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91.
Xin Ma Lien B. Lai Stella M. Lai Akiko Tanimoto Mark P. Foster Vicki H. Wysocki Venkat Gopalan 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2014,126(43):11667-11671
We demonstrate that surface‐induced dissociation (SID) coupled with ion mobility mass spectrometry (IM‐MS) is a powerful tool for determining the stoichiometry of a multi‐subunit ribonucleoprotein (RNP) complex assembled in a solution containing Mg2+. We investigated Pyrococcus furiosus (Pfu) RNase P, an archaeal RNP that catalyzes tRNA 5′ maturation. Previous step‐wise, Mg2+‐dependent reconstitutions of Pfu RNase P with its catalytic RNA subunit and two interacting protein cofactor pairs (RPP21⋅RPP29 and POP5⋅RPP30) revealed functional RNP intermediates en route to the RNase P enzyme, but provided no information on subunit stoichiometry. Our native MS studies with the proteins showed RPP21⋅RPP29 and (POP5⋅RPP30)2 complexes, but indicated a 1:1 composition for all subunits when either one or both protein complexes bind the cognate RNA. These results highlight the utility of SID and IM‐MS in resolving conformational heterogeneity and yielding insights on RNP assembly. 相似文献
92.
93.
Antony Wing Hung Ng Samuel Kin-Man Lai Chi-Chung Yee Ho Yu Au-Yeung 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2022,134(1):e202110200
A branched [8]catenane from an efficient one-pot synthesis (72 % HPLC yield, 59 % isolated yield) featuring the simultaneous use of three kinds of templates and cucurbit[6]uril-mediated azide–alkyne cycloaddition (CBAAC) for ring-closing is reported. Design and assembly of the [8]catenane precursors are unexpectedly complex that can involve cooperating, competing and non-influencing interactions. Due to the branched structure, dynamics of the [8]catenane can be modulated in different extent by rigidifying/loosening the mechanical bonds at different regions by using solvent polarity, acid-base and metal ions as the stimuli. This work not only highlights the importance of understanding the delicate interplay of the weak and non-obvious supramolecular interactions in the synthesis of high-order [n]catenane, but also demonstrates a complex control of dynamics and flexibility for exploiting [n]catenanes applications. 相似文献
94.
Pei-Ying Li Jia-Hui Zhao Nian Li Bo Liu Wen-Ge Zhang Zi-Fan Zhu Chao Yan Ning-Lan Xiao Hua-Jie Lai 《Journal of separation science》2022,45(14):2621-2631
Recently, pharmaceuticals and personal care products in the water environment exhibited potential risks to both human and aquatic organisms. In order to improve the sensitivity and accuracy of pharmaceutical detection, the polyimidazolyl acetate ionic liquid was synthesized by Radziszewski reaction and coated on cellulose filter papers as a thin-film extraction phase for extraction of non-steroidal anti-inflammatory drugs from water. The attenuated total reflection-infrared spectrometry, thermogravimetric analysis, and scanning electron microscope analyses demonstrated that the polyimidazolyl acetate ionic liquid was successfully prepared and attached to the surface of the cellulose filter paper through chemical bonding. The adsorption capacity of the homemade thin-film extraction material for the four non-steroidal anti-inflammatory drugs was greater than 8898 ng/cm2 under the optimum conditions, and the desorption rate was over 90%. Then, a paper-based thin-film extraction phase-high-performance liquid chromatography-tandem mass spectrometry method was established for the extraction of non-steroidal anti-inflammatory drugs in water. This method provided limits of detection and limits of quantification were in the range of 0.02–0.15 and 0.17–0.50 μg/L, respectively. Hence, the obtained thin-film extraction phase showed excellent recovery and reproducibility for the target non-steroidal anti-inflammatory drugs with carboxyl groups from water. 相似文献
95.
