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Dynamical Organometallic Mechanisms

动态有机金属机制

基本信息

批准号：
1952420
负责人：
Daniel Ess
金额：
$ 26.53万
依托单位：
Brigham Young University
依托单位国家：
美国
项目类别：
Standard Grant
财政年份：
2020
资助国家：
美国
起止时间：
2020-09-01 至 2023-08-31
项目状态：
已结题

来源：
https://www.nsf.gov/awardsearch/showAward?AWD_ID=1952420&HistoricalAwards=false
关键词：
Dynamical Organometallic Mechanisms

项目摘要

In this project, funded by the Chemical Structure, Dynamics, and Mechanisms B Program of the Chemistry Division, Professor Daniel Ess of the Department of Chemistry and Biochemistry at Brigham Young University is developing new experimentally testable theories about how the dynamic motion of atoms during the course of chemical reactions impacts how the reactions occur (reaction mechanisms). The goal of this research is to use the combination of a quantum mechanical treatment of the energy and forces with classical mechanical equations of motion to discover new reaction pathways and mechanisms for organometallic reactions. Quantum mechanics deals with the mathematical description of the motion and interaction of subatomic particles, incorporating the concepts of quantization of energy, wave-particle duality, and the uncertainty of how fast a tiny particle moves and how well we know its position. Classical mechanical describes the motion of macroscopic objects, from projectiles to parts of machinery, and astronomical objects, such as spacecraft, planets, stars and galaxies. This project combines the use of equations of physics, at both the atomic and macroscopic scales. The research project is a fruitful training ground to prepare undergraduate and graduate students for the scientific workforce. Undergraduate students will learn computational techniques that will be valuable in their future experimental careers. In addition to mentoring physical science students, this work provide cross disciplinary training in computer science.This work uses quasiclassical direct molecular dynamics trajectories to discover new dynamical organometallic reaction mechanisms, and examine major concepts that provide understanding and prediction of dynamical mechanisms. Many organometallic reactions involve highly reactive or weakly coordinated intermediates and their calculated energy landscapes provide an incomplete mechanistic picture. Quasiclassical direct molecular dynamics trajectories reveal new dynamical mechanisms. In this project, the focus is on direct dynamics studies of experimentally important alkane, arene, and alkene oxidative additions and reductive elimination reactions, which represent one of the largest and most important classes of organometallic reactions.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.

在本研究项目中，杨百翰大学化学与生物化学系的丹尼尔·埃斯教授（Professor B Program of the Chemistry Division），对化学反应过程中原子的动态运动如何影响反应的发生（反应机理）进行了新的实验验证理论的开发。本研究的目标是使用能量和力的量子力学处理与经典力学运动方程的结合来发现新的反应途径和有机金属反应的机制。量子力学涉及亚原子粒子运动和相互作用的数学描述，结合了能量量子化，波粒二象性和微小粒子运动速度的不确定性以及我们对它的位置的了解程度。经典力学描述了宏观物体的运动，从抛射体到机械部件，以及天文物体，如航天器，行星，恒星和星系。这个项目结合了物理方程的使用，在原子和宏观尺度。该研究项目是一个富有成效的培训基地，为本科生和研究生的科学劳动力做好准备。本科生将学习计算技术，这将是在他们未来的实验职业生涯中有价值的。除了指导物理科学的学生，这项工作提供了跨学科的培训，在计算机科学。这项工作使用准经典直接分子动力学轨迹，以发现新的动态有机金属反应机制，并检查主要概念，提供理解和预测的动力学机制。许多有机金属反应涉及高活性或弱配位的中间体，其计算的能量景观提供了一个不完整的机制图片。准经典直接分子动力学轨道揭示了新的动力学机制。在这个项目中，重点是对实验上重要的烷烃、芳烃和烯烃氧化加成和还原消除反应的直接动力学研究，这些反应代表了有机金属反应中最大和最重要的一类。这个奖项反映了NSF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。

项目成果

期刊论文数量（11）

专著数量（0）

科研奖励数量（0）

会议论文数量（0）

专利数量（0）

Catalysis with a Skip: Dynamically Coupled Addition, Proton Transfer, and Elimination during Au- and Pd-Catalyzed Diol Cyclizations

跳过催化：金和钯催化二醇环化过程中的动态耦合加成、质子转移和消除

DOI：
10.1021/acscatal.1c02408
发表时间：
2021
期刊：
ACS Catalysis
影响因子：
12.9
作者：
Teynor, Matthew S.;Scott, Windsor;Ess, Daniel H.
通讯作者：
Ess, Daniel H.

Direct Dynamics Trajectories Demonstrate Dynamic Matching and Nonstatistical Radical Pair Intermediates during Fe-Oxo-Mediated C–H Functionalization Reactions

直接动力学轨迹展示了 Fe-Oxo 介导的 C–H 功能化反应过程中的动态匹配和非统计自由基对中间体

DOI：
10.1021/jacs.3c01196
发表时间：
2023
期刊：
Journal of the American Chemical Society
影响因子：
15
作者：
Joy, Jyothish;Ess, Daniel H.
通讯作者：
Ess, Daniel H.

Exploring Cuneanes as Potential Benzene Isosteres and Energetic Materials: Scope and Mechanistic Investigations into Regioselective Rearrangements from Cubanes

探索古巴烷作为潜在苯等排体和含能材料：古巴烷区域选择性重排的范围和机制研究

DOI：
10.1021/jacs.3c03226
发表时间：
2023
期刊：
Journal of the American Chemical Society
影响因子：
15
作者：
Son, Jeong-Yu;Aikonen, Santeri;Morgan, Nathan;Harmata, Alexander S.;Sabatini, Jesse J.;Sausa, Rosario C.;Byrd, Edward F.;Ess, Daniel H.;Paton, Robert S.;Stephenson, Corey R.
通讯作者：
Stephenson, Corey R.

Mechanistic molecular motion of transition-metal mediated β-hydrogen transfer: quasiclassical trajectories reveal dynamically ballistic, dynamically unrelaxed, two step, and concerted mechanisms

过渡金属介导的β-氢转移的机械分子运动：准经典轨迹揭示动态弹道、动态非松弛、两步和协同机制