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21.
Enhanced Catalytic Activity in Liquid‐Exfoliated FeOCl Nanosheets as a Fenton‐Like Catalyst 下载免费PDF全文
Jian Zhang Prof. Xiu‐Ling Jiao Dr. Yu‐Guo Xia Fang‐Fang Liu Ying‐Ping Pang Xin‐Fu Zhao Prof. Dai‐Rong Chen 《Chemistry (Weinheim an der Bergstrasse, Germany)》2016,22(27):9321-9329
A facile liquid‐phase exfoliation method to prepare few‐layer FeOCl nanosheets in acetonitrile by ultrasonication is reported. The detailed exfoliation mechanism and generated products were investigated by combining first‐principle calculations and experimental approaches. The similar cleavage energies of FeOCl (340 mJ m?2) and graphite (320 mJ m?2) confirm the experimental exfoliation feasibility. As a Fenton reagent, FeOCl nanosheets showed outstanding properties in the catalytic degradation of phenol in water at room temperature, under neutral pH conditions, and with sunlight irradiation. Apart from the increased surface area of the nanosheets, the surface state change of the nanosheets also plays a key role in improving the catalytic performance. The changes of charge density, density of states (DOS), and valence state of Fe atoms in the exfoliated FeOCl nanosheets versus plates illustrated that surface atomistic relationships made the few‐layer nanosheets higher activity, indicating the exfoliation process of the FeOCl nanosheets also brought about surface state changes. 相似文献
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Mono‐ and Dinuclear Phosphorescent Rhenium(I) Complexes: Impact of Subcellular Localization on Anticancer Mechanisms 下载免费PDF全文
Rui‐Rong Ye Dr. Cai‐Ping Tan Mu‐He Chen Liang Hao Prof. Liang‐Nian Ji Prof. Zong‐Wan Mao 《Chemistry (Weinheim an der Bergstrasse, Germany)》2016,22(23):7800-7809
Elucidation of relationship among chemical structure, cellular uptake, localization, and biological activity of anticancer metal complexes is important for the understanding of their mechanisms of action. Organometallic rhenium(I) tricarbonyl compounds have emerged as potential multifunctional anticancer drug candidates that can integrate therapeutic and imaging capabilities in a single molecule. Herein, two mononuclear phosphorescent rhenium(I) complexes ( Re1 and Re2 ), along with their corresponding dinuclear complexes ( Re3 and Re4 ), were designed and synthesized as potent anticancer agents. The subcellular accumulation of Re1–Re4 was conveniently analyzed by confocal microscopy in situ in live cells by utilizing their intrinsic phosphorescence. We found that increased lipophilicity of the bidentate ligands could enhance their cellular uptake, leading to improved anticancer efficacy. The dinuclear complexes were more potent than the mononuclear counterparts. The molecular anticancer mechanisms of action evoked by Re3 and Re4 were explored in detail. Re3 with a lower lipophilicity localizes to lysosomes and induces caspase‐independent apoptosis, whereas Re4 with higher lipophilicity specially accumulates in mitochondria and induces caspase‐independent paraptosis in cancer cells. Our study demonstrates that subcellular localization is crucial for the anticancer mechanisms of these phosphorescent rhenium(I) complexes. 相似文献
24.
Copper‐Catalyzed Difunctionalization of Activated Alkynes by Radical Oxidation–Tandem Cyclization/Dearomatization to Synthesize 3‐Trifluoromethyl Spiro[4.5]trienones 下载免费PDF全文
Dr. Hui‐Liang Hua Yu‐Tao He Yi‐Feng Qiu Ying‐Xiu Li Bo Song Pin Gao Xian‐Rong Song Dong‐Hui Guo Prof. Dr. Xue‐Yuan Liu Prof. Dr. Yong‐Min Liang 《Chemistry (Weinheim an der Bergstrasse, Germany)》2015,21(4):1468-1473
A copper‐catalyzed difunctionalizing trifluoromethylation of activated alkynes with the cheap reagent sodium trifluoromethanesulfinate (NaSO2CF3 or Langlois’ reagent) has been developed incorporating a tandem cyclization/dearomatization process. This strategy affords a straightforward route to synthesis of 3‐(trifluoromethyl)‐spiro[4.5]trienones, and presents an example of difunctionalization of alkynes for simultaneous formation of two carbon–carbon single bonds and one carbon–oxygen double bond. 相似文献
25.
