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991.
Dr. Tarun Kumar Yan Yang Sirine Sghaier Dr. Yassir Zaid Dr. Xavier F. Le Goff Dr. Elodie Rousset Dr. Fabien Massicot Dr. Dominique Harakat Agathe Martinez Dr. Marc Taillefer Prof. Laurent Maron Prof. Jean-Bernard Behr Dr. Florian Jaroschik 《Chemistry (Weinheim an der Bergstrasse, Germany)》2021,27(12):4016-4021
The development of new fluorine-containing building blocks and their efficient synthetic access is currently a challenging research field. Herein, the highly regio- and stereoselective addition of a large range of aldehydes onto trifluoromethylated benzofulvenes was achieved using a simple La/I2/DIBAL-Cl system via a selective C−F bond activation process. This versatile methodology provided homodienyl alcohols bearing a terminal CF2-alkene with potential further applications, as shown by the dehydration to the first benzofulvenes carrying a difluorovinyl group. In addition, for certain electron-poor aldehydes, unprecedented ipso substitution of the CF3 group in a diene was observed, which, according to DFT studies, is related to the presence of the large, Lewis-acidic lanthanum metal. 相似文献
992.
Jingyi Cai Haoshan Wei Prof. Yong Zhang Rui Cai Dr. Xueru Zhang Prof. Yan Wang Prof. Jiaqin Liu Prof. Hark Hoe Tan Prof. Ting Xie Prof. Yucheng Wu 《Chemistry (Weinheim an der Bergstrasse, Germany)》2021,27(25):7300-7306
Efficient separation of photogenerated electron–hole pairs is a crucial factor for high-performance photocatalysts. Effective electron–hole separation and migration could be achieved by heterojunctions with suitable band structures. Herein, a porous SrTiO3/SrSO4 heterojunction is prepared by a sol-gel method at room temperature followed by an annealing process. XRD characterization suggests high crystallinity of the heterostructure. A well-defined interface between the two phases is confirmed by high-resolution (HR)TEM. The photocatalytic H2 evolution productivity of the SrTiO3/SrSO4 heterojunction with Pt as co-catalyst reaches 396.82 μmol g−1 h−1, which is 16 times higher than that of SrTiO3/Pt. The boosted photocatalytic activity of SrTiO3/SrSO4/Pt can be ascribed to the presence of SrSO4, which promotes the transfer and migration of photogenerated carriers by forming the heterojunction and porous structure, which provides a large amount of active sites. This novel porous heterostructure brings new ideas for the development of high-efficiency photocatalysts for H2 release. 相似文献
993.
Yao-Yao Liu Dr. Li-Jian Chen Dr. Xu Zhao Prof. Xiu-Ping Yan 《Chemistry (Weinheim an der Bergstrasse, Germany)》2021,27(39):10151-10159
Porphyrinic metal-organic frameworks (MOFs) are promising photosensitizers due to the lack of self-aggregation of porphyrin in aqueous solution. However, how the topology of porphyrinic MOFs affects the generation of singlet oxygen (1O2) is unclear. Here, the effect of the topology of porphyrinic MOFs on their photodynamic performance is reported. Four porphyrinic zirconium MOFs (MOF-525, MOF-545, PCN-223 and PCN-224 with different topologies: ftw , csq , shp and she , respectively) were selected to study the influence of topology on the photodynamic antibacterial performance. The 1O2 generation and the photodynamic antibacterial performance followed an decreasing order of MOF-545>MOF-525>PCN-224>PCN-223. The results reveal that the pore size, the distance between porphyrin, and the number of porphyrin per Zr6O8 cluster in MOFs greatly affected 1O2 generation. This work provides guidance for designing new MOFs for efficient photodynamic sterilization. 相似文献
994.
