Research Initiation Award: A Computational Study of Hydroformylation of Ethylene Over Heterogeneous Bimetallic Catalysts

研究启动奖：多相双金属催化剂上乙烯加氢甲酰化的计算研究

• 批准号: 2055012
• 负责人: Shyam Kattel
• 金额: $ 29.85万
• 依托单位: Florida Agricultural and Mechanical University
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2021
• 资助国家: 美国
• 起止时间: 2021-06-01 至 2025-05-31
• 项目状态: 未结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=2055012&HistoricalAwards=false
• 关键词: Research; Initiation; Award; Computational; Study

Research Initiation Awards provide support for junior and mid-career faculty at Historically Black Colleges and Universities who are building new research programs or redirecting and rebuilding existing research programs. It is expected that the award helps to further the faculty member's research capability and effectiveness, improve research and teaching at the home institution, and involves undergraduate students in research experiences. The award to Florida Agricultural and Mechanical University has potential to increase the understanding of hydroformylation which is an industrial process to produce aldehydes. The project will create undergraduate and graduate courses in materials modeling, provide research training in computational materials science and catalysis and create internal and external collaborations with local community colleges and high schools. Hydroformylation is a process to produce aldehydes by the reaction of synthesis gas with alkenes. Currently, hydroformylation is carried out using Rh and or Co-based transition metal complexes as a catalyst. The homogeneous nature of this reaction leads to difficulties in catalyst separation and recovery, active metal losses, metal species contamination, and corrosivity of catalytic solutions. The development of heterogeneous catalytic systems without sacrificing the activity and selectivity will avoid the drawbacks associated with homogeneous catalysts and be highly useful. This project employs computational methods such as first-principles density functional theory (DFT) calculations and kinetic Monte Carlo (KMC) simulations to gain a fundamental understanding of catalytic science of ethylene hydroformylation to C3-oxygenates on heterogeneous Rh and Rh-based bimetallic model catalysts. The DFT calculations will provide the energetics of the reaction network and KMC simulations will be employed to obtain the kinetics of the reaction at experimental reaction conditions. The theoretical calculations will provide atomistic insight into ethylene hydroformylation and help identify simple catalytic descriptors that can be used to screen potential bimetallic catalysts that are active and selective for ethylene conversion to C3-oxygenates. Moreover, the knowledge gained from this study will also shed light on the hydroformylation of other higher alkenes.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.

研究启动奖为历史悠久的黑人学院和大学的初级和中级教师提供了支持，他们正在构建新的研究计划，或重新指导和重建现有的研究计划。可以预期，该奖项有助于进一步进一步发展教职员工的研究能力和有效性，改善家庭机构的研究和教学，并让本科生参与研究经验。佛罗里达农业和机械大学的奖项有可能增加对氢甲基化的理解，这是产生醛的工业过程。该项目将在材料建模中创建本科和研究生课程，提供计算材料科学和催化的研究培训，并与当地社区大学和高中建立内部和外部合作。氢甲基化是通过合成气与烷烃的反应产生醛的过程。当前，使用RH和或基于CO的过渡金属复合物作为催化剂进行水甲基化。该反应的同质性质导致催化剂分离和恢复，活动金属损失，金属物种污染以及催化溶液的腐蚀性困难。在不牺牲活性和选择性的情况下的异质催化系统的发展将避免与均质催化剂相关的缺点，并且非常有用。该项目采用计算方法，例如第一原理密度功能理论（DFT）计算和动力学蒙特卡洛（KMC）模拟，以获得对C3-氧气对乙烯加氢甲氧基化催化科学的基本了解，从。 DFT计算将提供反应网络的能量，并将使用KMC模拟在实验反应条件下获得反应的动力学。理论计算将提供对乙烯氢甲基化的原子见解，并有助于识别简单的催化描述子，这些描述符可用于筛选活性和选择性的乙烯转化为C3-氧化物的潜在双金属催化剂。此外，这项研究所获得的知识还将阐明其他高级烷烃的氢甲基化。该奖项反映了NSF的法定任务，并且使用基金会的智力优点和更广泛的影响评估标准，认为值得通过评估来获得支持。

项目成果

A Density Functional Theory Study of Electrochemical Nitrogen Reduction to Ammonia on the (100) Surface of Transition-Metal Oxynitrides

• DOI: 10.1021/acs.jpcc.2c04119
• 发表时间: 2022-09
• 期刊: The Journal of Physical Chemistry C
• 作者: Damilola Ologunagba;Shyam Kattel

Density functional theory study of bulk properties of transition metal nitrides

过渡金属氮化物体性能的密度泛函理论研究

• DOI: 10.1039/d2cp06082e
• 发表时间: 2023
• 期刊: Physical Chemistry Chemical Physics
• 影响因子: 3.3
• 作者: Lynn, Michael O.;Ologunagba, Damilola;Dangi, Beni B.;Kattel, Shyam
• 通讯作者: Kattel, Shyam

Enhancing glycerol electrooxidation from synergistic interactions of platinum and transition metal carbides

• DOI: 10.1016/j.apcatb.2022.121648
• 发表时间: 2022-11-05
• 期刊: APPLIED CATALYSIS B-ENVIRONMENTAL
• 影响因子: 22.1
• 作者: Mou, Hansen;Chang, Qiaowan;Chen, Jingguang G.
• 通讯作者: Chen, Jingguang G.