Catalytic Activity For Oxidation Research Articles

A robust, eco-friendly, and biodegradable cellulose nanofiber composite film for highly effective formaldehyde removal at room temperature

Formaldehyde (HCHO) poses a significant threat as a common indoor air pollutant, leading to various health issues. However, effectively addressing HCHO removal at room temperature remains a considerable challenge. This paper presents the preparation of a robust, eco-friendly, and biodegradable composite cellulose nanofiber film, incorporating CeO2-Ag@MnO2 catalysts and TEMPO-oxidized cellulose nanofiber (TOCNF), for high-efficiency HCHO removal at room temperature. A CeO2-Ag@MnO2 ternary catalyst with a core–shell structure was constructed to enhance the catalytic oxidation activity and stability. This structure increased the number of active sites on the catalyst surface and enhanced the interfacial synergistic effect of Ce-Ag-Mn. The TOCNF physically adsorbed HCHO in the composite film, while the catalyst oxidized it to CO2 and water. The composite films, particularly those with 20 wt% CeO2-Ag@MnO2 catalyst, exhibited high HCHO removal rates of 91.2 % at 20 °C and 99.6 % at 60 °C. Furthermore, the TOCNF/20 CAM composite films demonstrated excellent mechanical properties and degradability. This composite film offers an efficient and eco-friendly solution for the catalytic oxidation of HCHO at room temperature.

N/Se co-doped porous carbon catalyst derived from a deep eutectic solvent and chitosan as green precursors: Investigation of catalytic activity for metal-free oxidation of alcohols

Heteroatom-doped porous carbon-based materials with high surface area compared to their metal-based homologs are considered environmentally friendly and ideal catalysts for organic reactions. In this paper, a new method for the convenient fabrication, cost-effective, and high efficiency of nitrogen/selenium co-doped porous carbon-based catalysis (marked as N/SePC-T) was designed. The N/SePC-T catalysts were created from the direct pyrolysis of a eutectic solvent containing choline chloride/urea as the nitrogen-rich carbon source, selenium dioxide as a source of heteroatom and chitosan as a secondary carbon source in different temperatures (T). The efficacy of the carbonization temperature on the pore structure, morphology, and catalytic activity of the N/SePC-T materials was investigated and displayed, the N/SePC-900 (having a surface area of 562.01 m2/g and total pore volume of 0.2351 cm3 g−1) has the best performance. The morphology, structure, and physicochemical properties of N/SePC-900 were characterized using various analyses including XRD, TEM, TGA, FE-SEM, EDX, FT-IR, XPS, and Raman. The optimized N/SePC-900 catalyst indicated excellent catalytic performance in the oxidation of benzylalcohols to corresponding aldehydes in very mild conditions.

Two-dimensional MXene supported single transition metal atom for HCHO catalytic oxidation: A first-principles study combined with Microkinetics

Catalytic oxidation is an efficient and environmentally friendly strategy for the removal of pollutant HCHO. Recent proof-of-concepts experiments indicate that single-atom catalysts (SACs) exhibit good activity for HCHO catalytic degradation, but a major obstacle is to look for an effective SAC. Herein, ten 3d transition metal SACs decorated on Mo2CS2 substrate were designed and constructed to catalyze HCHO using periodic density functional theory calculations. The results showed that the single atoms are inclined to locate at the Mo top site on the surface and most SACs can stay stable. Among these SCAs, Ti, V, Cr, and Mn SACs have shallow energy barriers of O2 activation and can facilitate O2 dissociation at room temperature. Therefore, two typical HCHO oxidation pathways on TM@Mo2CS2 (TM = Ti, V, Cr, and Mn) catalyst were investigated in detail. The V@Mo2CS2 has the lowest energy barrier of 1.72 eV for the rate-limiting step during HCHO oxidation via path-Ⅰ (O2 adsorption and activation, HCHO* → CHO* → CO* → CO2*). Correlation analysis verifies that the Bader charge and O2 adsorption are the appropriate descriptions for HCHO catalytic oxidation activity. Microkinetic simulations are further performed to reveal the relationship between HCHO oxidation rate and temperature.

