Collaborative Research: Tuning Hydrogen Mobility on Au/Spinel Catalysts to Develop the Isotopic Kinetic Resolution of H2 and D2

合作研究：调节 Au/尖晶石催化剂上的氢迁移率以开发 H2 和 D2 的同位素动力学分辨率

• 批准号: 2102525
• 负责人: Bert Chandler
• 金额: $ 29.8万
• 依托单位: Pennsylvania State Univ University Park
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2021
• 资助国家: 美国
• 起止时间: 2021-09-01 至 2024-08-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=2102525&HistoricalAwards=false
• 关键词: Collaborative; Research; Tuning; Hydrogen; Mobility

With funding from the Chemical Catalysis program in the Division of Chemistry, Professor Chandler at Penn State University and Professor Grabow at the University of Houston will collaborate to build the scientific foundations for a new H-D separation technique termed “isotopic kinetic resolution” (IKR). Due to the added mass of the neutron, deuterium tends to react more slowly in H-atom transfer reactions. The research team will conduct an experimental and computational study of hydrogen mobility and diffusion across aluminum oxide surfaces to understand the important factors in controlling the speed of H- and D- atom transport. This will include developing methods to control the spacing between catalytic H2/D2 activation sites and H/D reaction sites on the oxide surface. The team will then screen spinel oxides, a class of transition doped aluminum oxide materials with wide ranging electronic properties, for their H/D-atom transport properties using several computational and machine-learning techniques. Promising candidate oxides will be synthesized and their H-mobility fully evaluated and compared to predictions to begin developing the IKR. Both principal investigators will recruit graduate and undergraduate students from underrepresented minority (URM) groups. The principal investigators are also accomplished undergraduate mentors and will continue to involve UG students in this project.This collaborative research project will be focused on experimental and computational studies of hydrogen mobility and diffusion across tunable spinel oxide surfaces, with the aim of developing the novel concept of isotopic kinetic resolution (IKR). IKR is a kinetic tool capable of separating H/D isotopes by leveraging the large kinetic isotope effect for H/D transport on metal oxides. Further development of this technique may also lead to new design strategies for selective hydrogenation catalysts. To establish this new tool, the team will use density functional theory calculations combined with machine-learning techniques to screen for spinel oxides with suitable electronic structures. Promising candidates will be synthesized and their H-mobility evaluated through careful kinetic measurements and kinetic Monte Carlo simulations. Significant effort will be dedicated to the development of synthetic methods that will allow the research team to direct the spacing between primary reaction centers, where H2 is activated, and secondary reaction centers, where hydrogenation occurs.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.

在化学系化学催化项目的资助下，宾夕法尼亚州立大学的钱德勒教授和休斯顿大学的Grabow教授将合作为一种名为“同位素动力学解析”（IKR）的新H-D分离技术建立科学基础。 由于中子的质量增加，氘在氢原子转移反应中反应更慢。研究小组将对氢在氧化铝表面的迁移和扩散进行实验和计算研究，以了解控制H-和D-原子传输速度的重要因素。 这将包括开发控制氧化物表面上催化H2/D2活化位点和H/D反应位点之间间距的方法。 然后，该团队将使用多种计算和机器学习技术筛选尖晶石氧化物，这是一类具有广泛电子特性的过渡掺杂氧化铝材料，用于其H/D原子传输特性。 有希望的候选氧化物将被合成和他们的H-流动性充分评估和预测相比，开始发展IKR。 两位主要研究人员将从代表性不足的少数民族（URM）群体中招募研究生和本科生。主要研究人员也是本科生导师，并将继续参与UG学生在这个项目中，这个合作研究项目将集中在氢的流动性和可调尖晶石氧化物表面的扩散的实验和计算研究，与发展的同位素动力学分辨率（IKR）的新概念的目的。IKR是一种能够通过利用金属氧化物上H/D传输的大动力学同位素效应来分离H/D同位素的动力学工具。该技术的进一步发展也可能导致选择性加氢催化剂的新设计策略。为了建立这种新工具，该团队将使用密度泛函理论计算结合机器学习技术来筛选具有合适电子结构的尖晶石氧化物。有前途的候选人将合成和他们的H-流动性通过仔细的动力学测量和动力学蒙特卡罗模拟评估。该奖项将致力于开发合成方法，使研究团队能够指导初级反应中心（H2被激活的地方）和次级反应中心（氢化发生的地方）之间的空间。该奖项反映了NSF的法定使命，并通过使用基金会的知识价值和更广泛的影响审查标准进行评估，被认为值得支持。