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Direct pyrolysis to convert biomass to versatile 3D carbon nanotubes/mesoporous carbon architecture: conversion mechanism and electrochemical performance

《化学科学与工程前沿(英文)》 2023年 第17卷 第6期   页码 679-690 doi: 10.1007/s11705-022-2266-8

摘要: The massive conversion of resourceful biomass to carbon nanomaterials not only opens a new avenue to effective and economical disposal of biomass, but provides a possibility to produce highly valued functionalized carbon-based electrodes for energy storage and conversion systems. In this work, biomass is applied to a facile and scalable one-step pyrolysis method to prepare three-dimensional (3D) carbon nanotubes/mesoporous carbon architecture, which uses transition metal inorganic salts and melamine as initial precursors. The role of each employed component is investigated, and the electrochemical performance of the attained product is explored. Each component and precise regulation of their dosage is proven to be the key to successful conversion of biomass to the desired carbon nanomaterials. Owing to the unique 3D architecture and integration of individual merits of carbon nanotubes and mesoporous carbon, the as-synthesized carbon nanotubes/mesoporous carbon hybrid exhibits versatile application toward lithium-ion batteries and Zn-air batteries. Apparently, a significant guidance on effective conversion of biomass to functionalized carbon nanomaterials can be shown by this work.

关键词: biomass     direct pyrolysis     3D CNTs/MC hybrid     lithium-ion batteries     Zn-air batteries    

phosphonate-derived cobalt/nickel phosphide@N-doped carbon hybrids as efficient bifunctional oxygen electrodes for Znair batteries

《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    

Cobalt nanoparticle decorated N-doped carbons derived from a cobalt covalent organic framework for oxygen electrochemistry

《化学科学与工程前沿(英文)》 2021年 第15卷 第6期   页码 1550-1560 doi: 10.1007/s11705-021-2104-4

摘要: The low cost and highly efficient construction of electrocatalysts has attracted significant attention owing to the use of clean and sustainable energy technologies. In this work, cobalt nanoparticle decorated N-doped carbons (Co@NC) are synthesized by the pyrolysis of a cobalt covalent organic framework under an inert atmosphere. The Co@NC demonstrates improved electrocatalytic capabilities compared to N-doped carbon without the addition of Co nanoparticles, indicating the important role of cobalt. The well-dispersed active sites (Co-Nx) and the synergistic effect between the carbon matrix and Co nanoparticles greatly enhance the electrocatalytic activity for the oxygen reduction reaction. In addition, the Co content has a significant effect on the catalytic activity. The resulting Co@NC-0.86 exhibits a superb electrocatalytic activity for the oxygen reduction reaction in an alkaline electrolyte in terms of the onset potential (0.90 V), half-wave potential (0.80 V) and the limiting current density (4.84 mA·cm–2), and a high selectivity, as well as a strong methanol tolerance and superior durability, these results are comparable to those of the Pt/C catalyst. Furthermore, the superior bifunctional activity of Co@NC-0.86 was also confirmed in a home-built Zn-air battery, signifying the possibility for application in electrode materials and in current energy conversion and storage devices.

关键词: cobalt embedment     N-doped carbons     covalent organic framework     oxygen reduction     Zn-air battery    

g-CN-coated MnO hollow nanorod cathode for stable aqueous Zn-ion batteries

《化学科学与工程前沿(英文)》 2023年 第17卷 第2期   页码 217-225 doi: 10.1007/s11705-022-2214-7

摘要: Aqueous zinc-ion batteries are attracting considerable attention because of their high safety compared with conventional lithium-ion batteries. Manganese-based materials have been widely developed for zinc-ion batteries cathode owning to their low cost, high security and simple preparation. However, the severe volume expansion and poor stability during charging and discharging limit the further development of manganese-based cathodes. Herein, superior α-MnO2@g-C3N4 was successfully prepared for stable zinc-ion batteries (ZIBs) cathode by introducing g-C3N4 nanosheets. Compared with pure α-MnO2, α-MnO2@g-C3N4 has a specific capacity of 298 mAh·g–1 at 0.1 A·g–1. Even at 1 A·g–1, the α-MnO2@g-C3N4 still retains 100 mAh·g–1 (83.4% retention after 5000 cycles), implying its excellent cycling stability. The α-MnO2@g-C3N4-based cathode has the highest energy density (563 Wh·kg–1) and power energy density (2170 W·kg–1). This work provides new avenues for the development of a wider range of cathode materials for ZIBs.

