Collaborative Research: Preparation,Characterization,and Evaluation of Bimetallic Catalysts Using Electroless Deposition Methods for Selective Oxidation of Biomass-Related Alcohols

合作研究：利用化学沉积方法制备、表征和评价生物质相关醇的选择性氧化双金属催化剂

• 批准号: 0854339
• 负责人: John Monnier
• 金额: $ 32.99万
• 依托单位: University South Carolina Research Foundation
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2009
• 资助国家: 美国
• 起止时间: 2009-08-01 至 2012-07-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=0854339&HistoricalAwards=false
• 关键词: Collaborative; Research; Preparation; Characterization; Evaluation

0854339 MonnierA major goal of modern catalysis research is design and fabrication of catalysts that are selective toward reaction of a particular functional group. In attempting to tailor catalytic surfaces for selectivity, not only is it important to have a high level of control over the surface composition, but also to achieve this control using methods that can be scaled up for the economical production of large amounts of catalyst. 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 scaleable method that can be used to prepare truly bimetallic surfaces on supported catalyst particles, it shows great promise for catalytic applications in which selectivity can be tuned through adjustment of the surface composition. In the proposed effort, ED will be employed as a tool for tailoring bimetallic catalysts for the selective oxidation of biomass-related alcohols. In addition to being very important for the future production of fuels and chemicals, they serve as excellent probe molecules for assessing the capability of ED to prepare highly selective catalysts this class of reactions. The proposed effort will integrate a wide-ranging set of characterization techniques in pursuit of selective catalysts: 1. ED will be used to prepare a series of Au, Ag, and Cu-modified Pt and Pd catalysts having targeted metal compositions; these catalysts will be characterized using an array of spectroscopic techniques, and will be evaluated for glycerol oxidation. 2. DFT computational studies on the bimetallic compositions will be used to better understand and corroborate the characterization results and to suggest directions for further bimetallic catalyst compositions. 3. Catalyst evaluation results will be interpreted within the guidelines predicted by catalyst characterization and computation to make subsequent generations of catalysts. This iterative cycle should facilitate catalyst development leading to improved alcohol oxidation catalysts. The overall goal is to use these diverse capabilities to assess the utility of ED for preparation of bimetallic oxidation catalysts, and to take steps toward making rational improvements in catalyst design based on a fundamental understanding of electronic and structural features of the bimetallic catalysts. Intellectual Merit. The proposed work will help to develop ED as a potentially important technique for large-scale production of bimetallic catalysts. These efforts will also provide a template for programs aimed at identification of selective catalysts for reactions of multifunctional molecules. Furthermore, the close integration between (a) preparation and characterization of supported metal catalysts and (b) fundamental modeling and surface science studies will help to further develop the integration of basic science with applied catalysis, ultimately promoting rational design approaches for catalysis and materials synthesis. Broader Impact. The selective oxidation of biomass-related alcohols represents an important industrial target for production of a new class of bio-derived 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 PIs at different institutions, will allow those students to recognize the important contributions available from these different types of catalysis studies.

0854339 Monniera现代催化研究的主要目标是设计和制造催化剂，这些催化剂对特定功能组的反应有选择性。在尝试量身定制催化表面以提高选择性，不仅要对表面组成进行高水平的控制，而且还要使用可以对大量催化剂的经济生产进行扩展的方法来实现这种控制。一种有前途的技术是电气沉积（ED），它允许一种金属组件以受控量沉积在第二个金属的表面上。因为ED是一种可伸缩的方法，可用于在受支持的催化剂颗粒上准备真正的双金属表面，因此它对催化应用显示出很大的希望，在该应用中，可以通过调整表面组成来调整选择性。在拟议的工作中，ED将被用作调整双金属催化剂的工具，以选择性氧化生物质相关的醇。除了对未来的燃料和化学物质生产非常重要之外，它们还可以作为评估ED制备高度选择性催化剂能力的出色探针分子。提出的努力将集成一组广泛的表征技术，以追求选择性催化剂：1。ED将用于准备具有目标金属成分的一系列AU，Ag和Cu-Modified PT和PD催化剂；这些催化剂将使用一系列光谱技术来表征，并将评估用于甘油氧化。 2。关于双金属组合物的DFT计算研究将用于更好地理解和证实表征结果，并提出了进一步的双金属催化剂组成的方向。 3。将在通过催化剂表征和计算预测的指南中解释催化剂评估结果，以使后代的催化剂产生。这种迭代周期应促进催化剂的发育，从而改善酒精氧化催化剂。总体目标是利用这些多样化的能力来评估ED用于制备双金属氧化催化剂的实用性，并根据对双金属催化剂的电子和结构特征的基本了解，采取步骤进行催化剂设计的合理改进。智力优点。拟议的工作将有助于开发ED作为大规模生产双金属催化剂的潜在重要技术。这些努力还将为旨在识别多功能分子反应的选择性催化剂的程序提供模板。此外，（a）支持金属催化剂和（b）基本建模和表面科学研究之间的紧密整合将有助于进一步发展基础科学与应用催化的整合，最终促进催化和材料合成的合理设计方法。更广泛的影响。与生物质相关的醇的选择性氧化是生产新型生物衍生产品的重要工业目标。促进更高选择性的ED准备催化剂可以帮助降低过程分离成本，过度使用原料以及对环境的排放。这项合作努力还将使毕业生和本科生可以参与催化群落中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。从事该项目的学生获得的广泛经验以及不同机构与多个PI的互动将使这些学生能够认识到这些不同类型的催化研究中可获得的重要贡献。