SGER: Chemical Frustration and the Design of New Hydrogen Storage Materials

SGER：化学挫败与新型储氢材料的设计

• 批准号: 0844720
• 负责人: Peihong Zhang
• 金额: $ 9万
• 依托单位: SUNY at Buffalo
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2008
• 资助国家: 美国
• 起止时间: 2008-09-01 至 2010-02-28
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=0844720&HistoricalAwards=false
• 关键词: SGER; Chemical; Frustration; Design; New

CBET-0844720ZhangThe hydrogen storage challenge, and equally compelling issues in large-scale hydrogen generation, impedes the broad commercialization of this otherwise compelling energy carrier. Not only do existing storage technologies fail to meet requirements in capacity, cost and reversibility, but there are no clear optimization paths from known systems to fully practical on-board storage systems. In this research, the PI will perform an intense two-year theoretical materials design search, using powerful first-principles methods and exploiting several new concepts in hydrogen-substrate interaction, with the goal of discovering one or more new families of hydrogen sorbents. It will exploit the concept of electronic frustration, wherein intrinsic or geometrically-induced electron deficiency generates novel multi-center electronic configurations, unusual charge-transfer states, or anomalously large local fields that enhance hydrogen binding. Over the course of the two-year research effort, these calculations will identify targets for further investigation and optimization of hydrogen capacity and synthesizability, through studies of convex-hull phase stability and kinetic barriers. Boron-hydrogen molecules have a surprisingly rich and highly unconventional chemistry arising from an intrinsic electronic frustration associated with having just three valence electrons in the s-p shell. The PI will investigate several novel boron-based frameworks with build-in sites for multicenter hydrogen binding and will use doping to modulate the overall charge state of the framework to attain maximal framework stability, optimal hydrogen binding energetics, kinetics and reversibility within thermodynamic constraints on relative phase stability. Electronic frustration will also be induced geometrically, by means of topological and topographical constraints that prevent systems with well-known atomic constituents from attaining their traditional ground state structures. Topological barriers and topographical constraints will help induce novel electronic states with prospects to demonstrate new modes of binding to close-shell species such as molecular hydrogen. A solution to the hydrogen storage challenge would have a transformative impact throughout society, from environment issues to energy security, national security and transportation. The proposed research will educate one graduate student in interdisciplinary computational materials research. Student training in electronic structure theory relies upon a solid grounding in condensed matter theory, yet also requires important concepts from chemistry and materials science and naturally develops in students a strong familiarity with large-scale high-performance computation on massively parallel computers. This integrated multidisciplinary training on an application-oriented project will broaden the student's knowledge and experience and thereby prepare them for careers that span disciplines. Students will have opportunity to communicate their results both at research venues and to the general public.

CBET-0844720张氢存储挑战以及大规模制氢中同样引人注目的问题阻碍了这种引人注目的能源载体的广泛商业化。现有的存储技术不仅无法满足容量、成本和可逆性方面的要求，而且从已知系统到完全实用的车载存储系统也没有明确的优化路径。在这项研究中，首席研究员将进行为期两年的密集理论材料设计研究，使用强大的第一原理方法并开发氢-底物相互作用的几个新概念，目标是发现一个或多个新的氢吸附剂家族。它将利用电子挫败的概念，其中内在或几何诱导的电子缺陷会产生新颖的多中心电子构型、不寻常的电荷转移状态或增强氢结合的异常大的局部场。在两年的研究工作中，这些计算将通过凸包相稳定性和动力学势垒的研究，确定进一步研究和优化氢容量和合成性的目标。硼氢分子具有令人惊讶的丰富且高度非常规的化学性质，这是由于与 s-p 壳层中仅具有三个价电子相关的固有电子挫败而产生的。 PI将研究几种具有多中心氢结合内置位点的新型硼基框架，并将使用掺杂来调节框架的整体电荷状态，以在相对相稳定性的热力学约束内实现最大框架稳定性、最佳氢结合能量、动力学和可逆性。电子挫败也将通过拓扑和地形约束以几何方式引起，这些约束阻止具有众所周知的原子成分的系统获得其传统的基态结构。拓扑势垒和拓扑约束将有助于诱导新的电子态，并有望展示与分子氢等近壳层物种结合的新模式。氢存储挑战的解决方案将对整个社会产生变革性影响，从环境问题到能源安全、国家安全和交通。拟议的研究将培养一名跨学科计算材料研究的研究生。电子结构理论的学生培训依赖于凝聚态理论的坚实基础，但也需要化学和材料科学的重要概念，并自然地培养学生对大规模并行计算机上的大规模高性能计算的强烈熟悉。这种以应用为导向的项目的综合多学科培训将拓宽学生的知识和经验，从而为他们跨学科的职业生涯做好准备。学生将有机会在研究场所和向公众传达他们的成果。