isotherm results suggest that CNDE30 is a promising material for Cr(VI) removal from drinking water. Its cost-effectiveness, ease of synthesis, and potential for reuse make it particularly attractive for small-scale and decentralized water treatment applications. Full article

Catalytic oxidation has become a crucial technology for removing CO from industrial flue gas. However, the complex composition of flue gas (including NH₃, NO, SO₂, H₂O, etc.) poses significant challenges to the catalytic activity and stability of catalysts. In this work, we propose a new strategy for constructing highly efficient catalysts by loading a Pd component onto TiO₂ nanosheets (NSs) with predominantly exposed {001} facets. It has been revealed that the well-connected channels, abundant oxygen vacancies and Ti³⁺ species on the TiO₂(NS) support facilitate the formation of highly dispersed and electron-rich Pd nanoparticles. The weak adsorption of impurities such as NH₃, SO₂, NO and H₂O on these active sites promotes the adsorption and activation of the target reactants (CO and O₂), thereby enhancing catalytic activity. Furthermore, such reduced adsorption inhibits the aggregation of Pd nanoparticles and synergizes with the intrinsically weak NH₃ adsorption of TiO₂(NS) to suppress ammonium sulfate species deposition, thereby enhancing long-term catalytic stability. This work advances TiO₂ facet engineering in catalysis and offers new design concepts for efficient CO oxidation catalysts in complex atmospheres. Full article