胍盐离子液体捕获CO2温室气体的机理 (cited: 1)

通过量子力学与分子动力学对胍盐离子液体的模拟表明,胍阳离子与氯负离子之间存在较强的相互作用,其相互作用能约为-109.216 kcal/mol．从能量与几何分布可见,两种空间分布方式中最稳定构象为Middle作用模式．径向分布函数也验证了这一结论．CO₂含量的不断增加并没有对离子液体的结构产生影响,而是被离子液体的空腔捕获．     

理论研究二氧化碳在有机吸收剂1，3-二苯胍中的氢键相互作用

如今碳捕获和储存技术已得到了迅速发展以减少对环境的二氧化碳排放. 研究发现胺基有机分子溶剂能有效地吸收二氧化碳,并通过氢键和二氧化碳形成的碳酸氢盐相互作用. 最近,实验报道了一种1,3-二苯基胍溶液,在室温条件下能捕获环境中的二氧化碳并将其转化为有价值的化学品. 然而,1,3-二苯基胍分子在溶液状态下如何与二氧化碳相互作用的机理仍不清楚. 在这项工作中,利用分子动力学方法模拟研究了溶液相中1,3-二苯基胍分子与二氧化碳的复杂作用细节. 模拟结果表明,质子化的1,3-二苯基胍分子和碳酸氢根离子倾向通过不同的双氢键模式作用形成稳定的复合物. 精确的密度泛函方法计算表明,这些双氢键复合物在热力学上相当稳定. 本研究有助于理解溶液相中1,3-二苯基胍分子中催化转化二氧化碳的机理.     

Molecular Dynamics Simulations for Melting Temperatures of SrF2 and BaF2

利用壳层模型分子动力学方法,考虑萤石结构分子中的预熔化现象,对SrF₂和BaF₂的分子动力学模拟熔化温度进行修正,获得了高压下SrF₂和BaF₂的熔化温度. 同时给出了300 K、0.1 Mpa～7GPa和0.1 Mpa～3 GPa时SrF₂和BaF₂的状态方程,与已有研究结果的最大误差分别为0.3%和2.2%. 计算所得SrF₂和BaF₂常压下的熔点与已有的实验结果符合较好. 对于SrF₂和BaF₂分子体积变化和已有的熔化模拟的差别也做了比较和讨论.     

CO2 laser assisted removal of UO2 and ThO2 particulates from metal surface

Pulsed laser assisted removal of uranium dioxide and thorium dioxide particulates from stainless steel surface have been studied using a TEA CO₂ laser. Decontamination efficiency is measured as a function of laser fluence and number of pulses. Threshold fluence for the removal of UO₂ particulates has been found to be lower than that required for the removal ThO₂ particulates. Usage of a ZnSe substrate, that is transparent to the laser wavelength used here, enabled us to decouple the cleaning effect arising out of absorption in the particulates from that in the substrate and has contributed towards understanding the mechanism responsible for cleaning. The experimental observations are also corroborated by simple theoretical calculations.     

Absorption coefficients of O3 at CO2 laser wavelengths

The O₃ absorption coefficients for the rotational lines P(12)–P(28) of the 9.4 μm emission band of the CO₂ laser are presented. Measurements were made in O₃–air dilute mixtures (20–600 ppm) at 25°C and a total pressure of 1013.25 h Pa using a frequency stabilized cw CO₂ laser and values have been determined with greater precision than in previously reported studies.     

二氧化碳在柔性ZIF-8笼中平均停留时间的分子动力学模拟

采用巨正则蒙特卡洛和分子动力学模拟方法研究了二氧化碳分子在柔性ZIF-8材料中吸附位点和扩散机理. 通过构建合理的时间相关函数,得出了二氧化碳分子在柔性ZIF-8笼中的平均停留时间. 结果表明,二氧化碳分子待在同一个笼中的停留时间可达到几十个皮秒. 并且发现平均停留时间几乎随着压力(或负载量)的增加而线性增加.     

