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991.
Yonggui Liu Dr. Guoyong Luo Dr. Xing Yang Shichun Jiang Prof. Dr. Wei Xue Prof. Dr. Yonggui Robin Chi Prof. Dr. Zhichao Jin 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(1):450-456
The aromatic nitrogen atoms of heteroarylaldehydes are activated by carbene catalysts to react with ketone electrophiles. Multi-functionalized cyclic N,O-acetal products are afforded in good to excellent yields and optical purities. Our reaction involves the formation of an unprecedented aza-fulvene-type acylazolium intermediate. A broad range of N-heteroaromatic aldehydes and electron-deficient ketone substrates works effectively in this transformation. Several of the chiral N,O-acetal products afforded through this protocol exhibit excellent antibacterial activities against Ralstonia solanacearum (Rs) and are valuable in the development of novel agrichemicals for plant protection. 相似文献
992.
Zuojie Li Yan Chen Zhifang Liu Qingpeng Wang Yanna Zhao Jinjian Wei Min Liu Zhengping Wang Dacheng Li Jun Han 《Monatshefte für Chemie / Chemical Monthly》2020,151(3):353-367
Naphthalimide has emerged as an interesting DNA intercalator and possessed attracting antitumor properties. In this context, naphthalimide group was linked to platinum(IV) core to construct a series of new mono naphthalimide platinum(IV) derivatives. The title compounds exert effective antitumor activities to the tested tumor cells lines in vitro, especially the one with propionyl chain displays comparable or even better bioactivities than platinum(II) reference drugs cisplatin and oxaliplatin. Moreover, the mono naphthalimide platinum(IV) derivative displays comparable tumor growth inhibitory competence against CT26 xenograft tumors in BALB/c mice in vivo without severe toxic effects in contrast to oxaliplatin. A dual DNA damage mechanism was proven for the title complex. Both naphthalimide ligand and the liberated platinum(II) moiety could generate DNA lesions to tumor cells synergistically and active the apoptotic pathway by up-regulating the expression of caspase 9 and caspase 3. Meanwhile, the conversion of platinum(II) drug into tetravalent form by incorporating naphthalimide moiety increases the uptake of platinum in whole cells and DNA remarkably. All these facts might be the factors for the title platinum(IV) complexes to overcome platinum(II) drug resistance. Additionally, the mono naphthalimide platinum(IV) complex could interact with human serum albumin by hydrogen bond and van der Waals force which would further influence their storage, transport and bioactivities. 相似文献
993.
Photodynamic therapy (PDT) has been received broad attentions as a cancer treatment, and fullerenes are potential photosensitizer owing to their unique electronic structures. However, fullerenes show insolubility in water for the special structure, which will induce aggregation to hinder the production of reactive oxygen species (ROS). Furthermore, the size of fullerenes is not conducive to reach the tumors through the enhanced permeability and retention (EPR) effect. Herein, a polyhydroxy fullerene-loaded metal-organic framework is designed and prepared to address the mentioned problems encountering with fullerenes as photosensitizers. The nanocomposite PHF@ZIF-8, which is synthesized by a simple one-pot method, displays great biocompatibility and outstanding photodynamic performance under the 448 nm laser irradiation. This work provides strong evidence for PHF@ZIF-8 as a promising photosensitizer candidate. 相似文献
994.
Hao Guo Lie-Wei Zhang Hao Zhou Dr. Wei Meng Dr. Yu-Fei Ao Prof. Dr. De-Xian Wang Prof. Dr. Qi-Qiang Wang 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(7):2645-2649
An artificial system of substrate-induced dimerization assembly of chiral macrocycle catalysts enables a highly cooperative hydrogen-bonding activation network for efficient enantioselective transformation. These macrocycles contain two thiourea and two chiral diamine moieties and dimerize with sulfate to form a sandwich-like assembly. The macrocycles then adopt an extended conformation and reciprocally complement the hydrogen-bonding interaction sites. Inspired by the guest-induced dynamic assembly, these macrocycles catalyze the decarboxylative Mannich reaction of cyclic aldimines containing a sulfamate heading group. The imine substrate can be activated toward nucleophilic attack of β-ketoacid by a cooperative hydrogen-bonding network enabled by sulfamate-induced dimerization assembly of the macrocycle catalysts. Highly efficient (>95 % yield in most cases) and enantioselective (up to 97.5:2.5 er) transformation of a variety of substrates using only 5 mol % macrocycle was achieved. 相似文献
995.
