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Polyolefin-nanocomposites with special properties by in-situ polymerization

Walter Kaminsky

《化学科学与工程前沿（英文）》 2018年 第12卷 第3期   页码 555-563 doi: 10.1007/s11705-018-1715-x

摘要：

Exceptionally strong polyolefin nanocomposites are synthesized by in-situ polymerization using soluble metallocene/methylaluminoxane (MAO) as catalysts in a two-step process. First, the soluble metallocene/MAO or other single site catalysts are absorbed on the surface of the nanofillers. Then by addition of ethene or propene, a polyolefin film is formed, covering the nanoparticles, layered silicates, or fibers. The resulting polyethylene and polypropylene nanocomposites are characterized by better physical and chemical properties such as stiffness, gas barrier properties, degradation temperatures, and crystallization rates. They show better mechanical properties than materials produced by mechanical blending. The thickness of the polyolefin can be controlled by the pressure of ethene or propene and by the polymerization time. Carbon fibers and carbon nanotubes are covered with isotactic or syndiotactic polypropylene. Because of the hydrophobic character of the carbon surface, the polymer is drawn on the fiber. This leads to a reinforced combined polymer with special properties. The crystallization temperature is 10 °C higher and therefore the crystallization rate up to 20 times faster than that of pure syndiotactic polypropylene. The form stability increases by 100% if 3 wt-% of carbon nanotubes are incorporated.

关键词： polyolefin nanocomposites     metallocenes     methylaluminoxane    

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Development of an H reduction and moderate oxidation method for 3,5-dimethylpyridine hydrogenation in trickle bed reactor

《化学科学与工程前沿（英文）》 2022年 第16卷 第12期   页码 1807-1817 doi: 10.1007/s11705-022-2243-2

摘要： The Ru/C catalyst prepared by impregnation method was used for hydrogenation of 3,5-dimethylpyridine in a trickle bed reactor. Under the same reduction conditions (300 °C in H2), the catalytic activity of the non-in-situ reduced Ru/C-n catalyst was higher than that of the in-situ reduced Ru/C-y catalyst. Therefore, an in-situ H2 reduction and moderate oxidation method was developed to increase the catalyst activity. Moreover, the influence of oxidation temperature on the developed method was investigated. The catalysts were characterized by Brunauer–Emmett–Teller method, hydrogen temperature programmed reduction H2-TPR, hydrogen temperature-programmed dispersion (H2-TPD), X-ray diffraction, energy dispersive spectroscopy, X-ray photoelectron spectroscopy, Raman spectroscopy, O2 chemisorption and oxygen temperature-programmed dispersion (O2-TPD) analyses. The results showed that there existed an optimal Ru/RuOx ratio for the catalyst, and the highest 3,5-dimethylpyridine conversion was obtained for the Ru/C-i1 catalyst prepared by in-situ H2 reduction and moderate oxidation (oxidized at 100 °C). Excessive oxidation (200 °C) resulted in a significant decrease in the Ru/RuOx ratio of the in-situ H2 reduction and moderate oxidized Ru/C-i2 catalyst, the interaction between RuOx species and the support changed, and the hard-to-reduce RuOx species was formed, leading to a significant decrease in catalyst activity. The developed in-situ H2 reduction and moderate oxidation method eliminated the step of the non-in-situ reduction of catalyst outside the trickle bed reactor.

关键词： Ru/C catalyst     in-situ H2 reduction and moderate oxidation     in-situ reduction     non-in-situ reduction     hydrogenation of 3     5-dimethylpyridine    

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In-situ condition monitoring of reinforced concrete structures

Sanjeev Kumar VERMA,Sudhir Singh BHADAURIA,Saleem AKHTAR

《结构与土木工程前沿（英文）》 2016年 第10卷 第4期   页码 420-437 doi: 10.1007/s11709-016-0336-z

摘要： Performance of concrete structures is significantly influenced and governed by its durability and resistance to environmental or exposure conditions, apart from its physical strength. It can be monitored, evaluated and predicted through modeling of physical deterioration mechanisms, performance characteristics and parameters and condition monitoring of in situ concrete structures. One such study has been conducted using Non-destructive testing equipment in the city of Bhopal and around located in India. Some selected parameters influencing durability of reinforced concrete (RC) structures such as concrete cover, carbonation depth, chloride concentration, half cell potential and compressive strength have been measured, for establishing correlation among various parameters and age of structures. Effects of concrete cover and compressive strength over the variation of chloride content with time are also investigated.

