Frontiers of Chemical Science and Engineering

ISSN 2095-0179

ISSN 2095-0187(Online)

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A free-standing superhydrophobic film for highly efficient removal of water from turbine oil
Fan Shu, Meng Wang, Jinbo Pang, Ping Yu
Front. Chem. Sci. Eng.    2019, 13 (2): 393-399.   https://doi.org/10.1007/s11705-018-1754-3
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A free-standing superhydrophobic film is prepared by sequentially dip-coating a commercially available filter paper with nano SiO2 suspension, epoxy emulsion, and octyltrimethoxysilane solution. A surface with micro- or nano-roughness is formed because SiO2 nanoparticles are uniformly and firmly adhered on the backbone of the filter paper by the cured epoxy resin. Furthermore, the surface energy is significantly reduced because of introducing octytrimethoxysilane. Such a surface structure makes the prepared film a superhydrophobic material. Due to its free-standing nature, this superhydrophobic film can be used to remove water from turbine oil by filtration. The efficiency of water removal is high (up to 94.1%), and the filtration process is driven solely by gravity without extra energy consumption. Because of the facile fabrication process and the high efficiency of water removal, this free-standing superhydrophobic film may find application in power industry.

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Effect of adding a smart potassium ion-responsive copolymer into polysulfone support membrane on the performance of thin-film composite nanofiltration membrane
Meibo He, Zhuang Liu, Tong Li, Chen Chen, Baicang Liu, John C. Crittenden
Front. Chem. Sci. Eng.    2019, 13 (2): 400-414.   https://doi.org/10.1007/s11705-018-1757-0
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Thin-film composite (TFC) nanofiltration (NF) membranes were fabricated via the interfacial polymerization of piperazine (PIP) and 1,3,5-benzenetricarbonyl trichloride on polysulfone (PSf) support membranes blended with K+-responsive poly(N-isopropylacryamide-co-acryloylamidobenzo-15-crown-5) (P(NIPAM-co-AAB15C5)). Membranes were characterized by attenuated total reflection Fourier transform infrared spectroscopy, X-ray photoelectron spectroscopy, atomic force microscope, scanning electron microscope, contact angle, and filtration tests. The results showed that: (1) Under K+-free conditions, the blended P(NIPAM-co-AAB15C5)/PSf supports had porous and hydrophilic surfaces, thereby producing NF membranes with smooth surfaces and low MgSO4 rejections; (2) With K+ in the PIP solution, the surface roughness and water permeability of the resultant NF membrane were increased due to the K+-induced transition of low-content P(NIPAM-co-AAB15C5) from hydrophilic to hydrophobic; (3) After a curing treatment at 95 °C, the improved NF membrane achieved an even higher pure water permeability of 10.97 L·m−2·h−1·bar−1 under 200 psi. Overall, this study provides a novel method to improve the performance of NF membranes and helps understand the influence of supports on TFC membranes.

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Intrinsic kinetics and external diffusion of catalytic steam gasification of fine coal char particles under pressurized and fluidized conditions
Xuantao Wu, Jie Wang
Front. Chem. Sci. Eng.    2019, 13 (2): 415-426.   https://doi.org/10.1007/s11705-018-1725-8
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Catalytic steam gasification of fine coal char particles was carried out using a self-made laboratory reactor to determine the intrinsic kinetics and external diffusion under varying pressures (0.1–0.5 MPa) and superficial gas flow velocities (GFVs) of 13.8– 68.8 cm∙s−1. In order to estimate the in-situ gas release rate at a low GFV, the transported effect of effluent gas on the temporal gasification rate pattern was simulated by the Fluent computation and verified experimentally. The external mass transfer coefficients (kmam) and the effectiveness factors were determined at lower GFVs, based on the intrinsic gasification rate obtained at a high GFV of 55.0 cm∙s–1. The kmam was found to be almost invariable in a wider carbon conversion of 0.2–0.7. The variations of kmam at a median carbon conversion with GFV, temperature and pressure were found to follow a modified Chilton-Colburn correlation: Sh=0.311Re2.83Sc13(PP0)2.07 (0.04<Re<0.19), where P is total pressure and P0 is atmospheric pressure. An intrinsic kinetics/external diffusion integrating model could well describe the gasification rate as a function of GFV, temperature and pressure over a whole gasification process.

