Tailored Carbon-Supported Catalysts for the Conversion of Biomass in the Condensed Phase

从农业废弃物和非食用植物中产生的生物质提供了丰富、廉价和可再生的化学原料来源，可以升级为各种化学产品。生物质衍生原料的复杂性需要精细调整的催化剂，可以攻击特定的化学键以形成所需的产品。在这项研究中，由分散在碳载体上的贵金属组成的催化剂将被调整以产生特定的化学物质，重点是设计碳材料，以将化学作用导向目标化学产品。该研究产生的科学和工程将促进利用可再生原料生产化学品，从而减少对化石资源的依赖，减少全球碳足迹，刺激农村经济并使其多样化，并促进一系列教育机会。金属支持的相互作用提供了一个合适的处理工程的催化活性选定的金属功能，通过化学和电子效应。在碳的情况下，这种相互作用通常被忽视，因为这种材料通常被认为是惰性的催化。然而，材料科学中有充分的证据表明，碳的电子特性可以通过改变覆盖其表面的氧部分的性质和浓度来调整。因此，传统碳支架的功函数可以在4.4和5.4 eV之间调节，为研究和利用电子金属支撑相互作用提供了理想的平台，而没有氧化物常见的与原子迁移率相关的挑战。该项目将解耦氧部分引入的化学和电子相互作用，并揭示它们对负载型钯（Pd）和铂（Pt）纳米颗粒加氢性能的真正影响。肉桂醛和糠醛将被用作探测分子，因为它们具有碳-碳和碳-氧双键，这是生物基化学物质中常见的两种功能。相关的基本理解将产生革命性的概念，用于操纵碳负载催化剂的性能，特别是Pd/C和Pt/C，这两种催化剂在化学工业中有着广泛的应用。该项目的更广泛方面将包括以学生为主导的社区项目“聪明的爱荷华州”（Be Iowa Smart）为重点的几项教育和推广活动，该项目将吸引不同群体的学生学习科学、技术、工程和数学（STEM）学科，并在爱荷华州和中西部地区建立一支具有竞争力和全球参与的劳动力队伍。该奖项反映了美国国家科学基金会的法定使命，并通过使用基金会的知识价值和更广泛的影响审查标准进行评估，被认为值得支持。

Biomass, produced from agricultural waste and non-edible plants, offers an abundant, cheap, and renewable source of chemical raw materials that can be upgraded to a wide range of chemical products. The complexity of the biomass-derived raw materials necessitates finely tuned catalysts that can attack specific chemical bonds to form desired products. In this study, catalysts consisting of noble metals dispersed on carbon supports will be tuned to produce specific chemicals, with emphasis on engineering the carbon materials in ways that direct the chemistry towards the targeted chemical products. The science and engineering generated by the study will promote the production of chemicals from renewable feedstocks, thereby decreasing dependence on fossil resources, reducing global carbon footprint, stimulating and diversifying rural economies, and promoting a range of educational opportunities. Metal-support interactions provide a suitable handle to engineer the catalytic activity of a chosen metal function through both chemical and electronic effects. Such interactions have been generally overlooked in the case of carbon as this material is usually considered to be inert in catalysis. Yet, there is ample evidence in materials science that the electronic properties of carbons can be tailored by varying the nature and concentration of the oxygen moieties that cover their surface. As a result, the work function of conventional carbon scaffolds can be modulated between 4.4 and 5.4 eV, providing an ideal platform for studying and harnessing electronic metal-support interactions without the challenges associated with atom mobility that are common for oxides. The project will decouple the chemical and electronic interactions introduced by oxygen moieties and reveal their true effects on the hydrogenation performance of supported palladium (Pd) and platinum (Pt) nanoparticles. Cinnamaldehyde and furfural will be utilized as probe molecules as they present both carbon-carbon and carbon-oxygen double bonds - two functionalities common in bio-based chemicals. The associated fundamental understanding will yield transformative concepts for manipulating the performance of carbon-supported catalysts, in particular Pd/C and Pt/C, two catalysts with broad applications in the chemical industry. Broader aspects of the project will include several educational and outreach activities highlighted by a student-led community-based program "Be Iowa Smart" that will attract a diverse group of students to science, technology, engineering, and mathematics (STEM) disciplines, and build a competitive and globally engaged workforce in Iowa and the Midwest.This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.