Piao He Jian‐Guo Zhang Kun Wang Xin Yin Tong‐Lai Zhang 《Journal of Physical Organic Chemistry》2016,29(1):29-34
Two novel energetic nitrogen‐rich compounds 1,4‐diaminotetrazol‐5‐one ( DATO ) and 1,4‐dinitrotetrazol‐5‐one ( DNTO ) were proposed first and studied by quantum chemistry method with B3LYP/6‐31G* level of theory. The optimized geometry, IR predicted spectrum and thermochemical parameters, frontier molecular orbitals and molecular electrostatic potential were calculated for inspecting the electronic structure, molecular stability and chemical reactivity. The important macroscopic properties including density, enthalpy of formation, detonation parameters and impact sensitivity have been predicted as well. As a result, two designed compounds DATO and DNTO possess positive enthalpy of formation (395.79 and 342.77 kJ/mol), impressive detonation parameters (D = 8.80 km/s, P = 33.69 GPa; D = 8.89 km/s, P = 34.98 GPa) superior to the remarkable explosive RDX, acceptable sensitivities and might be promising candidates of energetic materials. Copyright © 2015 John Wiley & Sons, Ltd. 相似文献
96.
Back contact–absorber interface modification by inserting carbon intermediate layer and conversion efficiency improvement in Cu2ZnSn(S,Se)4 solar cell 下载免费PDF全文
Fangqin Zeng Kaiwen Sun Li Gong Liangxing Jiang Fangyang Liu Yanqing Lai Jie Li 《固体物理学:研究快报》2015,9(12):687-691
Carbon layers have been employed as intermediate layers between Mo back contact and Cu2ZnSn(S1–xSex)4(CZTSSe) absorber film prepared by sol–gel and post‐selenization method. Carbon layers with appropriate thickness can significantly inhibit the formation of MoSe2 and voids at bottom region of the absorber, and therefore reduce the series resistance remarkably. The conversion efficiency can be boosted by the introducing of the carbon layer from 6.20% to 7.24% by enhancement in short current density, fill factor and open voltage in comparison to the reference sample without carbon layer. However, excess thickness of carbon layer will worse device performance due to the deteriorated absorber crystallinity. In addition, the time‐resolved photoluminescence analysis shows that inserting the carbon layer with suitable thickness does not introduce recombination and lower minority lifetime. (© 2015 WILEY‐VCH Verlag GmbH &Co. KGaA, Weinheim) 相似文献
97.
Piao He Jian‐Guo Zhang Li‐Na Feng Kun Wang Tong‐Lai Zhang Shao‐Wen Zhang 《Journal of Physical Organic Chemistry》2015,28(6):423-427
1,5‐Daminotetrazole (DAT) is of much interest because of the practical significance and the diversity of characteristics. The study on the decomposition pathway and the kinetics of DAT has been performed based on the quantum chemistry theory. The minimum energy path (MEP) calculation has shown that NH2N3 and NH2CN are the initially detected products of DAT. And the structures of reactant, products and transition state were optimized with MP2 methods using 6‐311G** basis sets, and the energies were refined using CCSD(T)/6‐311G** levels of theory. The calculated rate constants were obtained using the conventional transition‐state theory (TST) and the canonical variational transition‐state theory (CVT) methods. The calculation results indicated that the energy barrier of decomposition reaction is 47.98 kcal mol?1 and the variational effect is small. In addition, the rate constants and the Arrhenius experience formula of DAT decomposition have been obtained between 200 and 2500 K temperature regions. The fitted three‐parameter expressions calculated using the TST and CVT methods are (TST) and (CVT). This work may provide the theoretical support for further experimental synthesis and testing. Copyright © 2015 John Wiley & Sons, Ltd. 相似文献
98.
