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Carbon-doped surface unsaturated sulfur enriched CoS@rGO aerogel pseudocapacitive anode and biomass-derivedporous carbon cathode for advanced lithium-ion capacitors

《化学科学与工程前沿（英文）》 2021年 第15卷 第6期   页码 1500-1513 doi: 10.1007/s11705-021-2086-2

摘要： As a hybrid energy storage device of lithium-ion batteries and supercapacitors, lithium-ion capacitors have the potential to meet the demanding needs of energy storage equipment with both high power and energy density. In this work, to solve the obstacle to the application of lithium-ion capacitors, that is, the balancing problem of the electrodes kinetic and capacity, two electrodes are designed and adequately matched. For the anode, we introduced in situ carbon-doped and surface-enriched unsaturated sulfur into the graphene conductive network to prepare transition metal sulfides, which enhances the performance with a faster lithium-ion diffusion and dominant pseudocapacitive energy storage. Therefore, the lithium-ion capacitors anode material delivers a remarkable capacity of 810 mAh∙g–1 after 500 cycles at 1 A∙g–1. On the other hand, the biomass-derived porous carbon as the cathode also displays a superior capacity of 114.2 mAh∙g–1 at 0.1 A∙g–1. Benefitting from the appropriate balance of kinetic and capacity between two electrodes, the lithium-ion capacitors exhibits superior electrochemical performance. The assembled lithium-ion capacitors demonstrate a high energy density of 132.9 Wh∙kg–1 at the power density of 265 W∙kg–1, and 50.0 Wh∙kg–1 even at 26.5 kW∙kg–1. After 10000 cycles at 1 A∙g–1, lithium-ion capacitors still demonstrate the high energy density retention of 81.5%.

关键词： in-situ carbon-doped     surface unsaturated sulfur enriched     pseudocapacitive energy storage     biomass-derived carbon     lithium-ion capacitors    

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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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Carbon-coated Ni-Co alloy catalysts: preparation and performance for aqueous phase hydrodeoxygenation

《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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Efficient hydrothermal deoxygenation of methyl palmitate to diesel-like hydrocarbons on carbon encapsulated

《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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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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Concurrent adsorption and reduction of chromium(VI) to chromium(III) using nitrogen-doped porous carbon

《环境科学与工程前沿（英文）》 2022年 第16卷 第5期 doi: 10.1007/s11783-021-1491-6

摘要：

• A high-efficiency N-doped porous carbon adsorbent for Cr(VI) was synthesized.

关键词： Chromium(VI)     Nitrogen-doped porous carbon     Adsorption     Reduction     Loofah sponge    

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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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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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Phosphorus-doped Ni–Co sulfides connected by carbon nanotubes for flexible hybrid supercapacitor

《化学科学与工程前沿（英文）》 2023年 第17卷 第5期   页码 491-503 doi: 10.1007/s11705-022-2257-9

摘要： As promising electrode materials for supercapacitors, nickel-cobalt bimetallic sulfides render the advantages of abundant redox reactions and inherently high conductivity. However, in general, unsatisfactory performance of low specific capacity, low rate capability, and fast capacity loss exist in Ni–Co sulfide electrodes. Herein, we rationally regulate phosphorus-doped nickel–cobalt sulfides (P-NCS) to enhance the electrochemical performance by gas–solid phosphorization. Moreover, carbon nanotubes (CNTs) as conductive additives are added to improve the cycle stability and conductivity and form the composite P-NCS/C/CNT. According to density functional theory, more electrons near the Fermi surface of P-NCS are demonstrated notionally than those of simple CoNi2S4. Electrochemical results manifest that P-NCS/C/CNT exhibits superior electrochemical performance, e.g., high specific capacity (932.0 C∙g‒1 at 1 A∙g‒1), remarkable rate capability (capacity retention ratio of 69.1% at 20 A∙g‒1), and lower charge transfer resistance. More importantly, the flexible hybrid asymmetric supercapacitor is assembled using P-NCS/C/CNT and activated carbon, which renders an energy density of 34.875 W·h∙kg‒1 at a power density of 375 W∙kg‒1. These results show that as-prepared P-NCS/C/CNT demonstrates incredible possibility as a battery-type electrode for high-performance supercapacitors.

