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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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    Co@C nanorods as both magnetic stirring nanobars and magnetic recyclable nanocatalysts for microcatalytic reactions

    Shao, ShihengDing, LeiHan, AijuanWang, Lianying...
    8页
    查看更多>>摘要：The rapid and effective mixing of reactants and catalysts is essential in liquid-phase catalytic reaction to boost mass transport. However, the routinely used magnetic stirring method is impractical for ultra-small systems such as lab-on-chip and flow cell due to the macroscale size of the magnetic bars. Herein, we developed a facile strategy to synthesize catalytically active magnetic Co@C nanorods, which could serve as both high-performance catalysts and magnetic stirring nanobars for micro-catalytic reactions. The Co@C core-shell structure endows the materials with high catalytic activity and excellent durability, while the strong magnetism of Co nanoparticles renders the nanorod catalyst unique stirring capability under an external rotating magnetic field, which significantly promotes the mass transport and also the catalytic efficiency in micro-catalytic reactions. Inspired by the unique structure and properties, the mixing ability and catalytic activity of Co@C nanorods were evaluated in several systems.
      原文链接:
    • NSTL
    • Elsevier

    Ultrastable and high-performance seawater-based photoelectrolysis system for solar hydrogen generation

    Gao, Rui-TingGuo, XiaotianLiu, ShujieZhang, Xueyuan...
    8页
    查看更多>>摘要：Solar hydrogen production from seawater, the most natural resource on the earth, is an economically appealing for renewable energy conversion. A photoelectrochemical (PEC) seawater-splitting system is greatly challenging for designing stable photoelectrodes and obtaining high and stable photocurrents, strongly preventing corrosion of semiconductors in seawater. In this context, we for the first time report an ultra-stable seawater splitting PEC cell based on the BiVO4 protected by a MoO3 barrier layer. The combination of MoO(3)and Mo/B co-doping on BiVO4 photoanode presents a resembled photocurrent density value of 4.30 mA cm(-2) at 1.23 VRHE in simulated seawater and natural seawater under 1 sun AM 1.5G illumination. Equally importantly, the resulting photoanode is quite stable during natural seawater splitting, which shows strong photocorrosion resistance over 70 h of continuous irradiation. Further theoretical calculations provide an insight into the roles of surface dopants for the reduction of substantial surface charge recombination and improving the photocorrosion resistance during long-term operation in the marine environment. This work provides a new avenue for the robust and stable PEC semiconductors design for hydrogen production by seawater photoelectrolysis. Broader context: Seawater photoelectrolysis is one of the promising alternatives for hydrogen production since sun and seawater represent the two most abundant and available resources reserved on earth. However, the corrosion resistance on photoelectrodes should be paid more attention to long-term operation, where the chloride ions from seawater corrode the electrodes. The highly robust and efficient photoelectrodes are thereby required as one of the critical points on potential application. The BiVO4 photoelectrode is a promising semiconductor for photoelectrochemical (PEC) seawater splitting with a suitable bandgap and favorable conduction band edge position. Unfortunately, this photoelectrode undergoes a poor charge carrier and serious photo corrosion which restricts practical applications for solar energy conversion. In this context, we develop a robust BiVO4 protected with a MoO3 barrier layer, constructing with surface dual-doping engineering, which serves as an outstanding PEC electrode for natural seawater photoelectrolysis. We further demonstrate that the optimized photoelectrode presents a resembled photocurrent density value in simulated seawater and natural seawater under 1 sun AM 1.5G illumination, which shows a strong photocorrosion resistance over 70 h of continuous irradiation, representing one of the targets directly avoiding chloride corrosion on seawater photoelectrolysis.
      原文链接:
    • NSTL
    • Elsevier

    Phosphate ions interfacial drift layer to improve the performance of CoFe-Prussian blue hematite photoanode toward water splitting

    Khan, Abdul ZeeshanKandiel, Tarek. A.Abdel-Azeim, SafwatJahangir, Tahir Naveed...
    13页
    查看更多>>摘要：Charge recombination at the surface of hematite photoanode is among the main issues that diminish its photoelectrochemical (PEC) water splitting efficiency. Herein, we address this issue by anchoring phosphate ions (Pi) layer between hematite's surface and CoFe-Prussian blue analogue (CoFe-PBA) water oxidation catalyst (WOC). The PEC results revealed that the Pi interfacial layer is crucial for boosting the PEC activity of CoFe-PBA/hematite photoanode. It improves the activity by 2.9-fold at 1.23 V-RHE. The analysis of time and frequency-resolved results revealed that the synergy between the Pi layer and CoFe-PBA catalyst prolongs the photogenerated holes lifetime, reduces their charge transfer resistance, and suppresses the surface recombination. The DFT simulations suggested that the Pi interfacial layer drifts the electrostatic potential of the hematite's surface toward more negative potential and thus facilities the diffusion of the photogenerated holes toward the hematite/CoFe-PBA/electrolyte interfaces making them dynamically apposite to oxidize water on CoFe-PBA WOC.
      原文链接:
    • NSTL
    • Elsevier