Catalytic Activity and Mechanical Stability of ZIFs‐Derived CoCeOx/Cordierite Monolithic Catalysts

AbstractBimetallic oxide catalysts derived from zeolitic imidazolate frameworks (ZIFs) have good catalytic oxidation activity, but their application is limited because the powder is not conducive to industrial production. In this study, CoCeOx/cordierite monolithic catalysts derived from ZIFs were prepared by a simple impregnation method. Firstly, a phase transition of Co‐ZIF was induced in ethanol solution by adding excessive Ce(NO3)3. Subsequently, tannic acid (TA) was used to chelate excess metal on the surface to expose more active sites. Meanwhile, TA staying on the surface of the precursor could also prevent the accumulation of Ce at high temperatures. After the activity test, CoCeOx/cordierite showed excellent activity for the catalytic oxidation of o‐xylene with a T90 of 295 °C. The mechanical stability of the catalyst was also tested by ultrasonic vibration method. In addition, we investigated the influence of factors such as impregnation cycles and TA treatment time on the physical and chemical properties. This paper provides a new idea for preparing monolithic catalysts derived from ZIFs.

Thermocatalytic oxidation potential of cobalt(II,III) oxide against gaseous formaldehyde in relation to hydrothermal synthesis temperature

The catalytic activity of various transition metal oxides has been reported to be tuned by controlling their synthesis conditions. In this perspective, the thermocatalytic oxidation performance of cobalt(II,III) oxides (Co3O4) against formaldehyde (FA) is studied in relation to the temperature selected for their hydrothermal synthesis (e.g., 30 (as room temperature (RT)), 60, 120, and 250℃) with the corresponding sample codes as Co3O4-RT, Co3O4-60, Co3O4-120, and Co3O4-250, respectively. The best performing Co3O4-RT records the lowest T90 (temperature required to obtain 90 % conversion) for 50 ppm FA at 72 °C when operated at 0 % relative humidity (RH), 30 mg (catalyst mass: mcat), and 100,000 mL g-1h−1 (weight hourly space velocity). The performance of Co3O4-RT, if assessed in terms of reaction kinetic rate (r) at XFA = 10 %, is 2.02E-02 mmol g-1h−1. According to X-ray photoelectron spectroscopy and temperature programmed characterization analysis, the catalytic activities of Co3O4-RT improve greatly through the synergistic combination of diverse factors (e.g., high Co3+ content, abundant oxygen vacancies (OVs) and surface adsorbed oxygen (Oβ) species, and good surface lattice oxygen (Oα) mobility). The analysis of in-situ diffuse reflectance infrared Fourier transform spectroscopy indicates that the FA should be oxidized into water (H2O) and carbon dioxide (CO2) via dioxymethylene (DOM) and formate (HCOO–) as reaction intermediates. The density functional theory simulations suggest the (111) surface of Co3O4 to be catalytically active against FA. The output of this research is expected to help establish effective strategies for designing high-performance transition metal oxide catalysts for the catalytic oxidation of FA.

Template Synthesis of Cyclometalated Macrocycle Iridium(III) Complexes Based on Photoinduced C-N Cross-Coupling Reactions In Situ.

The synthesis of metal macrocycle complexes holds paramount importance in coordination and supramolecular chemistry. Toward this end, we report a new, mild, and efficient protocol for the synthesis of cyclometalated macrocycle Ir(III) complexes: [Ir(L1)](PF6) (1), [Ir(L2)](PF6) (2), and [Ir(L3)](PF6) (3), where L1 presents 10,17-dioxa-3,6-diaza-2(2,8),7(8,2)-diquinolina-1,8(1,4)-dibenzenacyclooctadecaphane, L2 is 10,13,16,19,22,25-hexaoxa-3,6-diaza-2(2,8),7(8,2)-diquinolina-1,8(1,4)-dibenzenacyclohexacosaphane, and L3 is 4-methyl-10,13,16,19,22,25-hexaoxa-3,6-diaza-2(2,8),7(8,2)-diquinolina-1,8(1,4)-dibenzenacyclohexacosaphane. This synthesis involves the preassembly of two symmetric 2-phenylquinoline arms into C-shape complexes, followed by cyclization with diamine via in situ interligand C-N cross-coupling, employing a metal ion as a template. Moreover, the synthetic yield of these cyclometalated Ir(III) complexes, tethered by an 18-crown-6 ether-like chain, is significantly enhanced in the presence of K+ ion as a template. The resultant cyclometalated macrocycle Ir(III) complexes exhibit high stability, efficient singlet oxygen generation, and superior catalytic activity for the aerobic selective oxidation of sulfides into sulfoxides under visible light irradiation in aqueous media at room temperature. The photocatalyst 2 demonstrates recyclability and can be reused at least 10 times without a significant loss of catalytic activity. These results unveil a new and complementary approach to the design and in situ synthesis of cyclometalated macrocycle Ir(III) complexes via a mild interligand-coupling strategy.

