Hydrogen molecules in nanoscale confinement: A combined eigenstate-resolved/path integral study of the quantum translation-rotation dynamics, spectroscopy, and diffusion

纳米级限制中的氢分子：量子平移-旋转动力学、光谱学和扩散的本征态解析/路径积分组合研究

• 批准号: 1112292
• 负责人: Zlatko Bacic
• 金额: $ 54.5万
• 依托单位: New York University
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2011
• 资助国家: 美国
• 起止时间: 2011-07-01 至 2015-06-30
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1112292&HistoricalAwards=false
• 关键词: Hydrogen; molecules; nanoscale; confinement; combined

Zlatko Bacic (PI) and Mark E. Tuckerman (co-PI) of New York University are supported by an award from the Chemical Structures, Dynamics and Mechanisms program of the Chemistry Division for a computational study aimed at achieving a fundamental understanding and a comprehensive theoretical description of the quantum dynamics, spectroscopy, and diffusion of hydrogen molecules inside the nanoscale cavities of diverse host materials, such as clathrate hydrates, fullerenes and carbon nanotubes, and metal-organic frameworks (MOFs). This will provide a broad theoretical framework, as well as quantitative predictions, indispensable for the planning, analysis, and interpretation of various types of spectroscopic measurements of these systems presently carried out by groups around the world. An array of robust theoretical approaches, ranging from high-dimensional quantum bound state and scattering methods to diffusion Monte Carlo and path integral simulations, will be brought to bear on these objectives. Another goal of this proposal is the accurate determination of multidimensional, anisotropic and anharmonic interaction potentials of the nanoconfined hydrogen, and in certain cases H2O, with the host materials. Accomplishing this will involve the combination of sophisticated quantum dynamics and ab initio electronic structure calculations. The eigenstate-resolved calculations will be complemented by path integral simulations directed at elucidating the temperature and concentration dependence of the energetics, free-energetics, spatial distributions, and diffusion of molecular hydrogen, especially in bulk clathrate hydrates and MOFs. A major hurdle for the large-scale use of hydrogen as a clean and efficient energy carrier is developing ways to store it safely and economically. One possibility currently under intense investigation worldwide absorption in nanoporous materials. Quantitative understanding of the properties of molecular hydrogen under such conditions, and characterization of the interactions of hydrogen with various host environments is essential in joint experimental and theoretical efforts aimed at rational design of new media for hydrogen storage. If met, the challenge of developing efficient hydrogen-storage materials will have an enormous impact on emerging energy technologies. This research will be carried out by graduate and undergraduate students at NYU, including those from traditionally underrepresented groups. In addition, one of our experimental collaborators, Prof. Stephen FitzGerald, is at an undergraduate institution (Oberlin), and his students will be directly involved in the project.

Zlatko Bacic（PI）和Mark E.纽约大学的塔克曼（共同PI）获得了化学系化学结构，动力学和机制计划的奖项，用于计算研究，旨在实现对不同主体材料（如笼形水合物，富勒烯和碳纳米管）纳米级空腔内氢分子的量子动力学，光谱学和扩散的基本理解和全面的理论描述，和金属有机框架（MOFs）。这将提供一个广泛的理论框架，以及定量预测，不可或缺的规划，分析和解释这些系统的各种类型的光谱测量目前正在进行的团体在世界各地。一系列强有力的理论方法，从高维量子束缚态和散射方法扩散蒙特卡罗和路径积分模拟，将承担这些目标。该提案的另一个目标是准确测定纳米限制氢和在某些情况下H2O与主体材料的多维、各向异性和非谐相互作用势。实现这一目标将涉及复杂的量子动力学和从头计算电子结构计算的结合。本征态分辨计算将补充路径积分模拟，旨在阐明温度和浓度依赖的能量，自由能，空间分布和扩散的分子氢，特别是在散装笼形水合物和MOFs。大规模使用氢作为一种清洁高效的能源载体的一个主要障碍是开发安全经济的储存方法。一种可能性，目前正在激烈的调查，世界范围内的纳米多孔材料的吸收。定量的了解在这种条件下的分子氢的性质，和表征的氢与各种主机环境的相互作用是必不可少的联合实验和理论的努力，旨在合理设计的新媒体储氢。如果能够实现，开发高效储氢材料的挑战将对新兴能源技术产生巨大影响。这项研究将由纽约大学的研究生和本科生进行，包括那些传统上代表性不足的群体。此外，我们的实验合作者之一，斯蒂芬·菲茨杰拉德教授，是在一个本科院校（奥伯林），他的学生将直接参与该项目。