SusChEM: Theoretical Studies of Inorganic, Organometallic, and Bioinorganic Systems

SusChEM:无机、有机金属和生物无机系统的理论研究

基本信息

  • 批准号:
    1664866
  • 负责人:
  • 金额:
    $ 48万
  • 依托单位:
  • 依托单位国家:
    美国
  • 项目类别:
    Continuing Grant
  • 财政年份:
    2017
  • 资助国家:
    美国
  • 起止时间:
    2017-05-01 至 2021-04-30
  • 项目状态:
    已结题

项目摘要

In this project funded by the Chemical Structure, Dynamics, and Mechanisms B Program of the Division of Chemistry, Professor Michael B. Hall at Texas A&M University, College Station, investigates important problems in catalytic chemistry by using modern computational techniques. The project studies the naturally occurring hydrogenase enzymes and related model complexes, as these systems hold promise for low-cost replacements for expensive platinum electrodes that are now used for the development of hydrogen as an energy resource. Additional studies are on the activation and formation of chemical bonds by reactions with inexpensive metal catalysts rather than precious metals, developments that are important for the chemical industry. In addition to the education of students and postdoctoral associates at Texas A&M University, a number of experimental collaborators bring the educational aspects to a broader audience. The Laboratory for Molecular Simulation, directed by Professor Hall, provides researchers across campus with access to the latest atomistic modeling software and hardware. The Laboratory also supports the free world-wide distribution of the Fenske-Hall method. This method, with its simple graphical user interface and ability to run large transition metal calculations on a laptop, allows it to be easily used by a wide audience and to be incorporated into teaching courses. Full-gradient geometry optimizations with non-local density-functional theory (DFT) and ab initio energy calculations, primarily coupled cluster, complete active space and multireference configuration interaction, are being used to solve problems of current interest in inorganic, organometallic, and bioinorganic chemistry. Specific systems include: (1) non-innocent thiolate ligands in alkene and hydrogen activation, where the metal-sulfur pi bonding is sufficiently weak, such that the substantial multireference character cannot be handled by DFT; (2) cobalt catalyzed borylation reactions (in collaboration with Paul Chirik), where development of abundant first-transition-row metals as catalysts are needed, but where the mechanism appears to be different from those for second-transition-row metals; (3) unexpected non-innocent behavior in nickel phosphine complexes (in collaboration with Morris Bullock), where the ligands that are well known to assist in providing protons for proton reduction become active in other transformations; (4) regioselective functionalization of unactivated sp3 carbon-hydrogen bonds; (5) fluoroalkane metathesis (in collaboration with Tom Baker), where the formation and stability of the metallocycle competes with its further transformation to the final metathesis products; (6) Nickel iron hydrogenase studies to include more of the protein backbone, where there are still several competing mechanisms in the literature, but where there is insufficient calibration of the functionals; (7) modeling new nickel iron hydrogenases and their mutants (in collaboration with David Barondeau), where changes in the residues near the bridging carbonyl site change the reactivity; and (8) hydrogenase synthetic models (in collaboration with Marcetta Darensbourg), where exploration of new ligands opens up unexpected new mechanisms.
在这个由化学系化学结构、动力学和机理B计划资助的项目中,德克萨斯农工大学的迈克尔·B·霍尔教授利用现代计算技术研究了催化化学中的重要问题。该项目研究自然产生的氢酶和相关的模型复合体,因为这些系统有望以低成本取代昂贵的铂电极,而铂电极现在用于开发氢作为一种能源。更多的研究是关于通过与廉价的金属催化剂而不是贵金属反应来激活和形成化学键,这一发展对化学工业很重要。除了为德克萨斯农工大学的学生和博士后提供教育外,许多实验合作者还将教育方面带给了更广泛的受众。由霍尔教授领导的分子模拟实验室为校园内的研究人员提供了访问最新的原子模拟软件和硬件的途径。该实验室还支持在世界范围内免费分发芬斯克-霍尔法。这种方法具有简单的图形用户界面和在笔记本电脑上运行大型过渡金属计算的能力,使其易于被广泛的受众使用,并被纳入教学课程。采用非局域密度泛函理论(DFT)和从头算能量计算的全梯度几何构型优化,主要是团簇耦合、完全活性空间和多参考构型相互作用,正被用来解决目前无机、有机金属和生物无机化学中感兴趣的问题。具体的体系包括:(1)烯烃中的非无辜硫代配体和氢活化,其中金属-硫pi键足够弱,使得DFT无法处理实质性的多重引用特征;(2)钴催化的硼化反应(与Paul Chirik合作),其中需要开发丰富的第一过渡排金属作为催化剂,但其机理似乎不同于第二过渡排金属的反应;(3)镍膦络合物中出人意料的非无辜行为(与Morris Bullock合作),其中众所周知有助于提供质子还原质子的配体在其他转化中变得活跃;(4)未活化的SP3碳氢键的区域选择性官能化;(5)氟烷烃歧化反应(与Tom Baker合作),其中金属环的形成和稳定性与其进一步转化为最终复分解产物竞争;(6)镍铁氢酶研究以包括更多的蛋白质主链,在文献中仍有几种竞争机制,但没有对官能团进行充分的校准;(7)模拟新的镍铁氢酶及其突变体(与David Barondeau合作),其中桥式羰基附近残基的变化改变反应活性;以及(8)氢酶合成模型(与Marcetta Darensburg合作),其中新配体的探索打开了意想不到的新机制。

