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101.
Ning-Fang Li Jiuyang Ji Wei Jiang Jia-Peng Cao Ye-Min Han Peng Yuan Yan Xu 《无机化学与普通化学杂志》2020,646(10):463-468
The usage of the achiral ligand, in lanthanide chemistry, successfully obtained two series of chiral lanthanide complexes, formulated d - and l -{Gd[IN][HIN][CH2OCH2O]}n (abbreviated as Gd ) and d - and l -{Dy[IN][HIN][CH2OCH2O]}n (abbreviated as Dy , HIN = isonicotinic acid). Crystallographic researches determined that four compounds are all one-dimensional (1D) chain structures and crystallized in a chiral space group. In addition, CH2OHCH2OH acts as not only solvent but also the bridge ligand. Besides, single crystal circular dichroism (CD) spectra conformed compounds Gd-L and Gd-D , Dy-L and Dy-D are enantiomers respectively. Magnetically, compound Gd showed predominant magnetocaloric effect (MCE) of 26.20 J · kg–1 · K–1 at 2.5 K for ΔH = 7 T, while there is ferromagnetic interactions in compound Dy . 相似文献
102.
103.
Dr. Feifan Wang Jie Tian Dr. Mengzhu Li Dr. Weizhen Li Dr. Lifang Chen Xiaozhi Liu Dr. Jian Li Aidaer Muhetaer Prof. Dr. Qi Li Prof. Dr. Yuan Wang Prof. Dr. Lin Gu Prof. Dr. Ding Ma Prof. Dr. Dongsheng Xu 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(21):8280-8286
Fully utilizing solar energy for catalysis requires the integration of conversion mechanisms and therefore delicate design of catalyst structures and active species. Herein, a MOF crystal engineering method was developed to controllably synthesize a copper–ceria catalyst with well-dispersed photoactive Cu-[O]-Ce species. Using the preferential oxidation of CO as a model reaction, the catalyst showed remarkably efficient and stable photoactivated catalysis, which found practical application in feed gas treatment for fuel cell gas supply. The coexistence of photochemistry and thermochemistry effects contributes to the high efficiency. Our results demonstrate a catalyst design approach with atomic or molecular precision and a combinatorial photoactivation strategy for solar energy conversion. 相似文献
104.
Dr. Yuan Liu Dr. Jin-Cheng Liu Teng-Hao Li Zeng-Hui Duan Dr. Tian-Yu Zhang Ming Yan Dr. Wan-Lu Li Prof. Dr. Hai Xiao Prof. Dr. Yang-Gang Wang Prof. Dr. Chun-Ran Chang Prof. Dr. Jun Li 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(42):18745-18749
The direct, nonoxidative conversion of methane on a silica-confined single-atom iron catalyst is a landmark discovery in catalysis, but the proposed gas-phase reaction mechanism is still open to discussion. Here, we report a surface reaction mechanism by computational modeling and simulations. The activation of methane occurs at the single iron site, whereas the dissociated methyl disfavors desorption into gas phase under the reactive conditions. In contrast, the dissociated methyl prefers transferring to adjacent carbon sites of the active center (Fe1©SiC2), followed by C−C coupling and hydrogen transfer to produce the main product (ethylene) via a key −CH−CH2 intermediate. We find a quasi Mars–van Krevelen (quasi-MvK) surface reaction mechanism involving extracting and refilling the surface carbon atoms for the nonoxidative conversion of methane on Fe1©SiO2 and this surface process is identified to be more plausible than the alternative gas-phase reaction mechanism. 相似文献
105.
It has been two months since a boom of online education triggered by the epidemic in China. At present, we are keeping focus on how to optimize our online class. In the case of chemistry laboratory courses, there's not much that can be done to experimental operations through online teaching. While for the traditional teaching procedure, there is still room for improvement in terms of integrating research to teaching, interactivity, etc. This paper will present some design strategies for improving teaching the organic chemistry laboratory online. To be specific, it describes how teaching materials like the lesson plan and virtual lab were coordinated into the online teaching. And we will also discuss the holistic approach to a better outcome for students' active learning and integration research into teaching by redesigning multiple phases, such as the pre-laboratory preparation, live online class, experimental operations. 相似文献
106.
Chunyu Qiu Suqi He Dr. Yuan Wang Prof. Qingxiang Wang Prof. Chuan Zhao 《Chemistry (Weinheim an der Bergstrasse, Germany)》2020,26(18):4120-4127
Interface engineering has been applied as an effective strategy to boost the electrocatalytic performance because of the strong coupling and synergistic effects between individual components. Here, we engineered vertically aligned FeOOH/CoO nanoneedle array with a synergistic interface between FeOOH and CoO on Ni foam (NF) by a simple impregnation method. The synthesized FeOOH/CoO exhibits outstanding electrocatalytic activity and stability for both hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) in an alkaline medium. For the overall water splitting, the bifunctional FeOOH/CoO nanoneedle catalyst requires only a cell voltage of 1.58 V to achieve a current density of 10 mA cm−2, which is much lower than that required for IrO2//Pt/C (1.68 V). The FeOOH/CoO catalyst has been successfully applied for solar cell-driven water electrolysis, revealing its great potential for commercial hydrogen production and solar energy storage. 相似文献
107.