Synergistic inhibition effect of 2-mercaptobenzothiazole and Tween-80 on the corrosion of brass in NaCl solution

The corrosion inhibition of brass in 0.2 M NaCl in the presence of 2-mercaptobenzothiazole (MBT) and polyoxyethylene sorbitan monooleate (Tween-80) has been investigated using potentiodynamic polarization, X-ray photoelectron spectroscopy and inductively coupled plasma analysis. Analysis of the results revealed that the addition of MBT and Tween-80 inhibits the corrosion of brass in 0.2 M NaCl. Potentiodynamic polarization measurements showed that MBT acts as a mixed-type inhibitor and Tween-80 as an anodic inhibitor. Corrosion inhibition occurs through adsorption of the inhibitor on brass surface without modifying the corrosion mechanism. The adsorption of MBT and Tween-80 both follow Langmuir adsorption isotherm. Potentiodynamic polarization results suggested that the mixture of MBT and Tween-80 acts as a mixed-type inhibitor. Inhibition efficiency of 79.0 and 62.5% were obtained in the presence of optimum concentration of MBT and Tween-80, respectively. The addition of the mixture of MBT and Tween-80 enhanced the inhibition efficiency to 94.0% and showed a synergism of inhibition. XPS analysis indicated that MBT adsorbed on brass surface along with Tween-80 in the presence of the mixture of MBT and Tween-80. The results of solution analysis using ICP showed that the mixture of MBT and Tween-80 effectively controlled the dezincification of brass.     

New CH2F2 FIR laser lines pumped by a tunable WG CO2 laser

8 new large offset FIR laser lines of CH₂F₂ have been discovered by pumping with a high tunability waveguide CW CO₂ laser. Optoacoustic measurements of CH₂F₂ have also been performed and the pump offsets of the new and of previously known lines have been measured and checked. Some assignments are proposed and a few assignments found in literature are checked     

H++CO2散射在30电子伏能量下电荷转移和非电荷转移的非绝热分子动力学模拟

在大气化学、天体物理学和癌症质子疗法中都涉及到高能H⁺+CO₂散射反应.本文在最简电子-核动力学（SLEND）基础上系统研究在30 eV下的H⁺+CO₂散射.SLEND用经典力学描述核,用单行列式Thouless波函数描述电子.本文模拟了CO₂在42个取向共3402条轨线,为理解H⁺+CO₂散射中的各个反应过程和机制提供了系统描述：非电荷转移散射（NCTS）,电荷转移散射（CTS）和C=O双键的断裂,这些关于反应的有用信息不能完全从实验中获取.本文提供了散射的详尽细节,包括随CO₂取向不同主彩虹角和次彩虹角的出现和合并.SLEND NCTS和CTS的微分散射截面通过高等半经典方法计算,显示NCTS散射截面对所有散射角都同实验符合得很好,而CTS散射截面只大散射角时同实验结果符合得很好而在小角散射时稍差.无论是CTS还是NCTS SLEND都预言了主彩虹角的特征,这同实验完全一致.     

CO2/CO2 isotopic ratio measurements with a continuous-wave quantum cascade laser in exhaled breath

A laser spectrometer based on a continuous-wave thermoelectrically-cooled distributed feedback quantum cascade laser at ∼2308 cm⁻¹ has been evaluated for measurement of ¹³CO₂/¹²CO₂ isotopic ratio (δ¹³C) changes in exhaled breath samples and in CO₂ gas flows in the concentration range 1-5%. Mid-infrared CO₂ absorption spectra were measured in a 54.2-cm long optical cell using balanced detection whereby the beam passing through the cell was ratioed against a reference beam split-off from the main beam before the cell. Signal-to-noise ratios (SNR) were estimated for CO₂ concentration measurements determined from either absorption peak amplitude or absorption peak area. The highest SNR were achieved in the measurements based upon a fitted absorption peak area. Typical short-term δ¹³C precisions of 1.1⁰/₀₀ (1-s integration time) and 0.5⁰/₀₀ (8-12-s integration time) were estimated from the two-sample (Allan) variance plots of data recorded in the optical cell at a pressure of 20 Torr and with no active temperature stabilization of the cell and gas flow. The best precision of 0.12⁰/₀₀ was achieved for averaging 80 successive 1-s integration time measurements.     

