Bimetallic Fe-Cu modified SSZ-13 catalyst (FeCu-SSZ-13) was prepared by a sequential ion-exchange method and tested for catalytic oxidation of dichloromethane. It was found that the FeCu-SSZ-13 catalyst was more active than the Cu-and Fe-SSZ-13 catalysts, giving a very high reaction rate of 5.04 mmolCH2Cl2 gcat-1 h-1 at 250 degrees C. The catalyst was highly resistant to water vapor during the reaction, thus showing potential in practical application. The improved performance was attributed to the strong Fe-Cu interaction, not only enhancing the surface acidity and redox capability of the catalyst for higher activity, but stabilizing isolated Cu cations for better catalyst stability particularly under wet condition. Moreover, the in situ spectroscopic investigation on the reaction route revealed that C-Cl cleavage on the surface acid site while the oxidation of reactive intermediates is related to metal cations, which thus showed a clear synergy and accounted for higher mineralization rate.
Improving the low-temperature activity, hydrothermal stability as well as sulfur-resistance of Cu-SSZ-13 zeolite catalysts for selective catalytic reduction of NO with NH3 (NH3-SCR) reaction remains challenging. Herein, we reported that a Ce/Cu-SSZ-13 prepared by a simple impregnation method exhibited good resistance to hydrothermal aging and sulfur-poisoning compared to a CeCu-SSZ-13 catalyst prepared by an ion-exchange method. Various characterizations revealed that CeO2 nanoparticles were deposited on the zeolite surface to effectively stabilize the zeolite framework and the active Cu2+ species during the aging process, which thus can maintain the catalytic activity. Meanwhile, the CeO2 NPs posed Cu-Ce synergy to regulate the Cu2+/Cu+ redox pair. Furthermore, in situ diffuse reflectance infrared Fourier transform spectroscopy results indicated that CeO2 NPs effectively promoted the oxidation of NO which is favorable for fast-SCR, thus promoting the catalytic performance. These findings thus provide a simple but effective strategy for the improvement of low-temperature deNOx performance and hydrothermal stability as well as sulfur-resistance of Cu-SSZ-13 catalysts.
A defective Co3O4 oxide was synthesized by the addition of urea during the preparation procedure, which exhibited 2-fold higher activity than the pristine Co3O4 in the oxidation of dichloromethane (reaction rates of 7.9 x 10(-8) versus 3.4 x 10(-8) mol g(-1) s(-1) at 180 degrees C). Sulfate-modification on the defective Co3O4 further improved the reactivity up to 32.5 x 10(-8) mol g(-1) s(-1) at 180 degrees C. More importantly, the sulfate modification remarkably inhibited the formation of undesired byproducts such as CH3Cl, CHCl3 and CO, giving nearly 100% selectivity to CO2. Various characterizations revealed that the decomposition of urea resulted in the enrichment of structural defects, thus improving the mobility of reactive oxygen species in the reaction. Sulfate-modification intensified surface acidity and defect evolution in Co3O4 and promoted the adsorption and oxidization of the reactants, which accounted for its excellent performance in the reaction.
The CO2-assisted oxidative dehydrogenation of propane (CO2-ODHP) over Cr-based catalysts represents a promising approach to produce propylene, while the nature of active Cr species and associated reaction mechanisms remains debatable. In this work, a series of Cr-containing MFI-structured zeolite catalysts (i.e., S-1, ZSM-5-100, and ZSM-5-13) were synthesized and evaluated for CO2-ODHP to elucidate active Cr sites and reaction pathways. Through reaction rate analysis combined with multiple characterizations, we quantitatively correlated the distribution of Cr species with their intrinsic activities. It is found that the isolated Cr6+ cations and their reduced form, coordinatively unsaturated Cr3+ cations (denoted as isolated Cr3+), give turnover frequencies (TOFs) of 1.9 & times; 10-3 and 2.5 & times; 10-3 s-1 at 550 degrees C, respectively, which are much higher than those of crystalline Cr2O3 (0.24 & times; 10-3 s-1), polymeric Cr6+ (0.023 & times; 10-3 s-1), and its reduced form Cr3+ (0.016 & times; 10-3 s-1). Density functional theory calculations further illustrate the feasible dehydrogenation of propane on both isolated Cr6+ species and isolated Cr3+ species. The Cr6+/Cr4+ redox pair highlights a Mars-van Krevelen mechanism with the involvement of CO2 as a soft oxidant. Both direct propane dehydrogenation and oxidative dehydrogenation with activated CO2 can readily occur on isolated Cr3+ sites, with notably lower energy barriers for the former. Therefore, our findings unequivocally clarify the active sites and the main reaction network, in which the role of CO2 is also highlighted.
