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101.
Robert Lindner Xinghua Lou Jochen Reinstein Robert L Shoeman Fred A Hamprecht Andreas Winkler 《Journal of the American Society for Mass Spectrometry》2014,25(6):1018-1028
Hydrogen–deuterium exchange (HDX) experiments analyzed by mass spectrometry (MS) provide information about the dynamics and the solvent accessibility of protein backbone amide hydrogen atoms. Continuous improvement of MS instrumentation has contributed to the increasing popularity of this method; however, comprehensive automated data analysis is only beginning to mature. We present Hexicon 2, an automated pipeline for data analysis and visualization based on the previously published program Hexicon (Lou et al. 2010). Hexicon 2 employs the sensitive NITPICK peak detection algorithm of its predecessor in a divide-and-conquer strategy and adds new features, such as chromatogram alignment and improved peptide sequence assignment. The unique feature of deuteration distribution estimation was retained in Hexicon 2 and improved using an iterative deconvolution algorithm that is robust even to noisy data. In addition, Hexicon 2 provides a data browser that facilitates quality control and provides convenient access to common data visualization tasks. Analysis of a benchmark dataset demonstrates superior performance of Hexicon 2 compared with its predecessor in terms of deuteration centroid recovery and deuteration distribution estimation. Hexicon 2 greatly reduces data analysis time compared with manual analysis, whereas the increased number of peptides provides redundant coverage of the entire protein sequence. Hexicon 2 is a standalone application available free of charge under http://hx2.mpimf-heidelberg.mpg.de. Figure
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102.
Soot particles characteristics were investigated numerically for high temperature oxidation of C2H4/O2/N2 (C/O ratio of 2.2) in a closed jet-stirred/plug-flow reactor (JSR/PFR) system. Based on the growth mechanism of polycyclic aromatic hydrocarbons (PAHs), two mechanisms were used to explore the formation pathways of soot precursors and soot. Numerical results were compared with the experimental and reference data. The simulation results show that the value predicted for small molecule intermediates within A1 gives a strong regularity, consistent trend with reference data. However, with the hydrogen-abstraction-carbon-addition (HACA) growth mechanism, the predicted value for beyond-A1 PAH macromolecules and soot volume fraction are smaller than the experimental data. The results also show that the predicted soot volume fraction is in good agreement with experimental data when a combination of the HACA and PAHs condensation (HACA + PAH-PAH) growth mechanisms is used. Analyses of the A1 sensitivity and reaction pathway elucidated that A1 are mainly formed from C2H3, C2H2, C3H3, C6H5OH, A1C2H and A1-. The reaction 2C3H3 → A1 is the dominant route of benzene formation. The prediction results and an analysis of the A3 reaction pathway indicate that the growth process from benzene to larger aromatic hydrocarbons (beyond two-ring polycyclic aromatic hydrocarbons [PAHs]) goes by two pathways, i.e., HACA combined with the PAH-PAH radical recombination and addition reaction growth mechanisms. 相似文献
103.
Ben Qi Lan-Lan Lou Ying Yang Yanbing Wang Wenyue Bian Shuangxi Liu 《Research on Chemical Intermediates》2014,40(8):2973-2982
Manganese oxides supported on γ-Al2O3, amorphous SiO2, MCM-41, and TiO2 prepared by an impregnation method were used as heterogeneous catalysts for epoxidation of alkenes with 30 % H2O2 in the presence of NaHCO3 aqueous solution. The effect of support and manganese loading on their activity was studied. The 1.3-MnO x /γ-Al2O3 exhibited superior epoxidazing activity of styrene, compared with other supported MnO x . Hydrogen temperature-programmed reduction, UV–vis and ESR analyses suggested that Mn2+ (catalytic activity species) dominated in 1.3 % MnO x /γ-Al2O3 due to a strong interaction between MnO x and γ-Al2O3. Recycling studies showed the catalyst was a heterogeneous one and retained its activity after recycling four times. 相似文献
104.