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Tailoring electrical conductivity of two dimensional nanomaterials using plasma for edge electronics: A mini review
Aswathy Vasudevan, Vasyl Shvalya, Aleksander Zidanšek, Uroš Cvelbar
Front. Chem. Sci. Eng.    2019, 13 (3): 427-443.   https://doi.org/10.1007/s11705-019-1805-4
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Since graphene has been discovered, two-dimensional nanomaterials have attracted attention due to their promising tunable electronic properties. The possibility of tailoring electrical conductivity at the atomic level allows creating new prospective 2D structures for energy harvesting and sensing-related applications. In this respect, one of the most successful way to manipulate the physical properties of the aforementioned materials is related to the surface modification techniques employing plasma. Moreover, plasma-gaseous chemical treatment can provide a controlled change in the bandgap, increase sensitivity and significantly improve the structural stability of material to the environment as well. This review deals with recent advances in the modification of 2D carbon nanostructures for novel ‘edge’ electronics using plasma technology and processes.

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Microwave-assisted catalytic oxidation of gaseous toluene with a Cu-Mn-Ce/cordierite honeycomb catalyst
Longli Bo, Shaoyuan Sun
Front. Chem. Sci. Eng.    2019, 13 (2): 385-392.   https://doi.org/10.1007/s11705-018-1738-3
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A novel Cu-Mn-Ce/cordierite honeycomb catalyst was prepared by an incipient wetness method and the catalyst was characterized. The active ingredients were present as various spinel species of Cu, Mn and Ce oxides with different valences and they were unevenly dispersed over the surface of the catalyst. The catalytic oxidation of gaseous toluene was primarily investigated using a fixed bed reactor under microwave heating in the continuous flow mode. Under the optimal conditions of 6.7 wt-% loading of the active component, a bed temperature of 200°C, a flow rate of 0.12 m3·h−1 and an initial concentration of toluene of 1000 mg·m−3, the removal and mineralization efficiencies of toluene were 98% and 70%, respectively. Thus the use of the microwave effectively improved the oxidation of toluene and this is attributed to dipole polarization and hotspot effects. After four consecutive cycles (a total of 1980 min), the Cu-Mn-Ce/cordierite catalyst still exhibited excellent catalytic activity and structural stability, and the toluene removal was higher than 90%. This work demonstrates the possibility of treating volatile organic compounds in exhaust gases by microwave-assisted catalytic oxidation.

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Dealumination and desilication for Al-rich HZSM-5 zeolite via steam-alkaline treatment and its application in methanol aromatization
Yuehua Fang, Fan Yang, Xuan He, Xuedong Zhu
Front. Chem. Sci. Eng.    2019, 13 (3): 543-553.   https://doi.org/10.1007/s11705-018-1778-8
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The hierarchical HZSM-5 was prepared via dealumination and desilication of commercial Al-rich HZSM-5, and characterized by X-ray diffraction, 27Al magic-angle spinning nuclear magnetic resonance, inductively coupled plasma mass spectrometry, scanning electron microscope, transmission electron microscope, N2 adsorption-desorption, NH3 temperature-programmed desorption, performed thermogravimetric and Raman spectrum. The results showed that partial framework of HZSM-5 was removed after steam treatment at 0.15 MPa, 500°C for 3 h. HZSM-5 with high specific surface area and much mesoporosity was obtained by the subsequent alkaline treatment. The regulation of acid quantity was achieved by altering the concentration of alkaline. Dealumination and desilication of Al-rich HZSM-5 zeolites became more effective using a combination of steam and alkaline treatments than using alkaline treatment alone. Methanol aromatization reaction was employed to evaluate the catalytic performance of treated HZSM-5 at 0.15 MPa, 450°C and MHSV of 1.5 h−1. The results indicated that after steam treatment, HZSM-5 further treated with 0.2 mol/L NaOH exhibits the best catalytic performance: the selectivity of aromatics reached 42.1% and the lifetime of catalyst attained 212 h, which are much better than untreated HZSM-5.

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Molecular tailoring to improve polypyrrole hydrogels’ stiffness and electrochemical energy storage capacity
Evelyn Chalmers, Yi Li, Xuqing Liu
Front. Chem. Sci. Eng.    2019, 13 (4): 684-694.   https://doi.org/10.1007/s11705-019-1817-0
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This research looks at ways of tailoring and improving the stiffness of polypyrrole hydrogels for use as flexible supercapacitor electrodes. Molecules providing additional cross-linking between polypyrrole chains are added post-polymerisation but before gelation, and are found to increase gel stiffness by up to 600%, with the degree of change dependent on reactant type and proportion. It was also found that addition of phytic acid led to an increase in pseudocapacitive behaviour of the hydrogel, and thus a maximum specific capacitance of 217.07 F·g1 could be achieved. This is an increase of 140% compared to pristine polypyrrole hydrogels produced by this method.