Submillimeter-wave spectroscopy of HN2 and DN2 in the excited vibrational states

The pure rotational transitions of HN₂⁺ and DN₂⁺ in the first excited vibrational states for all the fundamental vibrational modes have been observed in the range of 300-750 GHz. The molecular constants determined are much more accurate compared with those obtained from the infrared spectroscopy. The equilibrium rotational constants, B_e = 46832.45 (71) MHz for HN₂⁺ and B_e = 38708.38 (58) MHz for DN₂⁺, have been determined by correcting for the higher-order vibration-rotation interaction effects, γ_ij, obtained by an infrared investigation. The equilibrium bond lengths are derived from these equilibrium rotational constants: r_e(H-N) = 1.03460 (14) Å and r_e (N-N) = 1.092698 (26) Å.     

Molecular dynamics simulations of CFx (x = 2, 3) molecules at Si3N4 and SiO2 surfaces

Molecular dynamics simulations of the interaction between CF_x (x = 2, 3) molecules and crystalline as well as amorphous Si₃N₄ and SiO₂ surfaces using a density-functional based method are reported. The binding energies of various configurations at the crystalline surfaces were calculated. The effect of hydrogen substitution was studied.     

Spatial-dependent simulation of TEA CO2 lasers

We have developed a 1-D spatially-dependent model and simulation code to study the dynamics of TEA CO₂ lasers. In this paper we will discuss the motivation for developing the model and present the simulation details. We have compared and verified the simulation results with the previous 0-D model, and with the measurements of a TEA CO₂ laser. With spatial resolution, the 1-D simulation is in better agreement with experimental results compared with the existing 0-D model.     

Characteristics of CO2 corrosion scale formed on N80 steel in stratum water with saturated CO2

The component and structure of CO₂ corrosion scale formed on N80 tubing steel were studied by using X-ray photoelectron spectroscopy (XPS), X-ray diffraction (XRD) and scanning electron microscopy (SEM); the electrochemical property of N80 steel covered by corrosion scale was investigated by electrochemical impedance spectroscopy (EIS). The results shows a double-layer structure of the corrosion scale, in which the principal component of the outer layer is FeCO₃ with a limited amount of ∂-FeOOH; while for the inner scale, FeCO₃ is still the major component, but some Fe positions in FeCO₃ lattice are substituted by Ca, and form a composite compound of (Fe,Ca)CO₃ in the inner scale. EIS study shows that the anodic impedance spectrum has three time constants, i.e., the capacitance at high frequency, Warburg impedance at middle frequency and capacitance at low frequency.     

Molecular modeling study on inhibition performance of imidazolines for mild steel in CO2 corrosion

Corrosion inhibiting performance of 1-hydroxyethyl-2-heptadecylimidazoline (A) and 1-aminoethyl-2-heptadecylimidazoline (B) for mild steel was evaluated by combination of quantum chemistry calculation, molecular mechanics, and molecular dynamics simulation. The calculated results by quantum chemistry method demonstrated that frontier orbitals of A and B molecules are mainly located on imidazoline rings, and molecule B possesses higher reactivity than molecule A. The calculated results by molecular mechanics and molecular dynamics simulation presented that these two inhibitor molecules could form dense and high-coverage membranes to prevent diffusion of reactive corrosive species to metal surface. Furthermore, the adsorption energy, cohesive energy, and adsorption angle demonstrated that the binding affinity and stability of B membrane was remarkably greater than that of A, which indicated that B had better inhibition performance in CO₂ corrosion. The calculated results were well accorded with previous reported experimental results. These researches implied that molecular modeling might be an effective approach to assess inhibition performance, which has potential application in design of new inhibitors.     