关键词： concrete     carbonation     chloride     corrosion     monitoring     models    

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Development and application of ex-situ presulfurization technology for hydrotreating catalysts in China

Yulan GAO, Xiangchen FANG, Zhenmin CHENG

《化学科学与工程前沿（英文）》 2011年 第5卷 第3期   页码 287-296 doi: 10.1007/s11705-010-0529-2

摘要： The development and application of ex-situ presulfurization (EPRES) technology for hydrotreating catalysts has been reviewed in the present article. The studies in laboratory scale and commercial practice indicated that the adoption of the EPRES catalyst in industrial application can significantly enhance the degree of presulfurization of metal oxide components, shorten the start-up period, and effectively reduce the environmental impact as well as the danger of start-up procedure in industrial hydrotreating unit. This catalyst has been proved to be versatile for different types of hydrogenation reactions. Different types of active site models are also discussed for better understanding the nature of presulfurized catalysts.

关键词： ex-situ presulfurization     in situ presulfurization     hydrotreating catalyst     sulfur utilization ratio    

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Organics Recovery from Waste Activated Sludge In-situ Driving Efficient Nitrogen Removal from Mature

Fangzhai Zhang,Shang Ren,Haoran Liang,Zhaozhi Wang,Ying Yan,Jiahui Wang,Yongzhen Peng,

《工程（英文）》 doi: 10.1016/j.eng.2023.03.005

摘要： The sustainable recovery and utilization of sludge bioenergy within a circular economy context has drawn increasing attention, but there is currently a shortage of reliable technology. This study presents an innovative biotechnology based on free nitrous acid (FNA) to realize sustainable organics recovery from waste activated sludge (WAS) in-situ, driving efficient nitrogen removal from ammonia rich mature landfill leachate by integrating partial nitrification, fermentation, and denitrification process (PN/DN–F/DN). First, ammonia ((1708.5 ± 142.9) mg·L−1) in mature landfill leachate is oxidized to nitrite in the aerobic stage of a partial nitrification coupling denitrification sequencing batch reactor (PN/DN-SBR), with nitrite accumulation ratio of 95.4% ± 2.5%. Then, intermediate effluent (NO2−–N = (1196.9 ± 184.2) mg·L−1) of the PN/DN-SBR, along with concentrated WAS (volatile solids (VSs) = (15119.8 ± 2484.2) mg·L−1), is fed into an anoxic reactor for fermentation coupling denitrification process (F/DN-SBR). FNA, the protonated form of nitrite, degrades organics in the WAS to the soluble fraction by the biocidal effect, and the released organics are utilized by denitrifiers to drive NOx− reduction. An ultra-fast sludge reduction rate of 4.89 kg·m−3·d−1 and nitrogen removal rate of 0.46 kg·m−3·d−1 were realized in the process. Finally, F/DN-SBR effluent containing organics is refluxed to PN/DN-SBR for secondary denitrification in the post anoxic stage. After 175 d operation, an average of 19350.6 mg chemical oxygen demand organics were recovered per operational cycle, with 95.2% nitrogen removal and 53.4% sludge reduction. PN/DN–F/DN is of great significance for promoting a paradigm transformation from energy consumption to energy neutral, specifically, the total benefit in equivalent terms of energy was 291.8 kW·h·t−1 total solid.

关键词： Waste activated sludge     Bioresource recovery     Simultaneous treatment of wastewater and sludge     Mature landfill leachate     Free nitrous acid    

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Development of lunar regolith-based composite for - 3D printing via high-pressure extrusion system