关键词: α-MnO2 hollow nanorods     g-C3N4     heterojunction     aqueous Zn-ion batteries    

“Charging” the cigarette butt: heteroatomic porous carbon nanosheets with edge-induced topological defects for enhanced oxygen evolution performance

《化学科学与工程前沿(英文)》 2023年 第17卷 第11期   页码 1755-1764 doi: 10.1007/s11705-023-2318-8

摘要: Owing to the complexity of electron transfer pathways, the sluggish oxygen evolution reaction process is defined as the bottleneck for the practical application of Zn–air batteries. In this effort, metal nanoparticles (Co, Ni, Fe, etc.) encapsulated within nitrogen-doped carbon materials with abundant edge sites were synthesized by one-step pyrolysis treatment using cigarette butts as raw materials, which can drastically accelerate the overall rate of oxygen evolution reaction by facilitating the adsorption of oxygenated intermediates by the edge-induced topological defects. The prepared catalyst of nitrogen-doped carbon porous nanosheets loaded with Co nanoparticles (Co@NC-500) exhibits enhanced catalytic activity toward oxygen evolution reaction, with a low overpotential of 350 mV at the current density of 10 mA·cm–2. Furthermore, the Zn–air battery assembled with Co@NC-500 catalyst demonstrates a desirable performance affording an open-circuit potential of 1.336 V and power density of 33.6 mW·cm–2, indicating considerable practical application potential.

关键词: oxygen evolution reaction     porous carbon nanosheets     Co nanoparticles     edge-induced topological defects     Zn–air batteries    

CC@BCN@PANI core-shell nanoarrays as ultra-high cycle stability cathode for Zn-ion hybrid supercapacitors

《能源前沿(英文)》 2023年 第17卷 第4期   页码 555-566 doi: 10.1007/s11708-023-0882-8

摘要: Exploring cathode materials that combine excellent cycling stability and high energy density poses a challenge to aqueous Zn-ion hybrid supercapacitors (ZHSCs). Herein, polyaniline (PANI) coated boron-carbon-nitrogen (BCN) nanoarray on carbon cloth surface is prepared as advanced cathode materials via simple high-temperature calcination and electrochemical deposition methods. Because of the excellent specific capacity and conductivity of PANI, the CC@BCN@PANI core-shell nanoarrays cathode shows an excellent ion storage capability. Moreover, the 3D nanoarray structure can provide enough space for the volume expansion and contraction of PANI in the charging/discharging cycles, which effectively avoids the collapse of the microstructure and greatly improves the electrochemical stability of PANI. Therefore, the CC@BCN@PANI-based ZHSCs exhibit superior electrochemical performances showing a specific capacity of 145.8 mAh/g, a high energy density of 116.78 Wh/kg, an excellent power density of 12 kW/kg, and a capacity retention rate of 86.2% after 8000 charge/discharge cycles at a current density of 2 A/g. In addition, the flexible ZHSCs (FZHSCs) also show a capacity retention rate of 87.7% at the current density of 2 A/g after 450 cycles.

关键词: CC@BCN@PANI cathode     Zn-ion hybrid supercapacitor     core-shell nanoarrays     high energy density     ultra-high cycle stability    

Experimental and modeling studies on installation of arc sprayed Zn anodes for protection of reinforced

Xianming SHI

《结构与土木工程前沿(英文)》 2016年 第10卷 第1期   页码 1-11 doi: 10.1007/s11709-016-0312-7

摘要: Arc sprayed zinc (Zn) anode on concrete surfaces has been an emerging technology for protecting reinforced concrete structures from rebar corrosion in coastal environments. Many cathodic protection (CP) systems with arc sprayed Zn anodes will reach or exceed their design life in the near future and thus may function improperly or insufficiently, making it necessary to replace the aged anodes. However, prior to this study, little was known about the most effective profile for the concrete surface, for either new concrete or old concrete with existing Zn anodes removed. This work develops criteria to properly prepare the concrete surface before the application of new Zn anode. Experimental studies were conducted both in the laboratory and for a field structure in Oregon. Artificial neural network was used to achieve better understanding of the complex cause-and-effect relationships inherent in the Zn-mortar or Zn–concrete systems and was successful in finding meaningful, logical results from the bond strength data. The goal is to achieve strong initial bond strength of new Zn to concrete, which is essential for long-term performance of the CP system. The results from this case study suggest that it is necessary to adjust the anode removal and surface sandblasting based on the electrochemical age of the existing concrete. In all cases of sandblasting, minimize the exposure of large aggregates (e.g., those bigger than 19 mm in diameter).

