CAS: Fundamental Experimental-Theoretical Investigations of New Metal Alloy Nanocatalysts for Natural Gas Repurposing

CAS：用于天然气再利用的新型金属合金纳米催化剂的基础实验理论研究

• 批准号: 2109120
• 负责人: Simon Humphrey
• 金额: $ 58.93万
• 依托单位: University of Texas at Austin
• 依托单位国家: 美国
• 项目类别: Continuing Grant
• 财政年份: 2022
• 资助国家: 美国
• 起止时间: 2022-01-01 至 2024-12-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=2109120&HistoricalAwards=false
• 关键词: CAS; Fundamental; Experimental; Theoretical; Investigations

With the support of the Macromolecular, Supramolecular and Nanochemistry Program in the Division of Chemistry, Profs. Simon M. Humphrey and Graeme Henkelman at the University of Texas at Austin are leading a highly collaborative research program involving the synthesis and reactivity studies of nano-sized alloys capable of converting methane into stable liquid fuels such as methanol, at the location where the methane is released. Meanwhile, natural gas flaring is an increasingly significant environmental issue worldwide and particularly in the USA. Natural gas (i.e., methane) that is released at oil recovery sites or in refineries is remediated by direct combustion to give carbon dioxide. While methane is a much more powerful greenhouse gas than carbon dioxide, the act of flaring still wastes the methane and adds millions of tones of extra carbon dioxide into the atmosphere each year. This is because compression of methane for transportation and eventual use is not cost-effective. This research project is fundamental and aims to understand how certain compositions of alloys of non-precious metals can perform the target reactions in a controlled and desirable manner. The scientific project is also significantly enhanced through integration with an innovative undergraduate educational program, called the Austin-International Framework (AIF), which provides a fully immersive, scholarship-supported international exchange experience to UT Austin undergraduates. It provides students the unique opportunity to broaden their horizons, while simultaneously earning course credit for their research experiences.This a collaborative experimental-computational research program between the groups of Profs. Simon M. Humphrey and Graeme Henkelman at the University of Texas at Austin. The overarching aims are to leverage expertise in the formation of novel metallic nanoalloys via microwave-assisted heating techniques, and to use theory in silico to guide synthetic studies and to elucidate the resulting reactivity of the nanoparticle catalysts, as a function of surface structure and composition. The specific goals of this project are to prepare new binary and ternary catalysts using combinations of catalytically less valuable and abundant coinage metals along with more highly oxophilic metals such as Ru and Re, to generate systems that can mimic the reactivity of scarcer noble metals. In addition to model gas-phase chemical reaction studies that mimic realistic reaction conditions, structure-function relationships will be elucidated using a palette of spectroscopic techniques (e.g., electron microscopy, total X-ray scattering, extended X-ray fine structure, chemisorption, etc.), to provide realistic theoretical models at the atomic scale. This structural information will then be used to build and refine theoretical models that can identify then most important active site ensembles. Ultimately this enables accurate predictions of reactivity and selectivity, which can be leveraged to inform future synthetic targets, toward the identification of eventual catalysts with desired reactivity: those that are able to selectively activate CH4 to CH3 and H in the presence of atomic oxygen.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.

在化学划分的大分子，超分子和纳米化学计划的支持下，教授。德克萨斯大学奥斯汀分校的西蒙·汉弗莱（Simon M. 同时，天然气爆炸是全球尤其是美国越来越重大的环境问题。 在油回收地点或炼油厂中释放的天然气（即甲烷）通过直接燃烧来补充以给出二氧化碳。 虽然甲烷比二氧化碳更强大，但燃烧的行为仍会浪费甲烷，并每年在大气中添加数百万个额外的二氧化碳。 这是因为甲烷用于运输和最终使用的压缩不是成本效益。 该研究项目是基本的，旨在了解非贵金属合金的某些合金成分如何以受控且期望的方式执行目标反应。 科学项目还通过与创新的本科教育计划（称为Austin-International框架（AIF）的创新本科教育计划（AIF）相结合，该计划也得到了显着增强，该计划为UT Austin本科生提供了完全沉浸式，奖学金支持的国际交流经验。 它为学生提供了拓宽视野的独特机会，同时为他们的研究经验赢得了课程学分。这是教授群体之间的协作实验性计算研究计划。 Simon M. Humphrey和Graeme Henkelman在德克萨斯大学奥斯汀分校。 总体目的是利用通过微波辅助加热技术形成新型金属纳米合金的专业知识，并在硅中使用理论来指导合成研究并阐明纳米粒子催化剂作为表面结构和成分的功能。 该项目的具体目标是使用催化性较低和丰富的造币金属以及更高的氧金属（例如RU和RE）的组合制备新的二元和三元催化剂，以产生可以模仿稀有金属反应性的系统。 除了模拟模仿模仿逼真反应条件的模型化学反应研究外，还将使用光谱技术（例如电子显微镜，总X射线散射，扩展的X射线X射线结构，化学剂等）来阐明结构功能关系，以在原子质尺度上提供现实的理论模型。 然后，这些结构信息将用于构建和完善理论模型，以识别最重要的活性站点集合。 最终，这可以实现反应性和选择性的准确预测，可以利用这些预测以告知未来的合成目标，以确定最终具有所需反应性的催化剂：能够选择性地激活CH4至CH4至CH3和H的催化剂，在存在原子的情况下，这些奖项通过NSF的法定宣称和构成的构成，是由NSF的范围进行的，并且在宽广的范围内得到了良好的影响。 标准。