Dr. Xi-Sha Zhang Yan-Ying Huang Jing Zhang Dr. Wei Meng Dr. Qian Peng Ruirui Kong Zhenwei Xiao Dr. Jie Liu Miaofei Huang Dr. Yuanping Yi Liangliang Chen Qingrui Fan Dr. Gaobo Lin Dr. Zitong Liu Dr. Guanxin Zhang Dr. Lang Jiang Prof. Dr. Deqing Zhang 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(9):3557-3561
Polycyclic aromatic hydrocarbons with hexagons/pentagons or hexagons/heptagons have been intensively investigated in recent years, but those with simultaneous presence of hexagons, pentagons and heptagons remain rare. In this paper, we report dicyclohepta[ijkl,uvwx]rubicene ( DHR ), a non-benzenoid isomer of dibenzo[bc,kl]coronene with two pentagons and two heptagons. We developed an efficient and scalable synthetic method for DHR by using Scholl reaction and dehydrogenation. Crystal structure of DHR shows that the benzenoid rings, two pentagons and two heptagons are coplanar. The bond lengths analysis and the ICSS(1)zz and LOL-π calculations indicate that the incorporation of two formal azulene moieties has an effect on the conjugated structure. The π-electrons of benzenoid and pentagon rings are more delocalized. Cyclic voltammetry studies indicate that DHR shows multiple oxidation and reduction potentials. Interestingly, DHR exhibits unusual S0 to S2 absorption and abnormal anti-Kasha S2 to S0 emission. Moreover, crystals of DHR exhibit semiconducting behaviour with hole mobility up to 0.082 cm2 V−1 s−1. 相似文献
996.
Dr. Ying Huang Prof. Bo Chen Jian Duan Fei Yang Tengrui Wang Zhengfeng Wang Dr. Wenjuan Yang Dr. Chenchen Hu Prof. Wei Luo Prof. Yunhui Huang 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(9):3728-3733
Solid-state Li metal batteries (SSLMBs) have attracted considerable interests due to their promising energy density as well as high safety. However, the realization of a well-matched Li metal/solid-state electrolyte (SSE) interface remains challenging. Herein, we report g-C3N4 as a new interface enabler. We discover that introducing g-C3N4 into Li metal can not only convert the Li metal/garnet-type SSE interface from point contact to intimate contact but also greatly enhance the capability to suppress the dendritic Li formation because of the greatly enhanced viscosity, decreased surface tension of molten Li, and the in situ formation of Li3N at the interface. Thus, the resulting Li-C3N4|SSE|Li-C3N4 symmetric cell gives a significantly low interfacial resistance of 11 Ω cm2 and a high critical current density (CCD) of 1500 μA cm−2. In contrast, the same symmetric cell configuration with pristine Li metal electrodes has a much larger interfacial resistance (428 Ω cm2) and a much lower CCD (50 μA cm−2). 相似文献
997.
Shan Jin Manman Zhou Xi Kang Xiaowu Li Wenjun Du Xiao Wei Shuang Chen Dr. Shuxin Wang Prof. Manzhou Zhu 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(10):3919-3923
The high-dimensional (that is, three-dimensional (3D)) assembly of nanomaterials is an effective means of improving their properties; however, achieving this assembly at the atomic level remains challenging. Herein, we obtained a novel nanocluster, [Au8Ag57(Dppp)4(C6H11S)32Cl2]Cl (Dppp=1,3-bis(diphenylphosphino)propane) showing a 3D octameric assembly mode involving the kernel penetration of eight complete icosahedral Au@Ag10Au2 units for the first time. The atomically precise structure was determined by single-crystal X-ray diffraction, and further confirmed by thermogravimetric analysis, X-ray photoelectron spectroscopy, and electrospray ionization mass spectrometry measurements. Furthermore, ligand-induced transformation prompted the conversion of [Au8Ag57(Dppp)4(C6H11S)32Cl2]Cl, with complete octameric fusion into [Au8Ag55(Dppp)4(C6H11S)34][BPh4]2, with incomplete octameric fusion. These observations will hopefully facilitate further research on the assembly of M13 nanobuilding blocks. 相似文献
998.