Andrea Marchesi Dr. Fabio Parmeggiani João Louçano Ashley P. Mattey Dr. Kun Huang Tanistha Gupta Dr. Mario Salwiczek Prof. Sabine L. Flitsch 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(50):22642-22645
Automated chemical oligosaccharide synthesis is an attractive concept that has been successfully applied to a large number of target structures, but requires excess quantities of suitably protected and activated building blocks. Herein we demonstrate the use of biocatalysis to supply such reagents for automated synthesis. By using the promiscuous NmLgtB-B β1-4 galactosyltransferase from Neisseria meningitidis we demonstrate fast and robust access to the LacNAc motif, common to many cell-surface glycans, starting from either lactose or sucrose as glycosyl donors. The enzymatic product was shown to be successfully incorporated as a complete unit into a tetrasaccharide target by automated assembly. 相似文献
105.
Dr. Ze-Jun Xu Yan Zong Ya-Nan Qiao Jiao-Zhen Zhang Xuyuan Liu Ming-Zhu Zhu Yuliang Xu Hongbo Zheng Liyuan Fang Dr. Xiao-ning Wang Prof. Hong-Xiang Lou 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(45):20091-20095
A divergent synthetic approach to biogenetically related diterpenoids such as ent-kauranes, ent-trachylobanes, ent-beyerane, and ent-atisane has been developed. The unified synthetic route involves the De Mayo reaction to rapidly generate the bicyclo[3.2.1]-octane moiety of ent-kaurane. The key reactions also include bioinspired nucleophilic cyclopropanation generating the [3.2.1.02,7]-tricyclic core of ent-trachylobane and regioselective cyclopropane fragmentation furnishing ent-beyerane and ent-atisane through the nucleophilic attack and protonation of the cyclopropane ring. This strategy enables the asymmetric total syntheses of six diterpenoids from the commercially available geraniol. 相似文献
106.
Youshan Li Dr. Zhenbang Lou Hongyun Li Dr. Haijun Yang Prof. Dr. Yufen Zhao Prof. Dr. Hua Fu 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(9):3700-3706
A bioorthogonal ligation and cleavage method via reactions of chloroquinoxalines (CQ) and ortho-dithiophenols (DT) is presented. Double nucleophilic substitutions of ortho-dithiophenols to chloroquinoxalines provide conjugates containing tetracyclic benzo[5,6][1,4]dithiino[2,3-b]quinoxaline with strong built-in fluorescence together with release of the other functional molecules. Three cleavable linkers were designed and successfully used in release of the molecules containing biotin from the protein conjugates. The CQ-DT bioorthogonal reactions can be applied for the bioorthogonal ligations, bioorthogonal cleavages, and trans-tagging of proteins, and show advantages of readily accessible unnatural orthogonal groups, appealing reaction kinetics (k2≈1.3 m −1 s−1), excellent biocompatibility of orthogonal groups, and high stability of conjugates. This complements previous bioorthogonal reactions and is a new route for protein-fishing applications and in-gel fluorescence analysis. 相似文献
107.
Dr. Yongjin Fang Dr. Deyan Luan Dr. Ye Chen Prof. Shuyan Gao Prof. Xiong Wen Lou 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(18):7245-7250
Hybrid materials, integrating the merits of individual components, are ideal structures for efficient sodium storage. However, the construction of hybrid structures with decent physical/electrochemical properties is still challenging. Now, the elaborate design and synthesis of hierarchical nanoboxes composed of three-layered Cu2S@carbon@MoS2 as anode materials for sodium-ion batteries is reported. Through a facile multistep template-engaged strategy, ultrathin MoS2 nanosheets are grown on nitrogen-doped carbon-coated Cu2S nanoboxes to realize the Cu2S@carbon@MoS2 configuration. The design shortens the diffusion path of electrons/Na+ ions, accommodates the volume change of electrodes during cycling, enhances the electric conductivity of the hybrids, and offers abundant active sites for sodium uptake. By virtue of these advantages, these three-layered Cu2S@carbon@MoS2 hierarchical nanoboxes show excellent electrochemical properties in terms of decent rate capability and stable cycle life. 相似文献
108.
