KIT-6负载CeO2催化CO2和甲醇合成碳酸二甲酯

采用不同老化温度(80、100、120和150℃)合成了一系列KIT-6载体,并通过浸渍法制备了相应的CeO_2/KIT-6催化剂。结合X射线衍射、N_2物理吸附、NH_3程序升温脱附、CO_2程序升温脱附、透射电子显微镜、傅里叶变换红外光谱和X射线光电子能谱等表征结果,详细考察了老化温度对KIT-6结构以及CeO_2/KIT-6催化剂直接催化CO_2和甲醇合成碳酸二甲酯(DMC)反应活性的影响。结果表明,不同老化温度下制备的KIT-6均保持其独特的三维孔道结构。随着老化温度升高,KIT-6比表面积先增大后减小,当老化温度为100℃时,KIT-6比表面积达到最大(683 m~2·g~(-1))。KIT-6较高的比表面积有利于提高CeO_2分散度,进而提高暴露的活性位点数量,催化活性随催化剂表面中等碱/酸性吸附位数量和Ce~(3+)含量的增加而逐渐提高。其中,CeO_2/100-KIT-6催化剂中CeO_2颗粒尺寸最小(5.9 nm),暴露的活性位数量最高,催化活性最佳。随后,考察了反应温度和压力对CeO_2/100-KIT-6催化活性的影响。随着反应温度提高,催化活性先升高后降低,当反应温度为140℃时,催化活性最高;且催化活性随反应压力的提高而逐渐增加。在反应温度为140℃、压力为6.8 MPa条件下,催化剂经6次循环后,DMC收率由15 mmol·g_(CeO_2)~(-1)逐渐降低至2.8 mmol·g_(CeO_2)~(-1),原因归结为反应过程中CeO_2纳米颗粒发生团聚,使暴露出的活性位数量减少。     

Dissipative quantum phase transition in a biased Tavis-Cummings model

We study the dissipative quantum phase transition(QPT)in a biased Tavis–Cummings model consisting of an ensemble of two-level systems(TLSs)interacting with a cavity mode,where the TLSs are pumped by a drive field.In our proposal,we use a dissipative TLS ensemble and an active cavity with effective gain.In the weak drive-field limit,the QPT can occur under the combined actions of the loss and gain of the system.Owing to the active cavity,the QPT behavior can be much differentiated even for a finite strength of the drive field on the TLS ensemble.Also,we propose to implement our scheme based on the dissipative nitrogen-vacancy(NV)centers coupled to an active optical cavity made from the gainmedium-doped silica.Furthermore,we show that the QPT can be measured by probing the transmission spectrum of the cavity embedding the ensemble of the NV centers.     

A new probe of neutron skin thickness

The correlation between neutron-to-proton yield ratio (R_np) and neutron skin thickness (δ_np) in neutron-rich projectile induced reactions is investigated within the framework of the Isospin-Dependent Quantum Molecular Dynamics (IQMD) model. The density distribution of the Droplet model is embedded in the initialization of the neutron and proton densities in the present IQMD model. By adjusting the diffuseness parameter of neutron density in the Droplet model for the projectile, the relationship between the neutron skin thickness and the corresponding R_np is obtained. The results show strong linear correlation between R_np and δ_np for neutron-rich Ca and Ni isotopes. It is suggested that R_np may be used as an experimental observable to extract δ_np for neutron-rich nuclei, which is very interesting in the study of the nuclear structure of exotic nuclei, the equation of state (EOS) of asymmetric nuclear matter and neutron-rich matter in astrophysics, etc.     