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An overview of carbon nanotubes role in heavy metals removal from wastewater
Leila Ouni, Ali Ramazani, Saeid Taghavi Fardood
Front. Chem. Sci. Eng.    2019, 13 (2): 274-295.   https://doi.org/10.1007/s11705-018-1765-0
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The scarcity of water, mainly in arid and semi-arid areas of the world is exerting exceptional pressure on sources and necessitates offering satisfactory water for human and different uses. Water recycle/reuse has confirmed to be successful and promising in reliable water delivery. For that reason, attention is being paid to the effective treatment of alternative resources of water (other than fresh water) which includes seawater, storm water, wastewater (e.g., dealt with sewage water), and industrial wastewater. Carbon nanotubes (CNTs) are called the technology of 21st century. Nowadays CNTs have been widely used for adsorption of heavy metals from water/wastewater due to their unique physical and chemical properties. This paper reviews some recent progress (from 2013 to 2018) in the application of CNTs for the adsorption of heavy metals in order to remove toxic pollutants from contaminated water. CNTs are expected to be a promising adsorbent in the future because of its high adsorption potential in comparison to many traditional adsorbents.

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Carbon-based materials for photodynamic therapy: A mini-review
Di Lu, Ran Tao, Zheng Wang
Front. Chem. Sci. Eng.    2019, 13 (2): 310-323.   https://doi.org/10.1007/s11705-018-1750-7
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Carbon-based materials have been extensively applied in photodynamic therapy owing to the unique optical characteristics, good biocompatibility and tunable systematic toxicity. This mini-review mainly focuses on the recent application of carbon-based materials including graphene, carbon nanotube, fullerene, corannulene, carbon dot and mesoporous carbon nanoparticle. The carbon-based materials can perform not only as photosensitizers, but also effective carriers for photosensitizers in photodynamic therapy, and its combined treatment.

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Plasma for cancer treatment: How can RONS penetrate through the cell membrane? Answers from computer modeling
Annemie Bogaerts, Maksudbek Yusupov, Jamoliddin Razzokov, Jonas Van der Paal
Front. Chem. Sci. Eng.    2019, 13 (2): 253-263.   https://doi.org/10.1007/s11705-018-1786-8
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Plasma is gaining increasing interest for cancer treatment, but the underlying mechanisms are not yet fully understood. Using computer simulations at the molecular level, we try to gain better insight in how plasma-generated reactive oxygen and nitrogen species (RONS) can penetrate through the cell membrane. Specifically, we compare the permeability of various (hydrophilic and hydrophobic) RONS across both oxidized and non-oxidized cell membranes. We also study pore formation, and how it is hampered by higher concentrations of cholesterol in the cell membrane, and we illustrate the much higher permeability of H2O2 through aquaporin channels. Both mechanisms may explain the selective cytotoxic effect of plasma towards cancer cells. Finally, we also discuss the synergistic effect of plasma-induced oxidation and electric fields towards pore formation.

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Special Issue on future directions in plasma nanoscience
Erik C. Neyts
Front. Chem. Sci. Eng.    2019, 13 (2): 199-200.   https://doi.org/10.1007/s11705-019-1843-y
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Two-dimensional SnS2 nanosheets on Prussian blue template for high performance sodium ion batteries
Glenn J. Sim, Kakui Ma, Zhixiang Huang, Shaozhuan Huang, Ye Wang, Huiying Yang
Front. Chem. Sci. Eng.    2019, 13 (3): 493-500.   https://doi.org/10.1007/s11705-019-1826-z
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Three-dimensional Prussian blue (PB) nanostructures was obtained via a one-step hydrothermal method. Subsequently, two-dimensional tin disulfide (SnS2) nanosheets were grown onto PB through a facile hydrothermal synthesis. The as prepared SnS2/PB is further employed as the anode of sodium ion batteries (SIBs). SnS2/PB nanoarchitecture delivers a specific capacity of 725.7 mAh∙g−1 at 50 mA∙g−1. When put through more than 200 cycles, it achieved a stable cycling capacity of 400 mAh∙g−1 at 200 mA∙g−1. The stable Na+ storage properties of SnS2/PB was attributed to the synergistic effect among the conductive PB carbon, used as the template in this work. These results obtained potentially paves the way for the development of excellent electrochemical performance with stable performance of SIBs.

