SusChEM: Metal Complexes Containing New Tin Ligands for Applications in Homogeneous Catalysis
SusChEM:含有新型锡配体的金属配合物在均相催化中的应用
基本信息
- 批准号:1300206
- 负责人:
- 金额:$ 39万
- 依托单位:
- 依托单位国家:美国
- 项目类别:Standard Grant
- 财政年份:2013
- 资助国家:美国
- 起止时间:2013-04-01 至 2017-03-31
- 项目状态:已结题
- 来源:
- 关键词:
项目摘要
With this award from the Chemical Synthesis (SYN) Program of the Chemistry Division, Professor Burjor Captain of the Department of Chemistry at the University of Miami will explore the structures and reactivity of transition metal complexes containing bulky tin ligands. The main drive is to indice activation of hydrogen and small molecules as well as to investigate their potential as hydroformylation and hydrogenation catalysts. The work will consist of incorporating sterically encumbered tin ligands to bring about electronic and/or coordinative unsaturation around the metal atoms in transition metal complexes. This work will begin by exploring synthetic, structural, and catalytic chemistry on platinum-tin systems and then be extended to include complexes of non-precious transition metals such as Ni and Fe. The central theme is the use of tin which offers significant advantages and is largely untested. There is precedent for the potential scope and effectiveness of this strategy in the widely investigated use of phosphine ligands to modify both binding sites and catalytic properties. However, bulky tin ligands offer additional incentives for their investigation compared to phosphine ligands. Because the stannyl group is a radical with an odd number of electrons, its utilization at a metal site changes formal oxidation numbers, but more importantly electron densities at the metal center, in ways quite different from that of coordinated phosphines. The long range goal of this work is development of robust, economic, and efficient catalysts of use to chemical industry.The broader impact of this project is that it calls for synthesis of a new class of materials in a relatively unexplored area of inorganic chemistry. This provides the opportunity to discover new binding patterns of small molecules. Some of these may be predictable, but some may be unanticipated and lead to new insights of broad impact in fundamental chemical science. There has been a renaissance in main group chemistry, and this work combines main group with transition metal chemistry in an exciting and potentially breakthrough area. The proposed small molecule activation studies center on hydrogen- by trying to understand how it behaves in a main group metal-transition group metal setting. Transition metal complexes have and always will play the crucial part in the chemistry of hydrogen, but this may be modified by the presence of the added bulky tin ligand. The question is how and to what extent it will be modified. The long term impact of this work will be in helping to better utilize this important resource in binding and catalytic reactivity. A final area of impact is in student training (undergraduate and graduate) to be scientists and professionals. Students will be trained to prepare and handle air-sensitive compounds, and will learn various methods such as X-Ray crystallography, Fourier transform infrared spectroscopy, nuclear magnetic resonance spectroscopy, mass spectrometry, calorimetry and computational analysis. The results will be broadly disseminated in refereed research journals and through presentations at meetings. Due to the diversity of the proposed research, students trained in this program will have the skill set and creative attitude needed to find viable solutions for the emerging energy crisis and contribute to sustainability.
