CAS: Quantifying the Systematic Catalytic Surface Chemistry of Non-Noble Metal Intermetallic Compounds to Achieve Diol and Olefin Production in Polyol Deoxygenation Reactions

在化学系化学催化项目的支持下，田纳西大学的Siris Laursen正在开发廉价的、土壤丰富的催化剂，用于生物质热解和生物柴油生产中的废物的增值。一个完全一体化的生物精炼厂的未来取决于有效和选择性地将生物质的所有部分转化为增值化合物。劳尔森博士和他的团队正在研究非贵金属金属间化合物作为催化剂，从生物质加工过程中产生的废水流中选择性地形成二醇和烯烃（构建块化学物质）。这些催化剂将被调整，以提供从废物中去除氧原子的更大活性，降低碳-碳键断裂的活性，降低烯烃加氢的活性。同时，对催化剂的组成-活性关系的一般理解正在发展，以提高预测性能，加速催化剂的发现，并推进催化剂的可持续性。该研究项目预计将影响K-12、本科和研究生教育，通过暑期体验将学生直接纳入研究小组，建立一支受过良好教育的劳动力队伍，以支持新的可再生化学工业。机构项目被用来支持这些经历的包容性，并确定可能从这些活动中受益最大的学生。非贵重金属间化合物是由过渡金属和后过渡金属或半金属组成的有序固体，具有将甘油部分或完全脱氧为1,2-丙二醇和丙烯的良好性质。Siris Laursen和他的研究小组正在利用量子化学表面反应模型和实验研究的结合来确定这些组成复杂催化剂的组成-活性关系，并加速发现可以从多元醇中产生有价值的化学物质的材料。正在确定促进从多元醇中部分和完全去除氧以产生有价值的二醇和烯烃的表面化学的特定范围。同样，催化剂组合物表现出更强的表面化学性质，以驱动多元醇完全分解产生氢（H2）和CO。通过了解金属间化合物在原子和电子水平上的特殊表面化学的起源，Laursen博士和他的学生们正在努力为非贵金属催化剂开发简单的基本设计规则，这些催化剂可能用于广泛的化学转化，这些化学转化仍然缺乏有效的催化材料。此外，通过整合研究和教育，该项目促进了未来科学家多样化群体的教育，并为生物炼制部门建立了一支受过良好教育的劳动力队伍。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。

With the support of the Chemical Catalysis Program in the Division of Chemistry, Siris Laursen of the University of Tennessee, Knoxville is developing inexpensive, earth-abundant catalysts for the valorization of waste from biomass pyrolysis and bio-diesel production. The future of a fully integrated biorefinery is contingent upon the efficient and selective conversion of all parts of biomass to value-added compounds. Dr. Laursen and his team are studying non-noble metal intermetallic compounds as catalysts to selectively form diols and olefins (building block chemicals) from water waste streams generated during biomass processing. These catalysts will be tuned in an effort to provide greater activity for the removal of oxygen atoms from the waste products, lower activity for carbon-carbon bond fragmentation, and lower activity for olefin hydrogenation. Simultaneously, a general understanding of the composition-activity relationships of the catalysts is being developed to improve predictive performance, accelerate catalyst discovery, and advance catalyst sustainability. This research project is expected to impact K-12, undergraduate, and graduate education by integrating students directly into the research group through summer experiences to build an educated workforce to support new renewable chemicals industries. Institutional programs are being used to support the inclusivity of these experiences and to identify students who may benefit the most from these activities.Non-noble intermetallic compounds are compositionally ordered solids composed of transition metals and post-transition metals or semimetals that have exhibited promising properties for the partial or complete deoxygenation of glycerol to 1,2-propanediol and propene. Siris Laursen and his research group are utilizing a combination of quantum chemical surface reaction modeling and experimental investigations to determine the composition-activity relationships of these compositionally complex catalysts and accelerate the discovery of materials that can produce valuable chemicals from polyols. Specific ranges of surface chemistry that promote the partial and complete removal of oxygens from polyols to produce valuable diols and olefins are being determined. Likewise, catalyst compositions that exhibit more aggressive surface chemistry to drive the complete breakdown of polyols to produce hydrogen (H2) and CO are also being noted. By understanding the origin of the special surface chemistry of intermetallic compounds at the atomic and electronic levels, Dr. Laursen and his students are working to develop simple fundamental design rules for non-noble metal catalysts that may be used in a wide range of chemical transformations that still lack efficient catalytic materials. Moreover, by integrating research and education, this project is promoting the education of a diverse group of future scientists and building an educated workforce for the biorefinery sector.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.