CAS: Collaborative Research: Tailoring the Distribution of Transient vs. Dynamic Active Sites in Solid-Acid Catalysts and Their Impacts on Chemical Conversions

在化学系化学催化项目的资助下，俄克拉荷马州立大学的Jeffrey White和俄克拉荷马大学的Steven Crossley、Daniel Resasco和Bin Wang将开展新型沸石催化剂的跨学科研究。人们需要强大而可持续的催化剂，将各种来源的分子（包括传统碳氢化合物、废物流和植物原料）转化为能源载体以及消费品和耐用品的构件，需要对催化剂设计变量、最终功能和环境影响有基本的了解。 固体酸催化剂，包括被称为沸石的一类重要材料，由于具有多种可设计的结构和拓扑，对于新原料的加工以及减少传统碳氢化合物转化中的有害副产物具有吸引力。 这些催化剂对环境无害，不需要使用贵金属。该团队将进行研究合作，以确定新的催化剂材料，以应对非常规和富含水的原料带来的挑战，并减少环境足迹。 该合作团队将培训所有大学级别的学生，包括本科生、研究生和代表性不足的群体，使其成为国家 STEM（科学、技术、工程和数学）基础设施的积极贡献者。通过出版物以及地方、州、国家和国际会议，该团队将提高人们对基础催化研究如何影响当前和未来重要经济行业的认识，并将吸引工业合作伙伴的关注。该合作团队将使用跨学科的合成、表征、模拟和反应分析方法来创建和表征新型沸石催化剂，其中孤立、配对、邻近和协同活性位点的分布受到控制。博士。 White、Resasco、Wang 和 Crossley 将从事沸石的定制合成、沸石的合成后改性、原位光谱核磁共振测量以及不同温度和压力下的反应器研究，以确定催化剂活性位点的放置、分布和时间行为在涉及传统和非传统原料的关键反应中如何响应。 目标包括减少不需要的化学副产品（最终导致二氧化碳排放量增加），以及控制可逆与不可逆活性位点降解途径。该团队将努力通过每个校园的项目，推动代表性不足的群体纳入 STEM 学科，并通过大学和州一级的公共媒体提高公众对催化益处的认识。该奖项反映了 NSF 的法定使命，并通过使用基金会的智力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 funding from the Chemical Catalysis Program of the Chemistry Division, Jeffrey White of Oklahoma State University and Steven Crossley, Daniel Resasco and Bin Wang of University of Oklahoma will carry out an interdisciplinary study of new zeolite catalysts. The need for robust but sustainable catalysts that can convert molecules derived from a variety of sources, including traditional hydrocarbons, waste streams, and plant-based feedstocks into energy carriers and building blocks for consumable and durable goods requires fundamental understanding of catalyst design variables, resulting function, and environmental impacts. Solid-acid catalysts, including the important class of materials known as zeolites, are attractive for the processing of new feedstocks as well as reducing harmful byproducts in conversion of traditional hydrocarbons, due to the variety of designable structures and topologies. These catalysts are environmentally benign and do not require use of precious metals. The team will be engaged in a research collaboration to identify new catalyst materials that meet the challenges posed by unconventional and water-rich feeds, as well as reduce environmental footprints. The collaborative team will train students at all college levels, including undergraduate, graduate, and under-represented groups, to be active contributors to the national STEM (science, technology, engineering, and mathematics) infrastructure. Through publication outlets and local, state, national, and international meetings, the team will increase awareness of how fundamental catalysis research impacts economically important industries, both present and future, and will attract attention from industrial partners.The collaborative team will use an interdisciplinary synthesis, characterization, simulation, and reaction analysis approach to create and characterize new zeolite catalysts where the distribution of isolated, paired, proximate, and synergistic active sites are controlled. Drs. White, Resasco, Wang and Crossley will be engaged in tailored synthesis of zeolites, post-synthetic modifications of zeolites, in-situ spectroscopic NMR measurements, and reactor studies at varying temperature and pressure to determine how catalyst active site placement, distribution, and temporal behavior respond in key reactions involving both traditional and non-traditional feedstocks. Goals include reduction of unwanted chemical byproducts, which ultimately lead to increased CO2 emissions, and control of reversible vs. irreversible active site degradation pathways. The team will endeavor to advance inclusion of underrepresented groups in STEM disciplines through programs on each campus, and increase public awareness of the benefit of catalysis through public media outlets at the university and state level.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.