催化化学发光分析系统研究进展

催化化学发光是分子通过催化剂表面时被氧气氧化过程中产生的一种光辐射现象。在过去的三十几年里,催化化学发光技术发展迅速,特别是在传感器方面快速发展,成为一项新型分析检测技术,在公众安全、排放检测、环境保护等方面发挥了巨大的作用。基于催化发光技术设计的传感器具有检测限低、灵敏度高、快速、仪器简单易操作、易实现小型化,便携等优点,在无机小分子气体及易挥发有机物的分析检测中展现了其独特的优势。应用于催化发光的催化材料发展至今已达上千种,囊括了金属、金属氧化物,非金属氧化物、硫化物、硒化物、金属盐类、有机物、陶瓷玻璃类等各类材料;复合材料的应用丰富了催化材料的种类;纳米新材料的引入为其发展提供了新的契机;材料的形貌等也得以深入研究。催化发光新技术也不断发展,催化发光与其他技术(雾化、分离富集、等离子体等)联用的发展,静态催化发光技术、多级催化发光技术、循环催化发光技术等的开发应用进一步提高了催化法光分析系统的灵敏度与选择性,拓展了催化发光的应用范围。本文综述了近年来催化发光的催化材料、联用技术及其他新技术的发展,并对其发展趋势进行了展望。     

The Progress on Cataluminescence-Based Analytical SystemSCIEI北大核心CSCD

Cataluminescence(CTL) is a phenomenon of light radiation generated when analyte moleculars were oxidized by catalyst. In the past few decades, CTL has developed rapidly and become a promising detection technique, especially in gas sensing, and has attracted much attention of researchers for its potential versatile applications in emission control, public safety, and environmental protection. The analytical system based on CTL has low detection limit, high sensitivity and simple instrument which easy to operate, which shows huge advantages in the detection of inorganic gases and volatile organic compounds. The library of sensing materials has been greatly enriched to thousands kinds, which contains metals, metal/non-metal oxides, sulfide, metal salts, organic compounds, ceramic, glass and other types of materials; Composite materials have been developed; The decreasing of material dimensions to nanoscale provided new opportunities for its development; The morphology of material has also been explored. Some novel hyphenated techniques based on CTL coupled to other techniques including preconcentration/sepration, nebulization, plasma have been developed, as well as some new CTL technique including static CTL, cyclic CTL and ect. Thanks to development of sensing material and the appearance of these novel techniques, the selectivity and sensitivity of CTL system has been improved, and the range of CTL application has been extended. In this article, the progress made in the field of cataluminescence, especially in latest developments of analytical applications were reviewed. The catalysts used in CTL, the recent novel CTL techniques were sumerized. The future of the cataluminescence was also forecasted.     

SnO2-碳纳米管复合纳米材料催化发光传感器测定甲醇

以碳纳米管（CNT）为模板，采用液相沉积法合成了SnO2-CNT复合纳米材料。建立了一种SnO2-CNT复合纳米材料测定甲醇的纳米催化发光传感船，并测定了甲醇含量，甲醇的线性范围在50-3000ppm，探讨了SnO2-CNT复合纳米材料催化发光传感器测定甲基叔丁基醚（MTBE）中甲醇的可行性。     

Reveal the large open-circuit voltage deficit of all-inorganicCsPbIBr2 perovskite solar cells

Due to excellent thermal stability and optoelectronic properties, all-inorganic perovskite is one of the promising candidates to solve the thermal decomposition problem of conventional organic—inorganic hybrid perovskite solar cells (PSCs), but the larger voltage loss (V_loss) cannot be ignored, especially CsPbIBr₂, which limits the improvement of efficiency. To reduce V_loss, one promising solution is the modification of the energy level alignment between the perovskite layer and adjacent charge transport layer (CTL), which can facilitate charge extraction and reduce carrier recombination rate at the perovskite/CTL interface. Therefore, the key issues of minimum V_loss and high efficiency of CsPbIBr₂-based PSCs were studied in terms of the perovskite layer thickness, the effects of band offset of the CTL/perovskite layer, the doping concentration of the CTL, and the electrode work function in this study based on device simulations. The open-circuit voltage (V_oc) is increased from 1.37 V to 1.52 V by replacing SnO₂ with ZnO as the electron transport layer (ETL) due to more matching conduction band with the CsPbIBr₂ layer.     

