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

用于凝相生物质转化的定制碳负载催化剂

• 批准号: 1804436
• 负责人: Jean-Philippe Tessonnier
• 金额: $ 30万
• 依托单位: Iowa State University
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2018
• 资助国家: 美国
• 起止时间: 2018-09-01 至 2022-02-28
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1804436&HistoricalAwards=false
• 关键词: Tailored; Carbon; Supported; Catalysts; Conversion

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.

由农业废物和非食用植物生产的生物质提供了丰富，便宜且可再生的化学原料来源，可以升级到广泛的化学产品。 生物质衍生的原材料的复杂性需要精心调整的催化剂，这些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，将调整由碳载体上的贵金属组成的催化剂，以生产特定的化学物质，重点是以将化学物质指向目标化学产品的方式来设计碳材料。 该研究产生的科学和工程将促进可再生原料的化学物质生产，从而减少对化石资源的依赖，减少全球碳足迹，刺激和多样化的农村经济以及促进一系列教育机会。 金属辅助相互作用提供了合适的手柄，可通过化学和电子效应来设计所选金属功能的催化活性。在碳的情况下，这种相互作用通常被忽略了，因为这种材料通常被认为是在催化中惰性的。然而，有充分的材料科学证据表明，可以通过改变覆盖其表面的氧气部分的性质和浓度来量身定制碳的电子性质。结果，可以在4.4和5.4 eV之间调节常规碳支架的工作函数，为研究和利用电子金属支持相互作用提供了理想的平台，而没有与氧化物常见的原子迁移率相关的挑战。该项目将使氧部分引入的化学和电子相互作用解脱，并揭示其对支持钯（PD）和铂（PT）纳米颗粒的氢化性能的真实影响。肉桂醛和呋喃醛将被用作探针分子，因为它们同时提出了碳碳和碳 - 氧气双键 - 在基于生物的化学物质中常见的两个功能。相关的基本理解将产生可转化的概念，以操纵碳支持的催化剂的性能，尤其是PD/C和PT/C，这是两个在化学工业中具有广泛应用的催化剂。 该项目的更广泛的方面将包括几项以学生为基础的社区为基础的教育和外展活动，该计划“ Be Iowa Smart”将吸引一群多样化的学生进入科学，技术，工程和数学（STEM）学科，并通过IOWA和MEDWEST的竞争范围来建立竞争性和全球范围的劳动力。优点和更广泛的影响审查标准。

项目成果

Oxygen-Doped Carbon Supports Modulate the Hydrogenation Activity of Palladium Nanoparticles through Electronic Metal–Support Interactions

• DOI: 10.1021/acscatal.2c01063
• 发表时间: 2022-06
• 期刊: ACS Catalysis
• 影响因子: 12.9
• 作者: R. G. Rao;R. Blume;M. Greiner;Pei Liu;T. Hansen;Kathleen S Dreyer;D. Hibbitts;J. Tessonnier

Bottom-Up Synthesis Strategies Enabling the Investigation of Metal Catalyst-Carbon Support Interactions

• DOI: 10.3390/c8030037
• 发表时间: 2022-06
• 期刊: C
• 作者: H. Bateni;Prathamesh T. Prabhu;Hannah E. Gebur;J. Tessonnier