Exploring the Water Oxidation Catalytic Activity of a Mn-Based Magnetic Metal-Organic Framework: The Role of Proton Conductivity and Oxygen Evolution Reaction Overpotential.

The present work evaluates the water oxidation catalytic activity of a Mn-based metal-organic framework (MOF), which we envisioned to reduce the oxygen evolution reaction (OER) overpotential because of its high electrical conductivity, facilitated by solvent-encapsulated structural features. The presence of Mn centers induces interesting magnetic features in the MOF, which exhibits impressive cryogenic magnetic refrigeration with a ΔSM value of 29.94 J kg-1 K-1 for a field change of ΔH = 5T at 2.3 K. To the best of our knowledge, the ΔSM value of the current system ranked the highest position among the published examples. The crystal structure aligns perfectly with the thematic expectations and features as many as ten metal-coordinated water molecules, forming an extensive web of a hydrogen-bonded network while facing toward the porous channel filled with another set of much-anticipated entrapped lattice water molecules. Such structural features are expected to manifest high proton conductivity, and detailed investigation indeed yields the best value for the system at 1.57 × 10-4 S/cm at 95% humidity and 85 °C. In order to evaluate the thematic notion of a one-to-one relationship between OER and improved electrical conductivity, extensive electrocatalytic water splitting (WS) investigations were carried out. The final results show highly encouraging WS ability of the Mn-MOF, showing the electrocatalytic surface area value of the active species as 0.0686 F/g with a turnover frequency value of 0.043 [(mol. O2) (mol. Mn-MOF)-1 s-1]. Another fascinating aspect of the current communication is the excellent synergy observed between the experimental WS outcomes and the corresponding theoretical data calculated using density functional theory (DFT). Consequently, a plausible mechanism of the overall OER and the role of the Mn-MOF as a water oxidation catalyst, along with the importance of water molecules, have also been derived from the theoretical calculations using DFT.

Enhancing catalytic activity of CuCoFe-layered double oxide towards peroxymonosulfate activation by coupling with biochar derived from durian peel for antibiotic degradation: The role of C=O in biochar and underlying mechanism of built-in electric field

CuCoFe-LDO/BCD was successfully synthesized from CuCoFe-LDH and biochar derived from durian shell (BCD). Ciprofloxacin (CFX) degraded more than 95% mainly by O2•− and 1O2 in CuCoFe-LDO/BCD(2/1)/PMS system within 10 min with a rate constant of 0.255 min−1, which was 14.35 and 2.66 times higher than those in BCD/PMS and CuCoFe-LDO/PMS systems, respectively. The catalytic system exhibited good performance over a wide pH range (3–9) and high degradation efficiency of other antibiotics. Built-in electric field (BIEF) driven by large difference in the work function/Fermi level ratio between CuCoFe-LDO and BCD accelerated continuous electron transfer from CuCoFe-LDO to BCD to result in two different microenvironments with opposite charges at the interface, which enhanced PMS adsorption and activation via different directions. As a non-radical, 1O2 was mainly generated via PMS activation by C=O in BCD. The presence of C=O in BCD resulted in an increase in atomic charge of C in C=O and redistributed the charge density of other C atoms. As a result, strong adsorption of PMS at C atom in C=O and other C with a high positive charge was favorable for 1O2 generation, whereas an enhanced adsorption of PMS at negatively charged C accounted for the generation of •OH and SO4•−. After adsorption, electrons in C of BCD became deficient and were fulfilled with those transferred from CuCoFe-LDO driven by BIEF, which ensured the high catalytic activity of CuCoFe-LDO/BCD. O2•−, on the other hand, was generated via several pathways that involved in the transformation of •OH and SO4•− originated from PMS activation by the transition of metal species in CuCoFe-LDO and negatively charged C in BCD. This study proposed a new idea of fabricating a low-cost metal-LDH and biomass-derived catalyst with a strong synergistic effect induced by BIEF for enhancing PMS activation and antibiotic degradation.