CTLA-4 blockade during dendritic cell based booster vaccination influences dendritic cell survival and CTL expansion

Dendritic cells (DCs) are potent antigen-presenting cells and critical for the priming of CD8+ T cells. Therefore the use of these cells as adjuvant cells has been tested in a large number of experimental and clinical vaccination studies, in particular cancer vaccine studies. A number of protocols are emerging that combine vaccination with CTL expanding strategies, such as e.g. blockade of CTLA-4 signalling. On the other hand, the lifespan and in vivo survival of therapeutic DCs have only been addressed in a few studies, although this is of importance for the kinetics of CTL induction during vaccination. We have previously reported that DCs loaded with specific antigens are eliminated by antigen specific CTLs in vivo and that this elimination affects the potential for in vivo CTL generation. We now show that CTLA-4 blockade increases the number of DC vaccine induced LCMV gp33 specific CTLs and the lysis of relevant in vivo targets. However, the CTLA-4 blockage dependent expansion of CTLs also affect DC survival during booster DC injections and our data suggest that during a booster DC vaccine, the largest increase in CTL levels is already obtained during the first vaccination.     

Squared Eigenfunction Symmetries for the BTL and CTL Hierarchies

In this paper, the squared eigenfunction symmetries for the BTL and CTL hierarchies are explicitly constructed with the suitable modification of the ones for the TL hierarchy, by considering the BTL and CTL constraints. Also the connections with the corresponding additional symmetries are investigated: the squared eigenfunction symmetry generated by the wave function can be viewed as the generating function for the additional symmetries.     

Charge transfer luminescence kinetics in a YAG:Yb monocrystal and ceramics

The results of a study of charge transfer luminescence (CTL) in a YAG:Yb monocrystal and trans-parent ceramics obtained by vacuum sintering and nanocrystalline (VSN) technology from a weakly agglomerated powder are presented. The kinetics of CTL decay at temperatures of 8, 100, and 300 K and different excitations were obtained. The results of the measurements are analyzed from the viewpoint of comparison of monocrystal and ceramics properties. The high quality of the latter is demonstrated.     

Single and multi-section CTL and branch-line CPW directional couplers with broadband performances for SIMMWIC

Single and multisection branch-line and coupled transmission line (CTL) directional couplers have been implemented in coplanar waveguide (CPW)-technology, showing broadband performances. The branch-line and CTL couplers had a phase balance of ±5° and a power variation of 1.5 dB in the coupling over a bandwidth of greater than 25% and 75% respectively. The experimental values for the couplers were found to agree well with simulated results. The CPW couplers provide larger bandwidth than comparable microstrip couplers. Investigation on different feeding structure for the branch-line couplers is also presented.     

Trapping and self-trapping in ytterbium-doped oxides with charge transfer luminescence

Temperature dependence of the charge transfer luminescence (CTL) of Yb-doped yttrium aluminum garnet Y₃Al₅O₁₂-Yb (YAG-Yb) and Yb-doped lutetium aluminum perovskite LuAlO₃-Yb (LuAP-Yb) crystals under X-ray excitation and their thermostimulated luminescence are investigated in the temperature range 30-350 K and compared to those of undoped crystals. Simulation using a set of kinetic equations describing the processes of creation of excitons, electron-hole pairs, their trapping and self-trapping, radiative relaxation and quenching is presented for the systems under investigation to analyze qualitatively two different types of experimentally observed temperature dependences: CTL yield decline with the temperature decrease below 110 K as in case of YAG-Yb and constant yield in the same temperature range as in case of LuAP-Yb.     

Synchronized frames for Gödel's universe

We exhibit Gödel's geometry in terms of a set of gaussian systems of coordinates, the union of which constitutes a complete cover for the whole manifold. We present a mechanism which induces a particle to follow a closed time-like line (CTL) present in this geometry. We generalize the construction of special class of observers (Generalized Milne Observers) which provides a way to define the largest causal domain allowing a standard field theory to be developed.     

Quasiparticle excitations and charge transition levels of oxygen vacancies in hafnia

We calculate the quasiparticle defect states and charge transition levels (CTLs) of oxygen vacancies in monoclinic hafnia using density functional theory (DFT) and the GW method. We introduce the criterion that the quality and reliability of CTLs may be evaluated by calculating the same CTL via two physical paths and show that it is necessary to include important electrostatic corrections previously neglected within the supercell DFT + GW approach. Contrary to previous reports, the oxygen vacancies in hafnia are large positive U centers, where U is the defect charging energy.     