关键词: arc sprayed Zn     anode replacement     reinforced concrete     bridge preservation     neural networks     surface profile    

电沉积Zn-Fe-SiO2复合镀层研究

张英杰,范云鹰,董鹏,罗少林

《中国工程科学》 2008年 第10卷 第3期   页码 93-96

摘要:

报告了电沉积Zn-Fe-SiO2复合镀层的研究结果,论述了电流密度、极间距、搅拌方式、阳极数量及排布方式、添加剂等对Zn-Fe-SiO2复合镀层的影响及试验所取得的技术指标试验结果表明,Zn-Fe-SiO2复合镀层工艺具有过程稳定性好,维护措施简单方便,生产的环保及安全性好等优点。

关键词: 电沉积     复合镀层     Zn-Fe-SiO2    

ZN - 1阻尼橡胶材料的老化机理研究

张凯,马艳,谭云,梅军

《中国工程科学》 2009年 第11卷 第2期   页码 48-52

摘要:

采用加速老化试验方法对ZN-1阻尼橡胶材料的热氧老化性能进行了研究,获得了不同老化温度 及老化时间对硅橡胶泡沫材料力学性能及阻尼性能的影响规律研究结果表明,随着老化温度的升高及老 化时间的延长, ZN-1的拉伸强度出现了先下降后升高的现象,而扯断伸长率则表现为单调下降的趋势。同 时,还研究了ZN-1阻尼橡胶材料在热氧老化条件下微观结构与性能变化之间的关系,得到了ZN- 1阻尼橡 胶材料的热老化机理。

关键词: ZN-1阻尼橡胶材料     老化性能     微观结构     老化机理    

Relationship between heavy metal concentrations of herbaceous plants and soils at four Pb-Zn mining sites

Yuan LI , Yanqun ZU , Qixian FANG , Zhaohua GAO , Christian SCHVARTZ ,

《环境科学与工程前沿(英文)》 2009年 第3卷 第3期   页码 325-333 doi: 10.1007/s11783-009-0024-5

摘要: This paper studied the relationship between heavy metal concentrations of herbaceous plants and soils at four Pb-Zn mining sites in Yunnan, China. 50 herbaceous plant samples of 9 plant species from 4 families and 50 soil samples were collected and then ana1yzed for the tota1 concentrations of Pb, Cd, and Zn. The results showed that the average concentrations of Pb, Cd, and Zn in soil samples were 3772.83, 168.81, and 5385.65 mg/kg, respectively. The average concentrations of Pb, Cd, and Zn were 395.68, 28.14, and 1664.20 mg/kg in the shoots, and 924.12, 57.25 , and 1778.75 mg/kg in the roots, respectively. Heterospecific plants at the same site and conspecific plants at various sites had different average levels of Pb, Cd, and Zn, both in the shoots and the roots. Enrichment coefficients of Pb, Cd, and Zn were greater than 1 in 2, 3, and 9 herbaceous plant samples, respectively. Translocation factors of Pb, Cd, and Zn were greater than 1 in 10, 17, and 25 herbaceous plant samples, respectively. In all 50 samples, the concentrations of Pb, Cd, and Zn between the shoots and the roots, the shoots, and the soils, and the roots and the soils had significant positive relationships.

关键词: Pb     Cd     Zn     herbaceous plants     Pb-Zn mining areas     enrichment coefficient     translocation factor    

Simultaneous removal of trihalomethanes by bimetallic Ag/Zn: kinetics study

Ahmed H A DABWAN, Satoshi KANECO, Hideyuki KATSUMATA, Kiyoyuki EGUSA, Tohru SUZUKI, Kiyohisa OHTA,

《化学科学与工程前沿(英文)》 2010年 第4卷 第3期   页码 322-327 doi: 10.1007/s11705-009-0261-y

摘要: In the present work, bimetallic silver/zinc was applied into the degradation of trihalomethanes, THMs: CHCl, CHBrCl, CHBrCl, and CHBr. The kinetics reaction rates and removal efficiencies of the THM compound mixtures, in the aqueous solutions, were investigated. Batch experiments were conducted under mild conditions, ambient temperature, and pressure. The primary degradation reaction followed a pseudo-first-order kinetic law. The first-order rate constants and the degradation efficiencies followed the decreasing order of CHBr>CHBrCl>CHBrCl>CHCl. The bond dissociation energy and hydrophilic/hydrophobic characteristics of the THM compounds may become the most important parameters affecting the degradation kinetics and efficiency by bimetallic Ag/Zn.

