Continuous generation of lattice oxygen via redox engineering for boosting toluene degradation performances

Excellent performances promoted by lattice oxygen have attracted wide attention for catalytic degradation of volatile organic compounds(VOCs).However,how to control the continuous regeneration of lattice oxygen from the support is seldom reported.In this study,we selected sepiolite supported manganese-cobalt oxides(Co_(x)Mn_(100-x)O_(y))as model catalysts by tuning Co/(Co+Mn)mass ratio(x=3%,10%,15%,and 20%)to enhance toluene degradation efficiency,owing to lattice oxygen regeneration by redox cycle existing at the interface and Mn species with high valence state,initiated by cobalt catalytic performance under the role of crystal field stability phase.The results of activity test show that the sepiolite-Co_(15)Mn_(85)O_(y)catalyst exhibit outperformances at 193℃with 10,000 h^(-1)GHSV.In addition,the catalyst existed at the bottom of the"volcano"curve correlated T_(50)or T_(90)with Co/(Co+Mn)weight ratio is sepiolite-Co_(15)Mn_(85)O_(y),conforming its outperformance.Further characterized by investigating active sites structural and electronic properties,the essential of superior catalytic activity is attributed to the grands of lattice oxygen continuous formation resulted from redox engineering based on the high atomic ratio of surface lattice oxygen with continuous refilled from the support and that of Mn^(4+)/Mn^(3+)cycle initiated by cobalt catalytic behaviors.All in all,redox engineering,not only promotes grands of active species reversible regeneration,but supplies an alternative catalyst design strategy towards the terrific efficiency-to-cost ratio performance.

Rational Design of LDH/Zn_(2)SnO_(4) Heterostructures for Efficient Mineralization of Toluene Through Boosted Interfacial Charge Separation

It is crucial to efficiently separate and transport photo-induced charge carriers for the effective implementation of photocatalysis toward environmental remediation.A rational design strategy is proposed to validate such proposition through the construction of an interfacial structure in the form of LDH/Zn_(2)SnO_(4) heterostructures in this research.The interfacial charge transfer on LDH/Zn_(2)SnO_(4) is greatly promoted via the unique charge transfer pathway,as characterized by transient photocurrent responses,X-ray photoelectron spectroscopy,electron paramagnetic resonance spectrum,and photoluminescence analysis.As such,it contributes to the generation of reactive oxygen species(ROS)and the activation of reactants for the mineralization of toluene.According to the in situ DRIFTS spectra analysis,the accumulation of benzoic acid takes place possibly through the partial oxidation of the methyl group on toluene at the interface of the LDH/Zn 2 SnO 4 heterostructure.This process can greatly promote the photocatalytic oxidation of toluene with the enhanced ring-opening efficiency.The LDH/Zn 2 SnO 4 is thus demonstrated as superior photocatalyst against toluene(removal efficiency of 89.5%;mineralization of 83.1%;and quantum efficiency of 4.55×10^(−6) molecules/photon).As such,the performance of this composite far exceeds that of their individual components(e.g.,P25,pure Mg-Al LDH,or Zn_(2)SnO_(4)).This study is expected to offer a new path to the interfacial charge transfer mechanism based on the design of highly efficient photocatalysts for air purification.

Defect-poor BaSn(OH)6 enhanced charge separation for efficient photocatalytic degradation of toluene

Crystal defect is well-known to have a significant effect on the photocatalytic performance of semiconductors. Herein, defect-rich and-poor BaSn(OH)6(BSOH-Sn and BSOH-Ba) photocatalysts were synthesized by exchanging the addition order of Ba and Sn. Results show that the defect-poor BSOH-Ba exhibited more efficient toluene degradation under ultraviolet(UV) light, which could attribute to the great suppression of photogenerated electron-hole(e--h+) pairs recombination by tuning the defect concentration. The low defect concentration in BSOH-Ba finally promotes the charge separation efficiency, the generation of reactive oxygen species(ROS), and the photocatalytic toluene degradation reactions. This work not only provides an effective way to inhibit the recombination of photogenerated carriers and improve the photocatalytic performance, but also promotes the understanding of defective perovskite-type hydroxide for more photoreactions.

