CAREER: Nanoparticle Non-Noble Metal Intermetallic Compounds as Tunable Catalysts for Selective Hydrogenation Reactions

职业：纳米颗粒非贵金属金属间化合物作为选择性加氢反应的可调催化剂

基本信息

批准号：
1752063
负责人：
Siris Laursen
金额：
$ 50.01万
依托单位：
University of Tennessee Knoxville
依托单位国家：
美国
项目类别：
Standard Grant
财政年份：
2018
资助国家：
美国
起止时间：
2018-03-15 至 2023-02-28
项目状态：
已结题

来源：
https://www.nsf.gov/awardsearch/showAward?AWD_ID=1752063&HistoricalAwards=false
关键词：
CAREER Nanoparticle Non Noble Metal

项目摘要

The project will investigate new, low-cost materials for catalyzing important chemical reactions associated with the refining of petroleum and bio-based materials to produce fuels and a wide range of chemical products. In addition, the project will explore the potential for improving the effectiveness of the catalytic materials by synthesizing them as nanoparticles rather than traditional micron-sized particles. The new materials can be formed through combinations of many different elements, and the study will also develop methods for predicting the best combinations of elements for specific chemical reactions, thereby streamlining the catalyst discovery process and promoting U.S. competitiveness in the fuels and chemicals manufacturing sectors. The project will be linked to educational and outreach efforts that will train the next generation of engineers, and increase public awareness of new energy-efficient technologies such as fuel cells and batteries.Preliminary efforts in the investigator's laboratory have established a working understanding of how supported nanoparticle intermetallic compounds (IMCs) may be synthesized with well-defined bulk and surface compositions. The project will utilize those findings to enable a systematic study of IMC surface chemistry as a function of constituent elements in the selective hydrogenation of unsaturated aldehyde and nitro compounds. Experimental and computational methods will be used to examine the selectivity of C=C, C=O, and N-O activation, dissociation, and hydrogenation as a function of IMC bulk and surface composition and electronic structure information. Synthesis of oxide-supported non-noble metal nanoparticle IMCs will focus on developing clear understanding of the physical phenomena that dictate their bulk and surface composition as a function of element selection, oxide choice, and preparation environment. Formation of the bulk crystal structure of the nanoparticles will be investigated by ex- and in-situ x-ray diffraction and neutron scattering. Complementary high-resolution energy-dispersive x-ray spectroscopy will verify bulk composition and quantify elements not incorporated into the IMC nanoparticles. Surface composition of the IMCs will be analyzed using low energy ion scattering. Diffusion of constituent elements, particle growth, and bulk crystal structure will be analyzed as a function of synthesis variables to produce a complete picture of how well-defined nanoparticle IMCs may be produced. Results of these studies will allow for a general procedure to be developed for the synthesis, characterization, reactivity evaluation, and stability analysis of the IMC catalysts. Beyond the targeted reactions, the project will enable atomic- and electronic-level understanding of how nanoparticle IMC catalysis can be controlled and widely utilized in chemical transformations important to the field of heterogeneous catalysis. The educational component of the proposed program will serve to develop a surface and materials chemistry education program at the University of Tennessee, Knoxville. In addition, a YouTube video series, focused on materials, surface, and catalytic science, will be developed in a format accessible to the general population to promote a greater understanding of the impact these sciences have on everyday life.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.

该项目将调查与催化与石油和生物基材料的精炼相关的重要化学反应的新的低成本材料，以生产燃料和广泛的化学产品。此外，该项目将通过将催化材料作为纳米颗粒而不是传统的微米大小颗粒合成来探索提高催化材料有效性的潜力。可以通过许多不同元素的组合形成新材料，该研究还将开发用于预测特定化学反应元素最佳组合的方法，从而简化催化剂发现过程并促进美国在燃料和化学制造业中的竞争力。该项目将与教育和外展工作有关，这些工作将培训下一代工程师，并提高公众对燃料电池和电池等新的节能技术的认识。研究人员的实验室中的优先努力已经确立了对纳米粒子的支持如何合成的纳米粒子构成纳米粒子的努力理解，可以与良好的构造和表面构成合成。该项目将利用这些发现来实现对IMC表面化学的系统研究，这是不饱和醛和硝基化合物的选择性氢化中组成元素的函数。实验和计算方法将用于检查C = C，C = O和N-O激活，解离和氢化的选择性，这是IMC批量和表面组成和电子结构信息的函数。氧化物支持的非缺失金属纳米颗粒IMC的合成将集中于对物理现象的清晰理解，这些现象将其散装和表面组成决定是元素选择，氧化物选择和制备环境的函数。纳米颗粒的大块晶体结构的形成将通过前和原位X射线衍射和中子散射研究。互补的高分辨率能量分散性X射线光谱法将验证散装组成并量化未掺入IMC纳米颗粒中的元素。 IMC的表面组成将使用低能离子散射分析。组成元素，颗粒生长和大量晶体结构的扩散将是合成变量的函数，以产生定义明确的纳米颗粒IMC的完整图像。这些研究的结果将允许制定一般程序，以对IMC催化剂的合成，表征，反应性评估和稳定性分析。除了靶向反应外，该项目还将使原子和电子水平了解如何控制纳米颗粒IMC催化，并广泛用于对异质催化领域重要的化学转化中。拟议计划的教育部分将用于在田纳西州诺克斯维尔大学制定表面和材料化学教育计划。此外，将以一般人群可以使用的格式开发YouTube视频系列，专注于材料，表面和催化科学，以提高对这些科学对日常生活的影响的更多了解。该奖项反映了NSF的法定任务，并被认为是通过基金会的智力功能和广泛影响来评估CRITERIA CREITERIA的评估。