Dr. Zheng Yi Song Jiang Dr. Jie Tian Yong Qian Prof. Shimou Chen Prof. Shiqiang Wei Dr. Ning Lin Prof. Yitai Qian 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(16):6521-6527
An amidation-dominated re-assembly strategy is developed to prepare uniform single atom Ni/S/C nanotubes. In this re-assembly process, a single-atom design and nano-structured engineering are realized simultaneously. Both the NiO5 single-atom active centers and nanotube framework endow the Ni/S/C ternary composite with accelerated reaction kinetics for potassium-ion storage. Theoretical calculations and electrochemical studies prove that the atomically dispersed Ni could enhance the convention kinetics and decrease the decomposition energy barrier of the chemically-absorbed small-molecule sulfur in Ni/S/C nanotubes, thus lowering the electrode reaction overpotential and resistance remarkably. The mechanically stable nanotube framework could well accommodate the volume variation during potassiation/depotassiation process. As a result, a high K-storage capacity of 608 mAh g−1 at 100 mA g−1 and stable cycling capacity of 330.6 mAh g−1 at 1000 mA g−1 after 500 cycles are achieved. 相似文献
999.
Mengjiao Huang Dr. Juanjuan Yang Teng Wang Dr. Jia Song Jinglu Xia Dr. Lingling Wu Dr. Wei Wang Dr. Qiaoyi Wu Prof. Zhi Zhu Dr. Yanling Song Prof. Chaoyong Yang 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(12):4830-4835
Immunotherapy has revolutionized cancer treatment, but its efficacy is severely hindered by the lack of effective predictors. Herein, we developed a homogeneous, low-volume, efficient, and sensitive exosomal programmed death-ligand 1 (PD-L1, a type of transmembrane protein) quantitation method for cancer diagnosis and immunotherapy response prediction (HOLMES-ExoPD-L1). The method combines a newly evolved aptamer that efficiently binds to PD-L1 with less hindrance by antigen glycosylation than antibody, and homogeneous thermophoresis with a rapid binding kinetic. As a result, HOLMES-ExoPD-L1 is higher in sensitivity, more rapid in reaction time, and easier to operate than existing enzyme-linked immunosorbent assay (ELISA)-based methods. As a consequence of an outstanding improvement of sensitivity, the level of circulating exosomal PD-L1 detected by HOLMES-ExoPD-L1 can effectively distinguish cancer patients from healthy volunteers, and for the first time was found to correlate positively with the metastasis of adenocarcinoma. Overall, HOLMES-ExoPD-L1 brings a fresh approach to exosomal PD-L1 quantitation, offering unprecedented potential for early cancer diagnosis and immunotherapy response prediction. 相似文献
1000.
采用失重法、电化学法、X射线光电子能谱(XPS)和扫描电子显微镜(SEM)研究了0.5 mol/L NaCl溶液中,山梨酸钾(PS)与Zn2+对Q235钢的缓蚀协同效应。 失重实验结果表明,在0.5 mol/L NaCl溶液中,PS对Q235钢具有一定的缓蚀效果,缓蚀效率随PS质量浓度的增加而增大,当添加PS的质量浓度为25.0 g/L时,最大缓蚀效率仅为38.37%,而PS与Zn2+复配后存在显著的缓蚀协同作用,缓蚀效率高达91.03%。 动电势极化结果表明,PS与Zn2+混合物可同时抑制Q235钢的阴、阳极反应,属于阳极型缓蚀剂。 阻抗谱表明,该混合物可在电极表面形成致密的保护膜。 XPS分析证明保护膜是由PS、铁的氧化物/氢氧化物和Zn(OH)2沉淀组成。 相似文献