Photocatalytic Activity of Porous Magnesium Oxychloride Cement Combined with AC/TiO2 Composites

As a decorative material, magnesium oxychloride cement was used as a photocatalyst supporter to purify the pollutants indoors. Due to excellent adsorption properties of activated carbon（AC）, the photocatalytic composties, TiO2/AC, were prepared and introduced into the porous magnesium oxychloride cement（PMOC） substrate to composite a sort of photocatalytic cementitious material（PCM）. The optimal composite processes were assessed by gas chromatograph, using toluene as the target. By comparing the perspective of toluene purification and thorough decomposition, it can be found that the optimal mass ratio for TiO2/AC composites is 4/25, and the heat treatment to TiO2/AC sample at 350 ℃ can play the optimal synergetic role of adsorbents in photocatalytic process. The synergistic effect of TiO2, AC and magnesium oxychloride cement（MOC） was also evaluated by gas chromatograph. One-take molding process was adopted to introduce the TiO2/AC into PMOC substrate, and its optimal mass fraction was 4 wt%, while the appropriate density of substrate was 0.35 g/cm3. Toluene degradation showed that the prepared PCM can degrade pollutants efficiently. The appropriate treatment process of TiO2/AC, mass of TiO2/AC, substrate density, and stable pore structure should be coordinated to maximize the adsorption-photodegradation performance. The combination of photocatalytic materials, adsorbents, and building materials provided a new idea for the application of photocatalysis.

Mesoporous carbon-supported cobalt catalyst for selective oxidation of toluene and degradation of water contaminants

Mesoporous carbon-supported cobalt （Co-MC） catalysts are widely applied as electrode materials for bat- teries. Conversely, the development of Co-MC as bifunctional catalysts for application in organic catalytic reactions and degradation of water contaminants is slower. Herein, the catalyst displayed high activity in the selective oxidation of toluene to benzaldehyde under mild conditions, attaining a high selectivity of 92.3%. Factors influencing the catalytic reaction performance were also investigated. Additionally, Co-MC displayed remarkable catalytic activity in degrading dyes relative to the pure metal counterpart. Moreover, the catalyst exhibited excellent reusability, as determined by the cyclic catalytic experiments. The paper demonstrates the potential of Co-MC as a bifunctional catalyst for both toluene selective oxidation and water contaminant degradation.

Accelerated oxidation of VOCs via vacuum ultraviolet photolysis coupled with wet scrubbing process

Vacuum ultraviolet(VUV) photolysis is a facile method for volatile organic compounds(VOCs) elimination, but is greatly limited by the relatively low removal efficiency and the possible secondary pollution. To overcome above drawbacks, we developed an efficient method for VOCs elimination via VUV photolysis coupled with wet scrubbing process. In this coupled process, volatile toluene, a representative of VOCs, was oxidized by the gas-phase VUV photolysis, and then scrubbed into water for further oxidation by the liquid-phase VUV photolysis. More than 96% of toluene was efficiently removed by this coupled process, which was 2 times higher than that in the gas-phase VUV photolysis. This improvement was attributed to the synergistic effect between gas-phase and liquid-phase VUV photolysis. O3and HO·are the predomination reactive species for the toluene degradation in this coupled process, and the generation of O3in gas-phase VUV photolysis can efficiently enhance the HO·production in liquid-phase VUV photolysis. The result from in-situ proton transfer reaction ionization with mass analyzer(PTR-MS) further suggested that most intermediates were trapped by the wet scrubbing process and efficiently oxidized by the liquid-phase VUV photolysis, showing a high performance for controlling the secondary pollution. Furthermore, the result of stability test and the reuse of solution demonstrated that this coupled process has a highly stable and sustainable performance for toluene degradation. This study presents an environmentally benign and highly efficient VUV photolysis for gaseous VOCs removal in the wet scrubbing process.