GOALI: A Scientific Synthesis of Bimetallic Catalysts

GOALI：双金属催化剂的科学合成

• 批准号: 1160036
• 负责人: John Regalbuto
• 金额: $ 32万
• 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: 2012
• 资助国家: 美国
• 起止时间: 2012-09-15 至 2016-08-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1160036&HistoricalAwards=false
• 关键词: GOALI; Scientific; Synthesis; Bimetallic; Catalysts

#1160036RegalbutoThe most common method of preparing supported metal catalysts begins by impregnating a porous oxide or carbon with an aqueous solution of dissolved metal complexes. The goal of most preparations is to convert the deposited precursor, often a coordination complex, into small metal particles firmly anchored onto the high surface area support. For a given amount of metal, the smaller the metal particles, the more catalytically active sites are created. In promoted or bimetallic catalysts, the goal is normally to maximize contact of the metal and promoter, or the two metals. How to achieve this effectively is the subject of many studies, both academic and industrial.In many cases these preparation steps are considered to be art. Professor John Regalbuto of the University of South Carolina has been effectively studying the fundamental phenomena that occur during supported metal catalyst impregnation, striving to transform the art of catalyst preparation into a science. With past support from NSF his research group has described the uptake of noble and base metal coordination complexes over many oxides and carbons during impregnation in terms of a simple electrostatic mechanism leading to an optimal pH at which the precursor-surface interaction is strongest. Fundamental aspects of the other preparation steps of these monometallic catalysts have also been studied. In this proposal, the strong electrostatic adsorption approach will be applied to the most complicated but highest impact preparations - bimetallic catalysts. Regalbuto postulates that this approach will yield unprecedented control of the morphology of bimetallic catalysts prepared with real, high surface area supports using common, commercially available metal precursors. Specifically, he hypothesizes that core-shell morphologies can be prepared by selectively adsorbing one metal precursor complex onto the oxide form of a second metal, and that core-shell morphology will be retained with low reduction temperatures and alloys will form at higher temperatures. Another alternative application of the science approach predicts that homogeneous alloys can be prepared with low temperature reductions by coadsorbing metal complexes in a single adsorption step.It is hoped that successful demonstrations of the proposed work will lead to a transformation in the understanding and practice of bimetallic catalyst preparation. The potential scientific impact is extremely broad, affecting all facets of the chemical industry which employ bimetallic catalysts. With that target, this award is a GOALI award. Regalbuto has teamed with the Johnson Matthey Technical Centre in Sonning, UK, a world leading company in noble metal catalyst manufacture. Measurements of point of zero charge and adsorption surveys over a wide range of noble metal oxides will be made for the first time at JMTC as well as at the University of South Carolina. Strategically, the partnership with industry will allow access to the copious amounts of noble metal oxides needed for the fundamental studies of adsorption properties.The project work has been formulated specifically for REU students; this work will be relatively easy to undertake, exciting to do, and will get noticed in peer reviewed publications and conference presentations. In addition the PI will tie into the comprehensive portfolio of outreach and diversity programs offered at USC: the Louis Stokes Alliance for Minority Participation, the SC Alliance for Minority Participation, and the South East Alliance for Graduate Education.

#1160036Regalbuto 制备负载型金属催化剂的最常见方法是用溶解的金属络合物的水溶液浸渍多孔氧化物或碳。大多数制备的目标是将沉积的前体（通常是配位络合物）转化为牢固锚定在高表面积载体上的小金属颗粒。对于给定量的金属，金属颗粒越小，产生的催化活性位点就越多。在助催化剂或双金属催化剂中，目标通常是使金属和助催化剂或两种金属的接触最大化。如何有效地实现这一目标是许多学术和工业研究的主题。在许多情况下，这些准备步骤被认为是艺术。南卡罗来纳大学的 John Regalbuto 教授一直有效地研究负载型金属催化剂浸渍过程中发生的基本现象，努力将催化剂制备艺术转变为一门科学。在 NSF 过去的支持下，他的研究小组描述了在浸渍过程中贵金属和贱金属配位络合物在许多氧化物和碳上的吸收，采用简单的静电机制，导致前体-表面相互作用最强的最佳 pH 值。还研究了这些单金属催化剂的其他制备步骤的基本方面。在该提案中，强静电吸附方法将应用于最复杂但影响最大的制剂——双金属催化剂。 Regalbuto 假设，这种方法将对双金属催化剂的形态产生前所未有的控制，该双金属催化剂是使用常见的市售金属前体制备的真正的高表面积载体。具体来说，他假设可以通过将一种金属前体复合物选择性吸附到第二种金属的氧化物形式上来制备核-壳形态，并且核-壳形态将在低还原温度下保留，合金将在较高温度下形成。 科学方法的另一种替代应用预测，可以通过在单个吸附步骤中共吸附金属配合物来低温还原制备均质合金。希望所提出的工作的成功示范将导致双金属催化剂制备的理解和实践的转变。 潜在的科学影响极其广泛，影响到使用双金属催化剂的化学工业的各个方面。出于这个目标，这个奖项是一个 GOALI 奖项。 Regalbuto 与位于英国桑宁的庄信万丰技术中心合作，这是一家世界领先的贵金属催化剂制造公司。 JMTC 和南卡罗来纳大学将首次对各种贵金属氧化物进行零电荷点测量和吸附调查。从战略上讲，与工业界的合作将允许获得吸附特性基础研究所需的大量贵金属氧化物。该项目工作是专门为 REU 学生制定的；这项工作相对容易开展，令人兴奋，并且会在同行评审的出版物和会议演讲中受到关注。此外，PI 将与南加州大学提供的综合外展和多元化项目组合相结合：路易斯斯托克斯少数族裔参与联盟、南卡罗来纳州少数族裔参与联盟和东南研究生教育联盟。