RUI: Preparation and Kinetic Characterization of New Bimetallic Au-M Selective Hydrogenation Catalysts

RUI：新型双金属Au-M选择性加氢催化剂的制备及动力学表征

• 批准号: 1566301
• 负责人: Bert Chandler
• 金额: $ 35.7万
• 依托单位: Trinity University
• 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: 2018-03-01 至 2021-08-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1566301&HistoricalAwards=false
• 关键词: RUI; Preparation; Kinetic; Characterization; New

This award is funded by the Chemical Catalysis Program in the Division of Chemistry. Professors Bert D. Chandler and Christopher J. Pursell of Trinity University are supported to investigate the advantages of combining inexpensive metals with gold (Au) to form bimetallic nanoparticle catalysts. The project addresses the need to find alternatives to scarce and expensive catalysts which are prohibitive to large-scale chemical production. Improving the fundamental understanding of bimetallic nanoparticles and their catalytic properties has the potential to positively impact both the U. S. catalysis industry and the national economy by providing cheaper materials and consumer products as well as reducing pollution and industrial waste. The project involves preparing tailored nanoparticles with an inexpensive metal, such as copper, nickel and iron, at the core and Au on the outside. This includes finding new synthetic means to assemble a few hundred atoms from two metals - which is a challenging chemical synthesis problem. The goals are to evaluate synthetic methods, understand how the inexpensive metal alters the catalytic chemistry of gold, and test the new catalysts for improved performance in some industrially important reactions. Integrating the research with education provides research opportunities for undergraduate students, giving them hands on experience in this nationally important area of research and training them to be the next generation of scientists. New nanoparticle and catalyst synthesis techniques are being employed to prepare bimetallic nanoparticles on alumina and titania. The primary goal is to take advantage of recent developments in solution nanoparticle synthesis to develop new routes to synthetically challenging bimetallic core-shell nanoparticle catalysts. Kinetics -based analytical techniques are being used to evaluate the new catalysts including (i) intentional poisoning studies to evaluate relative numbers of active sites, (ii) Michaelis-Menten analysis of poisoning experiments to evaluate the effects of thiol poisoning, and (iii) Hammett relationships to probe changes in nanoparticle surface charge. These studies enable new quantitative comparisons between catalysts and allow for assessing heterometals affect the chemistry of Au nanoparticles. In addition, these studies are addressing fundamental questions regarding the nature of the catalytic active sites. This project also expands on a recent discovery of "broad band IR absorption" for Au/TiO2 catalysts, and uses this phenomenon to characterize the strength of H2 and CO adsorption on the catalysts. These physical characterization studies, combined with detailed kinetics studies, are enabling the development of structure-property-activity relationships that guide researchers in designing the next generation of catalysts. In particular, these studies are (i) providing clear information regarding how Au nanoparticle chemistry and catalysts can be tuned using other transition metals, (ii) testing recent computational models, and (iii) providing insight into potential new applications for Au based catalysts.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.

该奖项由化学部的化学催化计划资助。 Bert D. Trinity大学的钱德勒和Christopher J. Pursell得到支持，研究将廉价金属与金（Au）结合形成纳米颗粒催化剂的优点。 该项目解决了寻找稀缺和昂贵的催化剂的替代品的需要，这些催化剂对大规模化学品生产是禁止的。 提高对纳米粒子及其催化性能的基本理解有可能对美国和欧洲产生积极影响。S.通过提供更便宜的材料和消费品以及减少污染和工业废物，催化工业和国民经济。 该项目涉及制备量身定制的纳米颗粒，其核心是廉价的金属，如铜、镍和铁，外部是Au。 这包括寻找新的合成方法，从两种金属中组装几百个原子-这是一个具有挑战性的化学合成问题。 目标是评估合成方法，了解廉价金属如何改变金的催化化学性质，并测试新催化剂在一些工业重要反应中的性能。 将研究与教育相结合，为本科生提供研究机会，让他们在这个国家重要的研究领域获得经验，并培养他们成为下一代科学家。 新的纳米颗粒和催化剂合成技术正在被用来制备氧化铝和二氧化钛上的纳米颗粒。 主要目标是利用溶液纳米颗粒合成的最新进展，开发新的合成具有挑战性的核-壳纳米颗粒催化剂的路线。 基于动力学的分析技术被用于评估新的催化剂，包括（i）有意中毒研究以评估活性位点的相对数量，（ii）中毒实验的Michaelis-Menten分析以评估硫醇中毒的影响，和（iii）Hammett关系以探测纳米颗粒表面电荷的变化。这些研究使催化剂之间的新的定量比较，并允许评估影响Au纳米粒子的化学的杂金属。 此外，这些研究正在解决有关催化活性部位的性质的基本问题。 该项目还扩展了最近发现的Au/TiO 2催化剂的"宽带IR吸收"，并使用该现象来表征催化剂上的H2和CO吸附强度。 这些物理表征研究与详细的动力学研究相结合，能够开发结构-性能-活性关系，指导研究人员设计下一代催化剂。 特别地，这些研究是（i）提供关于如何使用其他过渡金属调节Au纳米颗粒化学和催化剂的明确信息，（ii）测试最近的计算模型，以及（iii）为Au基催化剂的潜在新应用提供了深入的见解。该奖项反映了NSF的法定使命，并通过利用基金会的知识价值和更广泛的影响进行评估，被认为值得支持审查标准。