天山南北山前盆地中-新生代沉积记录及其动力学分析

It has been long known that intense multiple Mesozoic-Cenozoic intracontinental deformations have controlled the grand scale basin-range structural evolution of the Tianshan and its adjacent basins. So it is important to study the sedimentary records of the piedmont basins along the two sides of the Tianshan synthetically for the continental geodynamic research.We carried out a magnetostratigraphy study on Cretaceous- Tertiary succession and U-Pb dating analysis of detrital zircons from the representative sandstone samples of the Mesozoic-Cenozoic deposits in Kuqa Subbasin, northern Tarim Basin, combining our previous results of multiple depositional records from different profiles including paleocurrent data, conglomerate clast, sandstone framswork grains, detrital heavy minerals and geochemistry analysis, so the multiple intracontinental tectonic processes of Tianshan and their depositional response in the Kuqa Subbasin can be revealed. The results show that the tectonic evolution of the Tianshan Orogen and the sedimentary processes of the Kuqa Subbasin can be divided into four periods: early Triassic(active period), from middle Triassic to late Jurassic(placid period), from early Cretaceous to Tertiary Paleocene(active period) and from Neogene to present (intensely active period). Simultaneously，the depositional records reveal the provenance types and tectonic attributes in different periods. As follows, the lower Triassic with a dominant age ranging from 250 to 290Ma of the Zircons, which were principally derived from alkali feldspar granites and alkaline intrusion obviously, relative to the magma activity in Permian. In middle Triassic-late Jurassic, the two samples collected from the Taliqike formation and the Qiakemake formation respectively show the age peak at 350～450Ma, which was relative to the subduction of the Tarim Block to Yili-Central Tianshan Plate. In this period the provenance of the Kuqa deposits was the Central Tianshan arc orogenic belts distantly with little height predominance.During early Cretaceous-Paleogene, two major zircons age spectra at 240~330Ma and 370~480Ma have been acquired, with some other not dominant age ranges, indicating complicated provenance types. In Neogene, the detrital zircons age dating ranges from 460 to 390 Ma primarily. What’s more, the newer chronology of the stratigraphy and the older source age, indicating that Tianshan was uplifted and exhumated further strongly. Further study on the heavy mineral and the detrital zircons age dating of the Mesozoic-Paleogene representative profiles in southern Junggar Basin, combined with the published results of the sandstone framework grains, we consider that it occurred obvious sedimentary and tectonic changes occurred in the inside of Jurassic, from late Jurassic to early Cretaceous and form early Cretaceous to late Cretaceous. On this faces, there are remarkable changes of the steady minerals and unstable minerals, the sandstone maturity and the age spectra of the detrital zircons. Compared the sedimentary records from the two sides of the Tianshan, We find that they are different obviously since Middle Jurassic. It can be concluded that Tianshan have uplifted highly enough to influence the paleo-climatic. According to the current strata division, the structural activity apparently showed a migration from north to south. That is to say, the South Tianshan uplift later than the north, especially from late Jurassic to early Cretaceous , but it was uplifted and exhumated more strongly. Furthermore, correlating the depositional records and tectonic styles in the Kuqa-South Tianshan basin-range conjugation site in the east with the west, the obvious differentiation between the west and the east from the Cretaceous especially in Tertiary along the Tianshan-Kuqa belt was revealed, probably showing earlier uplifting in the east while greater exhumation depth and sediment rates in the west. In addition, the contacting style of Kuqa subbasin to the Tianshan Orogenic belts and the basement structure are also inconsistent at different basin-range conjugation sites. It is probably controlled by a series of N-S strike adjusting belts within the Kuqa subbasin, or probably correlated with the material difference at the complicated basin-range boundary. The research on the Mesozoic-Cenozoic tectonic-depositional response in the piedmont basins along the two sides of the Tianshan shows that the basin-filling process was controlled by the intracontinental multicyclic basin-range interactions, especially affected by the intense tectonic differentiations of basin-range system, which can’t be illuminated using a single evolutionary model.

