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Applied Catalysis
Elsevier Science Publishers
Applied Catalysis

Elsevier Science Publishers

0926-3373

Applied Catalysis/Journal Applied Catalysis
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    Synergistic effect of triphase interface and fluid control for efficient photosynthesis of residue-free H2O2

    Huining HuangRun ShiQitao Zhang
    9页
    查看更多>>摘要：Solar-to-chemical energy conversion is a challenging subject for renewable energy storage. Solar-driven hydrogen peroxide (H2O2) synthesis is a sustainable and potentially economic technology. Despite great efforts in catalyst engineering, photocatalytic H2O2 production is usually limited by the sluggish oxygen diffusion and H2O2 decomposition side reactions, leading to poor apparent photocatalytic H2O2 production efficiency. Herein, we developed a fluid triphase system that enables both the efficient interfacial oxygen mass transfer and the inhibited H2O2 decomposition side reactions. Such a synergistic effect endowed a residue-free H2O2 production rate of 6.03 μmol h~(-1) from pure water and oxygen without using any sacrificial agent or additive, with over 120 h continuous irradiation stability. We further designed a photosynthesis-concentration tandem system to produce high concentration H2O2 (10 mM), which demonstrated an effective water disinfection capability as a representative application.
      原文链接:
    • NSTL

    Superior visible light-mediated catalytic activity of a novel N-doped, Fe3O4-incorporating MgO nanosheet in presence of PMS: Imidacloprid degradation and implications on simultaneous bacterial inactivation

    Somaye AkbariGholamreza MoussaviJeremie Decker
    21页
    查看更多>>摘要：Impressive Imidacloprid (IMD) degradation and bacterial inactivation were attained through the photo catalytic activation of peroxymonosulfate (PMS) via a novel, N-doped MgO@Fe3O4, under visible light. After complete characterization (XPS, XRD, FT-IR, FE-SEM, EDX, HRTEM, DRS, BET, VSM, and EIS), using [PMS]=75 mg/L, [N-MgO@Fe3O4]=150 mg/L at pH=5.6, around 95% of 10 mg/L IMD was degraded within 60 min;; highly synergic interactions between the various catalytic routes were revealed. Extensive scavenger tests and EPR studies revealed that SO4~(·-), HO·, and ~1O2 are generated and play a key role in IMD degradation. Tap water experiments proceeded unhindered, and only the presence of high HCO3" and PO4~(3-) concentration resulted in a decrease in the IMD degradation efficiency, while negligible leaching, magnetization, notable separation, and reusability properties were well-preserved for six repetitive cycles. Finally, E. coli disinfection was achieved before IMD degradation, possibly affected by its transformation byproducts. The overall efficacy of N-MgO@Fe3O4 indicated the potential for implementation in contaminated waters.
      原文链接:
    • NSTL

    Ru/HxMoO_(3-y) with plasmonic effect for boosting photothermal catalytic CO2 methanation

    Hao GeYasutaka KuwaharaKazuki Kusu
    11页
    查看更多>>摘要：Utilizing localized surface plasmon resonance (LSPR) effect of catalysts to facilitate photothermal catalysis of CO2 to CH4 is an attractive strategy for mitigating CO2 emissions. Herein, we demonstrate that Ru/HxMoO_(3-y) synthesized via H-spillover exhibits plasmonic absorption in the visible-near-infrared (Vis-NIR) region, achieving a CH4 yield of 20.8 mmol/g_(cat)/h (520 mmol/g_(Ru)/h) with 100 % selectivity in the CO2 methanation under Vis-NIR light irradiation at 140 °C. Irradiation with Vis-NIR light substantialy increases the CH4 yield (～ 4.7 fold) compared with that under dark conditions. The abundant surface oxygen vacancies provide active sites for CO2 adsorption and activation. In situ infrared spectroscopic analysis reveals that photothermal catalytic CO2 methanation follows *CO pathway. This work represents a simple strategy for developing a plasmonic catalyst for efficient photothermal catalytic CO2 methanation.
      原文链接:
    • NSTL

    Scalable decomposition-catalysis of disposable COVID-19 face mask over self-assembly metal-doping carbocatalysts for tunable value-added products

