Spectroscopic and Simulation Studies of Ice Surface Interactions with Intermediate and Strong Adsorbates: Physics and Chemistry of Molecular Nanoparticles

冰表面与中强吸附物相互作用的光谱和模拟研究：分子纳米粒子的物理和化学

• 批准号: 9983185
• 负责人: J. Paul Devlin
• 金额: $ 22.36万
• 依托单位: Oklahoma State University
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2000
• 资助国家: 美国
• 起止时间: 2000-04-01 至 2003-03-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=9983185&HistoricalAwards=false
• 关键词: Spectroscopic; Simulation; Studies; Ice; Surface

Paul Devlin of Oklahoma State University is supported by a grant from the Experimental Physical Chemistry Program to perform experimental and theoretical studies on the structure and dynamics of free-standing ice using Fourier transform-infrared spectroscopy of nanocrystals and Grand Canonical Monte Carlo calculations. This work is giving information on the strengths of bonds between water molecules and the nature of the dangling, unsatisfied surface bonds. In detail, he is study (i) the interaction the surface of ice with both strong (ammonia, ethylene oxide, methanol, small ethers, strong acids) and intermediate strength (sulfur dioxide, hydrogen sulfide and cyanide, ethylene) absorbates, (ii) the quantitative kinetics of conversion of ice nanocrystals to acid hydrates, (iii) the catalytic role of small ether molecules in aiding the conversion of ice to clathrate hydrates and (iv) an exploration of the chemistry of organic nanoparticles in three dimensional arrays. Several stages are involved in these interactions including initial absorption, insertion of adsorbed molecules into weak hydrogen bonds, surface relaxation and subsurface relaxation or formation of the hydrate phase.These studies will give a more detailed understanding of the nature of the surface of ice and the mechanisms by which different molecules absorb strongly and weakly onto ice nanocrystals. The work has broad applications to the role of ice particles in the destruction of stratospheric ozone, their significance in the diurnal variations of the atmospheres of the icy moons of Jupiter, the chemistry on the ice mantles of interstellar dust particles and the control of hydrated species in fuel science.

俄克拉荷马州立大学的保罗·德夫林得到了实验物理化学计划的资助，他将利用纳米晶体的傅里叶变换红外光谱和大标准蒙特卡罗计算对自由冰的结构和动力学进行实验和理论研究。这项工作提供了有关水分子之间的键的强度和悬垂的、未令人满意的表面键的性质的信息。具体来说，他正在研究(I)冰表面与强(氨、环氧乙烷、甲醇、小分子醚、强酸)和中等强度(二氧化硫、硫化氢、氰化物、乙烯)吸收物的相互作用，(Ii)冰纳米晶体转化为酸性水合物的定量动力学，(Iii)小乙醚分子在帮助冰转化为笼状水合物方面的催化作用，以及(Iv)在三维阵列中探索有机纳米颗粒的化学。这些相互作用涉及几个阶段，包括初始吸附、吸附分子插入弱氢键、表面松弛和表面下松弛或水合物相的形成。这些研究将使人们更详细地了解冰表面的性质以及不同分子在冰纳米晶体上强吸附和弱吸附的机理。这项工作在以下方面有广泛的应用：冰粒在破坏平流层臭氧中的作用、它们在木星结冰卫星大气日变化中的意义、星际尘埃粒子冰盖上的化学以及燃料科学中的水合物控制。