《机械工程前沿（英文）》 2023年 第18卷 第2期 doi: 10.1007/s11465-022-0745-8

摘要： To fully utilize the in-situ resources on the moon to facilitate the establishment of a lunar habitat is significant to realize the long-term residence of mankind on the moon and the deep space exploration in the future. Thus, intensive research works have been conducted to develop types of 3D printing approach to adapt to the extreme environment and utilize the lunar regolith for in-situ construction. However, the in-situ 3D printing using raw lunar regolith consumes extremely high energy and time. In this work, we proposed a cost-effective melting extrusion system for lunar regolith-based composite printing, and engineering thermoplastic powders are employed as a bonding agent for lunar regolith composite. The high-performance nylon and lunar regolith are uniformly pre-mixed in powder form with different weight fractions. The high-pressure extrusion system is helpful to enhance the interface affinity of polymer binders with lunar regolith as well as maximize the loading ratio of in-situ resources of lunar regolith. Mechanical properties such as tensile strength, elastic modulus, and Poisson’s ratio of the printed specimens were evaluated systematically. Especially, the impact performance was emphasized to improve the resistance of the meteorite impact on the moon. The maximum tensile strength and impact toughness reach 36.2 MPa and 5.15 kJ/m2, respectively. High-pressure melt extrusion for lunar regolith composite can increase the effective loading fraction up to 80 wt.% and relatively easily adapt to extreme conditions for in-situ manufacturing.

关键词： in-situ resource utilization     melt extrusion molding     lunar regolith-based composites     mechanical properties     additive manufacturing    

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Thermodynamic analysis of liquid phase in situ hydrogenation of glycerol for 1,3-propanediol synthesis

Kun OUYANG, Yu HUANG, Haoyi CHEN, Tao LI, Fahai CAO, Dingye FANG

《化学科学与工程前沿（英文）》 2011年 第5卷 第1期   页码 67-73 doi: 10.1007/s11705-010-0541-6

摘要： Based on the combination of the glycerol aqueous-phase reforming (APR) and catalytic hydrogenation of glycerol, a novel reaction system of liquid phase in situ hydrogenation of glycerol for the synthesis of 1,3-propanediol is proposed, in which hydrogen is produced from glycerol aqueous-phase reforming in the same reactor. In this new system, the glycerol is the raw material of the aqueous-phase reforming reaction; the hydrogen generated from the APR of glycerol can be quickly transformed to the in situ hydrogenation of glycerol to produce 1,3-propanediol, which can improve the selectivity of hydrogen for the APR process of glycerol. Moreover, thermodynamic calculation of the coupling processes was carried out, and standard molar enthalpies and equilibrium constants of foregoing reactions were obtained. The above calculation results indicate that the combination process is feasible for 1,3-propanediol synthesis.

关键词： glycerol     aqueous-phase reforming     1     3-propanediol     in-situ reduction    

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density measurement for plastic injection molding via ultrasonic technology

《机械工程前沿（英文）》 2022年 第17卷 第4期 doi: 10.1007/s11465-022-0714-2

摘要： Density variation during the injection molding process directly reflects the state of plastic melt and contains valuable information for process monitoring and optimization. Therefore, in-situ density measurement is of great interest and has significant application value. The existing methods, such as pressure−volume−temperature (PVT) method, have the shortages of time-delay and high cost of sensors. This study is the first to propose an in-situ density measurement method using ultrasonic technology. The analyses of the time-domain and frequency-domain signals are combined in the proposed method. The ultrasonic velocity is obtained from the time-domain signals, and the acoustic impedance is computed through a full-spectral analysis of the frequency-domain signals. Experiments with different process conditions are conducted, including different melt temperature, injection speed, material, and mold structure. Results show that the proposed method has good agreement with the PVT method. The proposed method has the advantages of in-situ measurement, non-destructive, high accuracy, low cost, and is of great application value for the injection molding industry.

关键词： ultrasonic measurement     melt density     in-situ measurement     injection molding    

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A novel six-legged walking machine tool for

Jimu LIU, Yuan TIAN, Feng GAO

《机械工程前沿（英文）》 2020年 第15卷 第3期   页码 351-364 doi: 10.1007/s11465-020-0594-2

摘要： The manufacture and maintenance of large parts in ships, trains, aircrafts, and so on create an increasing demand for mobile machine tools to perform operations. However, few mobile robots can accommodate the complex environment of industrial plants while performing machining tasks. This study proposes a novel six-legged walking machine tool consisting of a legged mobile robot and a portable parallel kinematic machine tool. The kinematic model of the entire system is presented, and the workspace of different components, including a leg, the body, and the head, is analyzed. A hierarchical motion planning scheme is proposed to take advantage of the large workspace of the legged mobile platform and the high precision of the parallel machine tool. The repeatability of the head motion, body motion, and walking distance is evaluated through experiments, which is 0.11, 1.0, and 3.4 mm, respectively. Finally, an application scenario is shown in which the walking machine tool steps successfully over a 250 mm-high obstacle and drills a hole in an aluminum plate. The experiments prove the rationality of the hierarchical motion planning scheme and demonstrate the extensive potential of the walking machine tool for operations on large parts.