胞嘧啶核苷在纳米银膜上的NIR-SERS光谱检测

采用一种高活性的纳米银膜作为表面增强拉曼散射(SERS)基底,以近红外激光(785 nm)作为激发光源,对胞嘧啶核苷(胞苷)水溶液(10-2～10-8 mol·L-1)进行了近红外表面增强拉曼散射(NIR-SERS)光谱检测。实验结果表明,当胞苷水溶液浓度等于或低于10-7 mol · L-1时,可在300～2 000 cm-1范围内获得信噪比较好的NIR-SERS光谱。将胞苷水溶液(10-2～10-5 mol · L-1)分别滴在10片不同的纳米银薄膜上进行检测,结果表明该纳米银膜体现出了较好的光谱重现性。通过对纳米银膜表面形貌进行表征发现聚乙烯醇(PVA)包覆的纳米银颗粒在铝片表面形成“草状”结构。并通过对吸附了胞苷分子的纳米银膜进行紫外-可见光反射光谱检测,发现在800 nm处出现等离子共振峰。因此采用785 nm的近红外激光作为激发光时,该体系能够体现出强烈的表面等离子共振(surface plasmon resonance, SPR)特性。同时采用DFT-B3LYP/6-311G对胞苷分子进行了拉曼光谱计算,计算所采用入射光波长为785 nm,通过计算结果与实验测得的胞苷固体的拉曼光谱对比发现在300～2 000 cm-1范围内两者匹配得较好,进而对其振动进行了归属。最后通过比较胞苷的拉曼光谱和NIR-SERS光谱对胞苷分子在纳米银膜上的可能吸附方式进行了分析。分析结果表明胞苷分子主要为其核糖部分吸附纳米银颗粒上,同时该分子的17NH₂基团可能靠近局域电磁场增强区域。     

光中子源上吸收片功能研究

15 MeV电子直线加速器驱动的光中子源装置,将用于中国科学院战略性先导科技专项“钍基熔盐堆”中的核数据初步测量工作、中子探测器的研制和反应堆相关材料的辐照研究等。光中子源的中子能谱是连续的,中子能量通过中子飞行时间法测量得到,需要利用吸收片确认中子吸收峰,刻度飞行时间,计算等效飞行距离,扣除实验本底等,而实验本底的扣除对最终总截面计算有很大的影响。因此通过Geant4蒙特卡罗模拟软件构建了包括中子源、吸收片在内的模拟实验环境;研究了不同吸收片的吸收谱和吸收片厚度的关系,同理论计算值进行了比较,给出了推荐的吸收片厚度值;模拟计算了中子飞行时间谱,并和实验测量结果比较,确定中子等效飞行距离为5.70 m。Geant4的理论计算也可以模拟出多吸收片本底函数曲线,可用于实验数据的本底扣除和误差分析。实验测量、模拟分析以及理论公式计算的吸收片厚度和中子飞行时间参数得到了完全一致的结果,验证了实验测量的可靠性。A photo-neutron source driven by a 15 MeV electron LINAC is built for the "Strategic Priority Research Program" of the Chinese Academy of Sciences-the "thorium-based molten salt reactor" project to conduct the nuclear data measurement work,develop neutron detector and carry out reactor material irradiation studies.Since the neutron energy spectrum is continuous,the neutron energy is measured by the time of flight (TOF) method,and neutron filters are needed to confirm absorption peaks,calibrate the TOF,calculate the equivalent flight distance,and remove the experimental background which has great influence on the calculation accuracy of the total cross section.Based on the Monte Carlo simulation tool,Geant4 a simulation environment is set up,including neutron source and neutron filters,to study the energy absorption spectra and thickness of different filters and recommended data for the thickness are provided.The neutron TOF spectra are simulated and compared with experimental measurement,deciding the equivalent TOF distance to be 5.7 m.Geant4 can also simulate the background curve of multiple filters and be used to remove background and analyze errors for the experimental data.All the experiments,simulation and theoretical calculation show consistent results on filter thickness and neutron TOF parameters,indicating the accuracy of the measurement.     