凭借化学部化学合成(SYN)计划的这一奖项,迈阿密大学化学系的Burjor Captain教授将探索含有庞大锡配体的过渡金属络合物的结构和反应性。主要的驱动力是指示氢和小分子的活化以及研究它们作为加氢和加氢催化剂的潜力。 这项工作将包括纳入空间位阻的锡配体带来的电子和/或协调周围的金属原子在过渡金属配合物的不饱和度。这项工作将开始探索合成,结构和催化化学铂锡系统,然后扩展到包括非贵过渡金属,如镍和铁的配合物。中心主题是使用锡,它提供了显着的优势,并在很大程度上未经测试。在广泛研究使用膦配体来修饰结合位点和催化性能方面,这种策略的潜在范围和有效性有先例可循。然而,与膦配体相比,庞大的锡配体为它们的研究提供了额外的激励。由于锡烷基是一个具有奇数电子的基团,它在金属位点的利用改变了形式氧化数,但更重要的是改变了金属中心的电子密度,其方式与配位膦完全不同。这项工作的长期目标是开发用于化学工业的稳定、经济和有效的催化剂。该项目的更广泛影响是,它呼吁在相对未开发的无机化学领域合成一类新材料。这为发现小分子的新结合模式提供了机会。其中一些可能是可预测的,但有些可能是不可预见的,并导致在基础化学科学的广泛影响的新见解。主族化学的复兴,使主族化学与过渡金属化学在一个令人兴奋和潜在的突破性领域相结合。 所提出的小分子活化研究以氢为中心-通过试图了解它在主族金属-过渡族金属环境中的行为。过渡金属配合物在氢的化学中一直起着关键作用,但这可能会被添加的庞大锡配体的存在所改变。问题是如何以及在多大程度上进行修改。 这项工作的长期影响将有助于更好地利用这一重要资源的结合和催化反应。影响的最后一个领域是在学生培训(本科生和研究生)成为科学家和专业人士。学生将接受培训,以准备和处理空气敏感的化合物,并将学习各种方法,如X射线晶体学,傅里叶变换红外光谱,核磁共振光谱,质谱,量热法和计算分析。研究结果将在经过评审的研究期刊上广泛传播,并通过在会议上的介绍予以传播。 由于拟议的研究的多样性,在这个程序中培训的学生将有技能和创造性的态度需要找到可行的解决方案,为新兴的能源危机,并有助于可持续发展。
项目成果
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Burjor Captain其他文献
Intermediates and catalytic hydrostannylation. Characterization of a rare complex Pt(IPr)[<em>η</em><sup>2</sup>-<em>E</em>-(SnBu<sup>t</sup><sub>3</sub>)(H)C<img class="glyph" src="https://sdfestaticassets-eu-west-1.sciencedirectassets.com/shared-assets/16/entities/dbnd" />C(SiMe<sub>3</sub>)(H)]
- DOI:
10.1016/j.jorganchem.2017.03.024 - 发表时间:
2017-11-01 - 期刊:
- 影响因子:
- 作者:
Anjaneyulu Koppaka;Mohan M. Gamage;Burjor Captain - 通讯作者:
Burjor Captain
Build-up of a Ru<sub>6</sub> octahedral cluster core stabilized by <em>tert</em>-butyl germyl ligands
- DOI:
10.1016/j.jorganchem.2013.06.008 - 发表时间:
2014-02-01 - 期刊:
- 影响因子:
- 作者:
Sumit Saha;Derek Isrow;Burjor Captain - 通讯作者:
Burjor Captain
Activation of small molecules by the unsaturated complex Pt(IBu<sup>t</sup>)(PBu<sup>t</sup><sub>3</sub>): First structural characterization of a peroxycarbonate complex of platinum
- DOI:
10.1016/j.jorganchem.2021.121900 - 发表时间:
2021-08-01 - 期刊:
- 影响因子:
- 作者:
Mohan M. Gamage;Mark D. Smith;Burjor Captain - 通讯作者:
Burjor Captain
Synthesis, structure, and thermochemistry of adduct formation between N-heterocyclic carbenes and isocyanates or mesitylnitrile oxide
- DOI:
10.1007/s11224-013-0305-2 - 发表时间:
2013-07-16 - 期刊:
- 影响因子:2.200
- 作者:
Manuel Temprado;Subhojit Majumdar;Xiaochen Cai;Burjor Captain;Carl D. Hoff - 通讯作者:
Carl D. Hoff
Photochemical synthesis and radical generation of the nickel-tin dimer [Ni(SnBu<sup>t</sup><sub>3</sub>)(CNBu<sup>t</sup>)<sub>2</sub>(CO)]<sub>2</sub>
- DOI:
10.1016/j.jorganchem.2021.121715 - 发表时间:
2021-03-15 - 期刊:
- 影响因子:
- 作者:
Derek Isrow;Musa Ahmadi;Stefania Impellizzeri;Burjor Captain - 通讯作者:
Burjor Captain
Burjor Captain的其他文献
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