Regulating the oxidation state of Pd to enhance the selective hydrogenation for 5-hydroxymethylfurfural

The highly selective hydrogenation of 5-hydroxymethylfurfural to 2,5-dihydroxymethylfuran is an important reaction in the field of biomass hydrogenation, because it is a bridge between biomass resources and chemical industry. Here, we precisely constructed carbon nitride supported Pd-based catalysts by a simple impregnation-reduction method. By changing the reduction temperature, catalysts with different oxidation state could be precisely constructed. Moreover, the important correlation between the ratio of Pd0/Pd2+ and catalytic activity is revealed during the selective hydrogenation of HMF. The Pd/g–C3N4–300 catalyst with a Pd0/Pd2+ ratio of 3/2 showed the highest catalytic activity, which could get 96.9% 5-hydroxymethylfurfural conversion and 90.3% 2,5-dihydroxymethylfuran selectivity. Further density functional theory calculation revealed that the synergistic effect between Pd0 and Pd2+ in Pd/g–C3N4–300 system could boost the adsorption of the substrate and the dissociation of hydrogen. In this work, we highlight the important correlation between metal oxidation state and catalytic activity, which provides valuable insights for the rational design of precious metal catalysts for hydrogenation reactions.

Active learning driven discovery of novel alloyed catalysts for selective ammonia oxidation

Alloy catalysts design faces the contradiction of small sample and huge screen space, especially in rational design with multi-objective and multi-constraints. Here, we conduct the active learning enabled innovative catalyst screening in alloy space composed of transition metal elements. First, the small dataset and large search space are constructed based on knowledge informed feature group. Then, the surrogate model based on Gaussian process regression are trained for predicting catalytic activity and N2 selectivity descriptors for selective catalytic oxidation of ammonia (NH3-SCO) process, merely based on the small dataset. Furthermore, coupling pareto solution and Bayesian optimization, the active learning driven material searching are performed in the huge alloy spaces with more than 1000 configurations. After 3 iterations with high throughput calculation on 30 alloyed configurations and further theoretical validation based on microkinetic and stability analysis, 9 ensemble configurations are considered as innovative alloy catalysts of NH3-SCO with reactivity and selectivity trade-off. Our study provides the reliable framework for catalyst design with multi-objective and multi-constraints when facing with small sample data and huge searching space and gives the specific guidance for rational design of NH3−SCO alloy catalysts.

Catalytic hydropyrolysis of cashew de-oiled shell using Py-GC/MS

The present study delves into the impact of different metal oxides (Al2O3, Nb2O5, CaO, CeO2, and ZrO2) and temperatures (350, 450, and 550℃) on the flash pyrolysis of cashew de-oiled shell. Upon analysis using Pyrolysis Gas Chromatography and Mass Spectrometry (Py-GC/MS), the resulting functionalities, including carbonyls, furans, phenolics, hydrocarbons, sugars, and N-containing compounds, have been identified. Additionally, the potential of flash hydro-pyrolysis to upgrade pyrolysis vapors into fuel-grade hydrocarbons has also been studied. The study investigates the effect of hydrogen pressure variations (1, 5, and 10 bar) and the catalytic activity of metal oxides on hydropyrolysis. Characterization of the metal oxides through BET, XRD, SEM, and TPD reveals distinct properties. Notably, incorporating Al2O3 significantly enhances the production of aliphatic hydrocarbons, reaching 78.4 area% at 10 bar of hydrogen. This research advances our understanding of flash pyrolysis and provides insights into sustainable fuel production through targeted catalytic processes.

