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Synthesis of iron(II) complexes with asymmetric N

Wolfgang Bauer, Tanja Ossiander, Birgit Weber

《化学科学与工程前沿（英文）》 2018年 第12卷 第3期   页码 400-408 doi: 10.1007/s11705-018-1753-4

摘要：

The synthesis of new Schiff base-like ligands with asymmetric substituents pattern and their iron complexes with pyridine as axial ligand is described. Two of the ligands and one of the iron(II) complexes were characterized by single crystal X-ray structure analysis. One of the the iron(II) complexes shows spin crossover behavior while the others remain in the high spin state. The influence of the reduced symmetry of the ligand on the properties of the complexes is discussed.

关键词： iron     Schiff base-like ligands     magnetism     spin crossover     X-ray structures    

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chiral recognition of 1,1′-binaphthol through enantioselective collapse of gel based on an amphiphilic Schiff-base

Xuhong Zhang, Haimiao Li, Xin Zhang, Meng An, Weiwei Fang, Haitao Yu

《化学科学与工程前沿（英文）》 2017年 第11卷 第2期   页码 231-237 doi: 10.1007/s11705-017-1633-3

摘要： A novel gelator that contained both Schiff base and L-lysine moieties was synthesized and its gelation behavior was tested. This gelator can form gels in various organic solvents. The resulting gel can be applied as a fascinating platform for visual recognition of enantiomeric 1-(2-hydroxynaphthalen-1-yl)naphthalen-2-ol (BINOL) through selective gel collapse. In addition, the mechanism for the reaction of the gel with chiral BINOL was investigated by scanning electron microscope and H nuclear magnetic resonance.

关键词： gelator     Schiff base     chiral recognition     gel formation     gel collapse    

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Supramolecular self-assembly of two-component systems comprising aromatic amides/Schiff base and tartaric

Xin Wang, Wei Cui, Bin Li, Xiaojie Zhang, Yongxin Zhang, Yaodong Huang

《化学科学与工程前沿（英文）》 2020年 第14卷 第6期   页码 1112-1121 doi: 10.1007/s11705-019-1865-5

摘要： The gelating properties and thermotropic behaviors of stoichiometric mixtures of aromatic amides , and the aromatic Schiff base with tartaric acid (TA) were investigated. Among the three gelators, -TA exhibited superior gelating ability. Mixture -TA exhibits a smectic B phase and an unidentified smectic mesophase during both heating and cooling runs. The results of Fourier transform infrared spectroscopy and X-ray diffraction revealed the existence of hydrogen bonding and - interactions in -TA systems, which are likely to be the dominant driving forces for the supramolecular self-assembly. Additionally, it was established that all of the studied gel self-assemblies and mesophases possess a lamellar structure. The anion response ability of the tetrahydrofuran gel of -TA was evaluated and it was found that it was responsive to the stimuli of F , Cl , Br , I , AcO .

关键词： supramolecular self-assembly     organogel     liquid crystal     tartaric acid     hydrogen bond    

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Effects of ancillary ligands in acceptorless benzyl alcohol dehydrogenation mediated by phosphine-free

《化学科学与工程前沿（英文）》 2023年 第17卷 第3期   页码 314-325 doi: 10.1007/s11705-022-2219-2

摘要： Acceptorless alcohol dehydrogenation stands out as one of the most promising strategies in hydrogen storage technologies. Among various catalytic systems for this reaction, cost-effective molecular catalysts using phosphine-free ligands have gained considerable attention. However, the central challenge for using non-precious metals is to overcome the propensity of reacting by one-electron pathway. Herein, we synthesized a phosphine-free η5-C5Me5-Co complex by using the metal–ligand cooperative strategy and compared its activity with analogous catalysts toward acceptorless alcohol dehydrogenation. The catalyst showed excellent performance with a turnover number of 130.4 and a selectivity close to 100%. The improved performance among the class of η5-C5Me5-Co complexes could be attributed to the more accessible Co center and its cooperation with the redox-active ligand. To further study the systematic structure-activity relationship, we investigated the electronic structures of η5-C5Me5-Co complexes by a set of characterizations. The results showed that the redox-active ligand has a significant influence on the η5-C5Me5-Co moiety. In the meantime, the proximal O−/OH group is beneficial for shuttling protons. For the catalytic cycle, two dehydrogenation scenarios were interrogated through density functional theory, and the result suggested that the outer-sphere pathway was preferred. The formation of a dihydrogen complex was the rate-determining step with a ΔG value of 16.9 kcal∙mol‒1. The electron population demonstrated that the η5-C5Me5 ligand played a key role in stabilizing transition states during dehydrogenation steps. This work identified the roles of vital ligand components to boost catalytic performance and offered rationales for designing metal–ligand cooperative nonprecious metal complexes.

关键词： acceptorless alcohol dehydrogenation     η5-C5Me5-Co     metal–ligand cooperation     theoretical calculation    

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Study of base friction simulation tests based on a complicated engineered bridge slope

Liu HE, Guang WU, Hua WANG

《结构与土木工程前沿（英文）》 2012年 第6卷 第4期   页码 393-397 doi: 10.1007/s11709-012-0174-6

摘要： In this paper, a physical base friction test model of a slope is established. The model is based on similarity principles and the geological conditions of a complicated bridge slope during construction, deformation and failure. The behavior of the slope in both its natural state and during excavation loading is qualitatively analyzed through base friction tests. The base friction test results are then subjected to comparison and analysis using finite element numerical simulation. The findings show that the whole engineered slope tends to stabilize in its natural state, whereas instabilities will arise at faulted rock masses located near bridge piers during excavation loading. Therefore, to ensure normal construction operation of bridge works, it is suggested that pre-reinforcement of faulted rock masses be performed.