Li Zhu Kun Liu Shudong Zheng Dr. Xiacong Zhang Prof. Dr. Jiatao Yan Prof. Dr. Wen Li Prof. Dr. Afang Zhang 《Chemistry (Weinheim an der Bergstrasse, Germany)》2021,27(40):10470-10476
Water-soluble and thermoresponsive macrocycles with stable inclusion toward guests are highly valuable to construct stimuli-responsive supramolecular materials for versatile applications. Here, we develop such macrocycles – ureido-substituted cyclodextrins (CDs) which exhibit unprecedented upper critical solution temperature (UCST) behavior in aqueous media. These novel CD derivatives showed good solubility in water at elevated temperature, but collapsed from water to form large coacervates upon cooling to low temperature. Their cloud points are greatly dependent on concentration and can be mediated through oxidation and chelation with silver ions. Significantly, the amphiphilicity of these CD derivatives is supportive to host-guest binding, which affords them inclusion abilities to guest dyes. The inclusion complexation remained nearly intact during thermally induced phase transitions, which is in contrast to the switchable inclusion behavior of lower critical solution temperature (LCST)-type CDs. Moreover, ureido-substituted CDs were exploited to co-encapsulate a pair of guest dyes whose fluorescence resonance energy transfer process can be switched by the UCST phase transition. We therefore believe these novel thermoresponsive CDs may form a new strategy for developing smart macrocycles and allow for exploring smart supramolecular materials. 相似文献
995.
Sangni Jiang Wenliang Wang Lihua Dong Xinxin Yan Shengran Li Weikang Mei Xintao Xie Yuanhua Zhang Sanrong Liu Prof. Xifei Yu 《Chemistry (Weinheim an der Bergstrasse, Germany)》2021,27(49):12589-12598
Choline phosphate lipids have been designed and developed as new-generation zwitterionic nanocarriers with excellent biocompatibility and bioorthogonality to provide a more programmable performance for cancer therapy. However, there is a lack of spatiotemporal and reversible control for drug release at target tumor cells, which can lead to severe adverse effects to normal tissue and discounted treatment outcome. Here, light-inducible Lip-cRGDfk/ICG/Dox liposomes were developed for synergistic cancer therapy. ICG can effectively convert light energy into selective heating in a local environment upon laser irradiation, thus inducing thermal ablation of tumor cells, and further reversibly trigger the spatiotemporal release of anticancer drugs (Dox) at tumor cells due to the conformation transformation of CP lipids to synergistically kill tumor cells. That Lip-cRGDfk/ICG/Dox exhibited a significant improvement for breast cancer therapy in vitro and in vivo is also demonstrated, thus it can serve as an efficient platform to noninvasively and spatiotemporally control the activation of cytotoxicity at tumor cells for precision cancer therapy. 相似文献
996.
Distinguishing the types of partial discharge (PD) caused by different insulation defects in gas-insulated switchgear (GIS) is a great challenge in the power industry, and improving the recognition accuracy of the relevant models is one of the key problems. In this paper, a convolutional neural network and long short-term memory (CNN-LSTM) model is proposed, which can effectively extract and utilize the spatiotemporal characteristics of PD input signals. First, the spatial characteristics of higher-level PD signals can be obtained through the CNN network, but because CNN is a deep feedforward neural network, it does not have the ability to process time-series data. The PD voltage signal is related to the time dimension, so LSTM saves and analyzes the previous voltage signal information, realizes the modeling of the time dependence of the data, and improves the accuracy of the PD signal pattern recognition. Finally, the pattern recognition results based on CNN-LSTM are given and compared with those based on other traditional analysis methods. The results show that the pattern recognition rate of this method is the highest, with an average of 97.9%, and its overall accuracy is better than that of other traditional analysis methods. The CNN-LSTM model provides a reliable reference for GIS PD diagnosis. 相似文献
997.
Jiahui Liu Guangming Wang Xuepu Wang Yan Sun Bei Zhou Yunlong Zou Prof. Dr. Biaobing Wang Prof. Dr. Kaka Zhang 《Chemistry (Weinheim an der Bergstrasse, Germany)》2021,27(67):16735-16743
The fabrication of room-temperature organic phosphorescence and afterglow materials, as well as the transformation of their photophysical properties, has emerged as an important topic in the research field of luminescent materials. Here, we report the establishment of energy landscapes in dopant-matrix organic afterglow systems where the aggregation states of luminescent dopants can be controlled by doping concentrations in the matrices and the methods of preparing the materials. Through manipulation by thermodynamic and kinetic control, dopant-matrix afterglow materials with different aggregation states and diverse afterglow properties can be obtained. The conversion from metastable aggregation state to thermodynamic stable aggregation state of the dopant-matrix afterglow materials to leads to the emergence of intriguing afterglow transformation behavior triggered by thermal and solvent annealing. The thermodynamically unfavorable reversible afterglow transformation process can also be achieved by coupling the dopant-matrix afterglow system to mechanical forces. 相似文献
998.