关键词： cobalt nickel sulfide     phosphorus-doping     hybrid supercapacitor     carbon nanotube     density functional theory    

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Size-controllable synthesis of monodispersed nitrogen-doped carbon nanospheres from polydopamine for

《化学科学与工程前沿（英文）》 2023年 第17卷 第11期   页码 1788-1800 doi: 10.1007/s11705-023-2326-8

摘要： Monodispersed nitrogen-doped carbon nanospheres with tunable particle size (100–230 nm) were synthesized via self-polymerization of biochemical dopamine in the presence of hexamethylenetetramine as a buffer and F127 as a size controlling agent. Hexamethylenetetramine can mildly release NH3, which in turn initiates the polymerization reaction of dopamine. The carbon nanospheres obtained exhibited a significant energy storage capability of 265 F·g–1 at 0.5 A·g–1 and high-rate performance of 82% in 6 mol·L–1 KOH (20 A·g–1), which could be attributed to the presence of abundant micro-mesoporous structure, doped nitrogen functional groups and the small particle size. Moreover, the fabricated symmetric supercapacitor device displayed a high stability of 94% after 5000 cycles, revealing the considerable potential of carbon nanospheres as electrode materials for energy storage.

关键词： carbon nanospheres     size-controlled     nitrogen-doped     high-rate     supercapacitors    

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Sulfur and carbon co-doped g-CN microtubes with enhanced photocatalytic H production activity

《能源前沿（英文）》 doi: 10.1007/s11708-023-0899-z

摘要： Metal-free graphitic carbon nitride (g-C3N4) has captured significant attention as a low-cost and efficient hydrogen production photocatalyst through. Effectively regulating the microstructure and accelerating the separation of photogenerated carriers remain crucial strategies for promoting the photocatalytic performance of this material. Herein, a novel sulfur–carbon co-doped g-C3N4 (SCCN) hierarchical microtubules filled with abundant nanosheets inside by thermal polymerization is reported. Numerous nanosheets create abundant pores and cavities inside the SCCN microtubes, thereby increasing the specific surface area of g-C3N4 and providing sufficient reactant attachment sites. Besides, the hierarchical structure of SCCN microtubules strengthens the reflection and scattering of light, and the utilization of visible light is favorably affected. More importantly, co-doping S and C has greatly improved the photocatalytic performance of graphitic carbon nitride, optimized the band gap structure and enhanced the photogenerated carrier splitting. Consequently, the SCCN exhibits a remarkable photocatalytic H2 evolution rate of 4868 μmol/(g·h). This work demonstrates the potential of multi-nonmetal doped g-C3N4 as the ideal photocatalyst for H2 evolution.

关键词： carbon nitride     photocatalysis     hydrogen production    

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Fabrication of N-doped carbon nanobelts from a polypyrrole tube by confined pyrolysis for supercapacitors

