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961.
通过对前处理方法的比较,选择了快速溶剂萃取作为可吸入颗粒物中多环芳烃的提取方式,并且将ASE的萃取条件作了优化实验,确定ASE的优化结果为DCM:HEX=2:1,萃取温度为120℃,萃取压力为10.34 MPa。处理完的样品上气相色谱质谱-质谱测定,得到空白样品中24种PAHs均有检出,实际样品中的含量均低于10 ng/m L,6种替代物的标准曲线的相关系数在0.999以上,24种PAHs标准样品作了3个不同浓度范围的标准曲线,相关系数均在0.99以上。空白加标实验中得到6种替代物的回收率在58.7%~108.2%之间,24种PAHs的平均回收率在88.3%~104.0%之间,相对标准偏差均低于9.0%。样品加标实验中6种替代物的加标回收率在60.0%~106.5%之间,24种PAHs的回收率在78.0%~95.0%之间,相对标准偏差均低于6.0%。 相似文献
962.
Rongying Liu Dr. Zdravko Kochovski Long Li Yue-wen Yin Jing Yang Guang Yang Guoqing Tao Anqiu Xu Ensong Zhang Prof. Dr. Hong-ming Ding Prof. Dr. Yan Lu Prof. Dr. Guosong Chen Prof. Dr. Ming Jiang 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(24):9704-9710
A protein Pascal triangle has been constructed as new type of supramolecular architecture by using the inducing ligand strategy that we previously developed for protein assemblies. Although mathematical studies on this famous geometry have a long history, no work on such Pascal triangles fabricated from native proteins has been reported so far due to their structural complexity. In this work, by carefully tuning the specific interactions between the native protein building block WGA and the inducing ligand R-SL , a 2D Pascal-triangle lattice with three types of triangular voids has been assembled. Moreover, a 3D crystal structure was obtained based on the 2D Pascal triangles. The distinctive carbohydrate binding sites of WGA and the intralayer as well as interlayer dimerization of RhB was the key to facilitate nanofabrication in solution. This strategy may be applied to prepare and explore various sophisticated assemblies based on native proteins. 相似文献
963.
Qingyun Zheng Tian Wang Guo-Chao Chu Chong Zuo Rui Zhao Xin Sui Linzhi Ye Yuanyuan Yu Jingnan Chen Xiangwei Wu Wenhao Zhang Prof. Haiteng Deng Prof. Jing Shi Dr. Man Pan Prof. Yi-Ming Li Prof. Lei Liu 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(32):13598-13603
Triazole-based deubiquitylase (DUB)-resistant ubiquitin (Ub) probes have recently emerged as effective tools for the discovery of Ub chain-specific interactors in proteomic studies, but their structural diversity is limited. A new family of DUB-resistant Ub probes is reported based on isopeptide-N-ethylated dimeric or polymeric Ub chains, which can be efficiently prepared by a one-pot, ubiquitin-activating enzyme (E1)-catalyzed condensation reaction of recombinant Ub precursors to give various homotypic and even branched Ub probes at multi-milligram scale. Proteomic studies using label-free quantitative (LFQ) MS indicated that the isopeptide-N-ethylated Ub probes may complement the triazole-based probes in the study of Ub interactome. Our study highlights the utility of modern protein synthetic chemistry to develop structurally and new families of tool molecules needed for proteomic studies. 相似文献
964.
Dr. Weihui Ou Dr. Binbin Zhou Junda Shen Dr. Tsz Wing Lo Prof. Dangyuan Lei Dr. Shengliang Li Jing Zhong Prof. Yang Yang Li Prof. Jian Lu 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(17):6856-6859
Hot carriers (HCs) and thermal effects, stemming from plasmon decays, are crucial for most plasmonic applications. However, quantifying these two effects remains extremely challenging due to the experimental difficulty in accurately measuring the temperature at reaction sites. Herein, we provide a novel strategy to disentangle HCs from photothermal effects based on the different traits of heat dissipation (long range) and HCs transport (short range), and quantitatively uncover the dominant and potential-dependent role of photothermal effect by investigating the rapid- and slow-response currents in plasmon-mediated electrochemistry at nanostructured Ag electrode. Furthermore, the plasmoelectric surface potential is found to contribute to the rapid-response currents, which is absent in the previous studies. 相似文献
965.
Ying Liu Dr. Ximing Rong Mingze Li Prof. Maxim S. Molokeev Prof. Jing Zhao Prof. Zhiguo Xia 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(28):11731-11737
The incorporation of impurity ions or doping is a promising method for controlling the electronic and optical properties and the structural stability of halide perovskite nanocrystals (NCs). Herein, we establish relationships between rare-earth ions doping and intrinsic emission of lead-free double perovskite Cs2AgInCl6 NCs to impart and tune the optical performances in the visible light region. Tb3+ ions were incorporated into Cs2AgInCl6 NCs and occupied In3+ sites as verified by both crystallographic analyses and first-principles calculations. Trace amounts of Bi doping endowed the characteristic emission (5D4→7F6-3) of Tb3+ ions with a new excitation peak at 368 nm rather than the single characteristic excitation at 290 nm of Tb3+. By controlling Tb3+ ions concentration, the emission colors of Bi-doped Cs2Ag(In1−xTbx)Cl6 NCs could be continuously tuned from green to orange, through the efficient energy-transfer channel from self-trapped excitons to Tb3+ ions. Our study provides the salient features of the material design of lead-free perovskite NCs and to expand their luminescence applications. 相似文献
966.
