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.

研究启动奖为历史上黑人学院和大学的初级和中级职业教师提供支持，他们正在建立新的研究项目或重新定向和重建现有的研究项目。预计该奖项将有助于进一步提高教师的研究能力和效率，改善家庭机构的研究和教学，并使本科生参与研究经验。授予佛罗里达农业和机械大学的奖项有可能增加对加氢裂化的理解，加氢裂化是一种生产醛的工业过程。该项目将创建材料建模的本科生和研究生课程，提供计算材料科学和催化方面的研究培训，并与当地社区学院和高中建立内部和外部合作。加氢裂化是通过合成气与烯烃反应生产醛的方法。目前，加氢裂化使用Rh和/或Co基过渡金属络合物作为催化剂进行。该反应的均相性质导致催化剂分离和回收困难、活性金属损失、金属物质污染和催化溶液的腐蚀性。在不牺牲活性和选择性的情况下开发多相催化体系将避免与均相催化剂相关的缺点，并且是非常有用的。本项目采用第一性原理密度泛函理论（DFT）计算和动力学蒙特卡罗（KMC）模拟等计算方法，对乙烯加氢合成C3-含氧化合物在非均相Rh和Rh基催化剂上的催化科学进行了基本了解。DFT计算将提供反应网络的能量，KMC模拟将用于获得实验反应条件下的反应动力学。理论计算将提供对乙烯加氢裂化的原子洞察力，并帮助识别可用于筛选对乙烯转化为C3-含氧化合物具有活性和选择性的潜在加氢裂化催化剂的简单催化描述符。此外，从这项研究中获得的知识也将揭示其他高级烯烃的加氢精制。该奖项反映了NSF的法定使命，并被认为值得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。

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.