Abstract Stabilizing metal oxides is a prerequisite for elucidating their intrinsic mechanistic roles and sustaining high electrocatalytic activity. Here, we synthesize a high-temperature-phase La2O3-socketed sub-2 nm δ-Bi2O3 heterojunction (δ-Bi2O3/La2O3) that suppresses Bi3+ reduction to metallic Bi, achieving ≥95% formate Faradaic efficiency for ~200 hours in industrial-level electrolyzers. Electronic structure analyses reveal that strong electrostatic interactions between δ-Bi2O3 and La2O3 drive oxygen migration to the interface, contracting δ-Bi2O3 domains and enhancing La–Bi d-p orbital hybridization. This structural relaxation stabilizes interfacial Bi–O–La linkages and electron-deficient Bi2O3+x species under cathodic potentials, as confirmed by in situ X-ray absorption spectroscopy. Pourbaix diagrams and in situ infrared spectroscopy demonstrate that La2O3 promotes water dissociation to form a hydroxylated δ-Bi2O3 surface under working potentials, enhancing protonation propensity. Consequently, the energy barrier for the rate-determining step (*CO2 → *HCOO) is lowered to +0.15 eV on δ-Bi2O3/La2O3, significantly lower than the +0.83 eV barrier on pristine δ-Bi2O3. This work establishes a sub-nanoscale oxide/oxide heterojunction strategy to stabilize high-valent metal sites, enabling sustainable electrochemical conversion.
To address the challenges associated with global carbon emissions, this study developed a novel class of porous ionic polymer catalysts. Using a bipyridine-based porous organic polymer (POP-Bpy) as the framework, two Ionic liquid-functionalized materials, POP-Bpy-Et and POP-Bpy-OH, were successfully synthesized via quaternization with 1,2-dibromoethane and 2,3-dibromopropanol, respectively. Comprehensive structural characterization (including 13C NMR, FTIR, and XPS) confirmed the successful quaternization and formation of the desired ionic polymer architectures. Catalytic evaluation revealed that POP-Bpy-OH exhibits outstanding performance in the cycloaddition of CO2 with epoxides. Under mild conditions (60 degrees C, 1 atm CO2, 48 h), POP-Bpy-OH achieved 94.3% conversion of epichlorohydrin with 99% selectivity toward the corresponding cyclic carbonate, significantly outperforming the hydroxyl-free counterpart POP-Bpy-Et (78.4% conversion). Moreover, under industrially relevant low-CO2 conditions (15 %CO2, 96 h), POP-Bpy-OH maintained a high conversion of 83.3%, far exceeding that of POP-Bpy-Et (64.2%). This enhanced activity is attributed to a pronounced synergistic effect between the hydroxyl groups (acting as hydrogen-bond donors) and the bromide anions (Br-) in POP-Bpy-OH, which not only boosts reaction efficiency but also affords good substrate compatibility for epoxides with low to moderate steric hindrance. These results underscore that incorporating hydroxyl functionalities into the polymer backbone is a key strategy for improving CO2 cycloaddition catalysis. In addition to high activity, POP-Bpy-OH demonstrated excellent structural stability and recyclability. After five consecutive reaction cycles, its catalytic activity decreased by only about 3%, highlighting its potential for practical industrial application. To elucidate the origin of its superior performance, density functional theory (DFT) calculations were employed to probe the reaction mechanism. The simulations show that the hydroxyl groups lower the ring-opening energy barrier of the epoxide via hydrogen-bonding interactions, while the adjacent Br- facilitates the nucleophilic attack. This cooperative action efficiently drives the cycloaddition reaction forward, providing an atomic-level understanding of the catalyst's high activity and selectivity.
