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    南沙海区万安盆地构造演化与成因机制

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    本文基于地震、钻井和区域地质资料,运用回剥法和平衡剖面技术定量研究了万安盆地的构造沉降和伸展程度,重建盆地的构造演化史并探讨其成因机制。模拟结果表明,万安盆地构造沉降曲线为多段式,其南北部构造沉降差异明显,且沉降中心逐渐向南发展的趋势。晚始新世-渐新世(37.8~23.03Ma BP)盆地中、北部快速沉降,存在两个沉降中心;早中新世(23.03~16.0Ma BP)盆地南部也发生快速沉降,整个盆地存在3个沉降中心;中中新世(约16.0~11.63Ma BP)沉降作用减弱,盆地进入裂后热沉降期。万安盆地的伸展和形成演化呈现北早南晚的特征,与南海海底扩张密切相关,同时受控于万安断裂带交替地右旋-左旋走滑作用,是伸展和走滑双重作用的结果。盆地的构造演化过程可细分为4个阶段:初始裂谷期、主要裂谷期、走滑改造期和裂后加速沉降期

    紫外辐射对两种海洋微藻生长及培养体系碳流的影响

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    以硅藻威氏海链藻(Thalassiosira weissflogii)和甲藻锥状斯氏藻(Scrippsiella trochoidea)为实验材料,通过室内模拟华南地区秋季晴天紫外辐照强度,研究两种不同波段的紫外辐射(Ultraviolet radiation,UVR)对两种微藻生长以及培养体系碳流的影响。结果表明:UV-A对两种微藻的生长有显著的促进作用,而UV-B则表现为抑制作用。锥状斯氏藻对UV-B的耐受性更强。在UV-A的作用下,培养体系中溶解无机碳(Dissolved inorganic carbon,DIC)的净消耗量低于对照组,但释放出更多的溶解有机碳(Dissolved organic carbon,DOC)。对照组的有色溶解有机物(Chromophoric dissolved organic matter,CDOM)含量显著升高,表明浮游植物生长过程是CDOM的来源之一。然而,在UV-A的作用下,两种微藻培养体系的CDOM浓度变化呈现相反趋势,说明不同藻种的CDOM产物受光漂白和光腐殖化的影响不同。在UV-B的作用下,微藻碎屑的分解使水体DIC和DOC浓度轻微升高。总体上,锥状斯氏藻比威氏海链藻净释放出更多的DOC和CDOM

    Photo-assisted degradation of bisphenol A by a novel FeS2@SiO2 microspheres activated persulphate process: Synergistic effect, pathway and mechanism

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    In this study, FeS2@SiO2 microspheres were firstly employed as a heterogeneous catalyst to activate persulfate (PS) for the degradation of bisphenol A (BPA) from aqueous solutions. The most relevant findings revealed that UV irradiation induced a significant improvement in the degradation of BPA by the FeS2@SiO2 microspheres/PS system. Nearly 100% of BPA degradation by the FeS2@SiO2 microspheres/PS/UV system was achieved within 120 min at reaction conditions of 1 mM PS, 0.066 mM BPA, 1.0 g/L FeS2@SiO2 microspheres and pH 3.0. A high performance on the degradation of BPA might be attributable to a synergistic effect between the PS/UV and the FeS2@SiO2 microspheres/PS catalytic processes. It was found that the BPA degradation could be inhibited by the coexisting anions like Cl-, HCO3- and PO43- to different extents at much higher concentrations, whereas NO3 had a negligible effect. Organic acids such as ethylene diamine tetra-acetic acid (EDTA) and oxalic acid (OA) would lead to an enhancement with a lower dosage, whereas a significantly negative effect was observed at much higher dosages. Radical scavenging tests revealed that the SO4 center dot- radicals prevailed over HO center dot. A total of seven intermediates during the degradation of BPA were identified by GC/MS, and a possible reaction pathway and mechanism of BPA degradation by the FeS2@SiO2 microspheres/PS/UV system was proposed. This study demonstrated a simple water treatment method involving the use of low cost natural iron minerals for organic pollutants removal

    Bifunctional Ligand Enables Efficient Gold-Catalyzed Hydroalkenylation of Propargylic Alcohol