Wei Wang, Haijun Lv, Juan Du, Aibing Chen

《化学科学与工程前沿（英文）》 2021年 第15卷 第5期   页码 1312-1321 doi: 10.1007/s11705-020-2033-7

摘要： In this present work, N-doped carbon nanobelts (N-CNBs) were prepared by a confined-pyrolysis approach and the N-CNBs were derived from a polypyrrole (Ppy) tube coated with a compact silica layer. The silica layer provided a confined space for the Ppy pyrolysis, thereby hindering the rapid overflow of pyrolysis gas, which is the activator for the formation of carbonaceous materials. At the same time, the confined environment can activate the carbon shell to create a thin wall and strip the carbon tube into belt morphology. This process of confined pyrolysis realizes self-activation during the pyrolysis of Ppy to obtain the carbon nanobelts without adding any additional activator, which reduces pollution and preparation cost. In addition, this approach is simple to operate and avoids the disadvantages of other methods that consume time and materials. The as-prepared N-CNB shows cross-linked nanobelt morphology and a rich porous structure with a large specific surface area. As supercapacitor electrode materials, the N-CNB can present abundant active sites, and exhibits a specific capacitance of 246 F·g , and excellent ability with 95.44% retention after 10000 cycles. This indicates that the N-CNB is an ideal candidate as a supercapacitor electrode material.

关键词： carbon nanobelts     polypyrrole     N-doped     confined pyrolysis     supercapacitor    

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Metal phosphonate-derived cobalt/nickel phosphide@N-doped carbon hybrids as efficient bifunctional oxygen

《化学科学与工程前沿（英文）》 2022年 第16卷 第9期   页码 1367-1376 doi: 10.1007/s11705-022-2153-3

摘要： The exploration of efficient bifunctional electrocatalysts for oxygen reduction reaction and oxygen evolution reaction is pivotal for the development of rechargeable metal–air batteries. Transition metal phosphides are emerging as promising catalyst candidates because of their superb activity and low cost. Herein, a novel metal phosphonate-derived cobalt/nickel phosphide@N-doped carbon hybrid was developed by a carbothermal reduction of cobalt/nickel phosphonate hybrids with different Co/Ni molar ratios. The metal phosphonate derivation method achieved an intimately coupled interaction between metal phosphides and a heteroatom-doped carbon substrate. The resultant Co2P/Ni3P@NC-0.2 enables an impressive electrocatalytic oxygen reduction reaction activity, comparable with those of state-of-the-art Pt/C catalysts in terms of onset potential (0.88 V), 4e‒ selectivity, methanol tolerance, and long-term durability. Moreover, remarkable oxygen evolution reaction activity was also observed in alkaline conditions. The high activity is ascribed to the N-doping, abundant accessible catalytic active sites, and the synergistic effect among the components. This work not only describes a high-efficiency electrocatalyst for both oxygen reduction reaction and oxygen evolution reaction, but also highlights the application of metal phosphonate hybrids in fabricating metal phosphides with tunable structures, which is of great significance in the energy conversion field.

关键词： metal phosphonate     cobalt/nickel phosphide     N-doped carbon     oxygen electrochemistry     Zn−air battery    

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标题 作者 时间 类型 操作

Carbon-doped surface unsaturated sulfur enriched CoS@rGO aerogel pseudocapacitive anode and biomass-derivedporous carbon cathode for advanced lithium-ion capacitors

期刊论文

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

Carbon-coated Ni-Co alloy catalysts: preparation and performance for aqueous phase hydrodeoxygenation

期刊论文

Efficient hydrothermal deoxygenation of methyl palmitate to diesel-like hydrocarbons on carbon encapsulated

期刊论文

In-situ condition monitoring of reinforced concrete structures

Sanjeev Kumar VERMA,Sudhir Singh BHADAURIA,Saleem AKHTAR

期刊论文

Concurrent adsorption and reduction of chromium(VI) to chromium(III) using nitrogen-doped porous carbon

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

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

Phosphorus-doped Ni–Co sulfides connected by carbon nanotubes for flexible hybrid supercapacitor

期刊论文

Size-controllable synthesis of monodispersed nitrogen-doped carbon nanospheres from polydopamine for

期刊论文

Sulfur and carbon co-doped g-CN microtubes with enhanced photocatalytic H production activity

期刊论文

Fabrication of N-doped carbon nanobelts from a polypyrrole tube by confined pyrolysis for supercapacitors

Wei Wang, Haijun Lv, Juan Du, Aibing Chen

期刊论文

Metal phosphonate-derived cobalt/nickel phosphide@N-doped carbon hybrids as efficient bifunctional oxygen

期刊论文