    Yuan JiangRuolan XuChen Zeng
    16页
    查看更多>>摘要：This study explored a scalable decomposition-catalysis route to effectively valorize disposable COVID-19 face mask into tunable value-added products. The metal-doping carbonaceous catalysts (M/Cs) were successfully synthesized through a single-step energy-efficient thermal process. The modest decomposition-catalysis of face mask over Zn/C gave rise to a relatively high yield (73.52%) of liquid oil with 99% of selectivity toward jet fuel range (C8 - C_(16)) hydrocarbons. Besides, the scalable decomposition-catalysis of face mask over Ni(50)/C at 800 °C was observed to thoroughly transform face mask into gas with the cumulative gas yield of 967 NmL/g_(mask), involving 49.90 vol% of H2 and 40.90 vol% of CH4. Moreover, a dense, entangled growth of carbon nanotubes were formed on the surface of M/Cs. In brief this study developed a scalable and promising route by using M/Cs for the valorization of COVID-19 face mask into hydrocarbon fuel or coupling harvest of H2-enriched fuel gas and carbon nanotubes.
      原文链接:
    • NSTL

    Development of Ti/TiOx foams for removal of organic pollutants from water: Influence of porous structure of Ti substrate

    Jing MaClement TrelluNihal Oturan
    12页
    查看更多>>摘要：Ti/TiOx foams were obtained from plasma spraying technique using different porous Ti substrates. They were then applied for removal of organic pollutants from water by electro-oxidation. Effectiveness of these anodes was investigated using linear sweep voltammetry, probe molecules, quenchers and model pollutants. It was emphasized that surface morphology should allow for homogeneous coating of the surface in order to promote non-selective "OH-mediated oxidation of recalcitrant organic pollutants. Porous structure was also the key parameter for mass transport enhancement. Coarse roughness with characteristic scale that is larger than the diffusion boundary layer was more suitable in stirred-tank reactor. Flow-through application of Ti/TiOx foam further enhanced mass transport and allowed for 3.9-and 1.9-times enhancement of the degradation kinetic of paracetamol compared to Ti/TiOx plate and BDD plate, respectively. This work gives new insights on the role of porous structure of substrate for development and application of suitable electrodes in water treatment.
      原文链接:
    • NSTL

    Nb2CTx MXenes fimctionalized Co-NC enhancing electrochemical H2O2 production for organics degradation

    Xiao HuangWang ZhangWei Liu
    9页
    查看更多>>摘要：Cobalt-dispersed nitrogen-doped carbon nanotubes supported on oxygen-terminated Nb2CTx MXenes (Co-NC/MXenes) are successfully constructed, in which ZIF-67 are in-situ grown on Nb2CTx and then converted to Co-NC followed a pyrolysis process. The introduction of oxygen-terminated Nb2CTx MXenes can effectively regulate the structure of Co-NC and induces a strong interaction between Nb2CTx and Co-NC, promoting H2O2 electrosynthesis via two-electron (2e~-) oxygen reduction reaction (ORR) with high selectivity. Moreover, the assembled device with Co-NC/MXenes as cathode enables an accumulated H2O2 concentration of 4.8 wt% even under natural air diffusion. When combined with the dual-cathode system, the device achieves excellent total organic carbon (TOC) removal towards organic dyes (50 mg L~(-1)) and sulfamethoxazole (20 mg L~(-1)). This work provides a direction for the precise construction of 2e" ORR catalysts and expands an emerging application of the dual-cathode technique.
      原文链接:
    • NSTL

    Breaking the intrinsic activity barriers of perovskite oxides photocatalysts for catalytic CO2 reduction via piezoelectric polarization

    Jie HeXuandong WangShenyu Lan
    11页
    查看更多>>摘要：Breaking the limitations of the intrinsic redox potential of perovskite oxides photo catalysts for catalytic CO2 reduction remains a big challenge. Here we report a new process to achieve the durability yet efficient CO2 reduction activity of various perovskite oxides (BiFeO3, LaFeO3 and LaNiO3) with an inactive CO2 photo-reduction ability via piezoelectrically polarization. Taking BiFeO3 (BFO) as a representative sample, the band tilting and structure compression of BFO reach the redox potential of CO2 reduction and build a piezoelectric field for CO2 adsorption and activation by introducing vibration energy, inducing a piezoelectric catalytic CO2 reduction process. Continued ultrasonic vibration with BFO achieves durability CO2 reduction to high production rates of CH4 (17.9 μmol g~(-1) h~(-1)) and CO (28.7 μmol g~(-1) h~(-1)), respectively. This crucial feature highlights the feasibility of piezoelectric catalysis for CO2 conversion by utilizing mechanical energy, which can break the limitation of intrinsic redox properties ot the perovskite oxides.
      原文链接:
    • NSTL