弗林蛋白酶是前体蛋白转化酶家族中最具特色的酶之一,具有重要的生物学功能,其表达量水平与许多疾病有密切的关系,如癌症的发生和发展与弗林蛋白酶表达水平有着密切关联.目前文献中报道了一些单光子荧光探针用于弗林蛋白酶的检测,但这些探针不能应用于深层组织成像,且弗林蛋白酶在肿瘤发展过程的作用仍没有得到很好地研究.针对这些问题,本工作构建了一种新型双光子荧光探针Nap-F用于细胞和肿瘤组织内弗林蛋白酶的检测与双光子成像.Nap-F是由经典双光子荧光染料1,8-萘酰亚胺、弗林蛋白酶特异性多肽序列RVRR和自消除连接体整合而成.实验结果表明Nap-F对弗林蛋白酶具有很好的特异性,能够定量检测弗林蛋白酶的活性.在飞秒激光820 nm激发下,Nap-F能有效降低生物背景,并提高组织穿透深度,适用于细胞和组织的双光子成像.Nap-F成功地实现了几种活细胞中弗林蛋白酶的双光子成像,揭示了癌细胞和表达缺陷细胞中弗林蛋白酶含量的差异.更重要的是,我们将该探针用于CoCl2固定HIF-1构建的肿瘤细胞缺氧模型成像,实验结果表明弗林蛋白酶的表达与肿瘤细胞缺氧程度存在正相关性. 相似文献
109.
Peng Zhang Xue Feng Lu Deyan Luan Xiong Wen Lou 《Angewandte Chemie (International ed. in English)》2020,59(21):8128-8132
Photocatalysts with well‐designed compositions and structures are desirable for achieving highly efficient solar‐to‐chemical energy conversion. Heterostructured semiconductor photocatalysts with advanced hollow structures possess beneficial features for promoting the activity towards photocatalytic reactions. Here we develop a facile synthetic strategy for the fabrication of Fe2TiO5–TiO2 nanocages (NCs) as anode materials in photoelectrochemical (PEC) water splitting cells. A hydrothermal reaction is performed to transform MIL‐125(Ti) nanodisks (NDs) to Ti–Fe–O NCs, which are further converted to Fe2TiO5–TiO2 NCs through a post annealing process. Owing to the compositional and structural advantages, the heterostructured Fe2TiO5–TiO2 NCs show enhanced performance for PEC water oxidation compared with TiO2 NDs, Fe2TiO5 nanoparticles (NPs) and Fe2TiO5–TiO2 NPs. 相似文献
110.
Yongjin Fang Deyan Luan Ye Chen Shuyan Gao Xiong Wen Lou 《Angewandte Chemie (International ed. in English)》2020,59(18):7178-7183
Hybrid materials, integrating the merits of individual components, are ideal structures for efficient sodium storage. However, the construction of hybrid structures with decent physical/electrochemical properties is still challenging. Now, the elaborate design and synthesis of hierarchical nanoboxes composed of three‐layered Cu2S@carbon@MoS2 as anode materials for sodium‐ion batteries is reported. Through a facile multistep template‐engaged strategy, ultrathin MoS2 nanosheets are grown on nitrogen‐doped carbon‐coated Cu2S nanoboxes to realize the Cu2S@carbon@MoS2 configuration. The design shortens the diffusion path of electrons/Na+ ions, accommodates the volume change of electrodes during cycling, enhances the electric conductivity of the hybrids, and offers abundant active sites for sodium uptake. By virtue of these advantages, these three‐layered Cu2S@carbon@MoS2 hierarchical nanoboxes show excellent electrochemical properties in terms of decent rate capability and stable cycle life. 相似文献