Direct Synthesis,Characterization and Catalytic Performance of Iron-Containing SBA-15 for Phenol Degradation

An iron-containing SBA-15（Fe-SBA-15） has been synthesized via one-pot hydrothermal method under weak acidic conditions. A series of characterizations show nanocomposite materials of iron particles supported over mesostructured materials. The catalytic activity of these iron-containing SBA-15 materials has been tested for the heterogeneous Fenton degradation of phenolic aqueous solutions. The catalytic performance has beta monitored in terms of phenol conversion, whereas the catalytic stability was evaluated by catalyst recycle. The influence of concentration of hydrogen peroxide, catalyst loading, catalyst prepared with different Fe/Si molar ratios in the gel and pH values of the solution on phenol conversion has been studied. Achieving a good catalytic performance accompanied with a noteworthy stability, Fe-SBA-15 materials prepared by this method are shown as the successful catalyst for degradation of phenolic aqueous solutions by Fenton process.

Boosting CO_(2) hydrogenation to high-value olefins with highly stable performance over Ba and Na co-modified Fe catalyst

CO_(2)hydrogenation has been considered to be a highly promising route for the production of high-value olefins(HVOs)while also mitigating CO_(2)emissions.However,it is challenging to achieve high selectivity and maintain stable performance for HVOs(ethylene,propylene,and linear a-olefins)over a prolonged reaction time due to the difficulty in precise control of carbon coupling and rapid catalyst deactivation.Herein,we present a selective Ba and Na co-modified Fe catalyst enriched with Fe_(5)C_(2)and Fe_(3)C active sites that can boost HVO synthesis with up to 66.1%selectivity at an average CO_(2)conversion of 38%for over 500 h.Compared to traditional NaFe catalyst,the combined effect of Ba and Na additives in the NaBaFe-0.5 catalyst suppressed excess oxidation of FeCxsites by H_(2)O.The absence of Fe3O4phase in the spent NaBaFe-0.5 catalyst reflects the stabilization effect of the co-modifiers on the FeCxsites.This study provides a strategy to design Fe-based catalysts that can be scaled up for the stable synthesis of HVOs from CO_(2)hydrogenation.

Application of in-plasma catalysis and post-plasma catalysis for methane partial oxidation to methanol over a Fe_2O_3-CuO/γ-Al_2O_3 catalyst

Methane partial oxidation to methanol （MPOM） using dielectric barrier discharge over a Fe2O3-CuO/γ-Al2O3 catalyst was performed.The multicomponent catalyst was combined with plasma in two different configurations,i.e.,in-plasma catalysis （IPC） and post-plasma catalysis （PPC）.It was found that the catalytic performance of the catalysts for MPOM was strongly dependent on the hybrid configuration.A better synergistic performance of plasma and catalysis was achieved in the IPC configuration,but the catalysts packed in the discharge zone showed lower stability than those connected to the discharge zone in sequence.Active species,such as ozone,atomic oxygen and methyl radicals,were produced from the plasma-catalysis process,and made a major contribution to methanol synthesis.These active species were identified by the means of in situ optical emission spectra,ozone measurement and FT-IR spectra.It was confirmed that the amount of active species in the IPC system was greater than that in the PPC system.The results of TG,XRD,and N2 adsorption-desorption revealed that carbon deposition on the spent catalyst surface was responsible for the catalyst deactivation in the IPC configuration.

Investigation of High Catalyteal Durability for Porous Pt Films Deposited via Magnetron Sputtering

Porous Pt thin films were prepared on carbon papers by a single-step ultra-high dc magnetron sputtering method to obtain ideal electrodes for proton exchange membrane fuel cells.The platinum loading of the electrocatalyst layer is controlled at about 0.1 mg·cm^(-2).Structural characteristics and catalytic activities of the films were analyzed by scanning electron microscopy,atomic force microscopy,X-ray diffraction,cyclic voltammetry,and stress durability testing methods.The effect of treatment conditions of a substrate on the structural and performance characteristics of the catalytic films was shown as well.Films produced on acid-treated carbon papers at the argon pressure of 0.01 mbar possessed a homogeneous,highly developed surface along with a porous structure.Compared to Pt/TCPW(Toray carbon papers soaked in ultrapure water)electrodes,the film obtained on the acid-treated substrate had a larger electrochemical surface area(163.33 m^(2)·g^(-1))and exhibited better catalytic stability and durability due to a porous structure as a result of Pt particle accumulation.