The hydrogenation of ethylene carbonate (EC) is a crucial step in the indirect transformation of CO2 into methanol (MeOH) and ethylene glycol (EG) over Cu-based catalysts. In this work, a series of sorbitol-modified Cu/SiO2 catalyst were prepared and tested for continuous hydrogenation of EC. As a result, the MeOH selectivity displayed a volcano-like trend with the sorbitol/Cu molar ratios. The optimized Cu@0.04Cs/SiO2 catalyst exhibited excellent MeOH selectivity (91.4 %) and EG selectivity (99.6 %) at an EC conversion of 99.9 %. The results showed that copper-sorbitol complexes were preferentially formed, which could restrict the formation of copper phyllosilicate. However, a strong electronic interaction between copper and carbon, as confirmed by multiple characterizations, which may lead to possible formation of Cu-O-C bond located on the periphery of copper and carbon interface. This interfacial effect not only reduces the activation energy but also effectively enhances the Cu+/(Cu0 + Cu+) ratios, and thus improves the selectivity to MeOH. Furthermore, according to DFT calculation and kinetic study results, the interface between copper and carbon serves as active sites to facilitate the adsorption of H2 and EC, resulting in reduced activation energy.
An ion-exchanged Cu-SSZ-13 catalyst exhibited excellent performance in the deep oxidation of dichloromethane, achieving a high reaction rate of 2.41 mmol g-1 h-1 at 200 °C without producing chlorine-containing byproducts. Detailed characterizations indicated abundant isolated Cu species, specifically, [ZCu2+(OH)]+ and Z2Cu2+, in the catalyst. Quantitative analysis of the activity results demonstrated that the Z2Cu2+ in a 6-membered ring had the highest activity (with a turnover frequency of 1.8 × 10-3 s-1 at 200 °C), which was 5-fold higher than that of the [ZCu2+(OH)]+ species in an 8-membered ring and 9-fold higher than the acid sites in the SSZ-13 support. Importantly, the isolated Cu species remained intact during the reaction, ensuring good catalyst stability. In contrast, CuO particles, present in a higher amount in an impregnated Cu/SSZ-13 catalyst, were readily chlorinated, leading to notable deactivation. Moreover, theoretical calculations unraveled the reaction routes, clarifying the crucial role of the frustrated Lewis pair (Cu6mr···O4mr) species in accelerating the reaction. Therefore, this study not only broadens the application scope of SSZ-13-based catalysts but also provides valuable insights for designing efficient catalysts for the catalytic removal of chlorinated volatile organic compounds.
In the field of renewable fine chemicals, the selective hydrogenation of biomass-derived benzoic acid (BA) into cyclohexane carboxylic acid (CCA) holds a pivotal position. Herein, a series of nitrogen (N) and sulfur (S) codoped Ru-based porous carbon catalysts were synthesized using a combination of soft template and impregnation methods and tested for the hydrogenation of BA. The best performance was obtained on a Ru/N1.5S1.5C-800 catalyst, giving a cyclohexane carboxylic acid yield of 99.5% and a turnover frequency of 609.4 h-1 at 90 degrees C and 1 MPa. Such good reactivity is related to the synergy of S, N co-doping, which enhances the Ru dispersion and optimizes the electronic structure of Ru nanoparticles for BA adsorption. Furthermore, the Ru/N1.5S1.5C-800 catalyst exhibits good cycling stability. The porous structure, charge transfer, N, S co-doping synergistic effect, catalyst active sites, and catalytic reaction kinetics model were in-depth investigated by experimental and theoretical calculations, therefore, the findings in this work provides an efficient catalyst choice for the catalytic hydrogenation of BA under mild conditions.
Catalytic decomposition of dichloromethane was carried out over several phosphate-modified Co3O4 with different exposed crystal planes. It was found that the nanorod Co3O4 (Co3O4-R) exposing {110} planes was more active than the nanocube (Co3O4-C) exposing {100} planes and the octahedron Co3O4 (Co3O4-O) exposing {111} planes, giving a turnover frequency (TOF) of 3.5 lozenge 10-3 s-1 at 230 degrees C. Phosphate modification not only enhanced catalytic activity and stability but also achieved complete mineralization without generating chlorinated organic byproducts. The crystal plane dependency was related to the surface defects and surface acidity derived from the surface atom arrangement of different facets, as the {110} planes of Co3O4 has the highest concentration of oxygen vacancies and surface acid sites, and phosphate-modification intensified the two parameters. Density functional theory (DFT) calculations further demonstrated that the Co3O4 (110) surface has the lowest activation energy for the oxidation of CH2Cl2 compared to the other two surfaces and the phosphate modification hinders the formation of Cl-containing byproducts. These findings provide atomic-level insights into facet-engineered catalysis and establish a strategic framework for designing high performance catalysts for halogenated pollutant elimination.
