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

双功能金属/沸石催化剂上通过与 NH3 脱氢 C-N 偶联进行轻质烷烃升级

• 批准号: 2247058
• 负责人: Yizhi Xiang
• 金额: $ 29.81万
• 依托单位: Mississippi State University
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2023
• 资助国家: 美国
• 起止时间: 2023-07-15 至 2026-06-30
• 项目状态: 未结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=2247058&HistoricalAwards=false
• 关键词: Light; Alkane; Upgrading; Through; Dehydrogenative

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.

该项目介绍了一种新的工艺和催化剂设计，用于商品化学乙腈的过滤率。乙烷（天然气的低价和催化折射成分）在双功能金属/沸石催化剂上与氨反应，以在有可能在现有技术方面提供环境和经济利益的过程中产生乙腈。该项目着重于催化剂设计的基本方面以及提高催化剂性能和耐用性的反应机制。除了技术方面，该项目还采用了针对茎学科中潜在少数群体的教育和宣传活动。这项研究将为双功能金属/Zeolite催化剂而直接脱氢C-c-c-c-n偶联的基础研究奠定基础。该项目在催化剂设计中调查了钴（CO）和铂（PT）金属位点对沸石的Brønsted/Lewis酸度的影响，该催化剂设计将优化金属/酸性位点双桥接性。此外，通过操作数间漂移MS和弛豫类型的瞬态实验的组合，该项目将确定表面反应中间体与串联双功能金属/沸石催化剂的动力学和反应的机制相关。从项目中获得的基本知识可能是有效的肢解催化剂设计的基础。在该项目的支持下，PI将通过招募和保留承诺的化学工程专业的学生，​​尤其是来自代表性不足的团体来帮助解决密西西比州STEM人才丧失的问题。调查人员将与密西西比州立大学的各种外展计划紧密合作。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催化计划共同资助和启发竞争性研究的既定计划（EPSCOR）。该奖项反映了NSF的法定任务，并使用基金会的知识分子优点和更广泛的影响审查标准，认为通过评估被认为是宝贵的支持。