Exploring the Synthesis and Properties of Hybrid Perovskites with a "Gas" Atom, or Molecule, as a Structural Component

第一部分：非技术摘要在该项目中，合成并表征了一种新的固体材料家族，其结构中包含气体原子或分子。这项工作将对功能固体的基本理解带到了一个新的方向，也为新技术提供了机会。正在研究的材料可能在室温和压力下捕获大量气体，然后在变暖时释放气体。对于给定的体积，它们可以比通常用于容纳氢气、氦气和其他工业重要气体的高压储罐容纳更多的气体。高效和安全的气体储存是使用氢作为燃料的主要障碍之一。新的含气材料还具有气体分离和纯化过程的潜力，这对核工业和国防具有重要意义。利用机器学习方法的计算机模拟支持和指导实验工作。研究生和本科生在各种技术的培训，在新的功能材料的开发中具有广泛的实用性被集成到该项目，这是由材料研究部内的固态和材料化学计划的支持。第二部分：该项目探索钙钛矿的制备和性质，其中小的气体分子或原子，例如分子氢，氖或氦，是材料的结构组分。虽然有大量关于钙钛矿的先前工作，但由于其在广泛应用中的技术意义，几乎对含气体的钙钛矿一无所知。这种类型的材料可以以比在常规高压气体储罐中发现的高得多的密度容纳气体，并且其结构内的小孔可以通过量子筛分效应实现同位素分离。 合成方法包括三种不同的策略，用于制备不同组成家族的新材料。 高压衍射和拉曼光谱，沿着气体释放测量从回收的样品，提供有关材料的形成和性质的信息。 在该项目中，由材料研究部内的固态和材料化学计划支持，实验由先进的计算工具补充，因此计算既解释了实验结果，又指导了新材料的制备。蒙特卡罗和分子动力学模拟基于使用深度学习卷积神经网络方法从密度泛函理论计算中导出的力场，提供了真实捕获材料行为的机会。该奖项体现了NSF的法定使命，并通过使用基金会的智力价值和更广泛的影响审查标准进行评估，被认为值得支持。

Part 1: Non-Technical SummaryA new family of solid materials that contain gas atoms or molecules as part of their structure is being synthesized and characterized in this project. This work takes fundamental understanding of functional solids in a new direction and also opens opportunities for new technologies. The materials under study can potentially trap large amounts of gas at room temperature and pressure, and then release the gas on warming. For a given volume, they can contain more gas than the high pressure storage tanks typically used to contain hydrogen, helium and other industrially important gases. Efficient and safe gas storage is one of the major barriers to using hydrogen as a fuel. The new gas-containing materials also have potential for gas separation and purification processes that are of importance to the nuclear industry and national defense. Computer simulations, which make use of a machine learning approach, support and guide the experimental work. The training of graduate and undergraduate students in a variety of techniques that are of wide utility in the development of new functional materials is integrated into the project, which is supported by the Solid State and Materials Chemistry program within the Division of Materials Research. Parts 2: Technical SummaryThis project explores the preparation and properties of perovskites where a small gas molecule or atom, for example molecular hydrogen, neon or helium, is a structural component of the material. While there is vast body of prior work on perovskites, due to their technological significance across a wide range of applications, there is almost nothing known about gas-containing perovskites. Materials of this type can contain the gas at much higher densities than found in conventional high pressure gas storage tanks, and the small pores within their structures may enable isotope separation by quantum sieving effects. Synthetic approaches include three distinct strategies for preparing new materials in different compositional families. High pressure diffraction and Raman spectroscopy, along with gas release measurements from recovered samples, provide information on the formation and properties of the materials. In this project, supported by the Solid State and Materials Chemistry program within the Division of Materials Research, experiment is complemented by advanced computational tools, so that computation both explains experimental results and guides the preparation of new materials. Monte Carlo and molecular dynamics simulations, based on force fields derived from density functional theory calculations using a deep-learning convolution neural network approach, provide an opportunity to realistically capture the behavior of the materials. The training of graduate and undergraduate students in a variety of synthetic, computational and materials characterization techniques is integrated into the work.This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.