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Floret-like Fe–N nanoparticle-embedded porous carbon superstructures from a Fe-covalent triazine polymer

《化学科学与工程前沿（英文）》 2023年 第17卷 第5期   页码 525-535 doi: 10.1007/s11705-022-2232-5

摘要： Fe–Nx nanoparticles-embedded porous carbons with a desirable superstructure have attracted immense attention as promising catalysts for electrochemical oxygen reduction reaction. Herein, we employed Fe-coordinated covalent triazine polymer for the fabrication of Fe–Nx nanoparticle-embedded porous carbon nanoflorets (Fe/N@CNFs) employing a hypersaline-confinement-conversion strategy. Presence of tailored N types within the covalent triazine polymer interwork in high proportions contributes to the generation of Fe/N coordination and subsequent Fe–Nx nanoparticles. Owing to the utilization of NaCl crystals, the resultant Fe/N@CNF-800 which was generated by pyrolysis at 800 °C showed nanoflower structure and large specific surface area, which remarkably suppressed the agglomeration of high catalytic active sites. As expect, the Fe/N@CNF-800 exhibited unexpected oxygen reduction reaction catalytic performance with an ultrahigh half-wave potential (0.89 V vs. reversible hydrogen electrode), a dominant 4e– transfer approach and great cycle stability (> 92% after 100000 s). As a demonstration, the Fe/N-PCNF-800-assembled zinc–air battery delivered a high open circuit voltage of 1.51 V, a maximum peak power density of 164 mW·cm–2, as well as eminent rate performance, surpassing those of commercial Pt/C. This contribution offers a valuable avenue to exploit efficient metal nanoparticles-based carbon catalysts towards energy-related electrocatalytic reactions and beyond.

关键词： Fe–Nx nanoparticles     hypersaline-confinement conversion     floret-like carbon     covalent triazine polymers     oxygen reduction reaction    

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A facile synthesis of high activity cube-like Pt/carbon composites for fuel cell application

Reza B. MOGHADDAM, Samaneh SHAHGALDI, Xianguo LI

《能源前沿（英文）》 2017年 第11卷 第3期   页码 245-253 doi: 10.1007/s11708-017-0492-4

摘要： High activity catalyst with simple low-cost synthesis is essential for fuel cell commercialization. In this study, a facile procedure for the synthesis of cube-like Pt nanoparticle (Pt ) composites with high surface area carbon supports is developed by mixing precursor of Pt with carbon supports in organic batches, hence, one pot synthesis. The Pt grow with Vulcan XC-72 or Ketjen black, respectively, and then treated for 5.5 h at 185ºC (i.e., Pt /V and Pt /K). The resulting particle sizes and shapes are similar; however, Pt /K has a larger electrochemical active surface area (EASA) and a remarkably better formic acid (FA) oxidation performance. Optimization of the Pt /K composites leads to Pt /K that has been treated for 10 h at 185ºC. With a larger EASA, Pt /K is also more active in FA oxidation than the other Pt /K composites. Impedance spectroscopy analysis of the temperature treated and as-prepared (i.e., untreated) Pt /K composites indicates that Pt /K is less resistive, and has the highest limiting capacitance among the Pt /K electrodes. Consistently, the voltammetric EASA is the largest for Pt /K. Furthermore, Pt /K is compared with two commercial Pt/C catalysts, Tanaka Kikinzoku Kogyo (TKK), and Johnson Matthey (JM)Pt/C catalysts. The TKK Pt/C has a higher EASA than Pt /K, as expected from their relative particles sizes (3–4 nm vs. 6–7 nm for Pt /K), however, Pt /K has a significantly better FA oxidation activity.