项目成果

期刊论文数量(25)
专著数量(0)
科研奖励数量(0)
会议论文数量(0)
专利数量(0)
Computational Investigations of Enantioselection in Carbon–Carbon Bond Forming Reactions of Ruthenium Guanidinobenzimidazole Second Coordination Sphere Hydrogen Bond Donor Catalysts
钌胍基苯并咪唑第二配位球氢键供体催化剂碳-碳键形成反应中对映选择的计算研究
  • DOI:
    10.1021/acs.organomet.0c00072
  • 发表时间:
    2020
  • 期刊:
  • 影响因子:
    2.8
  • 作者:
    Wititsuwannakul, Taveechai;Mukherjee, Tathagata;Hall, Michael B.;Gladysz, John A.
  • 通讯作者:
    Gladysz, John A.
Theoretical Analysis of Competing Pathways for Carbon–Hydrogen Activation of Cyclopentadienyl–Triphenylphosphine–Iridium in Benzene
苯中环戊二烯基-三苯基膦-铱碳-氢活化竞争途径的理论分析
  • DOI:
    10.1021/acs.inorgchem.9b02580
  • 发表时间:
    2019
  • 期刊:
  • 影响因子:
    4.6
  • 作者:
    Yang, Xin;Hall, Michael B.
  • 通讯作者:
    Hall, Michael B.
Controlling O 2 Reactivity in Synthetic Analogues of [NiFeS]- and [NiFeSe]-Hydrogenase Active Sites
控制[NiFeS]-和[NiFeSe]-氢化酶活性位点的合成类似物中的O 2 反应性
  • DOI:
    10.1021/jacs.9b07448
  • 发表时间:
    2019
  • 期刊:
  • 影响因子:
    15
  • 作者:
    Yang, Xuemei;Elrod, Lindy C.;Le, Trung;Vega, Valeria S.;Naumann, Haley;Rezenom, Yohannes;Reibenspies, Joseph H.;Hall, Michael B.;Darensbourg, Marcetta Y.
  • 通讯作者:
    Darensbourg, Marcetta Y.
Platinum complexes containing or derived from olefinic phosphines P(X)((CH2)6CH CH2)2 (X = OH, Ph, (CH2)6CH CH2); ring closing metatheses, structures, and trans/cis isomerizations
含有或衍生自烯属膦 P(X)((CH2)6CH CH2)2 (X–=–OH, Ph, (CH2)6CH CH2) 的铂络合物;
  • DOI:
    10.1016/j.poly.2018.09.025
  • 发表时间:
    2019
  • 期刊:
  • 影响因子:
    2.6
  • 作者:
    Stollenz, Michael;Joshi, Hemant;Ehnbom, Andreas;Fiedler, Tobias;Kharel, Sugam;Reibenspies, Joseph H.;Bhuvanesh, Nattamai;Hall, Michael B.;Gladysz, John A.
  • 通讯作者:
    Gladysz, John A.
Controlling P–C/C–H Bond Cleavage in Nickel Bis(diphosphine) Complexes: Reactivity Scope, Mechanism, and Computations
控制镍双(二膦)络合物中的 P-C/C-H 键断裂:反应范围、机制和计算
  • DOI:
    10.1021/acs.organomet.0c00388
  • 发表时间:
    2020
  • 期刊:
  • 影响因子:
    2.8
  • 作者:
    Zhang, Shaoguang;Li, Haixia;Appel, Aaron M.;Hall, Michael B.;Bullock, R. Morris
  • 通讯作者:
    Bullock, R. Morris
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Michael Hall其他文献

