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

摘要提案标题：合作研究：多功能分子选择性反应的定制固体催化剂提案编号：CTS-0456899/CTS-0456908首席研究员：John Monnier/J. William Medlin机构：南卡罗来纳州大学研究基金会/科罗拉多大学博尔德分校分析（决定理由）：现代催化研究的一个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”催化剂。 双金属催化剂合成通常通过将两种金属盐同时共浸渍到催化剂载体上或通过金属盐添加的连续步骤来进行。 对于这些制备方法中的任一种，几乎不可能确保仅形成双金属颗粒;相反，可以并且确实发生两种金属的单独金属颗粒的形成。 因此，很难表征这样的催化体系，甚至更难将催化剂性能与可再生催化剂组合物相关联。 一种有前景的技术是无电沉积（艾德），其允许一种金属组分以受控的量沉积在第二金属的表面上。 由于艾德是一种可以按比例放大以经济地生产大量催化剂的方法，因此它在催化应用中显示出很大的前景，其中可以通过调节表面组成来调节选择性。 在这项工作中，艾德将被用作一种工具，用于定制纳米级的，可选择性的1-环氧-3-丁烯（EpB）和它的异构体，巴豆醛（CrH）的两个不同的官能团之一的氢化催化剂。 催化剂评估结果将与基础建模和表面科学研究相结合，以评估艾德在制备选择性加氢催化剂方面的效用，并采取措施，根据对双功能试剂表面化学的基本理解，对催化剂设计进行合理改进。EpB和CrH的选择性氢化是生产各种精细化学产品的重要工业目标。 ED制备的催化剂具有更高的选择性，有助于降低工艺分离成本、原料的过度使用和对环境的排放。 这种合作努力还将使研究生和本科生参与催化社区内的各种研究方法的整合，从表面科学实验到计算化学，再到现实催化剂的选择性探针。 从事该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.