Sorbents for the Direct Capture of CO2 from Ambient Air

The urgency to address global climate change induced by greenhouse gas emissions is increasing. In particular, the rise in atmospheric CO₂ levels is generating alarm. Technologies to remove CO₂ from ambient air, or “direct air capture” (DAC), have recently demonstrated that they can contribute to “negative carbon emission.” Recent advances in surface chemistry and material synthesis have resulted in new generations of CO₂ sorbents, which may drive the future of DAC and its large‐scale deployment. This Review describes major types of sorbents designed to capture CO₂ from ambient air and they are categorized by the sorption mechanism: physisorption, chemisorption, and moisture‐swing sorption.     

硝酰氯的大气化学

硝酰氯(nitryl chloride,ClNO₂)是大气中一种重要的气态污染物,对大气氧化性、一次污染物的降解和二次污染物的生成具有重要影响,并在全球氮循环和氯循环中扮演着不可忽视的角色。本文归纳了ClNO₂的基本物理化学性质及其在大气中的生成和去除机制,并介绍了实验室研究和外场观测中ClNO₂的主要测量方法。在此基础上,本文总结了过去十几年报道的ClNO₂在实际大气中的时空分布特征,通过分析实验室模拟和外场观测的研究结果系统讨论了ClNO₂非均相生成的机制、产率及其影响因素,探讨了ClNO₂对氯自由基、大气氧化性以及臭氧和硝酸盐形成的影响。我们指出,ClNO₂既耦合了气相化学和非均相化学,又耦合了夜间大气化学和日间光化学,在我国大气复合污染中可能起着非常重要的作用。最后,本文提出了ClNO₂大气化学研究中尚待解决的关键科学问题,并简要讨论了该领域的未来发展方向。     

Water Catalysis of the Reaction of Methanol with OH Radical in the Atmosphere is Negligible

Faced with the contradictory results of two recent experimental studies [Jara‐Toro et al., Angew. Chem. Int. Ed. 2017 , 56, 2166 and Chao et al., Angew. Chem. Int. Ed. 2019 , 58, 5013] of the possible catalytic effect of water vapor on CH₃OH + OH reaction, we report calculations that corroborate the conclusion made by Chao et al. and extend the rate constant evaluation down to 200 K. The rate constants of the CH₃OH + OH reaction catalyzed by a water molecule are computed as functions of temperature and relative humidity using high‐level electronic structure and kinetics calculations. The Wuhan–Minnesota Scaling (WMS) method is used to provide accurate energetics to benchmark a density functional for direct dynamics. Both high‐frequency and low‐frequency anharmonicities are included. Variational and tunneling effects are treated by canonical variational transition state theory with multidimensional small‐curvature tunneling. And, most significantly, we include multistructural effects in the rate constant calculations. Our calculations show that the catalytic effect of water vapor is not observable at 200–400 K.     

Wide-scope screening of polar contaminants of concern in water: A critical review of liquid chromatography-high resolution mass spectrometry-based strategies

The number of chemicals with potential to reach the environment is still largely unknown, which poses great challenges for both environmental scientists and analytical chemists. Liquid chromatography coupled to high-resolution mass spectrometry (LC-HRMS) is currently the instrumentation of choice for identification of wide-scope polar chemicals of concern (CECs) in water. This review critically evaluates all steps involved in screening for polar CECs in water, including sampling and extraction, analysis by LC-HRMS, data (pre-)treatment, evaluation and reporting. Passive samplers and direct injection, in combination with LC-HRMS, provide new opportunities compared with conventional grab water sampling, as do instrumental advances such as ion-mobility spectrometry coupled to HRMS (IM-HRMS). In this paper, we argue that target, suspect and non-target screening should not be viewed as three separate principles, but rather as conceptual approaches to general data treatment strategies that can be linked together. Due to the large amount of data generated, smart prioritisation strategies are needed, in particular for non-target screening, to reduce complexity and focus on data of high interest. We critically evaluate existing strategies and consider that each prioritisation step will result in data loss (as any other step in a screening study), requiring compromises depending on the research question to be tackled. Many different data treatment strategies have been developed in recent years, but structure elucidation remains a challenging and time-consuming task. We discuss current and potential future trends, e.g. effect-based methods that can be used as future prioritisation tools, technological advances like IM-HRMS and improved software solutions that can enable new data treatment strategies.     