磁层－电离层电流的暴时变化以及主磁场对空间环境的影响

Two problems are studied in this thesis, the relationship of the magneto-spheric - ionospheric current systems during storms, and the effects of the main field to the space environment. The thesis includes three parts. 1. Magnetic disturbances caused by magnetospheric - ionospheric current systems Transient variations of the geomagnetic field at middle-low latitudes are mainly caused by the ionospheric dynamo current (IDC), the symmetric ring current (SRC), the partial ring current-region II field-aligned current-ionospheric current system (PRFI), and the region I field-aligned current-ionospheric current system (FACI). The storm on May 1 ～ 6, 1998 is analyzed. Firstly, the S_q-field caused by IDC current is removed by using the modified Hibberd's method in which the effect of SRC is considered. The neglect of SRC-field can give as much as 40% error in S_q-field evaluation. Secondly, the disturbance fields at the middle and low latitudes are separated according to their origins. As a result, the disturbance caused by FACI-current is an important part of the asymmetrical depression of H-component in middle and low latitudes during storms. The results show that the relative intensity of the Sq-field increases in the main phase of the storm and decreases in the recovery phase. The latitudinal gradient of the Sq-field is positive during the whole storm. The storm of May 1 ～ 6, 1998 contains two events. In the first event on May 2, the SRC-field is similar to Dst index. But in the second event on May 4 ～ 5, the SRC-field delays to Dst index, and the SRC-field depresses while the PRFI- and FACI-fields recovery. 2. Analysis of S_q~p variation in CGM coordinates In order to study the conjugation of geomagnetic variations between northern and southern hemispheres, we use the corrected geomagnetic coordinates (CGM) instead of the geomagnetic coordinates (GM) to analyze the S_q~P equivalent current system. The CGM coordinates are built up by International Geomagnetic Reference Field (IGRF) model. The S_q~p variations and equivalent current systems in the northern and southern polar regions are more symmetrical in CGM coordinates than in GM co-ordinates. This fact implies that the current distributions in polar regions are governed by the configuration of the geomagnetic field lines. As the elaborate structure of S_q~p current system in quiet time is obtained, we summarize the seasonal variation of the electrojet in quiet time. 3. The magnetospheric configuration of non-parallel-dipole model The magnetospheric configurations are calculated for two possible geomag-netic field models during the geomagnetic field reversals. These models are the dipole field with the axis to the sun and the quadrupole field model. We use the finite element method to solve the magnetic equation, and use the surface evolution method to solve the equilibrium equation. The results show that the main field greatly affects the space environment.

Disseminação horizontal de genes que codificam para β-lactamases de espectro alargado em isolados de enterobacteriaceae de origem hospitalar

Projeto de Pós-Graduação/Dissertação apresentado à Universidade Fernando Pessoa como parte dos requisitos para obtenção do grau de Mestre em Ciências Farmacêuticas

Quantum chemical study of the effect of precursor stereochemistry on dissociative chemisorption and surface redox reactions during the atomic layer deposition of the transition metal copper

Using quantum chemical calculations, we investigate surface reactions of copper precursors and diethylzinc as the reducing agent for effective Atomic Layer Deposition (ALD) of Cu. The adsorption of various commonly used Cu(II) precursors is explored. The precursors vary in the electronegativity and conjugation of the ligands and flexibility of the whole molecule. Our study shows that the overall stereochemistry of the precursor governs the adsorption onto its surface. Formation of different Cu(II)/Cu(I)/Cu(0) intermediate complexes from the respective Cu(II) compounds on the surface is also explored. The surface model is a (111) facet of a Cu55 cluster. Cu(I) compounds are found to cover the surface after the precursor pulse, irrespective of the precursor chosen. We provide new information about the surface chemistry of Cu(II) versus Cu(I) compounds. A pair of CuEt intermediates or the dimer Cu2Et2 reacts in order to deposit a new Cu atom and release gaseous butane. In this reaction, two electrons from the Et anions are donated to copper for reduction to metallic form. This indicates that a ligand exchange between the Cu and Zn is important for the success of this transmetalation reaction. The effect of the ligands in the precursor on the electron density before and after adsorption onto the surface has also been computed through population analysis. In the Cu(I) intermediate, charge is delocalized between the Cu precursor and the bare copper surface, indicating metallic bonding as the precursor densifies to the surface.