The spinel Co-based catalysts have been extensively investigated for catalytic methane combustion. However, it remains a significant challenge to both achieve highly synergistic oxidation activity and elucidate the reaction mechanisms for commonly used doping of secondary metal cations in spinel oxide catalysts. Herein, density functional theory (DFT) fully elucidated the Cr promotion effect in spinel Co2CrO4(110) for CH4 oxidation, involving sequential methane dehydrogenation, O2 dissociation, and H2O formation. The magnetic ordering configurations significantly affect the catalytic activity and reaction mechanisms. The Cr-Cr-Co sites of the Co2CrO4(110) surface with antiferromagnetic structures substantially lower the activation barrier of the initial C-H bond in CH4 and boost O2 dissociation to O*. CH4 complete oxidation proceeds through a synergistic Eley-Rideal (ER) and Langmuir-Hinshelwood (L-H) mechanism, CH4 -> CH3O* -> OLCH2O* -> OLCHO* -> O*CO* -> CO2(g), rather than the Mars-van Krevelen (MvK) mechanism. Moreover, the coordination environment of surface Cr3+ or Co3+ ions modified by the neighboring preadsorbed O* species can increase the energy barriers for O2 activation, which becomes the rate-determining step (RDS) for the overall reaction. These findings provide theoretical guidance for the rational design of efficient transition metal oxide catalysts based on spin-catalytic synergy.
The effect of SO2 on the total oxidation of propane over supported Pt catalysts (e.g., Pt/AlF3, Pt/gamma-Al2O3, Pt/SiO2) was investigated in this work. The catalytic testing results revealed that the addition of 100 ppm SO2 in the reaction feed could significantly improve the activity. The largest improvement was obtained on the Pt/AlF3 catalyst, on which a 10-fold higher reaction rate (1.15 mu mol g(-1) s(-1) at 220 degrees C) was achieved in the presence of SO2 compared to that in the absence of SO2 (0.12 mu mol g(-1) s(-1) at 220 degrees C). Detailed characterizations such as Fourier transform infrared spectroscopy (FTIR), NH3 temperature-programmed desorption, and X-ray photoelectron spectra results revealed that the presence of SO2 in the reaction feed resulted in the formation of sulfates on the catalyst surface, which enhanced the surface acidity and lowered surface charge density of Pt species. The in-situ FTIR results of propane oxidation revealed an enhanced C-C bond cleavage of propane molecules by the addition of SO2. The kinetic investigation further clarified the origin of such enhancement, that is, the addition of SO2 slightly strengthened propane adsorption while greatly weakened the oxygen adsorption on the Pt species, and such synergy facilitated the kinetically-relevant surface reaction (i.e., C-C cleavage). Therefore, the findings establish a general agreement on the promoting roles of SO2 on the reaction. Moreover, the current work emphasizes the influence of surface sulfate on the adsorption/activation of oxygen, which has been rarely recognized in previous works.
Sorption-based atmospheric water harvesting (SAWH) offers a promising solution to address freshwater scarcity. Although many solid sorbents exhibit high water uptake capacities, their ability to achieve continuous, all-day water production still depends on complex system configurations. Here, a 24-h SAWH system is presented, enabled by wood-based ionogel (WIG) with simultaneous sorption-desorption functionality. The WIG is prepared by encapsulating 1-ethyl-3-methylimidazolium acetate ([EMIM][Ac]) into the natural wood channels, functioning as a sorption module. Meanwhile, carbonized wood, with photothermal and Joule heating properties, serves as the desorption module. Adjusting the sorption/desorption area ratio enables dynamic kinetic balance, allowing simultaneous moisture uptake and release within a single ionogel. The WIG leverages the water transport capability of wood channels and the fluidity of [EMIM][Ac] to shorten the sorption equilibrium time to 3 h and sustain directional water transfer from the sorption to the desorption zone. This system, driven by solar heating during the day and Joule heating at night, achieves 24-h continuous water production, yielding 47.62 g water per day under natural conditions, equivalent to 2.38 Lwatermsolar-2day-1 (Lwatermsolar-2day-1, defined as liters of water produced per solar absorbing area per day). This work demonstrates a sustainable and efficient SAWH strategy, highlighting the unique advantages of wood and offering a new avenue toward mitigating the global water crisis.