Absolute frequency measurement of CO2 laser lines with a femtosecond laser comb and new determination of the CO2 molecular constants and frequency grid

Absolute frequency measurements of a CO₂ laser stabilized on saturated absorption resonances of CO₂ laser lines are reported. They were performed using a femtosecond-laser frequency comb generator and two laser diodes at 852 and 782 nm as intermediate oscillators, with their frequency difference phase-locked to the CO₂ laser. Twenty ¹²C¹⁶O₂ laser lines in the P and R bands at 9 μm were measured with a relative uncertainty of a few 10⁻¹² limited by the CO₂ frequency reproducibility. A new determination of the CO₂ molecular constants was obtained from these data and previous measurements in the 10 μm band. The CO₂ frequency grid was also calculated, with an improvement of two orders of magnitude compared to the previous grid of Maki et al. [J. Mol. Spectrosc. 167 (1994) 211].     

Improvement of amine-modification with piperazine for the adsorption of CO2

Both selectivity and capacity of CO₂ adsorption were considerably increased when PZ (piperazine) was added in MDEA (methyldiethylamine) that used to modify the surface of silica gels. The adsorbent saturated with CO₂ was regenerated at ambient temperature through nitrogen purge. A set of PSA (pressure swing adsorption) operation with 200 cycles was carried out and applicability of the modified adsorbent was thus illustrated. The CO₂ content in the column-top stream decreased from 13% to below 0.05% at steady state.     

电化学析氢反应中单层MoSe2氢吸附机理第一性原理研究

基于密度泛函理论的第一性原理方法,本文计算了单层2H相MoSe₂纳米材料表面及两种边缘（Mo原子边缘、Se原子边缘）不同活性位点、不同氢原子吸附率下的氢吸附吉布斯自由能（Gibbs free energy,用△G_H⁰表示）,并且将对应的微观结构进行了系统分析比较,得出△G_H⁰最接近于0 eV的吸附位点及相应的吸附率.同时,结合差分电荷密度和电负性理论,分析了单层MoSe₂两种边缘氢吸附的电荷转移及成键特性,进一步解释了不同吸附位点呈现的结构与能量趋势.最后,通过基于密度泛函理论的第一性原理分子动力学模拟,研究了高温热运动对两种边缘氢吸附的影响,获得了氢原子发生脱附的临界温度及对应的微观动态过程.该理论研究从原子尺度揭示了单层2H相MoSe₂纳米材料边缘不同位点在不同温度下对氢原子吸附和脱附的微观机理,证实了Mo原子边缘的畸变和重构行为,加深了对实验中单层2H相MoSe₂边缘在不同温度下氢吸附机理的理解,为实验中通过控制MoSe₂边缘设计廉价高效的析氢催化剂提供理论参考.     

脉冲CO2激光器的多频动力学模型

建立了适用于各种气压下(20×133—20×10⁵ Pa)的脉冲CO₂激光器的六温度多频动力学模型，该模型考虑了增益谱线重叠效应，序列带、热带的影响，以及非洛伦兹线型效应.对模型进行数值求解可以预言和解释不同气压下的脉冲CO₂激光器的输出特性，有助于评价不同的抽运设计和研究可调谐特性，为设计脉冲CO₂激光系统提供理论支持. 关键词： 2激光器')" href="#">CO₂激光器 激光动力学 六温度模型 增益谱线重叠     

MgO-decorated carbon nanotubes for CO2 adsorption: first principles calculations

The global greenhouse effect makes it urgent to deal with the increasing greenhouse gases.In this paper the performance of MgO-decorated carbon nanotubes for CO 2 adsorption is investigated through first principles calculations.The results show that the MgO-decorated carbon nanotubes can adsorb CO 2 well and are relatively insensitive to O 2 and N 2 at the same time.The binding energy arrives at 1.18 eV for the single-MgO-decorated carbon nanotube adsorbing one CO 2 molecule,while the corresponding values for O 2 and N 2 are 0.55 eV and 0.06 eV,respectively.In addition,multi-molecule adsorption is also proved to be very satisfactory.These results indicate that MgO-decorated carbon nanotubes have great potential applications in industrial and environmental processes.