D-Amino acid peptide residualizing agents bearing N-hydroxysuccinimido- and maleimido-functional groups and their application for trastuzumab radioiodination.

INTRODUCTION: Proteins that undergo receptor-mediated endocytosis are subject to lysosomal degradation, requiring radioiodination methods that minimize loss of radioactivity from tumor cells after this process occurs. To accomplish this, we developed the residualizing radioiodination agent N(ϵ)-(3-[(*)I]iodobenzoyl)-Lys(5)-N(α)-maleimido-Gly(1)-D-GEEEK (Mal-D-GEEEK-[(*)I]IB), which enhanced tumor uptake but also increased kidney activity and necessitates generation of sulfhydryl moieties on the protein. The purpose of the current study was to synthesize and evaluate a new D-amino acid based agent that might avoid these potential problems. METHODS: N(α)-(3-iodobenzoyl)-(5-succinimidyloxycarbonyl)-D-EEEG (NHS-IB-D-EEEG), which contains 3 D-glutamates to provide negative charge and a N-hydroxysuccinimide function to permit conjugation to unmodified proteins, and the corresponding tin precursor were produced by solid phase peptide synthesis and subsequent conjugation with appropriate reagents. Radioiodination of the anti-HER2 antibody trastuzumab using NHS-IB-D-EEEG and Mal-D-GEEEK-IB was compared. Paired-label internalization assays on BT474 breast carcinoma cells and biodistribution studies in athymic mice bearing BT474M1 xenografts were performed to evaluate the two radioiodinated D-peptide trastuzumab conjugates. RESULTS: NHS-[(131)I]IB-D-EEEG was produced in 53.8%±13.4% and conjugated to trastuzumab in 39.5%±7.6% yield. Paired-label internalization assays with trastuzumab-NHS-[(131)I]IB-D-EEEG and trastuzumab-Mal-D-GEEEK-[(125)I]IB demonstrated similar intracellular trapping for both conjugates at 1h ((131)I, 84.4%±6.1%; (125)I, 88.6%±5.2%) through 24h ((131)I, 60.7%±6.8%; (125)I, 64.9%±6.9%). In the biodistribution experiment, tumor uptake peaked at 48 h (trastuzumab-NHS-[(131)I]IB-D-EEEG, 29.8%±3.6%ID/g; trastuzumab-Mal-D-GEEEK-[(125)I]IB, 45.3%±5.3%ID/g) and was significantly higher for (125)I at all time points. In general, normal tissue levels were lower for trastuzumab-NHS-[(131)I]IB-D-EEEG, with the differences being greatest in kidneys ((131)I, 2.2%±0.4%ID/g; (125)I, 16.9%±2.8%ID/g at 144 h). CONCLUSION: NHS-[(131)I]IB-D-EEEG warrants further evaluation as a residualizing radioiodination agent for labeling internalizing antibodies/fragments, particularly for applications where excessive renal accumulation could be problematic.

Enhanced surface attachment of protein-type targeting ligands to poly(lactide-co-glycolide) nanoparticles using variable expression of polymeric acid functionality

The density of reactive carboxyl groups on the surface of poly(lactide-co-glycolide) (PLGA) nanoparticles (NP) was modulated using a combination of high-molecular weight (MW) encapped and low MW non-encapped PLGA. Carboxyl groups were activated using carbodiimide chemistry and conjugated to bovine serum albumin and a model polyclonal antibody. Activation of carboxyl,groups in solution-phase PLGA prior to NP formation was compared with a postformation activation of peripheral carboxyl groups on intact NP. Activation before or after NP formation did not influence conjugation efficiency to NP prepared using 100% of the low-MW PLGA. The effect of steric stabilization using poly(vinyl alcohol) reduced conjugation of a polyclonal antibody from 62 mu g/(mg NP) to 32 mu g/(mg NP), but enhanced particulate stability. Increasing the amount of a high-MW PLGA also reduced Conjugation, with the activation post-formation still superior to the preformation approach. Drug release studies showed that high proportions of high-MW PLGA in the NP produced a longer sustained release profile of a model drug (celecoxib). It can be concluded that activating intact PLGA NP is superior to activating component parts prior to NP formation. Also, high MW PLGA could be used to prolong drug release, but at the expense of conjugation efficiency on to the NP surface. (C) 2008 Wiley Periodicals, Inc. J Biomed Mater Res 87A: 873-884, 2008