    Trap efficiency of exhaust gas pollutants in microporous sorbents under representative driving conditions

    Chaillou, C.Bourhis, G.Barbera-Italiano, K.Lecompte, M....
    14页
    查看更多>>摘要：The objective of this study is to develop a Neutral Air Quality Impact Vehicle (NAQIV) using a system able to reduce the tailpipe emissions of a gasoline powertrain engine. A possible configuration is a bypass in the exhaust, close to the tailpipe, that stores pollutants during the cold start phase when most emissions occur. For this purpose, adsorption efficiencies of commercial sieved powders Activated Carbon (AC), and zeolites (BEA, MFI) were screened at trap temperatures of 25, 50, and 150 degrees C using two different exhaust gas compositions. These compositions are obtained from two different phases of the World Harmonized Light-Duty Test Cycle (WLTC): the first 100 s after the engine start, and the first "5 km" after a cold start, the latter being representative of typical emissions of an automotive vehicle on an average trip in urban areas. The aim is also to provide sorption capacity not only in respect to the conventional pollutants (CO, NOx, CO2), and the most common NMHCs present in the exhaust gas (toluene, i-pentane, n-pentane, acetylene, ethylene, and methane), but also towards unregulated pollutants such as NH3, CH4 and N2O (to be introduced in Euro 7 regulations). The experimental results reveal a superior performance of AC NMHCs adsorption (and particularly toluene, n-pentane and ipentane) which is not affected by the presence of other pollutants, but is negatively impacted by rising temperature and flow gas composition. Among zeolites, only Cu/Beta and Cu/ZSM-5 display moderate adsorption capacity of NH3, NMHCs and NO. In particular, the adsorption of ethylene and acetylene over Cu/ZSM-5 is strongly promoted at lower H2O concentrations. Finally, desorption profiles of each pollutant were generated through Temperature Programmed Desorption (TPD) experiments, unraveling sorbate-sorbent interactions.
      原文链接:
    • NSTL
    • Elsevier

    Visible-light-driven semihydrogenation of alkynes via proton reduction over carbon nitride supported nickel

    Jia, TongtongMeng, DiJi, HongweiSheng, Hua...
    9页
    查看更多>>摘要：Semihydrogenation of alkynes represents one of the most viable route to produce functional alkene products. Herein we describe the visible-light-driven alcohol or water donating semihydrogenation catalyzed by nickel supported on carbon nitride scaffold (Ni/C3N4) under ambient condition, exhibiting excellent alkene selectivity and broad substrate scope. The catalyst design takes advantage of C3N4 to harvest visible irradiation and to tune the interaction of Ni with hydrogenation intermediates, which is essential for the excellent selectivity toward alkene products. The hydrogen atom incorporated in alkene products originates from hydroxyl group of methanol or water, via a Ni catalyzed proton reduction by photogenerated electrons to give the active surface hydrogen species (H*). Such hydrogenation pathway not only avoids harsh reaction condition but also enables facile synthesis of valuable deuterated alkenes using deuterated alcohols or D2O, promising enormous application potential for well-designed catalyst architectures in the light-driven selective transfer hydrogenation (deuteration) of alkynes and other organic substrates.
      原文链接:
    • NSTL
    • Elsevier

    Flexible, compressible, versatile biomass-derived freestanding carbon monoliths as binder- and substrate-free tri-functional electrodes for solid-state zinc-air batteries and overall water splitting

    Son, Hong JinCho, Ye RimPark, Ye-EunAhn, Sung Hoon...
    11页
    查看更多>>摘要：Highly flexible and compressible biomass-derived freestanding monoliths are directly utilized as binder-and substrate-free tri-functional electrodes for the wearable electronic devices. The introduction of Co nanoparticles, nanoclusters, and single atoms onto biomass-derived monoliths leads to the additional growth of CNTs for ensuring the interconnectivity of 3D cellulose-derived carbon network. Thus, superb flexibility and/or compressibility as well as high-efficiency tri-functional activity are achieved simultaneously. The alkaline water electrolyzer with monolithic electrodes requires only a potential of 1.56 V to generate hydrogen at a current density of 50 mA cm(-2) for over 120 h. Furthermore, the quasi-solid-state zinc-air batteries(ZABs) exhibit a high peak power density of 175.5 mW cm(-2), and an optimal charge-discharge overpotential with a remarkably small voltage gap (delta V) of 0.27 V at 5 mA cm(-2). The excellent charge-discharge cycle stability even under bending and compression conditions demonstrates its high potential for emerging next-generation electronics devices.
      原文链接:
    • NSTL
    • Elsevier

    Unique functionalities of carbon shells coating on ZnFe2O4 for enhanced photocatalytic hydroxylation of benzene to phenol