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    Using the previously designed biphenyl-2-ylphosphine ligand, featuring a remote tertiary amino group, the first gold-catalyzed intermolecular hydroalkenylation of alkynes has been developed. Synthetically valuable conjugated dienyl alcohols are formed in moderate to good yields. A range of alkenyltrifluoroborates are allowed as the alkenyl donor, and no erosion of alkene geometry and/or the propargylic configuration are detected. DFT calculations confirm the critical role of the remote basic group in the ligand as a general-base catalyst for promoting this novel gold catalysis with good efficiency

    A fibrinogen-related protein, LvFREP2, from Litopenaeus vannamei facilitates the clearance of Vibrio harveyi

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    Fibrinogen-related proteins (FREPs) play a crucial role in invertebrate immune response. In this study, we acquired a novel fibrinogen-related protein gene in Litopenaeus vannamei coding for one kind of fibrinogen-related protein, designated as LvFREP2. The complete cDNA sequence of LvFREP2 was 1903 bp long, containing an open reading frame of 1479 bp coding for LvFREP2. The LvFREP2 protein contained a putative signal peptide and a fibrinogen-related protein domain. qRT-PCRs indicated that LvFREP2 mRNA ubiquitously distributed in all examined tissues, and it was up-regulated in gills after V. harveyi and LPS challenges. The recombinant LvFREP2 agglutinated Gram-positive (Staphylococcus aureus) and Gram-negative bacteria (Vibrio alginolyticus, V. cholerae, V. vulnificus, V. parahaemolyticus, V. harveyi, Pseudomonas aeruginosa, P. fluorescens) in a calcium-dependent manner. LvFREP2 also facilitated the clearance of Vibrio harveyi in vivo. Therefore, our results suggested that lvFREP2 may have important roles in the anti-bacterial immunity of L. vannamei

    Molecular basis of dimer formation during the biosynthesis of benzofluorene-containing atypical angucyclines

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    Lomaiviticin A and difluostatin A are benzofluorene-containing aromatic polyketides in the atypical angucycline family. Although these dimeric compounds are potent antitumor agents, how nature constructs their complex structures remains poorly understood. Herein, we report the discovery of a number of fluostatin type dimeric aromatic polyketides with varied C-C and C-N coupling patterns. We also demonstrate that these dimers are not true secondary metabolites, but are instead derived from non-enzymatic deacylation of biosynthetic acyl fluostatins. The non-enzymatic deacylation proceeds via a transient quinone methide like intermediate which facilitates the subsequent C-C/C-N coupled dimerization. Characterization of this unusual property of acyl fluostatins explains how dimerization takes place, and suggests a strategy for the assembly of C-C and C-N coupled aromatic polyketide dimers. Additionally, a deacylase FlsH was identified which may help to prevent accumulation of toxic quinone methides by catalyzing hydrolysis of the acyl group

    Antimalarial Activity of Plant Metabolites

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    Malaria, as a major global health problem, continues to affect a large number of people each year, especially those in developing countries. Effective drug discovery is still one of the main efforts to control malaria. As natural products are still considered as a key source for discovery and development of therapeutic agents, we have evaluated more than 2000 plant extracts against Plasmodium falciparum. As a result, we discovered dozens of plant leads that displayed antimalarial activity. Our phytochemical study of some of these plant extracts led to the identification of several potent antimalarial compounds. The prior comprehensive review article entitled Antimalarial activity of plant metabolites by Schwikkard and Van Heerden (2002) reported structures of plant-derived compounds with antiplasmodial activity and covered literature up to the year 2000. As a continuation of this effort, the present review covers the antimalarial compounds isolated from plants, including marine plants, reported in the literature from 2001 to the end of 2017. During the span of the last 17 years, 175 antiplasmodial compounds were discovered from plants. These active compounds are organized in our review article according to their plant families. In addition, we also include ethnobotanical information of the antimalarial plants discussed

    Structural Basis of Transcription Inhibition by Fidaxomicin (Lipiarmycin A3)