In situ exsolution of Pt nanoparticles on low Pt-substituted A-site deficient perovskite for efficient CO oxidation

Platinum nanoparticles often lose their efficacy in challenging working environments. In this study, we developed a novel approach for the preparation of highly dispersed precious metal catalysts. The method involves the utilization of composite materials consisting of PtOx/(LC)0.9MP, achieved through the exsolution of a low Pt substituted A-site deficient perovskite (La0.97Ce0.03)0.9Mn0.99Pt0.01O3 ((LC)0.9MP). This procedure facilitates the in situ exsolution of Pt nanoparticles from (LC)0.9MP through heat treatment under 10 vol% H2/Ar environment. During this process, PtOx undergoes transformation to Pt0, exhibiting a high CO catalytic oxidation activity, with the T100(CO) decreasing from 213 to 141 °C. This capability primarily stems from the substantial number of oxygen vacancies and alterations in Pt species induced by the catalyst during the redox process. The active Pt nanoparticles are strongly integrated on the surface of (LC)0.9MP, demonstrate excellent CO oxidation activity and stability. This performance is attributed to the specific structure of perovskite. Upon reoxidation, these particles do not undergo direct reincorporation into the lattice structure. Instead, NPs result in the formation of stable, anchored oxide nanoparticles. This strategy can be extended to other metals oxides catalysts, thus may help the rational design of highly efficient transition metal oxide-based catalysts and beyond.

Metallophthalocyanine as ideal antibiotics without light: Mechanisms and applications

The urgent global health problem of antimicrobial resistance (AMR) calls for the discovery of new antibiotics with innovative modes of action while considering the low toxicity to mammalian cells. This paper proposes a novel strategy for designing antibiotics with selective bacterial toxicity by exploiting the positional differences of electron transport chains (ETC) in bacterial and mammalian cells. The focus is on cytochrome c (cyt C) and its maturation system in E. coli. The catalytic oxidative activity of metallophthalocyanine (MPc), which have a distinctive M-N4 structure, is being investigated. Unlike previous applications based on light-activated reactive oxygen species (ROS) generation, this study exploits the ability of MPcs to oxidize Fe2+ to Fe3+ in cyt C and catalyze the formation of disulfide bonds between cysteine residues to interfere with cyt C maturation, disrupt the bacterial respiratory chain and selectively kills bacteria. In contrast, in mammalian cells, these MPcs are located in the lysosomes and cannot access the ETC in the mitochondria, thus achieving selective bacterial toxicity. Two MPcs that showed effective antibacterial activity in a wound infection model were identified. This study provides a valuable reference for the design of novel antibiotics based on M-N4-based metal complex molecules.

Catalytic promiscuity, cytotoxicity and protein cleavage mediated by mononuclear copper(II) complexes: oxidative and hydrolytic activities

In this work, we describe the synthesis and structural and spectroscopic characterizations of two copper(II) complexes, [(Cu)(L1)(Cl2)].4H2O (1), where L1 is 2-(pyridin-2-yl)-1,3-bis(pyridin-2-ylmethyl)-hexahydropyrimidine, and [Cu(L2)](ClO4)2 (2), where L2 is N1,N1,N3-tris(pyridin-2-ylmethyl)propane-1,3-diamine. The crystalline structure analysis indicates that both complexes are mononuclear and pentacoordinated compounds. In the case of complex 1, it bears a neutral charge, with the ligand coordinating to the Cu(II) center in a tridentate manner, utilizing N-donor atoms. Additionally, two cis-chlorido ligands completing the coordination sphere. On the other hand, complex 2 is a cationic complex, with the ligand coordinated in a pentadentate manner, with only N-donor atoms for coordination around the Cu(II). Complex 1 showed catalytic promiscuity, displaying hydrolytic and oxidative activity. The hydrolytic activity was investigated using bis(2,4-dinitrophenyl) phosphate (2,4-BDNPP) as a phosphodiester substrate and applying the Michaelis–Menten approach, obtaining the following kinetic parameters: kcat = 1.21 × 10-4 s−1; KM = 3.35 × 10-3 molL-1. Complex 1 also accelerates the oxidation of the 3,5-di-tert-butylcatechol (3,5-DTBC) substrate with catalytic efficiency equal to 6.11 L mol-1s-1. Interestingly, we demonstrated that this Cu(II) complex 1 can also cleave the very stable peptide bonds from BSA (bovine serum albumin) through an oxidative mechanism using ascorbate as a reducing agent. Complexes 1 and 2 show good cytotoxic activity against two cancer cell lines: A431 from human squamous cell carcinoma and K562 from chronic myeloid leukemia. This study showed that complexes 1 and 2 are selective towards cancer cells.