关键词： synthesis     cube-like Pt     Pt/C composite     catalyst     impedance    

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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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Bamboo-like -doped carbon nanotubes encapsulating M(Co, Fe)-Ni alloy for electrochemical production of

《化学科学与工程前沿（英文）》 2022年 第16卷 第4期   页码 498-510 doi: 10.1007/s11705-021-2082-6

摘要： The electrochemical conversion of CO2-H2O into CO-H2 using renewable energy is a promising technique for clean syngas production. Low-cost electrocatalysts to produce tunable syngas with a potential-independent CO/H2 ratio are highly desired. Herein, a series of N-doped carbon nanotubes encapsulating binary alloy nanoparticles (MxNi-NCNT, M= Fe, Co) were successfully fabricated through the co-pyrolysis of melamine and metal precursors. The MxNi-NCNT samples exhibited bamboo-like nanotubular structures with a large specific surface area and high degree of graphitization. Their electrocatalytic performance for syngas production can be tuned by changing the alloy compositions and modifying the electronic structure of the carbon nanotube through the encapsulated metal nanoparticles. Consequently, syngas with a wide range of CO/H2 ratios, from 0.5:1 to 3.4:1, can be produced on MxNi-NCNT. More importantly, stable CO/H2 ratios of 2:1 and 1.5:1, corresponding to the ratio to produce biofuels by syngas fermentation, could be realized on Co1Ni-NCNT and Co2Ni-NCNT, respectively, over a potential window of –0.8 to –1.2 V versus the reversible hydrogen electrode. Our work provides an approach to develop low-cost and potential-independent electrocatalysts to effectively produce syngas with an adjustable CO/H2 ratio from electrochemical CO2 reduction.

关键词： electrochemical reduction of CO2     syngas     N-doped carbon nanotubes     encapsulated alloy nanoparticles     CO/H2 ratio    

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Templated synthesis of urchin-like zinc oxide particles by micro-combustion

Xintong ZHOU, Quan ZHANG, Chang-jun LIU

《化学科学与工程前沿（英文）》 2014年 第8卷 第1期   页码 73-78 doi: 10.1007/s11705-014-1404-3

摘要： Micro-combustion initiated by dielectric barrier discharge plasma has been applied for the removal of carbon template to prepare urchin-like ZnO particles. The combustion is operated at atmospheric pressure and low gas temperature (less than 150 °C), and the template is fully decomposed and rapidly removed. The obtained urchin-like ZnO possesses two distinct morphologies: nanosheets and sub-micro rods. The unique morphologies form on ZnO hexagonal nuclei with the template effect of activated carbon.

关键词： dielectric-barrier discharge     zinc oxide     carbon template     removal     plasma    

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Carbon nanotubes-incorporated MIL-88B-Fe as highly efficient Fenton-like catalyst for degradation of

Hang Zhang, Shuo Chen, Haiguang Zhang, Xinfei Fan, Cong Gao, Hongtao Yu, Xie Quan

《环境科学与工程前沿（英文）》 2019年 第13卷 第2期 doi: 10.1007/s11783-019-1101-z

摘要：

CNTs were incorporated into MIL-88B-Fe to get a new Fenton-like catalyst (C@M).

Fe(II) was introduced in C@M to get a fast initiation of Fenton-like reaction.

Fe(II) content in C@M was related with oxygen-containing functional groups on CNTs.

C@M shows efficient catalytic degradation of pollutants over a wide pH range.

关键词： Heterogeneous Fenton-like catalysts     MIL-88B-Fe     CNTs     Organic pollutants     Mechanism    

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Valorization of agro-industrial fruit peel waste to fluorescent nanocarbon sensor: Ultrasensitive detection of potentially hazardous tropane alkaloid

《环境科学与工程前沿（英文）》 2022年 第16卷 第3期 doi: 10.1007/s11783-021-1461-z

摘要：

• Transformation of agro-industrial waste to value-added material via green chemistry.

关键词： Agro-industrial waste     Orange peel     Valorization     Nanodiamond-like carbon     Atropine sulphate     Fluorescence sensing    

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Distinct immune escape and microenvironment between RG-like and pri-OPC-like glioma revealed by single-cell