A Pilot Randomized Controlled Trial of Augmented Reality Just-in-Time Guidance for the Performance of Rugged Field Procedures.
增强现实实时指导的随机对照试验,用于执行严格的现场程序。
  • DOI:
    10.1017/s1049023x24000372
  • 发表时间:
    2024
  • 期刊:
  • 影响因子:
    2.2
  • 作者:
    Laurel O'Connor;Sepahrad Zamani;Xinyi Ding;N. McGeorge;Susan Latiff;Cindy Liu;Jorge Acevedo Herman;Matthew Loconte;A. Milsten;Michael Weiner;Timothy Boardman;Martin Reznek;Michael Hall;J. Broach
  • 通讯作者:
    J. Broach
Improving pain management through better documentation
通过更好的文档改善疼痛管理
Novel Bio-Logging Tool for Studying Fine-Scale Behaviors of Marine Turtles in Response to Sound
用于研究海龟对声音响应的精细行为的新型生物测井工具
  • DOI:
  • 发表时间:
    2017
  • 期刊:
  • 影响因子:
    3.7
  • 作者:
    R. B. Tyson;W. Piniak;C. Domit;D. Mann;Michael Hall;D. Nowacek;M. Fuentes
  • 通讯作者:
    M. Fuentes
The Routledge handbook of tourism and sustainability
劳特利奇旅游与可持续发展手册
  • DOI:
    10.4324/9780203072332
  • 发表时间:
    2015
  • 期刊:
  • 影响因子:
    0
  • 作者:
    Michael Hall;S. Gössling;Daniel Scott;M. Rutty
  • 通讯作者:
    M. Rutty
No time for smokescreen skepticism: A rejoinder to Shani and Arad
没有时间进行烟幕怀疑:对沙尼和阿拉德的反驳
  • DOI:
  • 发表时间:
    2015
  • 期刊:
  • 影响因子:
    0
  • 作者:
    Michael Hall;B. Amelung;S. Cohen;E. Eijgelaar;S. Gössling;J. Higham;R. Leemans;P. Peeters;Yael Ram;D. Scott;C. Aall;B. Abegg;J. Araña;S. Barr;S. Becken;R. Buckley;P. Burns;T. Coles;J. Dawson;Rouven Doran;G. Dubois;D. Duval;D. Fennell;A. Gill;Martin Gren;W. Gronau;J. Guiver;D. Hopkins;E. Huijbens;K. Koens;M. Lamers;C. Lemieux;A. Lew;Patrick T. Long;F. Melissen;J. Nawijn;S. Nicholls;J. Nilsson;R. Nunkoo;Alan Pomering;A. Reis;D. Reiser;R. Richardson;C. Rogerson;J. Saarinen;Anna Dóra Sæþórsdóttir;R. Steiger;P. Upham;S. Linden;G. Visser;G. Wall;D. Weaver
  • 通讯作者:
    D. Weaver

Michael Hall的其他文献

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{{ truncateString('Michael Hall', 18)}}的其他基金

Theoretical Studies of Inorganic, Organometallic, and Bioinorganic Systems
无机、有机金属和生物无机系统的理论研究
  • 批准号:
    1300787
  • 财政年份:
    2013
  • 资助金额:
    $ 48万
  • 项目类别:
    Standard Grant
Pushing Back the Limits of Optical Microscopy - Enhancing dSTORM Resolution through Controlled Fluorophore Switching
突破光学显微镜的极限 - 通过受控荧光团切换提高 dSTORM 分辨率
  • 批准号:
    BB/K013971/1
  • 财政年份:
    2013
  • 资助金额:
    $ 48万
  • 项目类别:
    Research Grant
Diels-Alder/Ene Reactions for the Multi-Component Synthesis of Natural Product Inspired Bioactive Chemical Libraries
用于天然产物启发的生物活性化学库的多组分合成的 Diels-Alder/Ene 反应
  • 批准号:
    EP/I033959/1
  • 财政年份:
    2011
  • 资助金额:
    $ 48万
  • 项目类别:
    Research Grant
Theoretical Studies of Inorganic, Organometallic, and Bioinorganic Systems
无机、有机金属和生物无机系统的理论研究
  • 批准号:
    0910552
  • 财政年份:
    2009
  • 资助金额:
    $ 48万
  • 项目类别:
    Continuing Grant
Theoretical Studies of Inorganic, Organometallic, and Bioinorganic Systems
无机、有机金属和生物无机系统的理论研究
  • 批准号:
    0518074
  • 财政年份:
    2005
  • 资助金额:
    $ 48万
  • 项目类别:
    Continuing Grant
Support for Argos Data Collection and Location System
支持Argos数据采集和定位系统
  • 批准号:
    8341973
  • 财政年份:
    2000
  • 资助金额:
    $ 48万
  • 项目类别:
    Interagency Agreement
Theoretical Studies of Inorganic and Organometallic Systems
无机和有机金属体系的理论研究
  • 批准号:
    9800184
  • 财政年份:
    1998
  • 资助金额:
    $ 48万
  • 项目类别:
    Continuing Grant
Theoretical Studies of Inorganic and Organometallic Systems
无机和有机金属体系的理论研究
  • 批准号:
    9423271
  • 财政年份:
    1995
  • 资助金额:
    $ 48万
  • 项目类别:
    Continuing Grant
Workshop on ENSO and Seasonal to Interannual Climate Variability: Socio-Economic Impacts, Forecasting, and Applications to the Decision-Making Process
ENSO 和季节到年际气候变率研讨会:社会经济影响、预测和决策过程的应用
  • 批准号:
    9223264
  • 财政年份:
    1992
  • 资助金额:
    $ 48万
  • 项目类别:
    Interagency Agreement
Theoretical Studies of Inorganic and Organometallic Systems
无机和有机金属体系的理论研究
  • 批准号:
    9113634
  • 财政年份:
    1991
  • 资助金额:
    $ 48万
  • 项目类别:
    Continuing Grant

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  • 批准号:
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  • 批准号:
    23H00849
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