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91.
Dr. Song Song Vincent Fung Kin Yuen Dr. Lu Di Dr. Qiming Sun Prof. Dr. Kang Zhou Prof. Dr. Ning Yan 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(45):20018-20022
Production of renewable, high-value N-containing chemicals from lignocellulose will expand product diversity and increase the economic competitiveness of the biorefinery. Herein, we report a single-step conversion of furfural to pyrrole in 75 % yield as a key N-containing building block, achieved via tandem decarbonylation–amination reactions over tailor-designed Pd@S-1 and H-beta zeolite catalytic system. Pyrrole was further transformed into dl -proline in two steps following carboxylation with CO2 and hydrogenation over Rh/C catalyst. After treating with Escherichia coli, valuable d -proline was obtained in theoretically maximum yield (50 %) bearing 99 % ee. The report here establishes a route bridging commercial commodity feedstock from biomass with high-value organonitrogen chemicals through pyrrole as a hub molecule. 相似文献
92.
Dr. Haoxuan Li Haifei Wen Dr. Zhijun Zhang Dr. Nan Song Prof. Ryan T. K. Kwok Prof. Jacky W. Y. Lam Prof. Lei Wang Prof. Dong Wang Prof. Ben Zhong Tang 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(46):20551-20555
Using reverse thinking of the aggregation-induced emission (AIE) principle, we demonstrate an ingenious and universal protocol for amplifying molecular motions to boost photothermal efficiency of fibers. Core–shell nanofibers having the olive oil solution of AIE-active molecules as the core surrounded by PVDF-HFP shell were constructed by coaxial electrospinning. The molecularly dissolved state of AIE-active molecules allows them to freely rotate and/or vibrate in nanofibers upon photoexcitation and thus significantly elevates the proportion of non-radiative energy dissipation, affording impressive heat-generating efficiency. Photothermal evaluation shows that the core–shell nanofibers with excellent durability can reach up to 22.36 % of photothermal conversion efficiency, which is 26-fold as the non-core–shell counterpart. Such a core–shell fiber can be used for photothermal textiles and solar steam generation induced by natural sunlight with green and carbon-zero emission. 相似文献
93.
Jin Xie Yun-Wei Song Dr. Bo-Quan Li Dr. Hong-Jie Peng Prof. Jia-Qi Huang Prof. Qiang Zhang 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(49):22334-22339
Polysulfide intermediates (PSs), the liquid-phase species of active materials in lithium–sulfur (Li-S) batteries, connect the electrochemical reactions between insulative solid sulfur and lithium sulfide and are key to full exertion of the high-energy-density Li-S system. Herein, the concept of sulfur container additives is proposed for the direct modification on the PSs species. By reversible storage and release of the sulfur species, the container molecule converts small PSs into large organosulfur species. The prototype di(tri)sulfide-polyethylene glycol sulfur container is highly efficient in the reversible PS transformation to multiply affect electrochemical behaviors of sulfur cathodes in terms of liquid-species clustering, reaction kinetics, and solid deposition. The stability and capacity of Li-S cells was thereby enhanced. The sulfur container is a strategy to directly modify PSs, enlightening the precise regulation on Li-S batteries and multi-phase electrochemical systems. 相似文献
94.
Xinfeng Zhu Yanli Mao Hongpan Liu Haiyan Kang Biao Liu Zhongxian Song Xueping Liu Yifei Guo Huixian Du Qiulin Zhang 《应用有机金属化学》2020,34(2):e5285
FeOx, TiO2, and Fe–Ti–Ox catalysts were synthesized and used in the catalytic hydrolysis of hydrogen cyanide (HCN). Nearly 100% HCN conversion was achieved at 250 °C over the Fe–Ti–Ox catalyst. TiO2 rutile was detected over TiO2, but not over Fe–Ti–Ox, which suggested that the interaction between Fe and Ti species could inhibit the TiO2 phase transition. Furthermore, the interaction between Fe and Ti species over Fe–Ti–Ox could promote the selectivity of NH3 and CO. The mechanism of hydrolysis of HCN over FeOx, TiO2, and Fe–Ti–Ox can be given as follows: HCN + H2O → methanamide → ammonium formate → formic acid → H2O + CO. 相似文献
95.
Zhongxian Song Yun Xing Tingji Zhang Jinggang Zhao Junkai Wang Yanli Mao Baolin Zhao Xuejun Zhang Min Zhao Ziang Ma 《应用有机金属化学》2020,34(3):e5446
A series of Ce-Fe-Ox catalysts prepared by the different calcination temperatures (marked as CF-X, where X represented calcination temperature) were used to the selectivity catalytic reduction of NOx by NH3. The results explained the relationship between calcination temperature and the sulfate species over Ce-Fe-Ox, and then investigated the surface acidity and catalytic performance. The large amounts of sulfate species were formed over CF-450 and CF-550 while it was decomposed with further the increasing of calcination temperature, which resulted in the loss of surface acidity, causing a decrease in the catalytic activity over Ce-Fe-Ox. Thereby, the CF-450 catalyst showed the best catalytic activity and over 90% NOx conversion was obtained at 244–450 °C. Besides, the favored pore structure, more Fe3+ active species, higher Ce3+ concentration and the abundance of chemical adsorbed oxygen species, as well as the surface acid sites, would together contribute to the excellent catalytic activity of CF-450 catalyst. 相似文献
96.
