4.8 nm Concave {M_(72)}(M=Co,Ni,Fe) metal-organic polyhedra capped by 18 calixarenes

Three 4.8 nm isostructural{M₇₂}(M=Co^Ⅱ for CIAC-128,Ni^Ⅱ for CIAC-129,Fe^Ⅱ for CIAC-130) metal-organic polyhedra(MOPs) are constructed by eighteen M₄-p-tert-butylthiacalix[4]arene (M₄-TC4A) units bridged via sixteen four-connected 5,5′-(1H-1,2,4-triazole-3,5-diyl) diisophthalic acid (H₄TADIPA) linkers.These MOPs are featured with a rarely reported concave coordination cage,which can be simplified as a squeezed double-decker hexagonal prism pressed from the top and bottom hexagonal faces.Furthermore,CIAC-128,CIAC-129 and CIAC-130 are the highest nuclearity discrete clusters of Co,Ni and Fe reported so far.CIAC-128 has higher separation selectivity of C₃H₈ than CH₄ under ambient conditions,and also exhibits separation selectivity for C₂H₆/CH₄,C₂H₂/CH₄,and C₂H₄/CH₄.In addition,CIAC-128 can provide the cavity for the confined synthesis of noble metal nanoclusters such as Pd nanoclusters and the resulting Pd@CIAC-128 hybrids show higher electrocatalytic activity than commercial Pt/C towards hydrogen evolution reaction (HER).     

实际量子密钥分配扩展BB84协议窃听下的安全性分析

考虑强衰减激光脉冲技术实现的准单光子源和量子信道损耗以及窃听者Eve窃听能力有限等实际情况, 提出了一种窃听装置;同时对扩展BB84协议的各种窃听做了全面分析,计算得出发送者Alice/窃听者Eve所获得的交互信息量和发送者Alice/接收者Bob所能容忍的误码率上限,以此作为检测量子信道安全性的标准,同时得出Breidbart基/分束攻击相结合的方法是比截取/重发更为有效的窃听方案.     

Synthesis and characterization of visible light responsive N-TiO2 mixed crystal by a modified hydrothermal process

N doped TiO₂ with anatase and rutile mixed crystal were prepared by using tetrabutyl titanate as the precursor via a modified hydrothermal process and calcination at 320 °C. The microstructure and morphology of samples were characterized by XRD, UV-vis-DRS, FTIR and XPS. The results showed that N-TiO₂ particles were crystallized to anatase and rutile mixed crystal structure; they were presented narrow particle size distribution, and the average particle size was ca. 13.5 nm calculated from XRD results. It was found that the N-doped TiO₂ particles showed strong visible-light absorption and high photocatalytic activity for the mineralization of Rhodamine B under irradiation by visible light (400-500 nm). The high visible-light photocatalytic activity of the obtained N-doped TiO₂ might result from the synergetic effect of nitrogen doping and the mixed lattice structure of N-TiO₂. Possible mechanism of N-TiO₂ mixed crystal formed under hydrothermal conditions was discussed.     

扩散型气柱界面R-M失稳中混合率的实验研究

Richtmyer-Meshkov(R-M)不稳定性普遍存在于众多工程问题中,激波管实验是研究R-M失稳问题的主要手段.高精度的平面激光诱导荧光(planar laser-induced fluorescence,PLIF)技术具有分子量级的示踪能力,可获得界面气体浓度(摩尔分数)分布,为研究界面失稳混合问题提供了有力工具.在弱激波(Ma=1.25)冲击扩散型气柱界面实验中,采用PLIF技术对R-M失稳引起的SF6-Air界面混合问题进行了研究.通过改变椭圆形初始界面的长短轴比,得到了3种扩散型初始界面失稳演化过程中气体摩尔分数,观察到了斜压机制下界面的简单拉伸、二次不稳定性、挤压射流等现象.利用浓度分布进一步得到了界面的瞬时混合率,通过瞬时混合率、界面整体平均混合率以及混合率的概率密度分布,分析了界面在不同演化阶段的界面混合特征,初步讨论了界面失稳混合的机制.演化初期,界面在斜压涡的作用下发生拉伸卷曲,通过增大浓度梯度来促进界面的混合.当演化进一步发展,二次不稳定性出现后,界面通过小尺度对流的方式达到湍流混合状态,而浓度梯度驱使的分子间混合逐渐减弱.由浓度梯度引起的扩散与由二次不稳定性引起的对流存在着"竞争"关系,二者共同主导了界面的混合.     

高超声速飞行器气动热关联换算方法研究

气动热风洞实验是地面研究和预测飞行器气动热环境的重要手段之一, 但由于风洞实验模拟能力的限制, 风洞实验的流场参数和模型的几何尺度都会与实际飞行情况存在一定的差别, 导致地面风洞实验中得到的模型表面气动加热率数据无法直接用于飞行条件下的热环境预测和热防护设计. 以往通过针对具体飞行器的试验结果进行数据拟合后外插的气动热关联换算方法指向性较强, 没有考虑到气动热的具体影响参数, 存在一定局限性, 难以外推应用于其他外形的飞行器. 为解决通过气动热风洞实验数据外推预测飞行条件下气动热的技术难题, 基于无量纲NS方程和边界层理论分析研究了影响气动热的主要参数, 并通过推导化简边界层近似解热流公式, 针对层流流态建立了气动热关联换算方法, 可以考虑当地边界层外缘参数的影响, 具有一定通用性. 在此基础上, 利用建立的方法将Reentry-F飞行器缩比模型的风洞实验数据换算到该飞行器飞行条件下的典型工况, 并与飞行测量结果进行了比较, 外推预测结果与飞行测量结果符合较好, 表明建立的关联方法可以用于气动热风洞实验数据的外推换算.      