A series of Mo-doped CoAl2O4 spinel oxides were prepared and tested for deep oxidation of dichloromethane (CH2Cl2). The Mo-doping resulted in much improved surface acidity of the catalyst, and thus significantly enhanced the catalytic activity. The best performance was obtained on a CoAl1.7Mo0.3O4 catalyst, which gave a nearly 3-fold higher reaction rate than the pristine CoAl2O4 (26.5 x 10-8 versus 10.5 x 10-8 mol g- 1 s-1 at 230 degrees C). Moreover, the Mo-doped catalyst remarkably suppressed the formation of organic byproduct of CH3Cl. The good catalytic performance of the catalysts was ascribed to the fact that abundant Br & oslash;nsted acid sites derived from Mo5+-OH in the Mo-doped catalysts facilitated the C-Cl bond cleavage of the CH2Cl2 and CH3Cl reactants and their further oxidation. Water in the reaction feed was found to enhance the activity, due to its dissociation on the catalyst surface to hydroxyl groups that could react with CH2Cl2. Therefore, our findings revealed the vital roles of surface Br & oslash;nsted acidity and H2O in the catalytic combustion of chlorinated volatile organic compounds.
IrFe alloy nanoparticles with different Ir/Fe molar ratios were synthesized and exhibited good performance in the gas phase selective hydrogenation of crotonaldehyde (CRAL). The IrFe alloy with an Ir/Fe ratio of 19/1 gave a turnover frequency (TOF) of 0.022 s(-1) at 80 degrees C and a crotyl alcohol (CROL) selectivity of 91 %, while the bare Ir/BN catalyst gave a TOF of 0.0014 s(-1) and a CROL selectivity of 74 %. Detailed characterizations, kinetic investigation, and in situ spectroscopic study revealed that the altered electronic structure of the IrFe alloy with transfer from Fe to Ir species was essential for its improved performance. Also, density functional theory calculations indicated that such an electronic structure resulted in strong CRAL interaction with the Ir-Fe entity, thus higher adsorption capacity and lower reaction barrier than that on the Ir-Ir counterpart, which accounted for the higher activity. Moreover, the hydrogenation of C = O bond required lower barrier on the Ir-Fe site than that on the Ir-Ir, which well explained the higher selectivity to CROL.
The essential roles of octahedrally coordinated cations (B-site in AB(2)O(4) formula) in Co3-xCrxO4 spinel oxides in the total oxidation of propane were demonstrated, using a series of Co3-xCrxO4 spinel oxides with different Co/Cr molar ratios derived from layered double hydroxides. The catalytic activity was strongly related to the compositions of B-site cations. The Co2CrO4 catalyst with B-sites equally occupied with Co and Cr cations was more active than the Co3O4 (Co cations only in B-sites) and CoCr2O4 (Cr cations only in B-sites), giving turnover frequencies of 0.86 x 10(-3), 0.72 x 10(-3) and 0.11 x 10(-3) s(-1) at 250 degrees C (under kinetically-controlled reaction), respectively. Kinetics and density functional theory (DFT) calculations on the Co2CrO4 and CoCr2O4 catalysts indicated that the reaction followed a Langmuir-Hinshelwood mechanism, and the adsorption of oxygen on the former was easier. Moreover, the cleavage of the first C-H bond in the propane as the rate-determining step was more favored on the Co2CrO4, which accounted for its higher activity. These findings thus provide valuable insights on the mechanistic roles of B-site cations of spinel oxides in total oxidation of hydrocarbon.
Selective producing ethanol from CO2 electroreduction is highly demanded, yet the competing ethylene generation route is commonly more thermodynamically preferred. Herein, we reported an efficient CO2‐to‐ethanol conversion (53.5% faradaic efficiency at −0.75 V versus reversible hydrogen electrode (vs. RHE)) over an oxide‐derived nanocubic catalyst featured with abundant "embossment‐like" structured grain‐boundaries. The catalyst also attains a 23.2% energy efficiency to ethanol within a flow cell reactor. In situ spectroscopy and electrochemical analysis identified that these dualphase Cu(I) and Cu(0) sites stabilized by grain‐boundaries are very robust over the operating potential window, which maintains a high concentration of co‐adsorbed *CO and hydroxyl (*OH) species. Theoretical calculations revealed that the presence of *OHad not only promote the easier dimerization of *CO to form *OCCO (ΔG ~ 0.20 eV) at low overpotentials but also preferentially favor the key *CHCOH intermediate hydrogenation to *CHCHOH (ethanol pathway) while suppressing its dehydration to *CCH (ethylene pathway), which is believed to determine the remarkable ethanol selectivity. Such imperative intermediates associated with the bifurcation pathway were directly distinguished by isotope labelling in situ infrared spectroscopy. Our work promotes the understanding of bifurcating mechanism of CO2ER‐to‐hydrocarbons more deeply, providing a feasible strategy for the design of efficient ethanol‐targeted catalysts.