关键词： legged robot     parallel mechanism     mobile machine tool     in-situ machining    

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Comprehensive kinetostatic modeling and morphology characterization of cable-driven continuum robots for aero-engine maintenance

《机械工程前沿（英文）》 2023年 第18卷 第3期 doi: 10.1007/s11465-023-0756-0

摘要： In-situ maintenance is of great significance for improving the efficiency and ensuring the safety of aero-engines. The cable-driven continuum robot (CDCR) with twin-pivot compliant mechanisms, which is enabled with flexible deformation capability and confined space accessibility, has emerged as a novel tool that aims to promote the development of intelligence and efficiency for in-situ aero-engine maintenance. The high-fidelity model that describes the kinematic and morphology of CDCR lays the foundation for the accurate operation and control for in-situ maintenance. However, this model was not well addressed in previous literature. In this study, a general kinetostatic modeling and morphology characterization methodology that comprehensively contains the effects of cable-hole friction, gravity, and payloads is proposed for the CDCR with twin-pivot compliant mechanisms. First, a novel cable-hole friction model with the variable friction coefficient and adaptive friction direction criterion is proposed through structure optimization and kinematic parameter analysis. Second, the cable-hole friction, all-component gravities, deflection-induced center-of-gravity shift of compliant joints, and payloads are all considered to deduce a comprehensive kinetostatic model enabled with the capacity of accurate morphology characterization for CDCR. Finally, a compact continuum robot system is integrated to experimentally validate the proposed kinetostatic model and the concept of in-situ aero-engine maintenance. Results indicate that the proposed model precisely predicts the morphology of CDCR and outperforms conventional models. The compact continuum robot system could be considered a novel solution to perform in-situ maintenance tasks of aero-engines in an invasive manner.

关键词： kinetostatic modeling     morphology characterization     variable friction     continuum robots     in-situ maintenance    

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grown TiN/N-TiO composite for enhanced photocatalytic H evolution activity

《能源前沿（英文）》 2021年 第15卷 第3期   页码 721-731 doi: 10.1007/s11708-021-0766-8

摘要： Titanium nitride (TiN) decorated N-doped titania (N-TiO2) composite (TiN/N-TiO2) is fabricated via an in situ nitridation using a hydrothermally synthesized TiO2 and melamine (MA) as raw materials. After the optimization of the reaction condition, the resultant TiN/N-TiO2 composite delivers a hydrogen evolution activity of up to 703 μmol/h under the full spectrum irradiation of Xe-lamp, which is approximately 2.6 and 32.0 times more than that of TiO2 and TiN alone, respectively. To explore the underlying photocatalytic mechanism, the crystal phase, morphology, light absorption, energy band structure, element composition, and electrochemical behavior of the composite material are characterized and analyzed. The results indicate that the superior activity is mainly caused by the in situ formation of plasmonic TiN and N-TiO2 with intimate interface contact, which not only extends the spectral response range, but also accelerates the transfer and separation of the photoexcited hot charge carrier of TiN. The present study provides a fascinating approach to in situ forming nonmetallic plasmonic material/N-doped TiO2 composite photocatalysts for high-efficiency water splitting.

关键词： photocatalytic H2 evolution     TiN/N-TiO2 composite     plasmonic effect     in-situ nitridation    

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Carbon-coated Ni-Co alloy catalysts: preparation and performance for aqueous phase hydrodeoxygenation of methyl palmitate to hydrocarbons using methanol as the hydrogen donor

