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

在田纳西大学化学系化学催化计划的支持下，诺克斯维尔大学的Siris Laursen正在开发廉价的、富含地球的催化剂，用于生物质热解和生物柴油生产中产生的废物的价态。完全集成的生物炼油厂的未来取决于生物质所有部分能否有效和选择性地转化为增值化合物。劳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中选择性地生成二元醇和烯烃(积木化学品)。这些催化剂将进行调整，以努力提供更高的活性，以从废物中去除氧原子，降低碳-碳键断裂的活性，并降低烯烃加氢的活性。同时，正在发展对催化剂组成-活性关系的总体理解，以改进预测性能，加速催化剂发现，并提高催化剂的可持续性。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，以建立一支受过教育的劳动力队伍，以支持新的可再生化学品行业。非贵金属间化合物是由过渡金属和过渡后金属或半金属组成的成分有序的固体，在甘油部分或完全脱氧为1，2-丙二醇和丙烯方面表现出良好的性能。Siris Laursen和他的研究小组正在利用量子化学表面反应建模和实验研究相结合的方法来确定这些组成复杂的催化剂的组成-活性关系，并加速发现可以从多元醇中生产有价值的化学品的材料。正在确定促进部分和完全去除多元醇中的氧以产生有价值的二元醇和烯烃的特定表面化学范围。同样，表现出更具侵略性的表面化学反应的催化剂组合物也被注意到，这种催化剂组合物能够促使多元醇完全分解，产生氢(H2)和CO。通过在原子和电子水平上了解金属间化合物特殊表面化学的起源，Laursen博士和他的学生正在努力为非贵金属催化剂制定简单的基本设计规则，这些规则可以用于仍然缺乏有效催化材料的广泛的化学转化。此外，通过整合研究和教育，该项目正在促进未来科学家的多样化群体的教育，并为生物精炼部门建立一支受过教育的劳动力队伍。该奖项反映了NSF的法定使命，并通过使用基金会的智力优势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.