Searching for an antibacterial and anti-inflammatory dressing that can stably adhere to wet tissues remains a momentous clinical challenge, especially in the context of treatment failure due to multi-drug-resistant bacteria. Using a hard template method in combination with an in situ chelating strategy, three-dimensional nitrogen-doped graded porous carbon anchored 1.5–2.5 nm CeO2 quantum dots (CeO2-QDs) were tailor-designed in this study. Using the size effect, CeO2-QDs have a higher percentage of Ce3+ and oxygen vacancies that could amplify their antibacterial effects. Polyethyleneimine/polyacrylic acid (PEA) powder could self-gel and be adhesive due to its strong physical interactions, which make it an ideal carrier for CeO2-QDs. PEA@50 (mg/mL) CeO2-QDs hydrogel and PEA@75 (mg/mL) CeO2-QDs hydrogel with moderate doses of CeO2-QDs show a superior antibacterial effect against Staphylococcus aureus (S. aureus) and Escherichia coli (E. coli) strains. Furthermore, PEA@50CeO2-QDs hydrogels possess excellent anti-inflammatory capacity through their antioxidant activity, which could promote macrophage M2 phenotype polarization. More importantly, cytotoxicity assays on L929 fibroblasts show that PEA@CeO2-QDs hydrogels have no significant toxicity, and a significant proliferative effect could be observed. Overall, PEA@50CeO2-QDs hydrogels have the potential to become a multifunctional wet tissue dressing with anti-inflammatory and antiseptic properties to promote the healing of infected wounds.
Modulating the active sites in atomic level is very meaningful to optimize catalyst performance but still very challenge. Herein, Pt catalysts loaded on different supports (ZSM-5, Al2O3, ZrO2, CeO2) were sulfate modified by in situ pyrolysis of (NH4)(2)SO4 mixed with Pt catalyst. Sulfate remarkably improves these catalyst activities for propane combustion, particularly for the sulfate modified Pt/ZSM-5 catalyst with the highest activity among them. Through controlling the amount of (NH4)(2)SO4 used and the loading of Pt, Pt/S atomic ratio in the sulfate modified Pt/ZSM-5 catalyst was successfully regulated. Pt/S atomic ratio significantly affects the electron transfer from Pt species to sulfate and also their interaction strength, which is decisive to the synergetic catalysis of sulfate and Pt species. The 5S-2Pt/ZSM-5 with Pt/S atomic ratio of 0.5 shows a moderate strength of sulfate and Pt species interaction, which is responsible for its highest reaction rate of 86.5 mu mol.g(Pt)(-1).s(-1) at 200 degrees C.
The supported Pt-based catalysts exhibited excellent catalytic oxidation activity towards toluene, while the Pt metal was prone to aggregation at high temperatures, leading to catalyst sintering deactivation. A combination strategy was presented to enhance the reactivity and lifespan of catalysts for toluene catalytic oxidation in this work, which involved regulating the morphology and microstructure of Pt@D-Beta through a combination of recrystallization Pt confinement and zeolite dealumination to improve the stability and water resistance of the catalyst. The designed Pt@D-Beta catalyst with T-90 (temperatures for 90 conversion of toluene) at 158 degrees C was prepared by combining carrier dealumination and secondary crystallization method, which was 22 degrees C lower than that of traditional Pt/Beta. Importantly, the Pt@D-Beta catalyst exhibited excellent cycling performance and long-term stability, and great water resistance. After 5 cycle tests, the toluene conversion could also be maintained at similar to 85 % for at least 50 h with slight activity loss. The results of SEM and XPS show that a combination of recrystallization Pt confinement and zeolite dealumination could improve the reduction performance of the catalyst, increase the dispersion of Pt on zeolite and oxygen mobility, and improve the catalytic performance of the catalyst for toluene. The toluene catalytic degradation on Pt@D-Beta was researched via in situ DRIFTs (in situ diffuse reflectance infrared Fourier transform spectroscopy) combination with density functional theory (DFT) calculation, the hydroxyl groups on the catalyst can provide active oxygen for toluene catalytic oxidation, followed the Mars-van Krevelen (MvK) mechanism. This synthesis combination strategy is expected to provide an effective method for designing efficient zeolite limited noble metal catalysts for catalytic degradation of VOCs.