Immunocolloidal Targeting of the Endocytotic Siglec-7 Receptor Using Peripheral Attachment of Siglec-7 Antibodies to Poly(Lactide-co-Glycolide) Nanoparticles

Purpose: To prepare a nanoparticulate formulation expressing variable peripheral carboxyl density using non-endcapped and endcapped poly(lactide-co-glycolide), conjugated to antibodies recognising the siglec-7 receptor, which is expressed on most acute myeloid leukaemias. The aim is to exploit this receptor as a therapeutic target by constructing an internalising drug-loaded nanoparticle able to
translocate into cytoplasm by siglec receptor-mediated internalisation.

Materials and Methods: Antibodies to the siglec-7 (CD33-like) receptor were conjugated to dye-loaded nanoparticles using carbodiimide chemistry, giving 32.6 mg protein per mg of nanoparticles using 100% of the non-endcapped PLGA. Binding studies using cognate antigen were used to verify preservation of antibody function following conjugation.

Results: Mouse embryonic fibroblasts expressing recombinant siglec-7 receptor and exposed to NileRed-loaded nanoparticles conjugated to antibody accumulated intracellular fluorescence, which was not observed if either antibody or siglec-7 receptor was absent. Confocal microscopy revealed internalised perinuclear cytoplasmic staining, with an Acridine Orange-based analysis showing red staining in localised foci, indicating localisation within acidic endocytic compartments.

Conclusions: Results show antibody-NP constructs are internalised via siglec-7 receptor-mediated internalisation. If loaded with a therapeutic agent, antibody-NP constructs can cross into cytoplasmic
space and delivery drugs intracellularly to cells expressing CD33-like receptors, such as natural killer cells and monocytes.

Crystal structure and ab initio calculations of a cyano-carbamimidic acid ethyl ester

The structure of one tautomer (amine form) of cyano-carbamimidic acid ethyl ester or (amino-ethoxy-methylidene)aminoformonitrile (CAS: 13947-84-7) was determined by single crystal X-ray diffraction. Ab initio quantum chemical calculations at the B3LYP, MP2 and G3 levels were performed to investigate the stability and the formation of the different tautomers and conformers. The calculations indicate that the amine form is the more stable tautomer, showing a high degree of election conjugation. The most stable amine conformer located by the calculations corresponds to the crystallized structure. On the contrary, in the less stable imine form, the conjugation is separated by a N2-C2 single bond. (C) 2007 Elsevier B.V. All rights reserved.

High-performance IQ modulator-based phase conjugator for modular retrodirective antenna array implementation

In this paper, we verify a new phase conjugating architecture suitable for deployment as (lie core building block in retrodirective antenna arrays, which can be scaled to any number of elements in a modular way without impacting on complexity. Our solution is based on a modified in-phase and quadrature modulator architecture, which completely resolves four major shortcomings of the conventional mixer-based approach currently used for the synthesis of phase conjugated energy derived from a sampled incoming wavefront. 1) The architecture presented removes the need for a local oscillator running at twice the RF signal frequency to be conjugated. 2) It maintains a constant transmit power even if receive power goes as low as -120 dBm. 3) All unwanted re-transmit signal products are suppressed by at least 40 dB. 4) The issue of poor RF-IF leakage prevalent in mixer-based phase-conjugation solutions is completely mitigated. The circuit has also been shown to have high conjugation accuracy (better than +/-1 degrees at -60-dBm input). Near theoretically perfect experimental monostatic and bistatic results are presented for a ten-element retrodirective array constructed using the new phase conjugation architecture.