Wei‐Li Li Dr. Ya‐Fan Zhao Dr. Han‐Shi Hu Prof. Dr. Jun Li Prof. Dr. Lai‐Sheng Wang 《Angewandte Chemie (International ed. in English)》2014,53(22):5540-5545
Chirality is vital in chemistry. Its importance in atomic clusters has been recognized since the discovery of the first chiral fullerene, the D2 symmetric C76. 1 A number of gold clusters have been found to be chiral, 2 raising the possibility to use them as asymmetric catalysts. The discovery of clusters with enantiomeric structures is essential to design new chiral materials with tailored chemical and physical properties. 3 Herein we report the first inherently chiral boron cluster of [B30]? in a joint photoelectron spectroscopy and theoretical study. The most stable structure of [B30]? is found to be quasiplanar with a hexagonal hole. Interestingly, a pair of enantiomers arising from different positions of the hexagonal hole are found to be degenerate in our global minimum searches and both should co‐exist experimentally because they have identical electronic structures and give rise to identical simulated photoelectron spectra. 相似文献
99.
Wan-Feng Zhang Xiao-Ping Xia Takahashi Eiichi Li Li Qing Yang Yan-Qiang Zhang Ya-Nan Yang Ming-Liang Liu Chunkit Lai 《Surface and interface analysis : SIA》2020,52(5):224-233
Secondary ion mass spectrometry (SIMS) has a wide range of applications in Earth Science research, thanks to its high precision and sensitivity, and its capacity in direct insitu micromeasurement. The technique is operated in ultra-high vacuum (UHV) conditions, especially for the measurement of volatiles such as hydrogen, or the water content in nominally anhydrous minerals (NAMs). To minimize the water background and obtain accurate and precise water contents in NAMs (eg, olivine) critical parameters such as presputtering time, field aperture (FA), dynamic transfer on/off, and primary beam current intensity were investigated for a CAMECA IMS 1280-HR system. When the chamber vacuum reaches approximately 2 × 10−9 mbar, we set the DTOS OFF, raster size to 50 μm and primary beam current to 5 nA, and used 2000 μm FA and 170-second presputtering time. Consequently, an approximately 1.2 ppmw water background and 3.6 ppmw limit of detection (LOD) were yielded, from analyzing the San Carlos olivine. Meanwhile, the water content and homogeneity of a range of olivine minerals were characterized for potential use as reference materials for SIMS water content measurement. Olivine water content calibration curve was also established by comparing the Fourier transform infrared (FTIR) results with the SIMS-measured 16O1H−/16O− ratios. Accuracy and precision of water content measurement were estimated to be better than approximately 10% in this study. 相似文献
100.
Jiann-Jyh Huang Yu-Hsiang Lin Chun-Liang Lai Sheng-Chuan Yang Shu Fu Lin Ju-Ying Yang Hung-Jyun Huang Chiawei Liu Win-Yin Wei Shih-Hsien Chuang Chao-Cheng Chiang Ying-Shuen E. Lee Chu-Bin Liao Ching Yuh Chern 《中国化学会会志》2020,67(3):422-429
In this study, we reported the inhibition profiles of 4′-acylpyrrole–5-fluoroindolin-2-one 3 with a C-3′ side chain for VEGFR2, PDGFR-β, and FGFR-1 protein kinases. The pyrrole-fused cyclohexanone moiety provided 3 with the best potency to inhibit the three kinases, and the C-3′ side chains contributed to the different inhibition profiles of 3 . Compound 3b with a C-3′ 2-carboxylethyl side chain showed good potency for the three kinase (IC50: 25–260 nM), and compound 3g with a N,N-dialkyl-2-carbamoylethyl side chain was more active for VEGFR2 (IC50: 59 nM) and PDGFR-β (IC50: 16 nM) than FGFR-1 (IC50: 1.7 μM). The C-3′ 3-(dialkylamino)propyl side chain accomplished 3h – j as selective PDGFR-β inhibitors (IC50: 7.8–13 nM). Compound 3b was further investigated and found potent to inhibit VEGF- and FGF-dependent cell proliferation with moderate in vivo anticancer activity. Results from docking simulations revealed that the interactions of 3b with VEGFR2 and FGFR-1 which could account for the different inhibition profiles of 3 . 相似文献