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Molecular dynamics simulations of initial Pd and PdO nanocluster growth in a magnetron gas aggregation source
Pascal Brault, William Chamorro-Coral, Sotheara Chuon, Amaël Caillard, Jean-Marc Bauchire, Stève Baranton, Christophe Coutanceau, Erik Neyts
Front. Chem. Sci. Eng.    2019, 13 (2): 324-329.   https://doi.org/10.1007/s11705-019-1792-5
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Molecular dynamics simulations are carried out for describing growth of Pd and PdO nanoclusters using the ReaxFF force field. The resulting nanocluster structures are successfully compared to those of nanoclusters experimentally grown in a gas aggregation source. The PdO structure is quasi-crystalline as revealed by high resolution transmission microscope analysis for experimental PdO nanoclusters. The role of the nanocluster temperature in the molecular dynamics simulated growth is highlighted.

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The synthesis of 6-(tert-butyl)-8-fluoro-2,3-dimethylquinoline carbonate derivatives and their antifungal activity against Pyricularia oryzae
Long Cheng, Ruirui Zhang, Hongke Wu, Xinghai Liu, Tianming Xu
Front. Chem. Sci. Eng.    2019, 13 (2): 369-376.   https://doi.org/10.1007/s11705-018-1734-7
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A series of novel 6-(tert-butyl)-8-fluoro-2,3-dimethylquinoline carbonate derivatives were designed and synthesized. Bioassay results showed that some of them exhibited good activity against Pyricularia oryzae (P. oryzae). It was found that the compound 5q (benzyl (6-(tert-butyl)-8-fluoro-2,3-dimethylquinolin-4-yl) carbonate) possessed good activity against P. oryzae whatever protective activity (10 mg·L1) or curative activity (25 mg·L1), which was better than that of control tebufloquin. In addition, the frontier molecular orbit results revealed that the compound held higher activity against P. oryzae when the total energy was low and the ClogP was high, which may provide useful information for further design novel fungicides.

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Synthesis of Ag and Cd nanoparticles by nanosecond-pulsed discharge in liquid nitrogen
Mahmoud Trad, Alexandre Nominé, Natalie Tarasenka, Jaafar Ghanbaja, Cédric Noël, Malek Tabbal, Thierry Belmonte
Front. Chem. Sci. Eng.    2019, 13 (2): 360-368.   https://doi.org/10.1007/s11705-019-1802-7
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The synthesis of CdO, Ag2O (5 nm) and Ag (~20‒30 nm) nano-objects is achieved simultaneously by nanosecond-pulsed discharges in liquid nitrogen between one cadmium electrode and one silver electrode. Oxidation occurs when liquid nitrogen is fully evaporated and nanoparticles are in contact with the air. No alloy is formed, whatever the conditions, even though both elements are present simultaneously, as showed by time-resolved optical emission spectroscopy. This lack of reactivity between elements is attributed to the high pressure within the discharge that keeps each metallic vapor around the electrode it comes from. Each element exhibits a specific behavior. Cubic Cd particles, formed at 4 kV, get elongated with filamentary tips when the applied voltage reaches 7 and 10 kV. Cd wires are formed by assembly in liquid nitrogen of Cd nanoparticles driven by dipole assembly, and not by dielectrophoresis. On the contrary, silver spherical particles get assembled into 2D dendritic structures. The anisotropic growth of these structures is assumed to be due to the existence of pressure gradients.

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Towards an integrated modeling of the plasma-solid interface
Michael Bonitz, Alexey Filinov, Jan-Willem Abraham, Karsten Balzer, Hanno Kählert, Eckhard Pehlke, Franz X. Bronold, Matthias Pamperin, Markus Becker, Dettlef Loffhagen, Holger Fehske
Front. Chem. Sci. Eng.    2019, 13 (2): 201-237.   https://doi.org/10.1007/s11705-019-1793-4
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Solids facing a plasma are a common situation in many astrophysical systems and laboratory setups. Moreover, many plasma technology applications rely on the control of the plasma-surface interaction, i.e., of the particle, momentum and energy fluxes across the plasma-solid interface. However, presently often a fundamental understanding of them is missing, so most technological applications are being developed via trial and error. The reason is that the physical processes at the interface of a low-temperature plasma and a solid are extremely complex, involving a large number of elementary processes in the plasma, in the solid as well as fluxes across the interface. An accurate theoretical treatment of these processes is very difficult due to the vastly different system properties on both sides of the interface: Quantum versus classical behavior of electrons in the solid and plasma, respectively; as well as the dramatically differing electron densities, length and time scales. Moreover, often the system is far from equilibrium. In the majority of plasma simulations surface processes are either neglected or treated via phenomenological parameters such as sticking coefficients, sputter rates or secondary electron emission coefficients. However, those parameters are known only in some cases and with very limited accuracy. Similarly, while surface physics simulations have often studied the impact of single ions or neutrals, so far, the influence of a plasma medium and correlations between successive impacts have not been taken into account. Such an approach, necessarily neglects the mutual influences between plasma and solid surface and cannot have predictive power.