Detection of Binding of a Synthetic Granzyme B-like Peptide Fluorescent Conjugate within Platelet-like Structures in Cancer-related Peripheral Blood Specimens and Tissue Sections

Platelets and cytotoxic T lymphocytes (CTL) are important whole blood components in peripheral blood. Studies have shown that platelets, from precursor megakaryocytes, are significant factors in cancer prognosis, cancer progression, and metastasis; but a direct platelet-cancer relationship remains unclear. CTL play an essential role in cancer surveillance by inducing cancer cell death with granzyme B. A recent report has shown the presence of binding targets with binding affinity to a synthetic granzyme B-like peptide fluorescent conjugate (GP1R) in different types of cancer cells grown in vitro. It suggests that these binding targets may serve as a “universal-pathologic-biomarker”. It is not known if similar biomarkers may be present in platelets of cancer patients. We show with fluoroscopic images that GP1R can bind to binding targets: 1) within platelets in methanol-fixed whole blood smears of patients with breast cancer and lung cancer, and 2) within platelet-like structures in formalin-fixed-paraffin-embedded (FFPE) nude mouse xenogeneic breast tumor tissues. Samples without cancer-association displayed no discernible GP1R-binding in platelet-like structures. Our data demonstrate for the first time that a similar “universal-pathologic-biomarker” detectable by GP1R-binding is present in circulating platelets of cancer patients. The data depict a co-existence of animal-platelets and human-breast cancer cells, both have a common pathologic biomarker detectable by GP1R, in the tumor growth. The fluoroscopic images indicate a visual direct connection between pathologic platelets and cancer. These preliminary results may lead to developments of novel platelet-based cancer diagnostics and therapeutics and a better understanding of the potential multifunction of GP1R and its relationship to megakaryocytes and PD1.     

Detection of Cancer Cell Death Mediated by a Synthetic Granzyme B-like Peptide Fluorescent Conjugate and the same Peptide Binding in Bacteria

Granzyme-mediated apoptosis, supported by pore-forming perforin, plays an important role in CD8+ T lymphocytes (CTL)-dependent cellular immunity protection against both cancer and viral infection. Quantitative and qualitative problems with CTL are potential contributing factors to disease progression. The feasibility of developing CTL-independent cellular immunity is desired but must first overcome the barrier of CTL-independent target cell recognition. Granzyme B with its strong pro-apoptotic activity in many different target cells is investigated for use in the CTL-independent cellular immunity approach, and granzyme B or its bioactive peptides without the enzymatic activity are more desirable for use. Native granzyme B with enzymatic activity is usually investigated in cancer cells for its mediation of apoptosis by detection of DNA fragmentation. Detection of cell death mediated by such peptides in cancer cells is needed to demonstrate the potential therapeutic purposes. We show with never-before-seen microscopic images using fluorescence microscopy that a synthetic granzyme B-like peptide fluorescent conjugate (GP1R) can: 1) mediate cell death of different cancer cells via membrane extrusion, 2) bind to constitutively expressed binding targets in different cancer cells and bacteria, and 3) promote bacterial phagocytosis. The putative binding targets may serve as a universal pathologic biomarker detectable by GP1R. Our data taken together demonstrate the potential applications of GP1R for use in CTL-independent target cell recognition and target cell death induction. It may lead to development of rapid targeted detection and new treatment of cancer, viral and bacterial infections. The new treatment may show mutual benefits for two or more diseases.     

Frequency Reconfigurable and Multifunctional Metastructure Regulated by Nematic Liquid Crystal: Broadband Circular to Linear Polarization Converter

With the tunability of the nematic liquid crystal (NLC), a broadband frequency reconfigurable and versatile metastructure (MS) is proposed and theoretically investigated in this paper, combining circular-to-linear (CTL) polarization conversion (PC) and circular-to-circular (CTC) PC simultaneously. The MS is composed of two via-coupled modules, which can respond differently to the incident waves. Each module is connected utilizing a metal via a column, thus exceedingly enhancing the energy transmission and reducing the loss when transmitting. When the applied bias voltage (V_bias) is 0 V, the NCL molecules follow the initial orientation. The MS converts the incident right circular polarized (RCP) waves into linear polarized (LP) waves within 8.11–9.95 gigahertz (GHz) with a relative bandwidth of 20.38% and achieves the PC of left circular polarized (LCP) into RCP waves. As the V_bias reaches 20 V, the original operating interval reconfigures and shifts overall toward a lower frequency. The bandwidth of CTL is 7.66–9.02 GHz, and the CTC PC is broadened to 20.20%. Meanwhile, the structure justification is verified, and the inducing mechanism of PC is expounded. Possessing the merits of versatile collaborative processing and wide operating bands, such an MS is promising to be a polarization-controlled application candidate and enrich multifunctional designs.     

