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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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    Vanadium-phosphorus incorporation induced interfacial modification on cobalt catalyst and its super electrocatalysis for water splitting in alkaline media

    Zhu, ZizhengXu, KaiGuo, WenZhang, Hongyan...
    10页
    查看更多>>摘要：Co-based compounds have been considered as promising earth-abundant electrocatalysts for water splitting, however, the catalytic performance need to be further enhanced. Herein, we report a nickel foam (NF) supported Co-VOx-P nanoflower electrocatalyst that shows excellent catalytic performances, achieving a small over potential of 230 mV at 100 mA/cm(2) for OER. Such performances surpass the recently reported best-performing Co-based catalysts in alkaline media. In addition, the present Co-VOx-P electrocatalyst can deliver 10 mA/cm(2) with a small overpotential of 98 mV for HER. Experimental and DFT studies indicate that, due to the combination of P and V, the Co-VOx-P electrocatalyst shows improved intrinsic catalytic properties including enhanced conductivity, facile electron transfer and favorable surface adsorption strength. The strategy demonstrated here by incorporating metalloid with high valence states may be extended to design other cost-efficient electrocatalysts for more advanced water splitting performances.
      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

    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

    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

    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

    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

    Rational synthesis of BixFe(1-x)VO(4) heterostructures impregnated sulfur-doped g-C3N4: A visible-light-driven type-II heterojunction photo (electro)catalyst for efficient photodegradation of roxarsone and photoelectrochemical OER reactions

    Balu, SridharanChen, Yi-LunChen, Shih-WenYang, Thomas C. -K....
    15页
    查看更多>>摘要：Metal vanadate (MVO4) and graphitic carbon nitride (g-C3N4) semiconductor materials have attracted much interest due to their tremendous physicochemical and photocatalytic performances. In this prospect, BixFe(1_ x)VO(4) were prepared by mixing cation precursors (Bi and Fe) in different proportions (x = 0.7; 0.5; 0.3) via a simple one-pot hydrothermal route and impregnated on the surface of sulfur-doped g-C3N4(SCN) to attain a wide range of solar absorption and effective charge separation. Several spectroscopic techniques were used to analyze the physicochemical and optoelectronic properties of as-synthesized photocatalysts. The photocatalytic activities of as-synthesized photocatalysts were evaluated by photoelectrochemical oxygen evolution reactions (OER) and photodegradation of roxarsone (ROX). This work aims to investigate the formation, photocatalytic performance, and rational mechanism of BixFe1-xVO4/SCN photocatalytic nanocomposites. Among different BixFe(1_ x)VO(4) (x = 0.7; 0.5; 0.3), the BixFe(1_ x)VO(4)/SCN (Bi/Fe = 0.5) nanocomposite results in 85.66% of ROX photodegradation within 90 mins under visible-light irradiation. The photocatalytic performance of the nanocomposite is about 2.49, 2.87, 3.48 folds higher than that of pristine g-C3N4, BiVO4, and FeVO4 samples, respectively. The photo electrochemical OER results suggest the higher photocurrent density at 1.23 V (vs NHE) was achieved by BixFe(1_ x)VO(4)/SCN (0.987 mA cm(-2)) nanocomposite, and which is 16.73, 5.11, and 6.16 times higher than that of CN (0.059 mA cm(-2)), BiVO4 (0.193 mA cm(-2)), and FeVO4 (0.160 mA cm(-2)), respectively. The XPS and photo electrochemical (PEC) analysis depict the higher donor densities (ND) and excellent charge separations through type-II heterojunction of the BixFe(1_ x)VO(4) nanocomposite.
      原文链接:
    • NSTL
    • Elsevier

    Effective regulation of surface bridging hydroxyls on TiO2 for superior photocatalytic activity via ozone treatment

    Liu, BiyuanZhang, BogeJi, JianLi, Kai...
    10页
    查看更多>>摘要：A gas-solid and postsynthetic modification was proposed to enrich surface bridging hydroxyls (OHB) on TiO2 using ozone. It was found that the adsorbed ozone and its decomposition into oxygen atoms on oxygen vacancies would induce water dissociation and form OHB, narrowing the bandgap and enhancing the photoresponse. The increased OHB significantly doubled the efficiency of photogenerated charge carriers transfer, thus generating more reactive oxygen species. Additionally, OHB provided more adsorption sites for toluene, contributing to the excellent activity and stability. The degradation pathways of toluene containing OH addition and hydrogen abstraction were proposed based on in situ DRIFTS results. Ozone treatment was more effective than other reported surface treatments, and presented a universal improvement on both gas-solid and liquid-solid photodegradation. This work provides a facile, effective, and alternative strategy for the targeted regulation of OHB on TiO2 under mild conditions and insight into the mechanism underlying the process.
      原文链接:
    • NSTL
    • Elsevier