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231.
Organocopper(ii) complexes are a rarity while organocopper(i) complexes are commonplace in chemical synthesis. In the course of building a strategy to generate organocopper(ii) species utilizing electrochemistry, a method to form compounds with CuII–C bonds was discovered, that demonstrated remarkably potent reactivity towards different functionalized alkenes under catalytic control. The role of the organocopper(ii) complex is to act as a source of masked radicals (in this case ˙CH2CN) that react with an alkene to generate the corresponding γ-halonitrile in good yields through atom transfer radical addition (ATRA) to various alkenes. The organocopper(ii) complexes can be continuously regenerated electrochemically for ATRA (eATRA), which proceeds at room temperature, under low Cu loadings (1–10 mol%) and with the possibility of Cu-catalyst recovery.Electrochemical generation of a novel organocopper(ii) complex offers a new way to carry out atom transfer radical addition to alkenes under mild conditions with high yields and low catalyst loadings. 相似文献
232.
Kevin B. Wu Christopher J. A. Skrodzki Qiwen Su Jennifer Lin Jia Niu 《Chemical science》2022,13(23):6873
The functions of natural nucleic acids such as DNA and RNA have transcended genetic information carriers and now encompass affinity reagents, molecular catalysts, nanostructures, data storage, and many others. However, the vulnerability of natural nucleic acids to nuclease degradation and the lack of chemical functionality have imposed a significant constraint on their ever-expanding applications. Herein, we report the synthesis and polymerase recognition of a 5-(octa-1,7-diynyl)uracil 2′-deoxy-2′-fluoroarabinonucleic acid (FANA) triphosphate. The DNA-templated, polymerase-mediated primer extension using this “click handle”-modified FANA (cmFANA) triphosphate and other FANA nucleotide triphosphates consisting of canonical nucleobases efficiently generated full-length products. The resulting cmFANA polymers exhibited excellent nuclease resistance and the ability to undergo efficient click conjugation with azide-functionalized molecules, thereby becoming a promising platform for serving as a programmable and evolvable synthetic genetic polymer capable of post-polymerization functionalization.Polymerase-mediated incorporation of a “click handle”-modified fluoroarabinonucleic acid (cmFANA) triphosphate produces a new class of nuclease-resistant, evolvable genetic polymers that can be functionalized with azide-containing molecules. 相似文献
233.
Phenothiazine-based covalent organic frameworks with low exciton binding energies for photocatalysis
Weitao Wang Haotian Wang Xiaohui Tang Jinlei Huo Yan Su Chuangye Lu Yujian Zhang Hong Xu Cheng Gu 《Chemical science》2022,13(29):8679
Designing delocalized excitons with low binding energy (Eb) in organic semiconductors is urgently required for efficient photochemistry because the excitons in most organic materials are localized with a high Eb of >300 meV. In this work, we report the achievement of a low Eb of ∼50 meV by constructing phenothiazine-based covalent organic frameworks (COFs) with inherent crystallinity, porosity, chemical robustness, and feasibility of bandgap engineering. The low Eb facilitates effective exciton dissociation and thus promotes photocatalysis by using these COFs. As a demonstration, we subject these COFs to photocatalytic polymerization to synthesize polymers with remarkably high molecular weight without any requirement of the metal catalyst. Our results can facilitate the rational design of porous materials with low Eb for efficient photocatalysis.We report the construction of phenothiazine-based covalent organic frameworks, which exhibited diverse structures, the feasibility of bandgap engineering, and unprecedented ultralow exciton binding energy of ∼50 meV for photocatalytic polymerization. 相似文献
234.
In this paper, a penalty virtual element method (VEM) on polyhedral mesh for solving the 3D incompressible flow is proposed and analyzed. The remarkable feature of VEM is that it does not require an explicit computation of the trial and test space, thereby bypassing the obstacle of standard finite element discretizations on arbitrary mesh. The velocity and pressure are approximated by the practical significative lowest equal-order virtual element space pair which does not satisfy the discrete - condition. Combined with the penalty method, the error estimation is proved rigorously. Numerical results on the 3D polygonal mesh illustrate the theoretical results and effectiveness of the proposed method. 相似文献
235.
针对学生在学习理论力学课程过程中,各章知识点、解题方法、力学建模、分析和解决综合问题不容易掌握的特点,将力学竞赛辅导采用的科学方法论中3 种逻辑方法:比较-分类法、归纳-演绎法、分析-综合法,引入到理论力学的课程教学中. 实践证明,在理论力学课程教学中,采用了这几种逻辑方法,不仅提高了理论力学课程的教学质量,激发了学生的学习兴趣;而且学生也很容易掌握各章的知识点、解题方法、力学建模,并将它们熟练地应用于分析和解决综合问题. 相似文献
236.