《医学前沿（英文）》 doi: 10.1007/s11684-023-1017-7

摘要： The association of neurogenesis and gliogenesis with glioma remains unclear. By conducting single-cell RNA-seq analyses on 26 gliomas, we reported their classification into primitive oligodendrocyte precursor cell (pri-OPC)-like and radial glia (RG)-like tumors and validated it in a public cohort and TCGA glioma. The RG-like tumors exhibited wild-type isocitrate dehydrogenase and tended to carry EGFR mutations, and the pri-OPC-like ones were prone to carrying TP53 mutations. Tumor subclones only in pri-OPC-like tumors showed substantially down-regulated MHC-I genes, suggesting their distinct immune evasion programs. Furthermore, the two subgroups appeared to extensively modulate glioma-infiltrating lymphocytes in distinct manners. Some specific genes not expressed in normal immune cells were found in glioma-infiltrating lymphocytes. For example, glial/glioma stem cell markers OLIG1/PTPRZ1 and B cell-specific receptors IGLC2/IGKC were expressed in pri-OPC-like and RG-like glioma-infiltrating lymphocytes, respectively. Their expression was positively correlated with those of immune checkpoint genes (e.g., LGALS3) and poor survivals as validated by the increased expression of LGALS3 upon IGKC overexpression in Jurkat cells. This finding indicated a potential inhibitory role in tumor-infiltrating lymphocytes and could provide a new way of cancer immune evasion.

关键词： single-cell RNA-seq     glioma     radial glia     primitive oligodendrocyte precursor cell     immune escape    

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Self-sacrificial templating synthesis of flower-like nickel phyllosilicates and its application as high-performance

《化学科学与工程前沿（英文）》 2022年 第16卷 第4期   页码 484-497 doi: 10.1007/s11705-021-2074-6

摘要： The nanocomposites of flower-like nickel phyllosilicate particles incorporated into epoxy resin were fabricated via an in-situ mixing process. The flower-like nickel phyllosilicate particles were firstly synthesized using a mild self-sacrificial templating method, and the morphology and lamellar structure were examined carefully. Several properties of mechanical, thermal and tribological responses of epoxy nanocomposites were performed. It was demonstrated that adequate flower-like nickel phyllosilicate particles dispersed well in the matrix, and the nanocomposites displayed enhanced tensile strength and elastic modulus but decreased elongation at break as expected. In addition, friction coefficient and wear rate were increased first and then decreased along with the particle content, and showed the lowest values at a mass fraction of 5%. Nevertheless, the incorporated flower-like nickel phyllosilicate particles resulted in the continuously increasing thermal stability of epoxy resin (EP) nanocomposites. This study revealed the giant potential of flower-like particles in preparing high-quality EP nanocomposites.

关键词： nickel phyllosilicate     flow-like structure     mechanical property     thermal stability     tribological performance    

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Toll-like receptors in innate immunity and infectious diseases

Min-Hao WU, Ping ZHANG, Xi HUANG,

《医学前沿（英文）》 2010年 第4卷 第4期   页码 385-393 doi: 10.1007/s11684-010-0600-x

摘要： The protective ability of host defense system is largely dependent on germ-line encoded pattern-recognition receptors (PRRs). These PRRs respond to a variety of exogenous pathogens or endogenous danger signals, by recognizing some highly conserved structures such as pathogen-associated molecular patterns (PAMPs) and danger/damage associated molecular patterns (DAMPs). The most studied PRRs are Toll-like receptors (TLRs). Activation of TLRs triggers production of inflammatory cytokines and type I interferons (IFNs) via myeloid differentiation primary response gene 88 (MyD88)-dependent or-independent signaling respectively, thereby modulating innate and adaptive immunity, as well as inflammatory responses. This review introduces the classification, structure, and specific ligands of TLRs, and focuses on their signal pathways and biological activities, as well as clinical relevance. These studies of TLRs in the innate immune system have implications for the prevention and treatment of a variety of infectious diseases, including tuberculosis (TB), microbial keratitis, and hepatitis B and C.

关键词： Toll-like receptors     innate immunity     infectious disease     inflammation    

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Dispersion of “guava-like” silica/polyacrylate nanocomposite particles in polyacrylate matrix