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    Fidaxomicin is an antibacterial drug in clinical use for treatment of Clostridium difficile diarrhea. The active ingredient of fidaxomicin, lipiarmycin A3 (Lpm), functions by inhibiting bacterial RNA polymerase (RNAP). Here we report a cryo-EM structure of Mycobacterium tuberculosis RNAP holoenzyme in complex with Lpm at 3.5-angstrom resolution. The structure shows that Lpm binds at the base of the RNAP "clamp." The structure exhibits an open conformation of the RNAP clamp, suggesting that Lpm traps an open-clamp state. Single-molecule fluorescence resonance energy transfer experiments confirm that Lpm traps an open-clamp state and define effects of Lpm on clamp dynamics. We suggest that Lpm inhibits transcription by trapping an open-clamp state, preventing simultaneous interaction with promoter -10 and -35 elements. The results account for the absence of cross-resistance between Lpm and other RNAP inhibitors, account for structure-activity relationships of Lpm derivatives, and enable structure-based design of improved Lpm derivatives

    Dual roles of cystatin A in the immune defense of the pacific oyster, Crassostrea gigas

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    Cystatins are a large family of the proteins that function as reversible and tight-binding inhibitors of cysteine proteases, which consequently regulate multiple physiological activities including apoptosis and innate immunity. In the present study, we cloned a gene from Crassostrea gigas encoding cystatin, which is related to cystatin A superfamily. CgCytA was comprised of a cystatin-like domain with two conserved glycine residues (GG) near the N-terminal and a highly conserved glutamine-valine-glycine (Q-X-V-X-G) motif in the form of QVVAG loop. Transcription analysis of CgCytA indicated its constitutive expression in all tissues including mantle, gill, digestive tract, hemocytes, heart, adductor muscle, and gonads. Immune challenge with Vibrio alginolyticus, resulted in significant down-regulation of CgCytA expression at the initial stages of infection (till 12 h post infection) and the expression of cystatin increased 48 h post infection. Protease assay demonstrated the concentration of cystatin needed to inhibit half of the maximum biological response of cysteine protease is 14.4 mu g/L (IC50). Furthermore, RNAi of CgCytA resulted in increase of apoptotic cell population in hemocytes of C. gigas, suggesting protection role of CgCytA from hemocytes apoptosis. Unexpectedly, knockdown of CgCytA leaded to enhancement of bacterial clearance in vivo, implying that CgCytA may negatively regulate immune defense by suppressing endogenous cysteine protease. Therefore, CgCytA plays dual roles in protection of host hemocytes from apoptosis and control of bacterial clearance, which may server as one of key endogenous balancer between apoptosis and innate immunity in oyster

    Characterization and heterologous expression of the neoabyssomicin/abyssomicin biosynthetic gene cluster from Streptomyces koyangensis SCSIO 5802

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    Background: The deep-sea-derived microbe Streptomyces koyangensis SCSIO 5802 produces neoabyssomicins A-B (1-2) and abyssomicins 2 (3) and 4 (4). Neoabyssomicin A (1) augments human immunodeficiency virus-1 (HIV-1) replication whereas abyssomicin 2 (3) selectively reactivates latent HIV and is also active against Gram-positive pathogens including methicillin-resistant Staphylococcus aureus (MRSA). Structurally, neoabyssomicins A-B constitute a new subtype within the abyssomicin family and feature unique structural traits characteristic of extremely interesting biosynthetic transformations. Results: In this work, the biosynthetic gene cluster (BGC) for the neoabyssomicins and abyssomicins, composed of 28 opening reading frames, was identified in S. koyangensis SCSIO 5802, and its role in neoabyssomicin/abyssomicin biosynthesis was confirmed via gene inactivation and heterologous expression experiments. Bioinformatics and genomics analyses enabled us to propose a biosynthetic pathway for neoabyssomicin/abyssomicin biosynthesis. Similarly, a protective export system by which both types of compounds are secreted from the S. koyangensis producer was identified, as was a four-component ABC transporter-based import system central to neoabyssomicin/ abyssomicin biosynthesis. Furthermore, two regulatory genes, abmI and abmH, were unambiguously shown to be positive regulators of neoabyssomicin/abyssomicin biosynthesis. Consistent with their roles as positive regulatory genes, the overexpression of abmI and abmH (independent of each other) was shown to improve neoabyssomicin/ abyssomicin titers. Conclusions: These studies provide new insight into the biosynthesis of the abyssomicin class of natural products, and highlight important exploitable features of its BGC for future efforts. Elucidation of the neoabyssomicin/abyssomicin BGC now enables combinatorial biosynthetic initiatives aimed at improving both the titers and pharmaceutical properties of these important natural products-based drug leads

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