关键词： base friction test     slope stability evaluation     bridge slope    

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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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Base editors: development and applications in biomedicine

《医学前沿（英文）》 2023年 第17卷 第3期   页码 359-387 doi: 10.1007/s11684-023-1013-y

摘要： Base editor (BE) is a gene-editing tool developed by combining the CRISPR/Cas system with an individual deaminase, enabling precise single-base substitution in DNA or RNA without generating a DNA double-strand break (DSB) or requiring donor DNA templates in living cells. Base editors offer more precise and secure genome-editing effects than other conventional artificial nuclease systems, such as CRISPR/Cas9, as the DSB induced by Cas9 will cause severe damage to the genome. Thus, base editors have important applications in the field of biomedicine, including gene function investigation, directed protein evolution, genetic lineage tracing, disease modeling, and gene therapy. Since the development of the two main base editors, cytosine base editors (CBEs) and adenine base editors (ABEs), scientists have developed more than 100 optimized base editors with improved editing efficiency, precision, specificity, targeting scope, and capacity to be delivered in vivo, greatly enhancing their application potential in biomedicine. Here, we review the recent development of base editors, summarize their applications in the biomedical field, and discuss future perspectives and challenges for therapeutic applications.

关键词： base editing     CBE     ABE     ADAR     DdCBE     disease model     therapeutic application    

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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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Multistage-batch bipolar membrane electrodialysis for base production from high-salinity wastewater

《化学科学与工程前沿（英文）》 2022年 第16卷 第5期   页码 764-773 doi: 10.1007/s11705-021-2114-2

摘要： Bipolar membrane electrodialysis (BMED) is considered a state-of-the-art technology for the conversion of salts into acids and bases. However, the low concentration of base generated from a traditional BMED process may limit the viability of this technology for a large-scale application. Herein, we report an especially designed multistage-batch (two/three-stage-batch) BMED process to increase the base concentration by adjusting different volume ratios in the acid (Vacid), base (Vbase), and salt compartments (Vsalt). The findings indicated that performance of the two-stage-batch with a volume ratio of Vacid:Vbase:Vsalt = 1:1:5 was superior in comparison to the three-stage-batch with a volume ratio of Vacid:Vbase:Vsalt = 1:1:2. Besides, the base concentration could be further increased by exchanging the acid produced in the acid compartment with fresh water in the second stage-batch process. With the two-stage-batch BMED, the maximum concentration of the base can be obtained up to 3.40 mol∙L–1, which was higher than the most reported base production by BMED. The low energy consumption and high current efficiency further authenticate that the designed process is reliable, cost-effective, and more productive to convert saline water into valuable industrial commodities.

关键词： bipolar membrane electrodialysis     multistage-batch     base production     high-salinity wastewater    

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Enzyme@bismuth-ellagic acid: a versatile platform for enzyme immobilization with enhanced acid-base stability

《化学科学与工程前沿（英文）》 2023年 第17卷 第6期   页码 784-794 doi: 10.1007/s11705-022-2278-4

摘要： In situ encapsulation is an effective way to synthesize enzyme@metal–organic framework biocatalysts; however, it is limited by the conditions of metal–organic framework synthesis and its acid-base stability. Herein, a biocatalytic platform with improved acid-base stability was constructed via a one-pot method using bismuth-ellagic acid as the carrier. Bismuth-ellagic acid is a green phenol-based metal–organic framework whose organic precursor is extracted from natural plants. After encapsulation, the stability, especially the acid-base stability, of amyloglucosidases@bismuth-ellagic acid was enhanced, which remained stable over a wide pH range (2–12) and achieved multiple recycling. By selecting a suitable buffer, bismuth-ellagic acid can encapsulate different types of enzymes and enable interactions between the encapsulated enzymes and cofactors, as well as between multiple enzymes. The green precursor, simple and convenient preparation process provided a versatile strategy for enzymes encapsulation.

关键词： bismuth-ellagic acid     in situ encapsulation     enzyme@MOF biocomposites    

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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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标题 作者 时间 类型 操作

Synthesis of iron(II) complexes with asymmetric N

Wolfgang Bauer, Tanja Ossiander, Birgit Weber

期刊论文

chiral recognition of 1,1′-binaphthol through enantioselective collapse of gel based on an amphiphilic Schiff-base

Xuhong Zhang, Haimiao Li, Xin Zhang, Meng An, Weiwei Fang, Haitao Yu

期刊论文

Supramolecular self-assembly of two-component systems comprising aromatic amides/Schiff base and tartaric

Xin Wang, Wei Cui, Bin Li, Xiaojie Zhang, Yongxin Zhang, Yaodong Huang

期刊论文

Effects of ancillary ligands in acceptorless benzyl alcohol dehydrogenation mediated by phosphine-free

期刊论文

Study of base friction simulation tests based on a complicated engineered bridge slope

Liu HE, Guang WU, Hua WANG

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

Base editors: development and applications in biomedicine

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

Multistage-batch bipolar membrane electrodialysis for base production from high-salinity wastewater

期刊论文

Enzyme@bismuth-ellagic acid: a versatile platform for enzyme immobilization with enhanced acid-base stability

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