Fangping Zhou Zhao Zhao Ming Xu Prof. Ting Wang Huiru Yang Rong Wang Jiahui Wang Prof. Haibo Li Prof. Ming Feng 《Chemistry (Weinheim an der Bergstrasse, Germany)》2022,28(14):e202104157
Perovskite is a promising non-noble catalyst and has been widely investigated for the electrochemical oxygen evolution reaction (OER). However, there is still serious lack of valid approaches to further enhance their catalytic performance. Herein, we propose a spin state modulation strategy to improve the OER electrocatalytic activity of typical perovskite material of LaCoO3. Specifically, the electronic configuration transition was realized by a simple high temperature thermal reduction process. M-H hysteresis loop results reveal that the reduction treatment can produce more unpaired electrons in 3d orbit by promoting the electron transitions of Co from low spin state to high spin state, and thus lead to the increase of the spin polarization. Electrochemical measurements show that the catalytic performance of LaCoO3 is strongly dependent on its electronic configuration. With the optimized reduction treatment, the overpotential for the OER process in 0.5 M KOH electrolyte solution at 10 mA cm−2 current density was 396 mV, significantly lower than that of the original state. Furthermore, it can mediate efficient OER with an overpotential of 383 mV under an external magnetic field, which is attributed to the appropriate electron filling. Our results show that electron spin state regulation is a new way to boost the OER electrocatalytic activity. 相似文献
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A comprehensive study on the efficient one‐pot synthesis of polyhedral octaphenylsilsesquioxane (OPS) is reported via the hydrolytic condensation of phenyltrimethoxysilane (PTMS) in the presence of basic catalyst to investigate the specific synthesis mechanism. The synthetic reactions are monitored with real time infrared (RTIR) spectroscopy. Then RTIR coupled with 29Si nuclear magnetic resonance spectroscopy (NMR) and matrix‐assisted laser desorption/ionization time of flight mass spectrometry (MALDI‐TOF‐MS) are used to monitor the reactions and identify the intermediary species during the reaction. The rapid hydrolysis of PTMS is detected by RTIR. Contrary to previous reports, the ladder‐like structured species are identified as intermediates during the reaction process. It is suggested that formation of caged T8 OPS is realized through the chain break and rearrangement of the ladder‐like phenyltrimethoxysilanes. Accordingly, a scheme from hydrolysis of the PTMS to formation of the OPS is provided. 相似文献
29.
Characteristics of uranium sorption on illite in a ternary system: effect of phosphate on adsorption
Liao Rong Shi Zeming Chen Yuejiao Zhang Junji Wang Xinyu Hou Yun Zhang Kailiang 《Journal of Radioanalytical and Nuclear Chemistry》2020,324(1):159-167
Journal of Radioanalytical and Nuclear Chemistry - Na, Mg, Al and Cl in Roman glasses and pottery were analyzed by PIGE with 2.5 MeV protons and 2.0 MeV deuteron activation... 相似文献
30.
Jianxin Guan Rong Wei Antonio Prlj Jie Peng Kun-Han Lin Jitian Liu Han Han Prof. Clémence Corminboeuf Prof. Dahui Zhao Prof. Zhihao Yu Prof. Junrong Zheng 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(35):15013-15019
The mechanism of aggregation-induced emission, which overcomes the common aggregation-caused quenching problem in organic optoelectronics, is revealed by monitoring the real time structural evolution and dynamics of electronic excited state with frequency and polarization resolved ultrafast UV/IR spectroscopy and theoretical calculations. The formation of Woodward–Hoffmann cyclic intermediates upon ultraviolet excitation is observed in dilute solutions of tetraphenylethylene and its derivatives but not in their respective solid. The ultrafast cyclization provides an efficient nonradiative relaxation pathway through crossing a conical intersection. Without such a reaction mechanism, the electronic excitation is preserved in the molecular solids and the molecule fluoresces efficiently, aided by the very slow intermolecular charge and energy transfers due to the well separated molecular packing arrangement. The mechanisms can be general for tuning the properties of chromophores in different phases for various important applications. 相似文献