Dan-Dan Wang Li Song You-Yu Wang Jia-Yu Guo Hang-Yan Shen Xiao-Rong Wang Wen-Xiang Chai 《应用有机金属化学》2020,34(4):e5561
Four new heteroleptic [Cu(NN)P2]+-type cuprous complexes— 1 -TPP, 2 -POP, 3 -Xantphos, and 4 -DPPF—were designed and synthesized using a diimine ligand 2-(2′-pyridyl)benzoxazole (2-PBO) and different phosphine ligands (TPP, triphenylphosphine; POP, bis[2-(diphenylphosphino)phenyl]ether; Xantphos, 4,5-bis(diphenylphosphino)-9,9-dimethylxanthene; DPPF, 1,1′-bis(diphenylphosphino)-ferrocene). All complexes were characterized using single-crystal X-ray diffraction, spectroscopic analysis (infrared, UV–Vis.), elemental analysis, and photoluminescence (PL). Single-crystal X-ray diffraction revealed complexes 1 – 4 as isolated cation complex structures with a tetrahedral CuN2P2 coordination geometry and diverse P–Cu–P angles. Their UV–Vis. absorption spectra exhibited a blue-shift sequence in wavelength with an enlarged P–Cu–P angle from 4 to 2 then to 3 and then to 1 . The PL emission peaks of 1 – 3 also exhibited a similar blue-shift sequence ( 2 → 3 → 1 ). Their PL lifetime in microseconds (~7.5, 5.1, and 4.7 μs for 1 , 2 , and 3 , respectively) indicated that their PL behavior represents phosphorescence. Time-dependent density functional theory (TD-DFT) calculation and wavefunction analysis revealed that S1 and T1 states of 1 – 3 should be assigned as metal–ligand and ligand–ligand charge-transfer (ML + L'L)CT states. Their UV–Vis. absorption and phosphorescence should be attributed to the charge transfer from the P–Cu–P segment to the 2-PBO ligand. Therefore, as the P–Cu–P angle increased (lower HOMO), the energy of S1 and T1 states also increased, following the change of PL color. 相似文献
97.
Yi-Ying Lin Bao-Dong Song Xiang-Ming Wang Cong-Cong Zhang Xiao-Cong Zhang Shi-Wei Sun Song-Hai Wu Hai-Tao Ren Shao-Yi Jia Yong Liu Xu Han 《应用有机金属化学》2020,34(9):e5735
Pyrite catalyzes oxidation of various organic contaminants by dissolved oxygen (DO) under acidic conditions; however, the catalytic mechanism under alkaline conditions is still not clear. In this study, we observe increased oxidation rates of aniline with increasing pHs (7.0–11.0). Electron paramagnetic resonance (EPR) analysis and quenching experiments rule out contributions of •OH, O2•−, 1O2 and Fe (IV) to aniline oxidation and suggest that the Fe (III)–OOH peroxo and/or H2O2 are the primary oxidative species in the oxidation of aniline at pH 11.0. In addition, 200 mg L−1 H2O2 does not apparently increase the oxidation rate of aniline, which also rules out the predominant contribution of the produced H2O2 to aniline oxidation. We therefore suggest that the Fe (III)–OOH peroxo is indeed the primary oxidative species in the pyrite–DO system under alkaline conditions. Analyses of solid total organic carbon (TOC), gas chromatography–mass spectrometry and Fourier-transform infrared spectroscopy further reveal that more than 83.3% aniline has been polymerized to polyaniline, instead of being mineralized into CO2 and H2O, indicating that H-abstraction from aniline by the Fe (III)–OOH peroxo is an important step in the oxidation of aniline under alkaline conditions. This study provides new insight into the oxidative species in the pyrite–DO system, and opens a new door for organic degradations under alkaline conditions. 相似文献
98.
99.
Jing Zhao Yanan Zhu Xuehong Song Yuanyuan Xiao Guowei Su Xinyue Liu Zhangjie Wang Yongmei Xu Jian Liu David Eliezer Trudy F. Ramlall Guy Lippens James Gibson Fuming Zhang Robert J. Linhardt Lianchun Wang Chunyu Wang 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(5):1834-1843
Prion-like transcellular spreading of tau in Alzheimer's Disease (AD) is mediated by tau binding to cell surface heparan sulfate (HS). However, the structural determinants for tau–HS interaction are not well understood. Microarray and SPR assays of structurally defined HS oligosaccharides show that a rare 3-O-sulfation (3-O-S) of HS significantly enhances tau binding. In Hs3st1−/− (HS 3-O-sulfotransferase-1 knockout) cells, reduced 3-O-S levels of HS diminished both cell surface binding and internalization of tau. In a cell culture, the addition of a 3-O-S HS 12-mer reduced both tau cell surface binding and cellular uptake. NMR titrations mapped 3-O-S binding sites to the microtubule binding repeat 2 (R2) and proline-rich region 2 (PRR2) of tau. Tau is only the seventh protein currently known to recognize HS 3-O-sulfation. Our work demonstrates that this rare 3-O-sulfation enhances tau–HS binding and likely the transcellular spread of tau, providing a novel target for disease-modifying treatment of AD and other tauopathies. 相似文献
100.
Takumi Watanabe Yuichiro Nishizawa Haruka Minato Dr. Chihong Song Prof. Dr. Kazuyoshi Murata Prof. Dr. Daisuke Suzuki 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(23):8934-8938
The three-dimensional structure of nanocomposite microgels was precisely determined by cryo-electron micrography. Several nanocomposite microgels that differ with respect to their nanocomposite structure, which were obtained from seeded emulsion polymerization in the presence of microgels, were used as model nanocomposite materials for cryo-electron micrography. The obtained three-dimensional segmentation images of these nanocomposite microgels provide important insights into the interactions between the hydrophobic monomers and the microgels, that is, hydrophobic styrene monomers recognize molecular-scale differences in polarity within the microgels during the emulsion polymerization. This result led to the formation of unprecedented multi-layered nanocomposite microgels, which promise substantial potential in colloidal applications. 相似文献