《化学科学与工程前沿（英文）》 2022年 第16卷 第3期   页码 443-460 doi: 10.1007/s11705-021-2079-1

摘要： Carbon-coated Ni, Co and Ni-Co alloy catalysts were prepared by the carbonization of the metal doped resorcinol-formaldehyde resins synthesized by the one-pot extended Stöber method. It was found that the introduction of Co remarkably reduced the carbon microsphere size. The metallic Ni, Co, and Ni-Co alloy particles (mainly 10–12 nm) were uniformly distributed in carbon microspheres. A charge transfer from Ni to Co appeared in the Ni-Co alloy. Compared with those of metallic Ni and Co, the d-band center of the Ni-Co alloy shifted away from and toward the Fermi level, respectively. In the in-situ aqueous phase hydrodeoxygenation of methyl palmitate with methanol as the hydrogen donor at 330 °C, the decarbonylation/decarboxylation pathway dominated on all catalysts. The Ni-Co@C catalysts gave higher activity than the Ni@C and Co@C catalysts, and the yields of n-pentadecane and n-C6–n-C16 reached 71.6% and 92.6%, respectively. The excellent performance of Ni-Co@C is attributed to the electronic interactions between Ni and Co and the small carbon microspheres. Due to the confinement effect of carbon, the metal particles showed high resistance to sintering under harsh hydrothermal conditions. Catalyst deactivation is due to the carbonaceous deposition, and the regeneration with CO2 recovered the catalyst reactivity.

关键词： Stöber method     carbon-coated Ni-Co alloy     in-situ hydrodeoxygenation     methyl palmitate     decarbonylation/decarboxylation    

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Room temperature preparation of hydrazine-linked covalent organic frameworks coated capillaries for separation and determination of polycyclic aromatic hydrocarbons

《化学科学与工程前沿（英文）》 2023年 第17卷 第5期   页码 548-556 doi: 10.1007/s11705-022-2252-1

摘要： Covalent organic frameworks (COFs) have been increasingly used in capillary electrochromatography due to their excellent characteristics. In this work, hydrazine-linked TFPB-DHzDS (TFPB: 1,3,5-tris(4-formylphenyl)benzene; DHzDS: 2,5-bis(3-(ethylthio)propoxy)terephthalohydrazide) was first synthesized by a simpler and easier method at room temperature and introduced into capillary electrochromatography as coating material. The TFPB-DHzDS coated capillaries were prepared by an in-situ growth process at room temperature. After optimizing the coating concentration and experimental conditions of capillary electrochromatography, baseline separation of two groups of polycyclic aromatic hydrocarbons was achieved based on the TFPB-DHzDS coated capillary. And the established method was used successfully to determine PAHs in natural water and soil samples. The spiked recoveries of polycyclic aromatic hydrocarbons in these samples ranged from 90.01% to 111.0%, indicating that the method is reliable and could detect polycyclic aromatic hydrocarbons in natural samples. Finally, molecular simulation was applied to study and visualize the interaction between the analytes and coating COF materials to investigate the molecular level separation mechanism further.

关键词： hydrazine-linked TFPB-DHzDS     in-situ growth method     open-tubular capillary electrochromatography     molecular simulations    

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Efficient hydrothermal deoxygenation of methyl palmitate to diesel-like hydrocarbons on carbon encapsulated Ni–Sn intermetallic compounds with methanol as hydrogen donor

《化学科学与工程前沿（英文）》 2023年 第17卷 第2期   页码 139-155 doi: 10.1007/s11705-022-2217-4

摘要： Porous carbon-encapsulated Ni and Ni–Sn intermetallic compound catalysts were prepared by the one-pot extended Stöber method followed by carbonization and tested for in-situ hydrothermal deoxygenation of methyl palmitate with methanol as the hydrogen donor. During the catalyst preparation, Sn doping reduces the size of carbon spheres, and the formation of Ni–Sn intermetallic compounds restrain the graphitization, contributing to larger pore volume and pore diameter. Consequently, a more facile mass transfer occurs in carbon-encapsulated Ni–Sn intermetallic compound catalysts than in carbon-encapsulated Ni catalysts. During the in-situ hydrothermal deoxygenation, the synergism between Ni and Sn favors palmitic acid hydrogenation to a highly reactive hexadecanal that easily either decarbonylate to n-pentadecane or is hydrogenated to hexadecanol. At high reaction temperature, hexadecanol undergoes dehydrogenation–decarbonylation, generating n-pentadecane. Also, the C–C bond hydrolysis and methanation are suppressed on Ni–Sn intermetallic compounds, favorable for increasing the carbon yield and reducing the H2 consumption. The n-pentadecane and n-hexadecane yields reached 88.1% and 92.8% on carbon-encapsulated Ni3Sn2 intermetallic compound at 330 °C. After washing and H2 reduction, the carbon-encapsulated Ni3Sn2 intermetallic compound remains stable during three recycling cycles. This is ascribed to the carbon confinement that effectively suppresses the sintering and loss of metal particles under harsh hydrothermal conditions.