Cytosolic escape of mitochondrial DNA triggers cGAS-STING-NLRP3 axis-dependent nucleus pulposus cell pyroptosis

Low back pain (LBP) is a major musculoskeletal disorder and the socioeconomic problem with a high prevalence that mainly involves intervertebral disc (IVD) degeneration, characterized by progressive nucleus pulposus (NP) cell death and the development of an inflammatory microenvironment in NP tissue. Excessively accumulated cytosolic DNA acts as a damage-associated molecular pattern (DAMP) that is monitored by the cGAS-STING axis to trigger the immune response in many degenerative diseases. NLRP3 inflammasome-dependent pyroptosis is a type of inflammatory programmed death that promotes a chronic inflammatory response and tissue degeneration. However, the relationship between the cGAS-STING axis and NLRP3 inflammasome-induced pyroptosis in the pathogenesis of IVD degeneration remains unclear. Here, we used magnetic resonance imaging (MRI) and histopathology to demonstrate that cGAS, STING, and NLRP3 are associated with the degree of IVD degeneration. Oxidative stress induced cGAS-STING axis activation and NLRP3 inflammasome-mediated pyroptosis in a STING-dependent manner in human NP cells. Interestingly, the canonical morphological and functional characteristics of mitochondrial permeability transition pore (mPTP) opening with the cytosolic escape of mitochondrial DNA (mtDNA) were observed in human NP cells under oxidative stress. Furthermore, the administration of a specific pharmacological inhibitor of mPTP and self-mtDNA cytosolic leakage effectively reduced NLRP3 inflammasome-mediated pyroptotic NP cell death and microenvironmental inflammation in vitro and degenerative progression in a rat disc needle puncture model. Collectively, these data highlight the critical roles of the cGAS-STING-NLRP3 axis and pyroptosis in the progression of IVD degeneration and provide promising therapeutic approaches for discogenic LBP.Subject terms: Cell death, Diseases     

An adaptive trust region method and its convergence

In this paper, a new trust region subproblem is proposed. The trust radius in the new subproblem adjusts itself adaptively. As a result, an adaptive trust region method is constructed based on the new trust region subproblem. The local and global convergence results of the adaptive trust region method are proved. Numerical results indicate that the new method is very efficient.     

同伦分析方法：一种新的求解非线性问题的近似解析方法

本文描述了一种称为“同伦分析方法”（ＨＡＭ）的新的求解非线性问题的近似解析方法之基本思想·不同于摄动展开方法，“同伦分析方法”的有效性不依赖于所研究的非线性方程中是否含有小参数·因此，该方法提供了一个强有力的分析非线性问题的新工具·作为示例，我们应用一个典型的非线性问题来说明该方法的有效性及其巨大潜力·     

页岩矿物不同润湿性表征与吸附微观机理

无机矿物作为页岩气吸附的重要载体,其表面性质对甲烷吸附能力有着重要影响,而润湿性作为固体重要表面性质之一,对矿物气体吸附能力的影响不可忽视.文章以蒙脱石和石英作为研究对象,通过对矿物表面甲基化(-CH₃)和羟基化(-OH)处理来改变其润湿性,以探究无机矿物表面润湿性对甲烷吸附能力的影响.采用分子动力学方法研究矿物体系的润湿性,用接触角对润湿性进行定量表征,并构建纳米狭缝,结合巨正则蒙特卡罗方法模拟润湿性改变前后,CH₄在矿物中的吸附变化.研究结果表明,水滴在羟基化矿物表面迅速破裂并铺展在矿物表面,而在甲基化表面铺展程度较小,普遍呈半球形.羟基化蒙脱石和石英表面的润湿接触角分别为12.7°和26.5°,均小于其甲基化表面接触角62.5°和85.7°.甲基化矿物甲烷吸附量均高于其羟基化,气体几乎大都以吸附状态位于孔隙壁面,随着矿物亲水性的减弱,其对甲烷吸附能力增强.     

掺铥氟磷玻璃的结构、热学性质和光谱性质

制备了不同Al(PO3)3含量的掺铥系列氟磷玻璃,研究了其结构、热稳定性和光谱性质。随着Al(PO3)3含量的增加,该系列玻璃的密度降低,折射率增加,差热分析表明,转变温度、析晶起始温度、析晶峰温度和熔化温度增加。Al(PO3)3摩尔浓度在7%~9%时析晶稳定性最佳。采用归一化的拉曼光谱分析了材料的结构和声子状况,对于该系列氟磷玻璃,Al(PO3)3含量的增加不会影响声子能量,但使声子密度增大。测试了样品的吸收光谱,Tm3 的3H6→3F4在第三通信窗口的L波段有明显吸收。与在其它玻璃基质中相比,Tm3 的3F4能级对应能量偏高,3H4能级对应能量偏低,使得3H4→3F4跃迁波长较大,接近于增益迁移光纤放大器的放大波长。扎得奥菲而特(Judd-Ofelt)理论分析表明随着Al(PO3)3含量增加,离子强度参量Ω2增大,Ω6保持相对稳定,Tm3 的能级寿命降低。