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991.
Tianjiao Qiao Yicheng Wang Sujuan Zheng Huiying Kang Guangxin Liang 《Angewandte Chemie (International ed. in English)》2020,59(33):14111-14114
The first total syntheses of three unusual norrisolide‐type rearranged spongian diterpenes, cheloviolene C, seconorrisolide B, and seconorrisolide C, have been accomplished via a common intermediate through late‐stage ring‐scissoring. The synthesis features a Wolff ring contraction for the synthesis of the trans‐hydrindane system, and a crucial retro Diels–Alder reaction/intramolecular ene cyclization for the rapid stereoselective construction of the furo[2,3‐b]furan system, which is commonly seen in rearranged spongian diterpenes. 相似文献
992.
Biwei Xiao Hanshuo Liu Ning Chen Mohammad Norouzi Banis Haijun Yu Jianwen Liang Qian Sun Tsun‐Kong Sham Ruying Li Mei Cai Gianluigi A. Botton Xueliang Sun 《Angewandte Chemie (International ed. in English)》2020,59(34):14313-14320
Li‐ and Mn‐rich layered oxides are among the most promising cathode materials for Li‐ion batteries with high theoretical energy density. Its practical application is, however, hampered by the capacity and voltage fade after long cycling. Herein, a finite difference method for near‐edge structure (FDMNES) code was combined with in situ X‐ray absorption spectroscopy (XAS) and transmission electron microscopy/electron energy loss spectroscopy (TEM/EELS) to investigate the evolution of transition metals (TMs) in fresh and heavily cycled electrodes. Theoretical modeling reveals a recurring partially reversible LiMn2O4‐like sub‐nanodomain formation/dissolution process during each charge/discharge, which accumulates gradually and accounts for the Mn phase transition. From the modeling of spectra and maps of the valence state over large regions of the cathodes, it was found that the phase change is size‐dependent. After prolonged cycling, the TMs displayed different levels of inactivity. 相似文献
993.
Qun‐Liang Zhang Qin Xiong Miao‐Miao Li Wei Xiong Bin Shi Yu Lan Liang‐Qiu Lu Wen‐Jing Xiao 《Angewandte Chemie (International ed. in English)》2020,59(33):14096-14100
Higher‐order cycloadditions, particularly [8+2] cycloadditions, are a straightforward and efficient strategy for constructing significant medium‐sized architectures. Typically, configuration‐restrained conjugated systems are utilized as 8π‐components for higher‐order concerted cycloadditions. However, for this reason, 10‐membered monocyclic skeletons have never been constructed via catalytic asymmetric [8+2] cycloaddition with high peri‐ and stereoselectivity. Here, we accomplished an enantioselective [8+2] dipolar cycloaddition via the merger of visible‐light activation and asymmetric palladium catalysis. This protocol provides a new route to 10‐membered monocyclic architectures bearing chiral quaternary stereocenters with high chemo‐, peri‐, and enantioselectivity. The success of this strategy relied on the facile in situ generation of Pd‐containing 1,8‐dipoles and their enantioselective trapping by ketene dipolarophiles, which were formed in situ via a photo‐Wolff rearrangement. 相似文献
994.
Lin Yu Leiyang Lv Zihang Qiu Zhangpei Chen Ze Tan Yu‐Feng Liang Chao‐Jun Li 《Angewandte Chemie (International ed. in English)》2020,59(33):14009-14013
We have developed an unprecedented Pd‐catalyzed formal hydroalkylation of alkynes with hydrazones, which are generated in situ from naturally abundant aldehydes, as both alkylation reagents and hydrogen donors. The hydroalkylation proceeds with high regio‐ and stereoselectivity to form (Z)‐alkenes, which are more difficult to generate compared to (E)‐alkenes. The reaction is compatible with a wide range of functional groups, including hydroxy, ester, ketone, nitrile, boronic ester, amine, and halide groups. Furthermore, late‐stage modifications of natural products and pharmaceutical derivatives exemplify its unique chemoselectivity, regioselectivity, and synthetic applicability. Mechanistic studies indicate the possible involvement of Pd‐hydride intermediates. 相似文献
995.
Hai‐Dong Xia Zhong‐Liang Li Qiang‐Shuai Gu Xiao‐Yang Dong Jia‐Heng Fang Xuan‐Yi Du Li‐Lei Wang Xin‐Yuan Liu 《Angewandte Chemie (International ed. in English)》2020,59(39):16926-16932
We describe a photoinduced copper‐catalyzed asymmetric radical decarboxylative alkynylation of bench‐stable N‐hydroxyphthalimide(NHP)‐type esters of racemic alkyl carboxylic acids with terminal alkynes, which provides a flexible platform for the construction of chiral C(sp3)?C(sp) bonds. Critical to the success of this process are not only the use of the copper catalyst as a dual photo‐ and cross‐coupling catalyst but also tuning of the NHP‐type esters to inhibit the facile homodimerization of the alkyl radical and terminal alkyne, respectively. Owing to the use of stable and easily available NHP‐type esters, the reaction features a broader substrate scope compared with reactions using the alkyl halide counterparts, covering (hetero)benzyl‐, allyl‐, and aminocarbonyl‐substituted carboxylic acid derivatives, and (hetero)aryl and alkyl as well as silyl alkynes, thus providing a vital complementary approach to the previously reported method. 相似文献
996.