In this paper we discuss in some detail the physical processes of the plasma-solid interface which brings us to the necessity of coupled plasma-solid simulations. We briefly summarize relevant theoretical methods from solid state and surface physics that are suitable to contribute to such an approach and identify four methods. The first are mesoscopic simulations such as kinetic Monte Carlo and molecular dynamics that are able to treat complex processes on large scales but neglect electronic effects. The second are quantum kinetic methods based on the quantum Boltzmann equation that give access to a more accurate treatment of surface processes using simplifying models for the solid. The third approach are ab initio simulations of surface process that are based on density functional theory (DFT) and time-dependent DFT. The fourths are nonequilibrium Green functions that able to treat correlation effects in the material and at the interface. The price for the increased quality is a dramatic increase of computational effort and a restriction to short time and length scales. We conclude that, presently, none of the four methods is capable of providing a complete picture of the processes at the interface. Instead, each of them provides complementary information, and we discuss possible combinations.

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Plasma-catalysis: Is it just a question of scale?
J. Christopher Whitehead
Front. Chem. Sci. Eng.    2019, 13 (2): 264-273.   https://doi.org/10.1007/s11705-019-1794-3
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The issues of describing and understanding the changes in performance that result when a catalyst is placed into plasma are discussed. The different chemical and physical interactions that result and how their combination might produce beneficial results for the plasma-catalytic processing of different gas streams are outlined with particular emphasis being placed on the different range of spatial and temporal scales that must be considered both in experiment and modelling. The focus is on non-thermal plasma where the lack of thermal equilibrium creates a range of temperature scales that must be considered. This contributes in part to a wide range of inhomogeneity in different properties such as species concentrations and electric fields that must be determined experimentally by in situ methods and be incorporated into modelling. It is concluded that plasma-catalysis is best regarded as conventional catalysis perturbed by the presence of a discharge, which modifies its operating conditions, properties and outcomes often in a very localised way. The sometimes used description “plasma-activated catalysis” is an apt one.

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Review of plasma-assisted reactions and potential applications for modification of metal–organic frameworks
Tingting Zhao, Niamat Ullah, Yajun Hui, Zhenhua Li
Front. Chem. Sci. Eng.    2019, 13 (3): 444-457.   https://doi.org/10.1007/s11705-019-1811-6
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Plasma catalysis is drawing increasing attention worldwide. Plasma is a partially ionized gas comprising electrons, ions, molecules, radicals, and photons. Integration of catalysis and plasma can enhance catalytic activity and stability. Some thermodynamically unfavorable reactions can easily occur with plasma assistance. Compared to traditional thermal catalysis, plasma reactors can save energy because they can be operated at much lower temperatures or even room temperature. Additionally, the low bulk temperature of cold plasma makes it a good alternative for treatment of temperature-sensitive materials. In this review, we summarize the plasma-assisted reactions involved in dry reforming of methane, CO2 methanation, the methane coupling reaction, and volatile organic compound abatement. Applications of plasma for modification of metal–organic frameworks are discussed.

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Plasma-enabled healing of graphene nano-platelets layer
Xiuqi Fang, Carles Corbella, Denis B. Zolotukhin, Michael Keidar
Front. Chem. Sci. Eng.    2019, 13 (2): 350-359.   https://doi.org/10.1007/s11705-018-1787-7
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Graphene platelet networks (GPNs) were deposited onto silicon substrates by means of anodic arc discharge ignited between two graphite electrodes. Substrate temperature and pressure of helium atmosphere were optimized for the production of the carbon nanomaterials. The samples were modified or destroyed with different methods to mimic typical environments responsible of severe surface degradation. The emulated conditions were performed by four surface treatments, namely thermal oxidation, substrate overheating, exposition to glow discharge, and metal coating due to arc plasma. In the next step, the samples were regenerated on the same substrates with identical deposition technique. Damaging and re-growth of GPN samples were systematically characterized by scanning electron microscopy and Raman spectroscopy. The full regeneration of the structural and morphological properties of the samples has proven that this healing method by arc plasma is adequate for restoring the functionality of 2D nanostructures exposed to harsh environments.