关键词: reaction     first-order     dissociation     degradation reaction     aqueous    

Boosting the direct conversion of NHHCO electrolyte to syngas on Ag/Zn zeolitic imidazolate framework

《化学科学与工程前沿(英文)》 2023年 第17卷 第9期   页码 1196-1207 doi: 10.1007/s11705-022-2289-1

摘要: The electrochemical reduction of NH4HCO3 to syngas can bypass the high energy consumption of high-purity CO2 release and compression after the ammonia-based CO2 capture process. This technology has broad prospects in industrial applications and carbon neutrality. A zeolitic imidazolate framework-8 precursor was introduced with different Ag contents via colloid chemical synthesis. This material was carbonized at 1000 °C to obtain AgZn zeolitic imidazolate framework derived nitrogen carbon catalysts, which were used for the first time for boosting the direct conversion of NH4HCO3 electrolyte to syngas. The AgZn zeolitic imidazolate framework derived nitrogen carbon catalyst with a Ag/Zn ratio of 0.5:1 achieved the highest CO Faradaic efficiency of 52.0% with a current density of 1.15 mA·cm–2 at –0.5 V, a H2/CO ratio of 1–2 (–0.5 to –0.7 V), and a stable catalytic activity of more than 6 h. Its activity is comparable to that of the CO2-saturated NH4HCO3 electrolyte. The highly discrete Ag-Nx and Zn-Nx nodes may have combined catalytic effects in the catalysts synthesized by appropriate Ag doping and sufficient carbonization. These nodes could increase active sites of catalysts, which is conducive to the transport and adsorption of reactant CO2 and the stability of *COOH intermediate, thus can improve the selectivity and catalytic activity of CO.

关键词: Ag catalyst     zeolitic imidazolate framework     CO2 electroreduction     ammonium bicarbonate electrolyte     syngas    

Review on cellulose paper-based electrodes for sustainable batteries with high energy densities

《化学科学与工程前沿(英文)》 2023年 第17卷 第8期   页码 1010-1027 doi: 10.1007/s11705-023-2307-y

摘要: Powering the future, while maintaining strong socioeconomic growth and a cleaner environment, is going to be one of the biggest challenges faced by mankind nowadays. Thus, there is a transition from the use of fossil fuels to renewable energy sources. Cellulose, the main component of paper, represents a unique type of bio-based building blocks featuring exciting properties: low-cost, hierarchical fibrous structures, hydrophilicity, biocompatible, mechanical flexibility, and renewability, which make it perfect for use in paper-based sustainable energy storage devices. This review focuses on lithium-ion battery application of celluloses with cellulose at different scales, i.e., cellulose microfibers, and nanocellulose, and highlights the new trends in the field. Recent advances and approaches to construct high mass loading paper electrodes toward high energy density batteries are evaluated and the limitations of paper-based cathodes are discussed. This will stimulate the use of natural resources and thereby the development of renewable electric energy systems based on sustainable technologies with low environmental impacts and carbon footprints.

关键词: cellulose     paper electrodes     Li-ion batteries     high energy density    

Sequence of the main geochemical controls on the Cu and Zn fractions in the Yangtze River estuarine sediments

Shou ZHAO,Dongxin WANG,Chenghong FENG,Ying WANG,Zhenyao SHEN

《环境科学与工程前沿(英文)》 2016年 第10卷 第1期   页码 19-27 doi: 10.1007/s11783-014-0723-4

摘要: Metal speciation can provide sufficient information for environmental and geochemical researches. In this study, based on the speciation determination of Cu and Zn in the Yangtze Estuary sediments, roles of eight geochemical controls (i.e., total organic carbon (TOC), clay, Fe/Mn in five chemical fractions and salinity) are fully investigated and sequenced with correlation analysis (CA) and principal components analysis (PCA). Results show that TOC, clay and Fe/Mn oxides are key geochemical factors affecting the chemical speciation distributions of Cu and Zn in sediments, while the role of salinity appears to be more indirect effect. The influencing sequence generally follows the order: TOC>clay>Mn oxides>Fe oxides>salinity. Among the different fractions of Fe/Mn oxides, residual and total Fe content, and exchangeable and carbonate Mn exert the greatest influences, while exchangeable Fe and residual Mn show the poorest influences.