Wolfgang Dohle Xiangdong Su Yamni Nigam Edward Dudley Barry V. L. Potter 《Molecules (Basel, Switzerland)》2023,28(1)
A series of benzyl, phenyl guanidine, and aminoguandine hydrazone derivatives was designed and in vitro antibacterial activities against two different bacterial strains (Staphylococcus aureus and Escherichia coli) were determined. Several compounds showed potent inhibitory activity against the bacterial strains evaluated, with minimal inhibitory concentration (MIC) values in the low µg/mL range. Of all guanidine derivatives, 3-[2-chloro-3-(trifluoromethyl)]-benzyloxy derivative 9m showed the best potency with MICs of 0.5 µg/mL (S. aureus) and 1 µg/mL (E. coli), respectively. Several aminoguanidine hydrazone derivatives also showed good overall activity. Compounds 10a, 10j, and 10r–s displayed MICs of 4 µg/mL against both S. aureus and E. coli. In the aminoguanidine hydrazone series, 3-(4-trifluoromethyl)-benzyloxy derivative 10d showed the best potency against S. aureus (MIC 1 µg/mL) but was far less active against E. coli (MIC 16 µg/mL). Compound 9m and the para-substituted derivative 9v also showed promising results against two strains of methicillin-resistant Staphylococcus aureus (MRSA). These results provide new and potent structural leads for further antibiotic optimisation strategies. 相似文献
237.
238.
郑万国 魏晓峰 朱启华 景峰 胡东霞 张小民 粟敬钦 郑奎兴 王成程 袁晓东 周海 陈波 王健 马平 许乔 杨李茗 代万俊 周维 王方 许党朋 谢旭东 冯斌 彭志涛 郭良福 陈远斌 张雄军 刘兰琴 林东晖 党钊 向勇 陈晓东 张维岩 《强激光与粒子束》2016,28(01):019901
2015年9月15日,由中国工程物理研究院激光聚变研究中心承担研制的神光-Ⅲ主机装置成功完成了48束激光三倍频180 kJ/3 ns、峰值功率60 TW的输出测试实验,标志着神光-Ⅲ主机装置已全面建成并达到设计指标,成为现有输出能力世界排名第二、亚洲排名第一的惯性约束聚变激光驱动器。神光-Ⅲ主机装置可输出48束阵列化的大口径高功率脉冲激光(分为6个束组,每个束组为一个42的光束阵列),主要由前端、预放、主放、测量与光束控制、靶场、计算机集中控制等六大系统组成。神光-Ⅲ主机装置的研制,凝集了我国在光学、激光、脉冲功率、精密机械、快电子学、自动控制、化学清洗、超精密加工等多个学科领域的顶尖技术成就,堪称中国光学工程界的奇迹。神光-Ⅲ主机装置采用腔内四程放大+变口径90翻转U型反转器+助推三程放大的总体构型,在未使用大口径隔离组件的条件下,采用焦斑控制、精密准直、锥管镜面空间滤波及杂散光管理等技术措施,实现了基频光十万倍增益、10 kJ量级输出状态下的自激振荡抑制与反激光规避,在系统具备50%以上透过率的前提下确保了装置的运行安全,大大提高了装置的性价比。神光-Ⅲ主机装置的建设过程中攻克了高精度种子光源、高品质激光束的预放大、精密同步、辐射定标损伤检测、全光路精密波前校正、甚多束光路自动准直、自动化靶瞄准定位、计算机集中控制、高效谐波转换、一搁准精密安装、超精密光学加工、缺陷控制损伤阈值提升等多项光学工程技术难关,确保了装置具备优秀的技术指标性能。神光-Ⅲ主机装置打破了激光系统串行调试的规律,基于基准体系技术,通过不同束组间的错级并行,实现总体集成工作的满负荷运转,确保了装置建设的总体进度和集成效率。装置从第一个光机模块进场到基本完成集成调试,用时仅四年半,创造了又一个中国速度。在工程建设过程中以自主研发的传输放大动力学设计软件、激光泵浦动力学软件、杂散光树叉追迹软件等为基础,融合了部分光学设计商用软件,构建了覆盖光学、结构、电气、控制等多个学科的高功率激光装置数字化设计平台,基本实现了装置设计的全面数字化。工程建设过程中形成的质量、安全、进度控制体系保证了工程顺利进行。神光-Ⅲ主机装置的全面建成,标志着我国在大型激光驱动器方面的总体设计、总体集成、精密装校、加工制造、光学检测、关键技术等核心能力实现了体系化发展与成熟,面向更大规模的激光驱动器研制的光学工程体系已基本形成。 相似文献
239.
为了探讨铝飞片撞击陶瓷材料时的层裂现象,采用改进SPH方法模拟应力波在陶瓷材料中的传播。结果表明,当离散粒子分布不均匀时,数值模拟计算的自由面速度时程曲线与实测曲线吻合良好。对比CSPM方法,改进SPH方法的精度更高。提出适用于数值模拟的陶瓷材料损伤演化方程,对脉冲载荷下陶瓷/钢层合板层裂的破坏过程进行数值模拟,结果表明,由于陶瓷的波阻抗高于钢的,且抗压强度远高于抗拉强度,因此拉应力引起的层裂破坏是主要的。即使在材料内部传播的只是弹性压缩波,当弹性波到达材料界面时,由界面反射引起的卸载波也能导致陶瓷发生层裂破坏。 相似文献
240.