QI Dongming, YANG Lei, WU Minghua, SHAO Jianzhong, BAO Yongzhong

《化学科学与工程前沿（英文）》 2008年 第2卷 第2期   页码 127-134 doi: 10.1007/s11705-008-0033-0

摘要： A series of “guava-like” silica/polyacrylate nanocomposite particles with close silica content and different grafting degrees were prepared via mini-emulsion polymerization using 3-(trimethoxysilyl)propyl methacrylate (TSPM) modified silica/acrylate dispersion. The silica/polyacrylate composite particles were melt-mixed with unfilled polyacrylate (PA) resin to prepare corresponding silica/polyacrylate molded composites and the dispersion mechanism of these silica particles from the “guava-like” composite particles into polyacrylate matrix was studied. It was calculated that about 110 silica particles were accumulated in the bulk of every silica/polyacrylate composite latex particle. Both the solubility tests of silica/polyacrylate composite latex particles in tetrahydrofuran (THF) and the section transmission electron microscope (TEM) micrographs of silica/polyacrylate molded composites indicated that the grafting degree of silica particles played a crucial role in the dispersion of silica/polyacrylate composite particles into the polyacrylate matrix. When the grafting degree of polyacrylate onto silica was in a moderate range (ca. 20%–70%), almost all of silica particles in these “guava-like” composite particles were dispersed into the polyacrylate matrix in a primary-particle-level. However, at a lower grafting degree, massive silica aggregations were found in molded composites because of the lack of steric protection. At a greater grafting degree (i.e., 200%), a cross-linked network was formed in the silica/polyacrylate composite particles, which prevented the dispersion of composite particles in THF and polyacrylate matrix as primary particles.

关键词： silica/polyacrylate composite     cross-linked network     –70     guava-like     TEM    

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Layer-like FAU-type zeolites: A comparative view on different preparation routes

Bastian Reiprich, Tobias Weissenberger, Wilhelm Schwieger, Alexandra Inayat

《化学科学与工程前沿（英文）》 2020年 第14卷 第2期   页码 127-142 doi: 10.1007/s11705-019-1883-3

摘要： The creation of intergrown layer-like zeolite crystals is one route to form hierarchical zeolites. Faujasite-type (FAU-type) zeolites are among the industrially most important zeolites and the implementation of hierarchical porosity is a promising way to optimise their catalytic and adsorptive performance. After a short general survey into routes for the preparation of hierarchical pore systems in FAU, we will review the currently existing strategies for the synthesis of FAU with layer-like morphology. Those strategies are mainly based on the presence of morphology modifying agents in the synthesis mixture. However, a very recent approach is the synthesis of layer-like FAU-type zeolite crystals assembled in an intergrown manner in the absence of such additives, just by finely adjusting the crystallization temperature. This additive-free preparation route for layer-like FAU, which appears very attractive from an ecological as well as economic point of view, is highlighted in this review. Concluding, a comparison, including powder X-ray diffraction, scanning and transmission electron microscopy, nitrogen physisorption and elemental analysis, between conventional FAU and three layer-like FAU obtained by different synthesis routes was carried out to show the structural, morphological and textural differences and similarities of these materials.

关键词： FAU     hierarchical zeolite     layer-like morphology    

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Synthesis and characterization of well-defined comb-like branched polymers

LI Aixiang, LU Zaijun, LÜ Zijian

《化学科学与工程前沿（英文）》 2008年 第2卷 第4期   页码 407-411 doi: 10.1007/s11705-008-0064-6

摘要： Well-defined comb-like branched polymers having one branch in each repeating unit have been successfully synthesized by the coupling reaction of living polystyrene (PS) and polyisoprene (PI) anions with 1, 1-diphenylethenyl (DPE) groups along PS backbone prepared via atom transfer radical polymerization (ATRP) of 4-vinylbenzyloxy benzophenone (Sc) followed by Wittig reaction. The resulting comb-like branched polymers were characterized by IR, H-NMR, gel permeation chromatography (GPC) and static light scattering (SLS) in detail. The effect of living chains and DPE group molar ratio on grafting efficiency was discussed. The results show the coupling reaction of living chains and DPE groups was highly effective, and the coupling efficiency can be controlled via the feed molar ratios of living chains and DPE groups. Moreover, the effect of molecular weights of backbone (PSe) and PSLi or PILi on grafting efficiency was also discussed. The results show that when excess living polymers were used, the almost quantitative grafting efficiency could be achieved.