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Cryptosporidium parvum oocyst directed assembly of gold nanoparticles and graphene oxide
Sona Jain, Zhicheng Huang, Brent R. Dixon, Syed Sattar, Juewen Liu
Front. Chem. Sci. Eng.    2019, 13 (3): 608-615.   https://doi.org/10.1007/s11705-019-1813-4
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Understanding the interactions between inorganic nanomaterials and biological species is an important topic for surface and environmental chemistry. In this work, we systematically studied the oocysts of Cryptosporidium parvum as a model protozoan parasite and its interaction with gold nanoparticles (AuNPs) and graphene oxide (GO). The as-prepared citrate-capped AuNPs adsorb strongly on the oocysts leading to a vivid color change. The adsorption of the AuNPs was confirmed by transmission electron microscopy. Heat treatment fully inhibited the color change, indicating a large change of surface chemistry of the oocysts that can be probed by the AuNPs. Adding proteases such as trypsin and proteinase K partially inhibited the color change. DNA-capped AuNPs, on the other hand, could not be adsorbed by the oocysts. GO was found to wrap around the oocysts forming a conformal shell reflecting the shape of the oocysts. Both citrate-capped AuNPs and GO compromised the membrane integrity of the oocysts as indicated by the propidium iodide staining experiment, and they may be potentially used for inactivating the oocysts. This is the first example of using nanomaterials to probe the surface of the oocysts, and it suggests the possibility of using such organisms to template the assembly of nanomaterials.

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A non-lithographic plasma nanoassembly technology for polymeric nanodot and silicon nanopillar fabrication
Athanasios Smyrnakis, Angelos Zeniou, Kamil Awsiuk, Vassilios Constantoudis, Evangelos Gogolides
Front. Chem. Sci. Eng.    2019, 13 (3): 475-484.   https://doi.org/10.1007/s11705-019-1809-0
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In this work, we present plasma etching alone as a directed assembly method to both create the nanodot pattern on an etched polymeric (PMMA) film and transfer it to a silicon substrate for the fabrication of silicon nanopillars or cone-like nanostructuring. By using a shield to control sputtering from inside the plasma reactor, the size and shape of the resulting nanodots can be better controlled by varying plasma parameters as the bias power. The effect of the shield on inhibitor deposition on the etched surfaces was investigated by time-of-flight secondary ion mass spectroscopy (ToF-SIMS) measurements. The fabrication of quasi-ordered PMMA nanodots of a diameter of 25 nm and period of 54 nm is demonstrated. Pattern transfer to the silicon substrate using the same plasma reactor was performed in two ways: (a) a mixed fluorine-fluorocarbon-oxygen nanoscale etch plasma process was employed to fabricate silicon nanopillars with a diameter of 25 nm and an aspect ratio of 5.6, which show the same periodicity as the nanodot pattern, and (b) high etch rate cryogenic plasma process was used for pattern transfer. The result is the nanostructuring of Si by high aspect ratio nanotip or nanocone-like features that show excellent antireflective properties.

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Multifunctional antimicrobial chlorhexidine polymers by remote plasma assisted vacuum deposition
Ana Mora-Boza, Francisco J. Aparicio, María Alcaire, Carmen López-Santos, Juan P. Espinós, Daniel Torres-Lagares, Ana Borrás, Angel Barranco
Front. Chem. Sci. Eng.    2019, 13 (2): 330-339.   https://doi.org/10.1007/s11705-019-1803-6
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Novel antibacterial materials for implants and medical instruments are essential to develop practical strategies to stop the spread of healthcare associated infections. This study presents the synthesis of multifunctional antibacterial nanocoatings on polydimethylsiloxane (PDMS) by remote plasma assisted deposition of sublimated chlorhexidine powders at low pressure and room temperature. The obtained materials present effective antibacterial activity against Escherichia coli K12, either by contact killing and antibacterial adhesion or by biocide agents release depending on the synthetic parameters. In addition, these multifunctional coatings allow the endure hydrophilization of the hydrophobic PDMS surface, thereby improving their biocompatibility. Importantly, cell-viability tests conducted on these materials also prove their non-cytotoxicity, opening a way for the integration of this type of functional plasma films in biomedical devices.