A new indicator to measure the noise impact around airports: The Real Estate Tolerance Level (RETL) – Case study around Charles de Gaulle Airport

The Community Tolerance Level (CTL) is a new indicator which characterizes the impact of aircraft noise around local airport. It corresponds to the exposure sound level (DENL or DNL) where 50% of the population is highly annoyed. Inspired by this indicator, this paper aims at calculating the Real Estate Tolerance Level (RETL) which corresponds to the exposure sound level where a property price is 50% depreciated compared to the price of the same property which would be situated in an area whose DENL is below 50 dB(A). The use of a notarial database analyzed with the Hedonic Price Model (HPM) made it possible to calculate the percentage of property price depreciation around CDG airport, with 1-dB steps of DENL, and so far to calculate the RETL. 19,891 house transactions and 23,264 apartments have been localized with a Geographic Information Systems (GIS) and crossed with the Sound Environment Curves provided by Airport of Paris. The RETL value for single houses and for apartments around CDG is 75.8 dB. It is comparable to the mean CTL value which has been estimated to 73.3 dB from the DNL data of 43 airports over the world (about 73.9 dB from DENL data). The RETL is predictable without field survey and could characterize the impact of aircraft noise around local airports. It could be a good indicator to follow the evolution of population tolerance over the years.     

ESR investigations of burnt soil

Electron spin resonance (ESR) of transition metal ions (Mn^2?, Fe³⁺), radiation induced centres and pyrolytically formed radicals was studied to distinguish between burnt and unburnt soil. A testfire place and samples from an archaeological site were analyzed. The concentration of radiation induced centres decreases and pyrolytically formed radicals appear in a thermal annealing experiment. The spectral pattern of iron and manganese resonances changes during the heating process. These signals are useful to estimate temperature and atmosphere of the heating event. Chemithermoluminescence (CTL) of the soil was studied and could reveal its thermal history, too.     

操作参数对PEM燃料电池中水迁移的影响

质子膜内水分和阴极多孔电极中液态水含量是PEM燃料电池正常运行的控制因素。本文给出了一个用于研究PEM燃料电池内水迁移的稳态、等温、两相流模型。模型耦合了连续方程、动量守恒方程和物质守恒方程,以及水在质子膜中传递方程。运用试验结果验证了模型的有效性。分析模拟结果表明,增大系统操作压力、升高电池操作温度和降低加湿温度将会使质子膜中水的净迁移通量增大;增大操作压力、降低操作温度和升高加湿温度会增加阴极CTL与GDL界面上液态水含量。     

Study of the eigenwaves of a coplanar transmission line using the method of partial operator inversion

We propose a partial inversion procedure for the Cauchy singular integral and the integral with a logarithmic singularity determined on a finite set of bounded intervals. On the basis of this procedure, we constructed an electrodynamic model of a shielded coplanar transmission line (CTL). The results of calculation of the spectral characteristics and eigenwave field distributions of this structure are presented and the data on convergence of the approximate solution are given. Volga State Academy of Telecommunications and Information Sciences, Samara, Russia. Translated from Izvestiya Vysshikh Uchebnykh Zavedenii, Radiofizika, Vol. 43, No. 6, pp. 552–561, June, 2000.     

Use of ultraviolet-light irradiated multiple myeloma cells as immunogens to generate tumor-specific cytolytic T lymphocytes

Background

As the eradication of tumor cells in vivo is most efficiently performed by cytolytic T lymphocytes (CTL), various methods for priming tumor-reactive lymphocytes have been developed. In this study, a method of priming CTLs with ultraviolet (UV)-irradiated tumor cells, which results in termination of tumor cell proliferation, apoptosis, as well as upregulation of heat shock proteins (HSP) expression is described.

Methods

Peripheral blood mononuclear cells (PBMC) were primed weekly with UV-irradiated or mitomycin-treated RPMI 8226 multiple myeloma cells. Following three rounds of stimulation over 21 days, the lymphocytes from the mixed culture conditions were analyzed for anti-MM cell reactivity.

Results

By day 10 of cultures, PBMCs primed using UV-irradiated tumor cells demonstrated a higher percentage of activated CD8+/CD4- T lymphocytes than non-primed PBMCs or PBMCs primed using mitomycin-treated MM cells. Cytotoxicity assays revealed that primed PBMCs were markedly more effective (p < 0.01) than non-primed PBMCs in killing RPMI 8226 MM cells. Surface expression of glucose regulated protein 94 (Grp94/Gp96) and Grp78 were both found to be induced in UV-treated MM cells.

Conclusion

Since, HSP-associated peptides are known to mediate tumor rejection; these data suggest that immune-mediated eradication of MM cells could be elicited via a UV-induced HSP process. The finding that the addition of 17-allylamide-17-demethoxygeldanamycin (17AAG, an inhibitor of HSP 90-peptide interactions) resulted in decreased CTL-induced cytotoxicity supported this hypothesis. Our study, therefore, provides the framework for the development of anti-tumor CTL cellular vaccines for treating MM using UV-irradiated tumor cells as immunogens.