关键词: chemical speciation     geochemical factors     estuaries     sediments     correlation     salinity    

Fabrication of bimetallic Cu–Zn adsorbents with high dispersion by using confined space for gas adsorptive

《化学科学与工程前沿(英文)》   页码 1623-1631 doi: 10.1007/s11705-022-2202-y

摘要: The number of active components and their dispersion degree are two key factors affecting the performance of adsorbents. Here, we report a simple but efficient strategy for dispersing active components by using a confined space, which is formed by mesoporous silica walls and templates in the as-prepared SBA-15 (AS). Such a confined space does not exist in the conventional support, calcined SBA-15, which does not contain a template. The Cu and Zn precursors were introduced to the confined space in the AS and were converted to CuO and ZnO during calcination, during which the template was also removed. The results show that up to 5 mmol·g–1 of CuO and ZnO can be well dispersed; however, severe aggregation of both oxides takes place in the sample derived from the calcined SBA-15 with the same loading. Confined space in the AS and the strong interactions caused by the abundant hydroxyl groups are responsible for the dispersion of CuO and ZnO. The bimetallic materials were employed for the adsorptive separation of propene and propane. The samples prepared from the as-prepared SBA-15 showed superior performance to their counterparts from the calcined SBA-15 in terms of both adsorption capacity of propene and selectivity for propene/propane.

关键词: bimetallic adsorbents     confined space     mesoporous silica     propene/propane separation    

标题 作者 时间 类型 操作

Direct pyrolysis to convert biomass to versatile 3D carbon nanotubes/mesoporous carbon architecture: conversion mechanism and electrochemical performance

期刊论文

phosphonate-derived cobalt/nickel phosphide@N-doped carbon hybrids as efficient bifunctional oxygen electrodes for Znair batteries

期刊论文

Cobalt nanoparticle decorated N-doped carbons derived from a cobalt covalent organic framework for oxygen electrochemistry

期刊论文

g-CN-coated MnO hollow nanorod cathode for stable aqueous Zn-ion batteries

期刊论文

“Charging” the cigarette butt: heteroatomic porous carbon nanosheets with edge-induced topological defects for enhanced oxygen evolution performance

期刊论文

CC@BCN@PANI core-shell nanoarrays as ultra-high cycle stability cathode for Zn-ion hybrid supercapacitors

期刊论文

Experimental and modeling studies on installation of arc sprayed Zn anodes for protection of reinforced

Xianming SHI

期刊论文

电沉积Zn-Fe-SiO2复合镀层研究

张英杰,范云鹰,董鹏,罗少林

期刊论文

ZN - 1阻尼橡胶材料的老化机理研究

张凯,马艳,谭云,梅军

期刊论文

Relationship between heavy metal concentrations of herbaceous plants and soils at four Pb-Zn mining sites

Yuan LI , Yanqun ZU , Qixian FANG , Zhaohua GAO , Christian SCHVARTZ ,

期刊论文

Simultaneous removal of trihalomethanes by bimetallic Ag/Zn: kinetics study

Ahmed H A DABWAN, Satoshi KANECO, Hideyuki KATSUMATA, Kiyoyuki EGUSA, Tohru SUZUKI, Kiyohisa OHTA,

期刊论文

Boosting the direct conversion of NHHCO electrolyte to syngas on Ag/Zn zeolitic imidazolate framework

期刊论文

Review on cellulose paper-based electrodes for sustainable batteries with high energy densities

期刊论文

Sequence of the main geochemical controls on the Cu and Zn fractions in the Yangtze River estuarine sediments

Shou ZHAO,Dongxin WANG,Chenghong FENG,Ying WANG,Zhenyao SHEN

期刊论文

Fabrication of bimetallic Cu–Zn adsorbents with high dispersion by using confined space for gas adsorptive

期刊论文