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Cube-octameric silsesquioxane (POSS)-capped magnetic iron oxide nanoparticles for the efficient removal of methylene blue
Ali Akbari, Nasser Arsalani, Bagher Eftekhari-Sis, Mojtaba Amini, Gholamreza Gohari, Esmaiel Jabbari
Front. Chem. Sci. Eng.    2019, 13 (3): 563-573.   https://doi.org/10.1007/s11705-018-1784-x
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Octavinyl polyhedral oligomeric silsesquioxane (POSS) was polymerized on the surface of Fe3O4 nanoparticles (NPs) and then the NPs were functionalized with carboxylic acid groups using thiol-ene click reactions with thioglycolic acid. The as-prepared Fe3O4@POSS-COOH magnetic hybrid NPs had mesoporous structures with an average particle diameter of 15 nm and a relatively high specific surface area of 447 m2∙g−1. Experimental results showed that 4 mg of Fe3O4@POSS-COOH NPs efficiently adsorbed and removed methylene blue from water at 5 min. This is due to the presence of both carboxylic acid and pendant vinyl groups on the Fe3O4@POSS-COOH NPs. These NPs could be easily withdrawn from water within a few seconds under moderate magnetic field and showed high stability in acid and alkaline aqueous mediums.

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Continuous flow removal of acid fuchsine by dielectric barrier discharge plasma water bed enhanced by activated carbon adsorption
Rusen Zhou, Renwu Zhou, Xianhui Zhang, Kateryna Bazaka, Kostya (Ken) Ostrikov
Front. Chem. Sci. Eng.    2019, 13 (2): 340-349.   https://doi.org/10.1007/s11705-019-1798-z
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Continuous processes which allow for large amount of wastewater to be treated to meet drainage standards while reducing treatment time and energy consumption are urgently needed. In this study, a dielectric barrier discharge plasma water bed system was designed and then coupled with granular activated carbon (GAC) adsorption to rapidly remove acid fuchsine (AF) with high efficiency. Effects of feeding gases, treatment time and initial concentration of AF on removal efficiency were investigated. Results showed that compared to the N2 and air plasmas treatments, O2 plasma processing was most effective for AF degradation due to the strong oxidation ability of generated activated species, especially the OH radicals. The addition of GAC significantly enhanced the removal efficiency of AF in aqueous solution and shorten the required time by 50%. The effect was attributed to the ability of porous carbon to trap and concentrate the dye, increasing the time dye molecules were exposed to the plasma discharge zone, and to enhance the production of OH radicals on/in GAC to boost the degradation of dyes by plasma as well as in situ regenerate the exhausted GAC. The study offers a new opportunity for continuous effective remediation of wastewater contaminated with organic dyes using plasma technologies.

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Phosphorene: Current status, challenges and opportunities
Anandarup Goswami, Manoj B. Gawande
Front. Chem. Sci. Eng.    2019, 13 (2): 296-309.   https://doi.org/10.1007/s11705-018-1783-y
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The field of 2-dimensional (2D) materials has witnessed a sharp growth since its inception and can majorly be attributed to the substantial technical and scientific developments, leading to significant improvements in their syntheses, characterization and applications. In the list of 2D materials, the relatively newer addition is phosphorene, which ideally consists of a single layer of black phosphorous. Keeping in mind the past, and ongoing research activities, this short account offers a brief overview of the present status and the associated challenges in the field of phosphorene-related research, with special emphasis on their syntheses, properties, applications and future opportunities.

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Mass transport mechanisms within pervaporation membranes
Yimeng Song, Fusheng Pan, Ying Li, Kaidong Quan, Zhongyi Jiang
Front. Chem. Sci. Eng.    2019, 13 (3): 458-474.   https://doi.org/10.1007/s11705-018-1780-1
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Pervaporation is an energy-efficient membrane technology for separating liquid molecules of similar physical properties, which may compete or combine with distillation separation technology in a number of applications. With the rapid development of new membrane materials, the pervaporation performance was significantly improved. Fundamental understanding of the mass transport mechanisms is crucial for the rational design of membrane materials and efficient intensification of pervaporation process. Based on the interactions between permeate molecules and membranes, this review focuses on two categories of mass transport mechanisms within pervaporation membranes: physical mechanism (solution-diffusion mechanism, molecular sieving mechanism) and chemical mechanism (facilitated transport mechanism). Furthermore, the optimal integration and evolution of different mass transport mechanisms are briefly introduced. Material selection and relevant applications are highlighted under the guidance of mass transport mechanisms. Finally, the current challenges and future perspectives are tentatively identified.