Porphyrin and tetrabenzoporphyrin dendrimers: Tunable membrane-impermeable fluorescent pH nanosensors

The pH dependencies of the UV-vis and fluorescent spectra of new water-soluble dendritic porphyrins and tetrabenzoporphyrins were studied. Because of extended pi-conjugation and nonplanar distortion, the absorption and the emission bands of tetraaryltetrabenzoporphyrins (Ar4TBP) are red-shifted and do not overlap with those of regular tetraarylporphyrins (Ar4P). When encapsulated inside dendrimers with hydrophilic outer layers, Ar(4)Ps and Ar(4)TBPs become water soluble and can serve as pH indicators, with pKs adjustable by the peripheral charges on the dendrimers. Two new dendritic porphyrins, Gen 4 polyglutamic porphyrin dendrimer H2P-Glu(4)OH (1) with 64 peripheral carboxylates and Gen 1 poly(ester amide) Newkome-type tetrabenzoporphyrin dendrimer H2TBP-Nw(1)OH (2) with 36 peripheral carboxylates, were synthesized and characterized. The pKs of the encapsulated porphyrins (pK(H2P-Glu)(OH)(4) = 6.2 and pK(H2TBP)-Nw(1)OH = 6.3) were found to be strongly influenced by the dendrimers, revealing significant electrostatic shielding of the cores by the peripheral charges. The titration curves obtained by differential excitation using the mixtures of the dendrimers were shown to be identical to those determined for the dendrimers individually. Due to their peripheral carboxylates and nanometric molecular size, porphyrin dendrimers cannot penetrate through phospholipid membranes. Dendrimer 1 was captured inside phospholipid liposomes, which were suspended in a solution containing dendrimer 2. No response from 1 was detected upon pH changes in the bulk solution, while the response from 2 was predictably strong. When proton channels were created in the liposome walls, both compounds responded equally to the bulk pH changes. These results suggest that porphyrin dendrimers can be used as fluorescent pH indicators for proton gradient measurements.

Development of a high-throughput enzyme-linked immunosorbent assay for the routine detection of the carcinogen acrylamide in food, via rapid derivatisation pre-analysis

The spontaneous formation of the neurotoxic carcinogen acrylamide in a wide range of cooked foods has recently been discovered. These foods include bread and other bakery products, crisps, chips, breakfast cereals, and coffee. To date, the diminutive size of acrylamide (71.08Da) has prevented the development of screening immunoassays for this chemical. In this study, a polyclonal antibody capable of binding the carcinogen was produced by the synthesis of an immunogen comprising acrylamide derivatised with 3-mercaptobenzoic acid (3-MBA), and its conjugation to the carrier protein bovine thyroglobulin. Antiserum from the immunised rabbit was harvested and fully characterised. it displayed no binding affinity for acrylamide or 3-MBA but had a high affinity for 3-MBA-derivitised acrylamide. The antisera produced was utilised in the development of an ELISA based detection system for acrylamide. Spiked water samples were assayed for acrylamide content using a previously published extraction method validated for coffee, crispbread, potato, milk chocolate and potato crisp matrices. Extracted acrylamide was then subjected to a rapid 1-h derivatisation with 3-MBA, pre-analysis. The ELISA was shown to have a high specificity for acrylamide, with a limit of detection in water samples of 65.7 mu g kg(-1), i.e. potentially suitable for acrylamide detection in a wide range of food commodities. Future development of this assay will increase sensitivity further. This is the first report of an immunoassay capable of detecting the carcinogen, as its small size has necessitated current analytical detection via expensive, slower, physico-chemical techniques such as Gas or Liquid Chromatography coupled to Mass Spectrometry. (c) 2007 Elsevier B.V. All rights reserved.

Self-aligning wireless link using modulated backscatter

A self-tracking (aligning) radio communications system based on the principle of modulated backscatter detection is presented here. Using amplitude-modulated backscatter from a co-operating target, a modified IQ demodulation scheme is used to reproduce automatically and in real time both the received and conjugate of the received phase of an incoming signal. The phase conjugated demodulated IF signal can have incoming backscattered data removed and new data are inserted before being up-converted using IQ single side-band generation so that retro-directive re-transmission can be made to occur. In the absence of the backscattered modulation signal, no phase conjugation and hence no retro-directed re-transmission can occur. The system reported is therefore inherently self-authenticating a facility not readily available from previously reported retro-directive self-tracking systems. © 2010 © The Institution of Engineering and Technology.