Kai Wu Liang‐Liang Wu Cong‐Ying Zhou Chi‐Ming Che 《Angewandte Chemie (International ed. in English)》2020,59(37):16202-16208
A transition‐metal‐free C(sp2)?C(sp2) bond formation reaction by the cross‐coupling of diazo quinones with catechol boronic esters was developed. With this protocol, a variety of biaryls and alkenyl phenols were obtained in good to high yields under mild conditions. The reaction tolerates various functionalities and is applicable to the derivatization of pharmaceuticals and natural products. The synthetic utility of the method was demonstrated by the short synthesis of multi‐substituted triphenylenes and three bioactive natural products, honokiol, moracin M, and stemofuran A. Mechanistic studies and density functional theory (DFT) calculations revealed that the reaction involves attack of the boronic ester by a singlet quinone carbene followed by a 1,2‐rearrangement through a stepwise mechanism. 相似文献
997.
Shan-Shan Guo Xue Pang Yang Wang Zhu-Feng Geng Ju-Qin Cao Jun-Yu Liang 《Natural product research》2020,34(18):2595-2601
AbstractOne new sesquiterpene (α-iso-cubebenol acetate, 8), together with 9 known compounds (1-7, 9, 10) were isolated from the stems of Schisandra chinensis (Turcz.) Baill. by repeated silica gel column chromatography. Based on the results of MS, NMR spectra and comparing with literature data, the six dibenzocyclooctadiene lignans were identified as schizandrin A to C (1-3), schizandrin (4), schisantherin A (5) and gomisin J (6), the two sesquiterpenes were identified as α-iso-cubebenol (7) and α-iso-cubebenol acetate (8), while the two triterpenic acids were identified as ganwuweizic acid (9) and kadsuric acid (10). The antifeedant activity of the 10 compounds against Tribolium castaneum adults was tested. Gomisin J (6) exhibited activity at 1500?ppm concentration with 40.3% antifeeding index percentages. As for the dibenzocyclooctene lignans (compounds 1–3, 6), the number of methylenedioxies and the position of hydroxyl groups were the main factors to affect their antifeedant activities. 相似文献
998.
Fang Yuanxing Zheng Yun Fang Tao Chen Yong Zhu Yaodong Liang Qing Sheng Hua Li Zhaosheng Chen Chuncheng Wang Xinchen 《中国科学:化学(英文版)》2020,63(2):149-181
Photocatalysis,which is the catalyzation of redox reactions via the use of energy obtained from light sources,is a topic that has garnered a lot of attention in recent years as a means of addressing the environmental and economic issues plaguing society today.Of particular interest are photosynthesis can potentially mimic a variety of vital reactions,many of which hold the key to develop sustainable energy economy.In light of this,many of the technological and procedural advancements that have recently occurred in the field are discussed in this review,namely those linked to:(1)photocatalysts made from metal oxides,nitride,and sulfides;(2)photocatalysis via polymeric carbon nitride(PCN);and(3)general advances and mechanistic insights related to TiO2-based catalysts.The challenges and opportunities that have arisen over the past few years are discussed in detail.Basic concepts and experimental procedures which could be useful for eventually overcoming the problems associated with photocatalysis are presented herein. 相似文献
999.
Guozhen Liu Long Cheng Guining Chen Feng Liang Gongping Liu Wanqin Jin 《化学:亚洲杂志》2020,15(15):2364-2370
Mixed matrix membranes (MMMs) made from inorganic fillers and polymers is a kind of promising candidate for gas separation. In this work, two‐dimensional MXene nanosheets were synthesized and incorporated into a polyether‐polyamide block copolymer (Pebax) matrix to fabricate MMM for CO2 capture. The physicochemical properties of MXene nanosheets and MXene/Pebax membranes were studied systematically. The introduction of MXene nanosheets provided additional molecular transport channels and meanwhile enhanced the CO2 adsorption capacity, thereby enhancing both the CO2 peremance and CO2/N2 selectivity of Pebax membrane. The optimized MXene/Pebax membrane with a MXene loading of 0.15 wt % displayed a high separation performance with a CO2 permeance of 21.6 GPU and a CO2/N2 selectivity of 72.5, showing potential application in CO2 capture. 相似文献
1000.
Wenxin Xing Liang Zhou Bin Chen Juying Lei Lingzhi Wang Jinlong Zhang 《化学:亚洲杂志》2020,15(17):2749-2753
It's highly significant to develop a novel catalyst, which can be active at a wide range of pH, for an effective photo‐Fenton reaction. In this work, α‐FeOOH?MoO3 nanorod was prepared by a one‐step hydrothermal method and applied in photo‐Fenton degradation of organic pollutants. Benefit from the electron migration mechanism of Z‐scheme and excellent photoelectric performance, the catalyst exhibited superior photo‐Fenton activity in degradation of organic pollutants. In addition, the catalyst holds good stability after 5 recycles. These results demonstrated that this catalyst has wide application prospect in organic wastewater treatment. 相似文献