    Controlling the selectivity of high-surface-area Ru/TiO2 catalysts in CO2 reduction - modifying the reaction properties by Si doping of the support

    Sebastian CisnerosShilong ChenCorinna Fauth
    15页
    查看更多>>摘要：The influence of Si doping of high specific-surface-area Ru/TiO2 catalysts with similar structural properties on the CO2 reduction reaction was systematically investigated by kinetic measurements, combined with microscopic and spectroscopic methods for ex situ and in situ /operando catalyst characterization. While for undoped Ru/TiO2 a high-temperature treatment (350 °C) in reaction atmosphere results in a pronounced change of the selectivity from methanation to CO formation via the reverse water-gas shift (RWGS) reaction, CH4 formation is stabilized by Si doping of the catalyst support. For doping levels around 8 wt%, almost 100% CH4 selectivity is maintained. Comprehensive catalyst characterization is employed to identify trends in the physical and chemical properties with increasing Si doping and thus physical reasons responsible for the distinct differences in catalyst performance and stability. This work opens a route for improving the stability and selectivity of Ru/TiO2 catalysts in the CO2 hydrogenation reaction, a highly relevant application.
      原文链接:
    • NSTL

    Fe single-atom catalysts with pre-organized coordination structure for efficient electrochemical nitrate reduction to ammonia

    Wen-Da ZhangHongliang DongLang Zhou
    9页
    查看更多>>摘要：Single atom catalysts (SAC) have the potential to achieve large-scale production of NH3 through electrochemical nitrate reduction reaction (NO3~-RR). Tailoring the coordination structure of the SAC can effectively tune their electronic structure and thus promote their catalytic selectivity and activity. In this work, Fe SAC with unique FeN2O2 coordination was fabricated through direct pyrolysis of metal-organic frameworks that have pre-organized FeN2O4 environment. Fe SAC exhibits both high faradaic efficiency (-92%) and high ammonia yield rate (46 mg h~(-1) mg_(cat.)~(-1) ) in neutral electrolytes. Density functional theory calculations reveal that the O atoms in FeN2O2 can tune the d-band center of Fe and thus adjust the adsorption energies of the NO3~-RR intermediates. Compared to FeN4, FeN2O2 structure has higher conductivity and selectivity to NH3 and can spontaneously trigger the transformation of *NOH to N *, thus promoting the NO3~-RR. This work provides a simple method to fabricate O, N-coordinated Fe SAC and may stimulate the flourishing development of asymmetric SAC for electrocatalysis.
      原文链接:
    • NSTL

    Hierarchical pore enhanced adsorption and photocatalytic performance of graphene oxide/Ti-based metal-organic framework hybrid for toluene removal

    Jie JinJeong Pil KimShipeng Wan
    9页
    查看更多>>摘要：Metal-organic frameworks (MOFs) have been intensively hybridized with graphene oxide (GO) to enhance their catalytic performance;; however, the effect of the pore structure of MOFs on the activity of GO/MOF hybrids remains elusive. Herein, GO nanosheets were integrated with Ti-based MOF (MIL-125) that possesses the controlled pore structure. The toluene removal experiment results demonstrate that hierarchically porous MIL-125 (MIL-125 (H)) with 10 wt% GO (10% GO/MIL-125 (H)) exhibits concurrent enhancement of adsorption and photocatalytic performance compared to these of 10 wt% GO/microporous MIL-125 (MIL-125 (M)) (10% GO/MIL-125 (M)) counterpart. It is because the hierarchical pore structure of MIL-125 (H) endows hybrids with faster mass diffusion, stronger interaction between components, easier charge separation, better light adsorption ability, and superior photothermal effect. This work provides a reference for the relationship between the pore structure of MOFs and the efficiency of GO/MOF hybrids.
      原文链接:
    • NSTL