Far field subwavelength source resolution using Phase Conjugating Lens Assisted With Evanescent-to-Propagating Spectrum Conversion

The imaging properties of a phase conjugating lens operating in the far field zone of the imaged source and augmented with scatterers positioned in the source near field region are theoretically studied in this paper. The phase conjugating lens consists of a double sided 2D assembly of straight wire elements, individually interconnected through phase conjugation operators. The scattering elements are straight wire segments which are loaded with lumped impedance loads at their centers. We analytically and numerically analyze all stages of the imaging process; i) evanescent-to-propagating spectrum conversion; ii) focusing properties of infinite or finite sized phase conjugating lens; iii) source reconstruction upon propagating-to-evanescent spectrum conversion. We show that the resolution that can be achieved depends critically on the separation distance between the imaged source and scattering arrangement, as well as on the topology of the scatterers used. Imaged focal widths of up to one-seventh wavelength are demonstrated. The results obtained indicate the possibility of such an arrangement as a potential practical means for realising using conventional materials devices for fine feature extraction by electromagnetic lensing at distances remotely located from the source objects under investigation

An improved immunoassay for detection of saxitoxin by surface plasmon resonance biosensors

Saxitoxin and its analogs, the causative agents of paralytic shellfish poisoning (PSP), are a worldwide threat to seafood safety. Effective monitoring of potentially contaminated fishing areas as well as screening of seafood samples is necessary to adequately protect the public. While many analytical methods exist for detecting paralytic shellfish toxins (PSTs), each technique has challenges associated with routine use. One recently developed method [1] that overcomes ethical or performance-related issues of other techniques is the surface plasmon resonance (SPR) bioassay. Notwithstanding the advantages of this method, much research remains in optimizing the sensor substrate and assay conditions to create a robust technique for rapid and sensitive measurement of PSTs. This manuscript describes a more rigorous and stable SPR inhibition immunoassay through optimization of the surface chemistry as well as determination of optimum mixture ratios and mixing times. The final system provides rapid substrate formation (18 h saxitoxin conjugation with low reagent consumption), contains a reference channel for each assay, and is capable of triplicate measurements in a single run with detection limits well below the regulatory action level. Published by Elsevier B.V.

Acetylation of O-specific lipopolysaccharides from Shigella flexneri 3a and 2a occurs in Escherichia coli K-12 carrying cloned S. flexneri 3a and 2a rfb genes

Most of the Shigella flexneri O-specific serotypes result from O-acetyl and/or glucosyl groups added to a common O-repeating unit of the lipopolysaccharide (LPS) molecule. The genes involved in acetylation and/or glucosylation of S. flexneri LPS are physically located on lysogenic bacteriophages, whereas the rfb cluster contains the biosynthesis genes for the common O-repeating unit (D.A.R. Simmons and E. Romanowska, J. Med. Microbiol. 23:289-302, 1987). Using a cosmid cloning strategy, we have cloned the rfb regions from S. flexneri 3a and 2a. Escherichia coli K-12 containing plasmids pYS1-5 (derived from S. flexneri 3a) and pEY5 (derived from S. flexneri 2a) expressed O-specific LPS which reacted immunologically with S. flexneri polyvalent O antiserum. However, O-specific LPS expressed in E. coli K-12 also reacted with group 6 antiserum, indicating the presence of O-acetyl groups attached to one of the rhamnose components of the O-repeating unit. This was confirmed by measuring the amounts of acetate released from purified LPS samples and also by the chemical removal of O-acetyl groups, which abolished group 6 reactivity. The O-acetylation phenotype was absent in an E. coli strain with an sbcB-his-rfb chromosomal deletion and could be restored upon conjugation of F' 129, which carries sequences corresponding to a portion of the deleted region. Our data demonstrate that E. coli K-12 strains possess a novel locus which directs the O acetylation of LPS and is located in the sbcB-rfb region of the chromosomal map.