GOALI: The Engineering of Noble Metal Catalyst Impregnation

这个GOALI研究项目将研究贵金属配合物从溶液中吸附到广泛使用的氧化物和碳载体上的基本化学现象。一种被高度认可的预测工具，修订物理吸附（RPA）模型，已经被开发出来，它导致了阴离子或阳离子贵金属配合物与表面质子化或去质子化羟基的相互作用的新理解。“零电荷点”和溶液pH值决定了离子相互作用的性质。质子在本体溶液和表面之间的转移已被确定为一个关键的机械步骤。这项正在进行的研究的主要重点将是发展新的科学见解，这些见解可用于设计包括碳在内的几种重要工业催化剂载体的性能。由于这些催化剂对加氢反应和燃料电池的重要性，因此对活性贵金属如Pt和Pd的吸附将是主要的重点。控制对碳的吸附将主要通过加入特定类型的含o表面基团来实现；铌、硫酸氧化锆和混合金属氧化物也将被检查。工业合作者将提供关键的材料合成能力和互补的表征技术。进入阿贡国家实验室的先进光子源是这项工作所固有的。GOALI合作项目提供的实物和实际支持总额为50万美元，用于为期3年的研究项目。审稿人对这一提案的评价非常高，既基于其卓越的科学成就，也基于其对关键催化处理技术的重要性。先前的研究成果被认为是对催化剂制备的理解做出了创新的、突破性的贡献。表征技术，如EXAFS现在允许理论认识的关键方面得到确认。一个备受尊敬的工业团队是这个GOALI项目的一部分，大学调查员有与工业互动的记录。这项工作的广泛影响包括基础科学在重要国家研究重点中的实际应用，例如用于PEM燃料电池的改进碳基电极的开发。这项工作的其他方面将应用于改善催化剂制备的环境方法，特别是重金属。该研究项目的教育方面在研究生和本科生水平上都很强。学生将通过一个成功的NSF REU网站参与新材料，该网站涉及大量来自代表性不足群体的学生。

This GOALI research program will investigate the fundamental chemical phenomena associated with the adsorption of noble metal coordination complexes from solution onto widely used oxide and carbon supports. A highly recognized predictive tool, the Revised Physical Adsorption (RPA) model, has been developed which has led to a new understanding of the interaction of anionic or cationic noble metal complexes and the protonated or deprotonated hydroxyl groups at surfaces. The "point of zero charge" and the solution pH determine the nature of the ionic interaction. Proton transfer between the bulk solution and the surface has been identified as a key mechanistic step. The main focus on this ongoing research will be on the development of new scientific insight that can be used to engineer the properties of several important industrial catalyst supports including carbon. The adsorption of active noble metals such as Pt and Pd will the primary emphasis because of the importance of these catalysts for hydrogenation reactions and for fuel cells. Control of adsorption on carbon will be exercised primarily through the incorporation of specific types of O-containing surface groups; niobia, sulfated zirconia, and mixed metal oxides will also be examined. Industrial collaborators will provide key material synthesis capabilities and complementary characterization techniques. Access to the Advanced Photon Source at Argonne National Laboratories is inherent to the work. Combined in-kind and actual support from the GOALI collaborations is $500,000 for the 3-year research project.Reviewers rated this proposal very strongly, both on the basis of its scientific excellence and its importance to key catalytic processing technology. The prior research accomplishments have been recognized as making an innovative, ground-breaking contribution to the understanding of catalyst preparation. Characterization techniques such as EXAFS have now allowed key aspect of the theoretical understanding to be confirmed. A highly respected industrial team is part of this GOALI project, and the university investigator has a demonstrated record of interaction with industry.The broader impacts of the work include the practical applications of the fundamental science to important national research priorities, such as the development of improved carbon-based electrodes used in PEM fuel cells. Other aspects of the work will have applications in improved environmental approaches to catalyst preparation, especially for heavy metals. Educational aspects of the research project are strong at both the graduate and undergraduate level. Students will be involved through a successful NSF REU site on Novel Materials that has involved significant numbers of students from underrepresented groups.