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Low-k integration: Gas screening for cryogenic etching and plasma damage mitigation
Romain Chanson, Remi Dussart, Thomas Tillocher, P. Lefaucheux, Christian Dussarrat, Jean François de Marneffe
Front. Chem. Sci. Eng.    2019, 13 (3): 511-516.   https://doi.org/10.1007/s11705-019-1820-5
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The integration of porous organo-silicate low-k materials has met a lot of technical challenges. One of the main issues is plasma-induced damage, occurring for all plasma steps involved during interconnects processing. In the present paper, we focus on porous SiOCH low-k damage mitigation using cryogenic temperature so as to enable micro-capillary condensation. The aim is to protect the porous low-k from plasma-induced damage and keep the k-value of the material unchanged, in order to limit the RC delay of interconnexion levels while shrinking the microchip dimension. The cryogenic temperature is used to condense a gas inside the porous low-k material. Then, the etching process is performed at the temperature of condensation in order to keep the condensate trapped inside the material during the etching. In the first part of this work, the condensation properties of several gases are screened, leading to a down selection of five gases. Then, their stability into the porous structure is evaluated at different temperature. Four of them are used for plasma damage mitigation comparison. Damage mitigation is effective and shows negligible damage for one of the gases at –50°C.

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Important parameters in plasma jets for the production of RONS in liquids for plasma medicine: A brief review
Anna Khlyustova, Cédric Labay, Zdenko Machala, Maria-Pau Ginebra, Cristina Canal
Front. Chem. Sci. Eng.    2019, 13 (2): 238-252.   https://doi.org/10.1007/s11705-019-1801-8
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Reactive oxygen and nitrogen species (RONS) are among the key factors in plasma medicine. They are generated by atmospheric plasmas in biological fluids, living tissues and in a variety of liquids. This ability of plasmas to create a delicate mix of RONS in liquids has been used to design remote or indirect treatments for oncological therapy by treating biological fluids by plasmas and putting them in contact with the tumour. Documented effects include selective cancer cell toxicity, even though the exact mechanisms involved are still under investigation. However, the “right” dose for suitable therapeutical activity is crucial and still under debate. The wide variety of plasma sources hampers comparisons. This review focuses on atmospheric pressure plasma jets as the most studied plasma devices in plasma medicine and compiles the conditions employed to generate RONS in relevant liquids and the concentration ranges obtained. The concentrations of H2O2, NO2, NO3 and short-lived oxygen species are compared critically to provide a useful overview for the reader.

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Magnetic-porous microspheres with synergistic catalytic activity of small-sized gold nanoparticles and titania matrix
Kadriye Özlem Hamaloğlu, Ebru Sağ, Çiğdem Kip, Erhan Şenlik, Berna Saraçoğlu Kaya, Ali Tuncel
Front. Chem. Sci. Eng.    2019, 13 (3): 574-585.   https://doi.org/10.1007/s11705-019-1799-y
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Fe3O4 nanoparticles immobilized on porous titania in micron-size range were decorated with small-sized gold nanoparticles and used as a plasmonic catalyst for the reduction of 4-nitrophenol. Monodisperse-porous magnetic titania microspheres were synthesized with bimodal pore-size distribution by the sol-gel templating method. Small-sized gold nanoparticles obtained by the Martin method were attached onto the aminated form of the magnetic titania microspheres. A significant enhancement in the catalytic activity was observed using the gold nanoparticle-decorated magnetic titania microspheres compared to gold nanoparticle-decorated magnetic silica microspheres because of the synergistic effect between small-sized gold nanoparticles and titania. The synergistic effect for gold nanoparticle-attached magnetic titania microspheres could be explained by surface plasmon resonance-induced transfer of hot electrons from gold nanoparticles to the conduction band of titania. Using the proposed catalyst, 4-nitrophenol could be converted to 4-aminophenol in an aqueous solution within 0.5 min. The 4-nitrophenol reduction rates were 2.5–79.3 times higher than those obtained with similar plasmonic catalysts. The selection of micron-size, magnetic, and porous titania microspheres as a support material for the immobilization of small-sized gold nanoparticles provided a recoverable plasmonic catalyst with high reduction ability.

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Improvement in growth yield of single-walled carbon nanotubes with narrow chirality distribution by pulse plasma CVD
Bin Xu, Toshiro Kaneko, Toshiaki Kato
Front. Chem. Sci. Eng.    2019, 13 (3): 485-492.   https://doi.org/10.1007/s11705-019-1831-2
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A pulse plasma chemical vapor deposition (CVD) technique was developed for improving the growth yield of single-walled carbon nanotubes (SWNTs) with a narrow chirality distribution. The growth yield of the SWNTs could be improved by repetitive short duration pulse plasma CVD, while maintaining the initial narrow chirality distribution. Detailed growth dynamics is discussed based on a systematic investigation by changing the pulse parameters. The growth of SWNTs with a narrow chirality distribution could be controlled by the difference in the nucleation time required using catalysts comprising relatively small or large particles as the key factor. The nucleation can be controlled by adjusting the pulse on/off time ratio and the total processing time.

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