Oxygen reduction on polycobaltprotoporphyrin film Ⅰ.Catalytic activity and stability of polycobaltprotoporphyrin film toward oxygen reduction

The catalytic activity of polycobaltprotoporphyrin(PCoPP)was compared with adsorbed cobaltprotoporphyrin monolayer.The results have shown that PCoPP film shows higher catalytic activity and stability than monolayer on glass carbon electrode in both alkaline and acid solution. Catalytic activity of PCoPP goes through a maximum with increase of film thickness.A model was proposed to explain such dependence.The effect of film thickness and solution pH on the stability of PCoPP film was studied.

Synthesis and stability evaluation of hierarchical silicoaluminophosphates with different structural frameworks in the methanol to olefins process

Silicoaluminophosphates （SAPOs） with different pore structures were synthesized through the implementation of polyethylene glycol （PEG） as a mesopores impregnation agent. Using PEGs with different molecular weights （MWs） and concentrations in the synthesis precursor, several samples were synthesized and characterized. Applying a PEG capping agent to the precursors led to the formation of tuned mesopores within the microporous matrix of the SAPO. The effects of the PEG molecular weight and PEG/Al molar ratio were investigated to maximize the efficiency of the catalyst in the methanol-to-olefin （MTO） process. Using PEG with a MW of 6000 resulted in the formation of both Zeolite Rho and chabazite structural frameworks （i.e., DNL-6 and SAPO-34）. Pure SAPO-34 samples were successfully prepared using PEG with a MW of 4000. Our results showed that the PEG concentrations affect the porosity and acidity of the synthesized materials. Furthermore, the SAPO-34 sample synthesized with PEG （MW of 4000） and a PEG/Al molar ratio of 0.0125 showed a superior catalytic stability in the MTO reaction owing to the tuned bi-modal porosity and tailored acidity pattern. Finally, through reactivation experiments, it was found that the catalyst is stable even after several regeneration cycles.

Effects of support property on the catalytic performance of CeO_2-ZrO_2-CrO_x for 1,2-dichloroethane oxidation

HZSM-5, Al_2O_3, TiO_2 and SiO_2 supported CeO_2-ZrO_2-CrO_x catalysts were prepared by deposition-precipitation method and tested for deep catalytic oxidation of 1,2-dichloroethane（DCE）, as one of the common chlorinated organic pollutants. All the catalysts were characterized by means of N_2 adsorption-desorption, X-ray photoelectron spectroscopy（XPS）, ammonia-temperatureprogrammed desorption（NH_3-TPD） and hydrogen temperature-programmed reduction（H2-TPR）. The characterization results revealed that there was strongly synergistic effect between the oxidizability of CZCr species and the acidity of supports, which obviously promoted the catalytic activity for DCE degradation. 20% CZCr/HZSM-5 showed the highest activity and good durability during the long-term continuous test. The catalytic activity decreased in the order： 20%CZCr/HZSM-5〉CZCr〉20%CZCr/TiO_2〉20%CZCr/Al_2O_3〉20%CZCr/SiO_2.

Lanthanum incorporated in MCM-41 and its application as a support for a stable Ni-based methanation catalyst

Herein, lanthanum was incorporated via hydrothermal synthesis into a MCM-41 framework structure with La/Si molar ratios from 0.01 to 0.1. Samples of NiO supported on LaMCM-41 were prepared using the impregnation method. The catalyst performance was evaluated using a fixed bed CO methanation reactor. A Ni/LaMCM-41 catalyst with La/Si = 0.1 shows the best catalytic performance with a CO conversion of almost 100% and a CH4 selectivity of 89.5% at 250 ℃ under a pressure of 1.5 MPa and at an airspeed of 36,000 mL/（g·h）. Compared with Ni-La/MCM-41（La/Si = 0.1） and Ni/MCM-41 prepared via the impregnation method, Ni/LaMCM-41（La/Si = 0.1） shows a higher CO conversion and CH4 selectivity.In a 100 h stability test, the Ni/LaMCM-41（La/Si = 0.1） catalyst shows excellent stability; furthermore, the CO conversion is always greater than 98.0%, which is significantly better than the results for Ni/MCM-41.We experimentally demonstrate that elemental La enters the framework of MCM-41. The Ni/LaMCM-41 catalyst performs well because the La reduces the average particle size of the NiO particles and enhances the interaction between NiO and MCM-41; moreover, the introduction of La significantly inhibits the sintering of the catalyst and the formation of carbon deposits.

A new class of rhodium complexes containing free donor atoms and their intramolecular substitution reaction

A new class of rhodium complexes with high catalytic activity as well as excellent stability, which was used as catalyst for carbonylation of methanol to acetic acid, is reported. It contains free donor (namely un-coordinated donor) atoms which enable to improve its stability by intramolecular substitution reaction. Its synthesis, characteristic and catalytic reaction were discussed here.