Dr. Yan Peng Hagen Kaemmerer Prof. Annie K. Powell 《Chemistry (Weinheim an der Bergstrasse, Germany)》2021,27(61):15044-15066
In this Review we discuss the tuning handles which can be used to steer the magnetic properties of FeIII-4 f “butterfly” compounds. The majority of presented compounds were produced in the context of project A3 “Di- to tetranuclear compounds incorporating highly anisotropic paramagnetic metal ions” within the SFB/TRR88 “3MET”. These contain {FeIII2Ln2} cores encapsulated in ligand shells which are easy to tune in a “test-bed” system. We identify the following advantages and variables in such systems: (i) the complexes are structurally simple usually with one crystallographically independent FeIII and LnIII, respectively. This simplifies theory and anaylsis; (ii) choosing Fe allows 57Fe Mössbauer spectroscopy to be used as an additional technique which can give information about oxidation levels and spin states, local moments at the iron nuclei and spin-relaxation and, more importantly, about the anisotropy not only of the studied isotope, but also of elements interacting with this isotope; (iii) isostructural analogues with all the available (i. e. not Pm) 4 f ions can be synthesised, enabling a systematic survey of the influence of the 4 f ion on the electronic structure; (iv) this cluster type is obtained by reacting [FeIII3O(O2CR)6(L)3](X) (X=anion, L=solvent such as H2O, py) with an ethanolamine-based ligand L′ and lanthanide salts. This allows to study analogues of [FeIII2Ln2(μ3-OH)2(L′)2(O2CR)6] using the appropriate iron trinuclear starting materials. (v) the organic main ligand can be readily functionalised, facilitating a systematic investigation of the effect of organic substituents on the ligands on the magnetic properties of the complexes. We describe and discuss 34 {MIII2Ln2} (M=Fe or in one case Al) butterfly compounds which have been reported up to 2020. The analysis of these gives perspectives for designing new SMM systems with specific electronic and magnetic signatures 相似文献
999.
实验以潮州工夫茶文化为背景,在工夫茶传统冲泡工艺的基础上,采用茶汤抗氧化活性为评判指标,探讨工夫茶冲泡工艺的优化条件.实验内容包括文献调研、实验方案设计、实验操作、数据处理及小论文撰写等一系列学习任务.实践教学结果表明,将传统茶文化融入实验教学中,易于激发学生的学习兴趣,传递文化基因;引导学生从文化生活源头提出问题,运用科学方法分析问题、解决问题,利于学生熟悉科学过程,养成正确的科学思维习惯;同时,实践活动中学生会触及到多个学科领域、多重实验操作技能训练,可以全面提升学生的综合素养,达成课程育人目标. 相似文献
1000.
A new asymmetric Salamo‐based ligand H2L was synthesized using 3‐tert‐butyl‐salicylaldehyde and 6‐methoxy‐2‐[O‐(1‐ethyloxyamide)]‐oxime‐1‐phenol. By adjusting the ratio of the ligand H2L and Cu (II), Co (II), and Ni (II) ions, mononuclear, dinuclear, and trinuclear transition metal (II) complexes, [Cu(L)], [{Co(L)}2], and [{Ni(L)(CH3COO)(CH3CH2OH)}2Ni] with the ligand H2L possessing completely different coordination modes were obtained, respectively. The optical spectra of ligand H2L and its Cu (II), Co (II) and Ni (II) complexes were investigated. The Cu (II) complex is a mononuclear structure, and the Cu (II) atom is tetracoordinated to form a planar quadrilateral structure. The Co (II) complex is dinuclear, and the two Co (II) atoms are pentacoordinated and have coordination geometries of distorted triangular bipyramid. The Ni (II) complex is a trinuclear structure, and the terminal and central Ni (II) atoms are all hexacoordinated, forming distorted octahedral geometries. Furthermore, optical properties including UV–Vis, IR, and fluorescence of the Cu (II), Co (II), and Ni (II) complexes were investigated. Finally, the antibacterial activities of the Cu (II), Co (II), and Ni (II) complexes were explored. According to the experimental results, the inhibitory effect was found to be enhanced with increasing concentrations of the Cu (II), Co (II), and Ni (II) complexes. 相似文献