    Yang, BaoyingZhang, ShikunGao, YanHuang, Lianqi...
    9页
    查看更多>>摘要：Hydroxylation of benzene to phenol over a photocatalyst is a green approach toward phenol production. ZnFe2O4 (ZFO) with an intrinsic peroxidase-like catalytic behavior toward H2O2 activation is an emerging photocatalyst for benzene hydroxylation reaction; however, its catalytic performance is greatly limited by the fast charge recombination, inevitable metal leaching and hydrophilic surface structure. Herein, the encapsulation of ZFO by carbons (ZFO@C) is an effective solution to address these issues. The carbons conformably coating on ZFO not only protect them from corrosion and metal leaching, but also enable the generation of a strong electronic contact between them to facilitate charge separation. In addition, the carbons also increase the surface affinity for benzene adsorption. As a result, ZFO@C exhibited a significant enhanced photocatalytic activity and durability for phenol synthesis. Furthermore, ZFO@C with carbon derived unique functionalities will have a broad application in photocatalytic green synthesis of fine chemicals.
      原文链接:
    • NSTL
    • Elsevier

    High-density ultrafine RuP2 with strong catalyst-support interaction driven by dual-ligand and tungsten-oxygen sites for hydrogen evolution at 1 A cm(-2)

    Zhou, Ya-NanWang, Fu-LiNan, JunZhao, Hui-Ying...
    11页
    查看更多>>摘要：Ultrafine and high-density RuP2 based on coordination chemistry and catalyst-support correlation shows potential for hydrogen evolution reaction (HER). Herein, the uniform and high-density W-doped ultra-small RuP2 (W0.05-RuP2@C3N4-NC) are synthesized by incorporating oxygen-bridged [WO4] tetrahedron into tetraacetic acid (EDTA)-melamino-formaldehyde (MF) ligands. EDTA-MF shows strong metal-support interaction, dedicating to the optimal dispersion, highest Ru yields, and HER activity. W atoms regulate local electron structure and coordination environment, leading to faster proton supply and hydrogen release, thus achieving 10 mA cm(-2) at low overpotential of 27 mV (alkaline) and 66 mV (acidic). Notably, W-0.05-RuP2@C3N4-NC maintains stability with staged 500-1000 mA cm(-2) for 1000 h in alkaline, and 1000 mA cm(-2) for -300 h in acid, ascribing to the immobilized ultra-stable RuP2 nanoclusters via EDTA-MF and metal-oxygen sites. The excellent activity and stability hold promise for industrial hydrogen production, which provides deeper insights into catalyst-support interaction and reasonable design of high Ru-loading electrocatalysts.
      原文链接:
    • NSTL
    • Elsevier

    Stress-induced BiVO4 photoanode for enhanced photoelectrochemical performance

    Jiang, WeiyiAn, YangWang, ZeyanBao, Xiaolei...
    8页
    查看更多>>摘要：BiVO4 is a promising and environmental-benign photoanode material. However, the photoelectrochemical properties of BiVO4 are confined to its low charge separation efficiency. Herein, we have developed a simple method to introduce stress into the BiVO4 photoanode via the change of the unit cell volume of VO2 near the phase transition temperature. In this way, the crystal structure of BiVO4 is caused to be distorted and thus improve the photoelectrochemical properties of the BiVO4 photoanode, making the surface photopotential of the BiVO4-V photoanode nearly double that of the bare BiVO4 photoanode. At room temperature, the photocurrent density of the BiVO4-V photoanode is 2.35 times that of the BiVO4 photoanode. Intriguingly, at 85 C, the photocurrent density of the BiVO4-V photoanode is as high as 6.8 times that of the BiVO4 photoanode. Moreover, the photocurrent density of the BiVO4-V photoanode could reach 80% of the theoretical photocurrent density of the BiVO4 photoanode at 85 C in the presence of the sacrificial agent Na2SO3. This work illustrates a new stress engineering strategy to improve the photoelectrochemical properties of BiVO4 photoanodes and is expected to be applicable to other semiconductor photoanodes.
      原文链接:
    • NSTL
    • Elsevier

    Efficient NiFe-based oxygen evolution electrocatalysts and origin of their distinct activity

    Han, QinglinLuo, YuhongLi, JingdeDu, Xiaohang...
    10页
    查看更多>>摘要：Efficient oxygen evolution reaction (OER) electrocatalyst is essential for water electrolysis. Herein, high -performance NiFe-based layered double hydroxides (LDH), phosphide and sulfide OER pre-catalysts were fabricated and their distinct activity was unveiled. The as-prepared NixFe1-xS exhibits ultralow OER overpotential of 122 mV at 10 mA cm(-2) in 1 M KOH. The alkali-electrolyzer using NixFe1-xS electrodes achieve superior performance exhibiting a voltage of 1.46 V at 10 mA cm(-2). Experimental analysis reveals that, during OER, Fe dissolution into electrolyte occurs for NiFe LDH and NixFe1-xP, which were both converted into NiOOH, well explaining their similar activity. Interestingly, Fe dissolution is significantly mitigated in NixFe1-xS, forming partially oxidized Fe2O3/FeOOH species. Theoretical calculations confirmed that Fe2O3/FeOOH is responsible for the enhanced OER energetics of NixFe1-xS. These observations provide new insights on the distinct activity of NiFe-based electrocatalysts, guiding their rational design as well.
      原文链接:
    • NSTL
    • Elsevier