Unlocking the superior flexibility and enhanced catalytic oxidation performance of CoTiO3 nanofibrous membranes through zirconium doping

The development of continuous CoTiO3 (CTO) fibers with prominent catalytic oxidation activity, tunable fibrous structures, and improved recyclability is appealing for application in efficient organic wastewater treatment; however, inescapable flaws remain, such as their inherent brittleness and adverse operability. Herein, a facile and effective strategy is proposed for the fabrication of flexible and mechanically robust CTO nanofibrous membranes through a combination of element doping and sol–gel-assisted electrospinning. Compared with pristine CTO fibers, the resulting zirconium-doped CoTiO3 (ZCTO) nanofibrous membranes displayed remarkably enhanced flexibility and tensile mechanics, which were attributed to their lower crystallinity, smaller grain size, and fewer fiber surface defects. The developed ZCTO fibrous membrane demonstrated exceptional resistance to bending fatigue, retaining a polymer-like bending rigidity of approximately 25 mN even after undergoing 200 reciprocating bending cycles. Furthermore, the incorporation of zirconium into CTO clearly had an advantageous effect on the formation of oxygen vacancies, thereby enhancing the surface adsorption of peroxymonosulfate (PMS), accelerating the electron transfer process, and weakening the peroxy bonds. The tetracycline degradation efficiency of the ZCTO fibers remained at 81.4% within 10 min after 5 continuous cycles. Benefiting from their robust mechanical properties and excellent catalytic activity, the fabricated membranes demonstrated outstanding dynamic catalytic performance under gravity-driven conditions. More importantly, the reported strategy might be adopted and extended to develop a wide range of ceramic fibers with enhanced flexibility and mechanics for catalytic oxidation.

Effect of cobalt on CeO2 nanorod supported Pt catalyst: Structure, performance, kinetics and reaction mechanism in CO oxidation

Catalytic oxidation represents a highly efficient and extensively employed approach for the elimination of CO in exhaust gas. Rationally designing and preparing catalysts with exceptional activity and stability in the presence of H2O and SO2 at low temperatures represent crucial avenues for future advancements. In this work, a series of Pt catalysts supported on CeO2 nanorods incorporated with varying amounts of Cobalt (Co/CeO2 ratio ranging from 0 to 10 %) were prepared and evaluated for their catalytic activity in CO oxidation under both dry and wet conditions. The ultrahigh dispersion of Pt, outstanding redox properties, and abundant oxygen vacancies on the surface of Co-doped CeO2 nanorod supported Pt catalysts were revealed by XRD, TEM, Raman spectroscopy and H2-TPR techniques. The catalytic activity for CO oxidation strongly depends on the Co content and reaction conditions. Among them, Pt/Co-CeO2-5 % exhibits the highest CO oxidation performance with a T90 (the temperature to achieve 90 % conversion of CO) of 170 °C under dry conditions, which is significantly lower by 140 °C compared to T90 of Pt/CeO2. Pt/Co-CeO2-1 % demonstrates superior CO oxidation performance with a T90 of 195 °C under wet conditions, exhibiting a reduction in temperature by 65 °C compared to the T90 of Pt/CeO2. Moreover, Pt/Co-CeO2 exhibits excellent resistance to SO2 compared to Pt/CeO2. Kinetic studies, in situ DRIFT analysis and isotopic experiments demonstrated direct participation of H2O in the reaction. On the catalysts with a low Co/Ce ratio (Co/Ce < 0.03), CO readily reacts with hydroxyl groups dissociated from H2O to form carboxyl intermediates, which subsequently undergo rapid decomposition into CO2, resulting in an enhanced reaction rate of CO oxidation at low temperature.