大气压等离子体针产生空气均匀放电特性研究

大气压空气放电由于脱离了真空装置,易于实现流水线生产,因而在工业上具有广泛的应用. 采用等离子体针装置在空气中产生了稳定的大气压均匀放电. 利用光谱法对等离子体的相关参数进行了空间分辨率测量,并通过光学方法对放电机理进行了研究. 结果表明,等离子体针产生的放电存在电晕放电和等离子体羽放电两种模式. 在稳定的等离子体羽放电模式中,发光分为强光区和弱光区. 弱光区放电的发展速度远大于强光区的发展速度,电子能量和电子密度均是弱光区比强光区大. 对均匀放电的气体温度和振动温度的研究表明,强光区放电遵循汤生击穿机理而弱光区为流光放电. 这些结果对大气压空气放电的工业应用具有重要意义. 关键词： 大气压均匀放电 等离子体针 发射光谱 放电机理     

基于对比态原理的常压气体黏度关联式

本文依据对比态原理.通过关联常压下气态物质的无量纲黏度ηr与对比温度Tr以及临界压缩因子Zc,分别建立了适用于单原子气体、双原子气体、碳氢化合物气体以及卤代烃类气态物质的常压下黏度关联式.选用40种物质常压黏度数据对上述关联式分别进行了验证.与文献数据相比,气体黏度计算的相对偏差绝对平均值分别为:0.47%、0.45%...     

近场强度分布对线性相位反演算法复原效果的影响

利用数值仿真的方法详细的分析了近场强度分布对线性相位反演算法复原效果的影响.对近场强度分布分别为倾斜、环形和高斯随机型的情况下的复原结果与光强均匀时的复原结果进行对比,结果表明像倾斜型这种大部分为奇函数的近场强度分布对复原效果的影响比较恶劣;而像环形、随机型这样的偶函数或大部分为偶函数的近场强度分布对复原效果的影响则不...     

大气湍流随机相位差的相关解调算法研究

根据大气光学湍流的光纤干涉测量技术原理及其信号表现形式,针对湍流相位变化的随机性和复杂性,提出了能够实时解调湍流随机相位差的相关解调算法,数值模拟了固定相位差、波形相位差以及符合湍流频谱特征的随机相位差的解调.结果表明,此算法的绝对误差小于10-3,满足湍流测量的要求.该研究为实现光学湍流相位差的动态检测提供了必要的理...     

光纤激光阵列目标在回路自适应光学系统的数值模拟

研究了光纤激光阵列目标在回路自适应光学系统在实际大气环境中的传输.从光纤激光阵列、激光在大气中的传输、目标和优化算法四个方面,建立了光纤激光阵列目标在回路自适应光学系统的理论模型.在不同强度大气湍流下,对系统补偿大气湍流影响的效果进行了研究,并对系统控制参数优化进行了简单探讨.结果表明,目标在回路闭环控制结构能够有效补...     

双曲余弦高斯列阵光束在湍流大气中的光束传输因子

本文推导出了双曲余弦高斯(ChG)列阵光束在湍流大气中的光束传输因子( M ^{2因子)的解析公式,并采用相对 M 2因子研究了湍流对 M 2因子的影响.研究表明,在湍流大气中 M 2因子不再是一个传输不变量,湍流使得 M 2因子增大.非相干合成情况下, M 2因子随着传输距离、光束参数、相对子光束间距和子光束数目的增大而增大.相干合成情况下, M 2因子随光束参数和相对子光束间距的增大呈现振荡上升.相干合成情况下的 M 2因子比 关键词： M2因子)')" href="#">光束传输因子(M2因子) 光束质量 双曲余弦高斯列阵光束 大气湍流}