Light Alkane Upgrading Through Dehydrogenative C-N Coupling with NH3 over Bifunctional Metal/Zeolite Catalyst

该项目涉及乙烷转化为商品化学品乙腈的新工艺和催化剂设计。乙烷（天然气的一种低价值和催化折光成分）与氨在双功能金属/沸石催化剂上反应生成乙腈，相对于现有技术，该工艺具有潜在的环境和经济效益。该项目侧重于催化剂设计和反应机理的基本方面，以提高催化剂的性能和耐久性。除了技术方面，该项目还针对STEM学科中代表性不足的少数民族开展了教育和推广活动。本研究为乙烷脱氢C-N与氨气在双功能金属/沸石催化剂上直接偶联的基础研究奠定了基础。具体来说，该项目的目标是催化剂的结构/性能关系，以及对氨存在下金属官能团对C-H键活化的影响的基本理解。该项目研究了钴（Co）和铂（Pt）金属位点对沸石Brønsted/Lewis酸性的影响，并设计了一种优化金属/酸位点双功能的催化剂。此外，通过operando DRIFT-MS和弛缓型瞬态实验的结合，该项目将确定与串联双功能金属/沸石催化剂上反应动力学和机理相关的表面反应中间体。从该项目中获得的基本知识可以作为设计高效氨脱氢催化剂的基础。在该项目的支持下，PI将通过招募和留住有前途的化学工程学生，特别是来自代表性不足的群体的学生，帮助解决密西西比州STEM人才流失的问题。调查人员将与密西西比州立大学的各种外展项目密切合作。参与该项目的学生将获得在工业和学术职业道路上取得成功的技能。该项目由CBET催化项目和促进竞争研究的既定项目（EPSCoR）共同资助。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。

The project addresses a new process and catalyst design for on-purpose conversion of ethane to the commodity chemical acetonitrile. Ethane (a low-value and catalytically refractive component of natural gas) is reacted with ammonia over a bifunctional metal/zeolite catalyst to produce acetonitrile in a process that potentially offers both environmental and economic benefits with respect to existing technology. The project focuses on fundamental aspects of the catalyst design and the reaction mechanism to enhance catalyst performance and durability. Beyond the technical aspects, the project features educational and outreach activities targeting underrepresented minorities in STEM disciplines.This research will break ground for fundamental research for the direct ethane dehydrogenative C-N coupling with ammonia gas over bifunctional metal/zeolite catalysts. Specifically, the project targets catalyst structure/performance relationships and the fundamental understanding of the influence of metal functionality on C-H bond activation in the presence of ammonia. The project investigates the influence of cobalt (Co) and Platinum (Pt) metal sites on the Brønsted/Lewis acidity of the zeolite, in a catalyst design that would optimize metal/acid-site bifunctionality. Additionally, through the combination of operando DRIFT-MS and relaxation-type transient experiments, the project will identify the surface reaction intermediates as related to the kinetics and mechanism of the reaction over the tandem bifunctional metal/zeolite catalyst. The fundamental knowledge obtained from the project could be the basis for an efficient ammodehydrogenation catalyst design. With the support of this project, the PI will help address the problem of the loss of Mississippi’s STEM talent by recruiting and retaining promising chemical engineering students, especially from underrepresented groups. The investigator will work closely with various outreach programs at Mississippi State University. Students involved in this project will gain the skills to succeed in both industrial and academic career paths. This project is jointly funded by the CBET Catalysis program and the Established Program to Stimulate Competitive Research (EPSCoR).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.