Solvent-Free Synthesis Enables Encapsulation of Subnanometric FeOx Clusters in Pure Siliceous Zeolites for Efficient Catalytic Oxidation Reactions.

Metal/metal oxide clusters possess a higher count of unsaturated coordination sites than nanoparticles, providing multiatomic sites that single atoms do not. Encapsulating metal/metal oxide clusters within zeolites is a promising approach for synthesizing and stabilizing these clusters. The unique feature endows the metal clusters with an exceptional catalytic performance in a broad range of catalytic reactions. However, the encapsulation of stable FeOx clusters in zeolite is still challenging, which limits the application of zeolite-encapsulated FeOx clusters in catalysis. Herein, we design a modified solvent-free method to encapsulate FeOx clusters in pure siliceous MFI zeolites (Fe@MFI). It is revealed that the 0.3-0.4 nm subnanometric FeOx clusters are stably encapsulated in the 5/6-membered rings intersectional voids of the pure siliceous MFI zeolites. The encapsulated Fe@MFI catalyst with a Fe loading of 1.4 wt % demonstrates remarkable catalytic activity and recycle stability in the direct oxidation of methane, while also promoting the direct oxidation of cyclohexane, surpassing the performance of conventional zeolite-supported Fe catalysts.

Synthesis of thin-film CuMn2O4 for low-temperature CO oxidation

Thin films, 0.5- and 1.0-nm thick, of CuMn2O4 were synthesized on γ-Al2O3 using Atomic Layer Deposition (ALD); and their catalytic activities for CO oxidation were measured and compared to that of bulk CuMn2O4. For bulk CuMn2O4, the surface area decreased dramatically when the sample was calcined at 1073 K; but the area-specific rates for CO oxidation were the same for bulk samples calcined at 473 K and 1073 K. For thin films of CuMn2O4 on γ-Al2O3, both the surface area and spinel structure were maintained following oxidation at 1073 K or reduction at 973 K. Area-specific, CO-oxidation rates on the ALD-prepared catalysts were somewhat lower than those found on bulk CuMn2O4; however, adding an additional ALD cycle of Cu on the CuMn2O4/γ-Al2O3 increased the rates to the same level as that of the bulk CuMn2O4.

Supported palladium nanocubes reduced by graphene oxide and surface-cleaned for enhanced electrocatalytic activity

Highly dispersed Pd nanocubes (Pd NCs) supported on the surface of partially reduced graphene oxide (pRGO) were successfully prepared by a facile procedure. GO was used as reductant and support without any other external reducing agent been introduced, and potassium iodide (KI) was used as capping agent for morphology control respectively. Catalytic activities for ethanol oxidation and methanol oxidation were greatly enhanced after excess iodine on the surface of Pd NCs was removed by being surface-treated with NaBH4 solution.

Boosting catalytic oxidation of propane over CeO2-supported Co3O4 catalyst with strong interfacial interaction and electron transfer

Tuning the nanoparticle-support interaction can optimize the catalytic performance of supported metal oxide catalysts for VOCs removal. Herein, a series of Co3O4/CeO2 catalysts with different strengths of interfacial interaction and electron transfer were successfully constructed via various modified wetness impregnation procedures. With the introduction of ammonium hydroxide, citric acid or H2 pretreatment, a stronger interfacial interaction and electron transfer were achieved due to the highly Co3O4 dispersion and CeO2 surface reconstruction. The modified-synthesis Co3O4/CeO2 catalysts, particularly Co3O4/CeO2-CA (citric acid), demonstrated superior catalytic activity (T90 = 296 °C, TOF = 0.337 × 10−3 s−1) and stability for propane oxidation as compared to typical wetness impregnation Co3O4/CeO2-DI (T90 = 314 °C, TOF = 0.121 × 10−3 s−1). Through systematic characterizations and DFT calculation, the strong interfacial interaction and abundant reactive oxygen species facilitate the adsorption and activation of C3H8 and O2 on the catalyst surface, which further promote the intermediates (carbonate/carboxyl species) transformation. These findings highlight interfacial mechanism to catalytic performance optimization of supported metal oxides.