Prof. Dr. Su-Yun Zhang Dr. Han Miao Dr. He-min Zhang Jun-Hao Zhou Prof. Dr. Qiang Zhuang Prof. Dr. Yu-Jia Zeng Prof. Dr. Zhiming Gao Prof. Dr. Jiayin Yuan Prof. Dr. Jian-Ke Sun 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(49):22293-22300
The capability to significantly shorten the synthetic period of a broad spectrum of open organic materials presents an enticing prospect for materials processing and applications. Herein we discovered 1,2,4-triazolium poly(ionic liquid)s (PILs) could serve as a universal additive to accelerate by at least one order of magnitude the growth rate of representative imine-linked crystalline open organics, including organic cages, covalent organic frameworks (COFs), and macrocycles. This phenomenon results from the active C5-protons in poly(1,2,4-triazolium)s that catalyze the formation of imine bonds, and the simultaneous salting-out effect (induced precipitation by decreasing solubility) that PILs exert on these crystallizing species. 相似文献
967.
Dr. Hui Wang Dr. Changcheng Jing Dr. Adam Noble Prof. Dr. Varinder Kumar Aggarwal 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(39):17005-17018
The stereospecific 1,2-migration of boronate complexes is one of the most representative reactions in boron chemistry. This process has been used extensively to develop powerful methods for asymmetric synthesis, with applications spanning from pharmaceuticals to natural products. Typically, 1,2-migration of boronate complexes is driven by displacement of an α-leaving group, oxidation of an α-boryl radical, or electrophilic activation of an alkenyl boronate complex. The aim of this article is to summarize the recent advances in the rapidly expanding field of electrophile-induced stereospecific 1,2-migration of groups from boron to sp2 and sp3 carbon centers. It will be shown that three different conceptual approaches can be utilized to enable the 1,2-migration of boronate complexes: stereospecific Zweifel-type reactions, catalytic conjunctive coupling reactions, and transition metal-free sp2–sp3 couplings. A discussion of the reaction scope, mechanistic insights, and synthetic applications of the work described is also presented. 相似文献
968.
Yuan Xu Jing Xue Qing Zhou Yongjun Zheng Xinghua Chen Prof. Songqin Liu Prof. Yanfei Shen Prof. Yuanjian Zhang 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(34):14606-14611
Emerging as a cost-effective and robust enzyme mimic, nanozymes have drawn increasing attention with broad applications ranging from cancer therapy to biosensing. Developing nanozymes with both accelerated and inhibited biocatalytic properties in a biological context is intriguing to peruse more advanced functions of natural enzymes, but remains challenging, because most nanozymes are lack of enzyme-like molecular structures. By re-visiting and engineering the well-known Fe-N-C electrocatalyst that has a heme-like Fe-Nx active sites, herein, it is reported that Fe-N-C could not only catalyze drug metabolization but also had inhibition behaviors similar to cytochrome P450 (CYP), endowing it a potential replacement of CYP for preliminary evaluation of massive potential chemicals, drug dosing guide, and outcome prediction. In addition, in contrast to electrocatalysts, the highly graphitic framework of Fe-N-C may not be obligatory for a competitive CYP-like activity. 相似文献
969.
Yajie Liu Zelin Duan Jing Fang Fan Zhang Prof. Junyu Xiao Prof. Wen-Bin Zhang 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(37):16256-16261
Herein, we report the biosynthesis of protein heterocatenanes using a programmed sequence of multiple post-translational processing events including intramolecular chain entanglement, in situ backbone cleavage, and spontaneous cyclization. The approach is general, autonomous, and can obviate the need for any additional enzymes. The catenane topology was convincingly proven using a combination of SDS-PAGE, LC-MS, size exclusion chromatography, controlled proteolytic digestion, and protein crystallography. The X-ray crystal structure clearly shows two mechanically interlocked protein rings with intact folded domains. It opens new avenues in the nascent field of protein-topology engineering. 相似文献
970.
Xuan Wei Diao Zheng Ming Zhao Dr. Hongzhong Chen Xun Fan Bin Gao Dr. Long Gu Dr. Yi Guo Dr. Jianbin Qin Prof. Jing Wei Prof. Yanli Zhao Prof. Guangcheng Zhang 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(34):14747-14754
Heteroatom-doped polymers or carbon nanospheres have attracted broad research interest. However, rational synthesis of these nanospheres with controllable properties is still a great challenge. Herein, we develop a template-free approach to construct cross-linked polyphosphazene nanospheres with tunable hollow structures. As comonomers, hexachlorocyclotriphosphazene provides N and P atoms, tannic acid can coordinate with metal ions, and the replaceable third comonomer can endow the materials with various properties. After carbonization, N/P-doped mesoporous carbon nanospheres were obtained with small particle size (≈50 nm) and high surface area (411.60 m2 g−1). Structural characterization confirmed uniform dispersion of the single atom transition metal sites (i.e., Co-N2P2) with N and P dual coordination. Electrochemical measurements and theoretical simulations revealed the oxygen reduction reaction performance. This work provides a solution for fabricating diverse heteroatom-containing polymer nanospheres and their derived single metal atom doped carbon catalysts. 相似文献