关键词： extended Stöber method     carbon encapsulated Ni–Sn intermetallic compounds     confinement     in-situ hydrothermal deoxygenation     hydrogenation     decarbonylation    

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Spin polarization strategy to deploy proton resource over atomic-level metal sites for highly selective

《化学科学与工程前沿（英文）》 2022年 第16卷 第12期   页码 1772-1781 doi: 10.1007/s11705-022-2197-4

摘要： Unlocking of the extremely inert C=O bond during electrochemical CO2 reduction demands subtle regulation on a key “resource”, protons, necessary for intermediate conversion but also readily trapped in water splitting, which is still challenging for developing efficient single-atom catalysts limited by their structural simplicity usually incompetent to handle this task. Incorporation of extra functional units should be viable. Herein, a proton deployment strategy is demonstrated via “atomic and nanostructured iron (A/N-Fe) pairs”, comprising atomically dispersed iron active centers spin-polarized by nanostructured iron carbide ferromagnets, to boost the critical protonation steps. The as-designed catalyst displays a broad window (300 mV) for CO selectivity > 90% (98% maximum), even outperforming numerous cutting-edge M–N–C systems. The well-placed control of proton dynamics by A/N-Fe can promote *COOH/*CO formation and simultaneously suppress H2 evolution, benefiting from the magnetic-proximity-induced exchange splitting (spin polarization) that properly adjusts energy levels of the Fe sites’ d-shells, and further those of the adsorbed intermediates’ antibonding molecular orbitals.

关键词： CO2 electrolysis     single-atom catalysts     spin polarization     proton dynamics     in situ IR spectroscopy     kinetic isotope effect    

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标题 作者 时间 类型 操作

Polyolefin-nanocomposites with special properties by in-situ polymerization

Walter Kaminsky

期刊论文

Development of an H reduction and moderate oxidation method for 3,5-dimethylpyridine hydrogenation in trickle bed reactor

期刊论文

In-situ condition monitoring of reinforced concrete structures

Sanjeev Kumar VERMA,Sudhir Singh BHADAURIA,Saleem AKHTAR

期刊论文

Development and application of ex-situ presulfurization technology for hydrotreating catalysts in China

Yulan GAO, Xiangchen FANG, Zhenmin CHENG

期刊论文

Organics Recovery from Waste Activated Sludge In-situ Driving Efficient Nitrogen Removal from Mature

Fangzhai Zhang,Shang Ren,Haoran Liang,Zhaozhi Wang,Ying Yan,Jiahui Wang,Yongzhen Peng,

期刊论文

Development of lunar regolith-based composite for - 3D printing via high-pressure extrusion system

期刊论文

Thermodynamic analysis of liquid phase in situ hydrogenation of glycerol for 1,3-propanediol synthesis

Kun OUYANG, Yu HUANG, Haoyi CHEN, Tao LI, Fahai CAO, Dingye FANG

期刊论文

density measurement for plastic injection molding via ultrasonic technology

期刊论文

A novel six-legged walking machine tool for

Jimu LIU, Yuan TIAN, Feng GAO

期刊论文

Comprehensive kinetostatic modeling and morphology characterization of cable-driven continuum robots for aero-engine maintenance

期刊论文

grown TiN/N-TiO composite for enhanced photocatalytic H evolution activity

期刊论文

Carbon-coated Ni-Co alloy catalysts: preparation and performance for aqueous phase hydrodeoxygenation of methyl palmitate to hydrocarbons using methanol as the hydrogen donor

期刊论文

Room temperature preparation of hydrazine-linked covalent organic frameworks coated capillaries for separation and determination of polycyclic aromatic hydrocarbons

期刊论文

Efficient hydrothermal deoxygenation of methyl palmitate to diesel-like hydrocarbons on carbon encapsulated Ni–Sn intermetallic compounds with methanol as hydrogen donor

期刊论文

Spin polarization strategy to deploy proton resource over atomic-level metal sites for highly selective

期刊论文