Collaborative Research: Tailoring Solid Catalysts for Selective Reaction of Multifunctional Molecules

建议标题：协作研究：为多功能分子的选择反应量身定做固体催化剂建议编号：cts-0456899/cts-0456908主要研究员：John Monnier/J.William Medlin研究所：南卡罗来纳大学研究基金会/科罗拉多大学博尔德分析(决策的基本原理)：现代催化研究的主要目标是设计和制造对特定官能团的反应具有选择性的“下一代”双金属催化剂。双金属催化剂的合成通常是通过同时将两种金属盐共浸渍到催化剂载体上或通过连续的金属盐添加步骤来进行的。对于这两种制备方法中的任何一种，几乎不可能确保只形成双金属颗粒；相反，可以并且确实会形成两种金属的单独金属颗粒。因此，很难表征这种催化体系，更难将催化剂性能与双金属催化剂组成相关联。一种很有前途的技术是无电沉积(ED)，它允许在第二种金属的表面上以受控的数量沉积一种金属成分。由于ED是一种可以扩大规模以经济地生产大量催化剂的方法，因此它在通过调整表面组成来调节选择性的催化应用中显示出巨大的前景。在这项工作中，ED将被用作定制纳米级双金属催化剂的工具，这些催化剂可能对1-环氧基-3-丁烯(EPB)及其异构体巴豆醛(CRH)这两个不同官能团之一的加氢具有选择性。催化剂评价结果将与基础模拟和表面科学研究相结合，以评估ED在制备选择性双金属催化剂方面的有效性，并在对双功能试剂表面化学有基本了解的基础上，采取措施合理改进催化剂设计。就更广泛的技术影响而言，EPB和CRH的选择性加氢是生产各种精细化工产品的重要工业目标。促进更高选择性的ED制备的催化剂有助于减少工艺分离成本、原料的过度使用和对环境的排放。这一合作努力还将允许研究生和本科生参与催化社区内不同研究方法的整合，从表面科学实验到计算化学，再到现实催化剂的选择性探测器。从事这一项目的学生所获得的广泛经验，以及与不同机构的多名主要研究人员的互动，将使这些学生认识到这些不同类型的催化研究所做出的重要贡献。

AbstractProposal Title: Collaborative Research: Tailoring Solid Catalysts for Selective Reaction of Multifunctional Molecules Proposal Number: CTS-0456899/CTS-0456908Principal Investigator: John Monnier/J. William MedlinInstitution: University of South Carolina Research Foundation/University of Colorado at BoulderAnalysis (rationale for decision): A major goal of modern catalysis research is design and fabrication of "next generation" bimetallic catalysts that are selective toward reaction of a particular functional group. Bimetallic catalyst synthesis is typically carried out by either simultaneous co-impregnation of both metal salts onto the catalyst support or by successive steps of metal salt addition. For either of these preparative methods, it is virtually impossible to ensure formation of only bimetallic particles; rather, formation of separate metallic particles of both metals can and does occur. Thus, it is very difficult to characterize such catalytic systems, and even more difficult to correlate catalyst performance with bimetallic catalyst composition. One promising technique is electroless deposition (ED), which allows one metal component to be deposited in controlled quantities on the surface of a second metal. Because ED is a method that can be scaled up for the economical production of large amounts of catalyst, it shows great promise for catalytic applications in which selectivity can be tuned through adjustment of the surface composition. In this effort, ED will be employed as a tool for tailoring nanoscale, bimetallic catalysts that may be selective for hydrogenation of one of the two diverse functional groups of 1-epoxy-3-butene (EpB) and its isomer, crotonaldehyde (CrH). The catalyst evaluation results will be coupled with fundamental modeling and surface science studies to assess the utility of ED for preparation of selective bimetallic catalysts, and to take steps toward making rational improvements in catalyst design based on a fundamental understanding of bi-functional, reagent surface chemistry.In terms of broader technical impact, the selective hydrogenation of EpB and CrH represents an important industrial target for production of a variety of fine chemical products. ED-prepared catalysts that facilitate higher selectivity can help to reduce process separations costs, over-use of feedstocks, and emissions to the environments. This collaborative effort will also allow graduate and undergraduate students to be involved in the integration of diverse research approaches within the catalysis community, ranging from surface science experiments to computational chemistry to selectivity probes of realistic catalysts. The broad experience gained by the students who work on this project, as well as the interactions with multiple principal investigators at different institutions, will allow those students to recognize the important contributions available from these different types of catalysis studies.