关键词： grafting efficiency     polyisoprene     quantitative grafting     effective     molecular    

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Novel synthetic approaches and TWC catalytic performance of flower-like Pt/CeO

Zongcheng ZHAN,Xiaojun LIU,Dongzhu MA,Liyun SONG,Jinzhou LI,Hong HE,Hongxing DAI

《环境科学与工程前沿（英文）》 2014年 第8卷 第4期   页码 483-495 doi: 10.1007/s11783-013-0595-z

摘要： A novel Ultrasonic Assisted Membrane Reduction (UAMR)-hydrothermal method was used to prepare flower-like Pt/CeO catalysts. The texture, physical/chemical properties, and reducibility of the flower-like Pt/CeO catalysts were characterized by X-Ray Diffraction (XRD), Scanning Electron Microscope (SEM), Transmission Electron Microscope (TEM), N adsorption, and hydrogen temperature programmed reduction (H -TPR) techniques. The catalytic performance of the catalysts for treating automobile emission was studied relative to samples prepared by the conventional wetness impregnation method. The Pt/CeO catalysts fabricated by this novel method showed high specific surface area and metal dispersion, excellent three-way catalytic activity, and good thermal stability. The strong interaction between the Pt nanoparticles and CeO improved the thermal stability. The Ce ions were incorporated into the surfactant chains and the Pt nanoparticles were stabilized through an exchange reaction of the surface hydroxyl groups. The SEM results demonstrated that the Pt/CeO catalysts had a typical three-dimensional (3D) hierarchical porous structure, which was favorable for surface reaction and enhanced the exposure degree of the Pt nanoparticles. In brief, the flower-like Pt/CeO catalysts prepared by UAMR-hydrothermal method exhibited a higher Pt metal dispersion, smaller particle size, better three-way catalytic activity, and improved thermal stability versus conventional materials.

关键词： three-way catalyst     flower-like     Ultrasonic Assisted Membrane Reduction (UAMR)     Pt nanoparticles    

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Enhanced Fenton-like process over Cu/L(+)-ascorbic acid co-doping mesoporous silica for toxicity reduction

《环境科学与工程前沿（英文）》 2023年 第18卷 第4期 doi: 10.1007/s11783-024-1804-7

摘要：

● Cu-C-MSNs are developed via a co-doping step of Cu with L(+)-ascorbic acid.

关键词： Cation-π structures     Polarization electric field     Fenton-like process     Contaminants cleavage    

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标题 作者 时间 类型 操作

Floret-like Fe–N nanoparticle-embedded porous carbon superstructures from a Fe-covalent triazine polymer

期刊论文

A facile synthesis of high activity cube-like Pt/carbon composites for fuel cell application

Reza B. MOGHADDAM, Samaneh SHAHGALDI, Xianguo LI

期刊论文

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

期刊论文

Bamboo-like -doped carbon nanotubes encapsulating M(Co, Fe)-Ni alloy for electrochemical production of

期刊论文

Templated synthesis of urchin-like zinc oxide particles by micro-combustion

Xintong ZHOU, Quan ZHANG, Chang-jun LIU

期刊论文

Carbon nanotubes-incorporated MIL-88B-Fe as highly efficient Fenton-like catalyst for degradation of

Hang Zhang, Shuo Chen, Haiguang Zhang, Xinfei Fan, Cong Gao, Hongtao Yu, Xie Quan

期刊论文

Valorization of agro-industrial fruit peel waste to fluorescent nanocarbon sensor: Ultrasensitive detection of potentially hazardous tropane alkaloid

期刊论文

Distinct immune escape and microenvironment between RG-like and pri-OPC-like glioma revealed by single-cell

期刊论文

Self-sacrificial templating synthesis of flower-like nickel phyllosilicates and its application as high-performance

期刊论文

Toll-like receptors in innate immunity and infectious diseases

Min-Hao WU, Ping ZHANG, Xi HUANG,

期刊论文

Dispersion of “guava-like” silica/polyacrylate nanocomposite particles in polyacrylate matrix

QI Dongming, YANG Lei, WU Minghua, SHAO Jianzhong, BAO Yongzhong

期刊论文

Layer-like FAU-type zeolites: A comparative view on different preparation routes

Bastian Reiprich, Tobias Weissenberger, Wilhelm Schwieger, Alexandra Inayat

期刊论文

Synthesis and characterization of well-defined comb-like branched polymers

LI Aixiang, LU Zaijun, LÜ Zijian

期刊论文

Novel synthetic approaches and TWC catalytic performance of flower-like Pt/CeO

Zongcheng ZHAN,Xiaojun LIU,Dongzhu MA,Liyun SONG,Jinzhou LI,Hong HE,Hongxing DAI

期刊论文

Enhanced Fenton-like process over Cu/L(+)-ascorbic acid co-doping mesoporous silica for toxicity reduction

期刊论文