Jin Yuan Ling Wang Yitong Wang Prof. Dr. Jingcheng Hao 《Chemistry (Weinheim an der Bergstrasse, Germany)》2020,26(16):3545-3554
Copper nanoclusters (CuNCs) as a new class of fluorescent materials have attracted a great deal of interest due to their outstanding fluorescence properties. In this work, a variety of organic solvents were used to induce self-assembly of glutathione-capped CuNCs (GSH-CuNCs) to form ordered assemblies with enhanced fluorescence properties. Assemblies with multicolor fluorescence emission were constructed on the basis of the aggregation-induced emission (AIE) of GSH-CuNCs and the solvent effect. The fluorescence emission from these GSH-CuNCs assemblies can also be tuned from yellow to purple by changing the organic solvent. A possible mechanism based on the size of the assemblies and electron transfer was explored to explain the solvent effects on GSH-CuNCs. Stimuli-responsive nanoswitches with excellent reversibility can be controlled by changing the type of organic solvent and the ratio of the organic solvent to the aqueous solution of GSH-CuNCs. As the CuNCs assemblies exhibit strong, stable, and color-tunable fluorescence, they were employed as color-conversion materials for recognizing different organic solvents. 相似文献
108.
Dr. Karl P. J. Gustafson Arnar Guðmundsson Dr. Éva G. Bajnóczi Dr. Ning Yuan Prof. Xiaodong Zou Prof. Ingmar Persson Prof. Jan-E. Bäckvall 《Chemistry (Weinheim an der Bergstrasse, Germany)》2020,26(15):3411-3419
The activation process of a known Ru-catalyst, dicarbonyl(pentaphenylcyclopentadienyl)ruthenium chloride, has been studied in detail using time resolved in situ X-ray absorption spectroscopy. The data provide bond lengths of the species involved in the process as well as information about bond formation and bond breaking. On addition of potassium tert-butoxide, the catalyst is activated and an alkoxide complex is formed. The catalyst activation proceeds via a key acyl intermediate, which gives rise to a complete structural change in the coordination environment around the Ru atom. The rate of activation for the different catalysts was found to be highly dependent on the electronic properties of the cyclopentadienyl ligand. During catalytic racemization of 1-phenylethanol a fast-dynamic equilibrium was observed. 相似文献
109.
Zemin Sun Mengwei Yuan Kefan Shi Yuhui Liu Di Wang Dr. Caiyun Nan Dr. Huifeng Li Prof. Genban Sun Prof. Xiaojing Yang 《Chemistry (Weinheim an der Bergstrasse, Germany)》2020,26(32):7244-7249
NiFe layered double hydroxides (LDHs) have been denoted as benchmark non-noble-metal electrocatalysts for the oxygen evolution reaction (OER). However, for laminates of NiFe LDHs, the edge sites are active, but the basal plane is inert, leading to underutilization as catalysts for the OER. Herein, for the first time, light and electron-deficient Li ions are intercalated into the basal plane of NiFe LDHs. The results of theoretical calculations and experiments both showed that electrons would be transferred from near Ni2+ to the surroundings of Li+, resulting in electron-deficient properties of the Ni sites, which would function as “electron-hungry” sites, to enhance surface adsorption of electron-rich oxygen-containing groups, which would enhance the effective activity for the OER. As demonstrated by the catalytic performance, the Li−NiFe LDH electrodes showed an ultralow overpotential of only 298 mV at 50 mA cm−2, which was lower than that of 347 mV for initial NiFe LDHs and lower than that of 373 mV for RuO2. Reasonable intercalation adjustment effectively activates laminated Ni2+ sites and constructs the electron-deficient structure to enhance its electrocatalytic activity, which sheds light on the functional treatment of catalytic materials. 相似文献
110.
Peng Yang Xin Peng Ze-zhou Yang Prof. Ya-qin Chai Prof. Ruo Yuan Prof. Wen-bin Liang 《Chemistry (Weinheim an der Bergstrasse, Germany)》2020,26(40):8767-8773
The evident contradiction between high local-concentration-based substrate reactivity and free-diffusion-based high reaction efficiency remains one of the important challenges in chemistry. Herein, we propose an efficient aggregation-induced synergism through the hydrophobic-driven self-assembly of amphiphilic oligonucleotides to generate high local concentration whereas retaining high reaction efficiency through hydrophobic-based aggregation, which is important for constructing efficient DNA nanomachines for ultrasensitive applications. MicroRNA-155, used as a model, triggered strand displacement amplification of the DNA monomers on the periphery of the 3D DNA nanomachine and generated an amplified fluorescent response for its sensitive assay. The local concentration of substrates was increased by a factor of at least 9.0×105 through hydrophobic-interaction-based self-assembly in comparison with the traditional homogeneous reaction system, achieving high local-concentration-based reactivity and free-diffusion-based enhanced reaction efficiency. As expected, the aggregation-induced synergism by hydrophobic-driven self-assembly of amphiphilic oligonucleotides created excellent properties to generate a 3D DNA nanomachine with potential as an assay for microRNA-155 in cells. Most importantly, this approach can be easily expanded for the bioassay of various biomarkers, such as nucleotides, proteins, and cells, offering a new avenue for simple and efficient applications in bioanalysis and clinical diagnosis. 相似文献