光纤陀螺随机漂移补偿中的数据融合方法（英文）

为提高光电平台的控制性能和稳定性,以平台反馈回路所用的光纤陀螺传感器为研究对象,对光纤陀螺角速率的历史输出、当前量测以及随机漂移进行融合补偿。采用双自回归模型确定了光纤陀螺时间序列输出的自回归多项式和光纤陀螺随机漂移的自回归关系。以陀螺当前输出为量测量,结合卡尔曼滤波算法将陀螺历史输出和历史随机漂移融合进状态方程,并进行随机漂移在线估计补偿。实验结果表明,光纤陀螺随机漂移的AR模型能达到90%拟合效果,经卡尔曼滤波补偿后随机漂移能降到1/10。该方法能很好地抑制光电平台三个框架轴光纤陀螺的随机漂移,补偿率为80%~90%。     

固相反应制备无氯CuY催化剂及其催化氧化羰基化—固相反应温度和铜负载量的影响

以乙酰丙酮铜Cu(acac)₂为铜源、 NH₄Y分子筛为载体, 采用固相反应制备了无氯CuY催化剂, 考察了在甲醇氧化羰基化合成碳酸二甲酯过程中固相反应温度和Cu负载量对CuY催化剂催化性能的影响, 分析了CuY催化剂物相结构、 可还原性Cu物种和织构性质对催化性能的影响. 结果表明, 随着固相反应温度的升高, 与NH₄Y中N\begin{array}{c}{H}_4^{+}\end{array}发生离子交换的Cu²⁺交换度和活性中心Cu⁺含量先增大后降低, CuY催化剂活性也呈现出相同的变化趋势; 负载量(质量分数)低于10%时, 受分子筛残留B酸位影响, 碳酸二甲酯的选择性较低, 而负载量高于12%时, CuY催化剂中出现了CuO物种, 且粒子逐渐长大, 覆盖部分活性中心, 甚至堵塞孔道, 使催化剂活性降低. 当固相反应温度为250 ℃, Cu负载量为12%时, 活性中心Cu⁺含量最高, 催化剂表现出最佳的催化活性, 碳酸二甲酯基于甲醇的时空收率为267.3 mg·g^-1·h^-1, 甲醇转化率为6.9%, 碳酸二甲酯(DMC)的选择性为69.2%.     

CdS超薄片层包覆TiO2中空结构复合材料的形成和应用

本实验以钛酸四丁酯为钛源,醋酸镉为镉源,利用静电纺丝的方法制备了直径~250 nm的电纺丝纳米纤维。通过高温煅烧和硫化钠溶液进行水热处理,得到CdS超薄片层包覆TiO₂中空结构的纳米纤维。推测该复合结构形貌的形成过程为:在Ti/Cd(摩尔比)为1:1和2:1时,由于CdO的含量较高,反应过程中CdO溶解,并与反应溶液中的S^2-形成CdS超薄片层生长在纤维的外表面,剩余的TiO₂纳米粒子聚集形成中空的纳米管状结构;而Ti/Cd(摩尔比)为4:1和8:1时,由于溶解的CdO较少不足以形成TiO₂纳米管,同时,生成的CdS也不足以完全包覆TiO₂纳米纤维形成非管状结构。当Ti/Cd为1:1时,TiO₂@CdS复合材料具有最好的产氢活性。在300 W氙灯光照条件下和加UVCUT-420 nm滤光片下,50 mg催化剂产氢速率分别为19.7 μmol/h和3.4 μmol/h,这主要是由于所得到的复合结构中TiO₂为非晶材料。进一步在惰性气氛下煅烧,也很难将TiO₂晶化。     

近零排放双燃料多功能系统特性规律分析及优化

本文对煤/天然气双燃料氢电联产多功能系统进行了特性规律分析.从燃料互补和能量综合梯级利用角度,分析了重整条件、氢气分离率对系统节能率的影响,以及多功能系统特征参数的变化规律,得到了新系统可以提高燃料化学能利用效率,同时可以降低CO2分离能耗的结论.在能量利用上的优势和对CO2的有效控制,使得新系统相对参考系统可以实现低能耗分CO2.     

A novel technique for predicting ionizing radiation effects of commercial MOS devices

A nondestructive selection technique for predicting ionizing radiation effects of commercial metal-oxide-semiconductor (MOS) devices has been put forward. The basic principle and application details of this technique have been discussed. Practical application for the 54HC04 and 54HC08 circuits has shown that the predicted radiation-sensitive parameters such as threshold voltage, static power supply current and radiation failure total dose are consistent with the experimental results obtained only by measuring original electrical parameters. It is important and necessary to choose suitable information parameters. This novel technique can be used for initial radiation selection of some commercial MOS devices.