What Limits Turnover Number in NH3 Synthesis on a PNP Pincer Molecule?

Feibelman Peter J.

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What Limits Turnover Number in NH3 Synthesis on a PNP Pincer Molecule?

机译：什么限制PNP钳分子上NH3合成中的周转数？

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Abiological NH3 synthesis under mild conditions on a PNP [=2,6-bis(di-tert-butyl-phosphinomethyl)pyridine] pincer chelating an Mo(N-2)(3) group has been reported and attributed to a catalytic cycle wherein only the equatorial N-2 is reduced. The present calculations suggest that reduction of axial N-2 ligands was the reason the cycle ended after production of 23 equiv. of NH3. NH3 detachment from axial NNH3 initiates a terminal reaction pathway by leaving an axial nitrido N behind on the Mo. The transinfluence of the strong axial nitride bond causes the second axial N-2 to detach from the Mo, with N-Mo-N-2 remaining as a non-catalytic, pincer-chelated group.

机译：已报道在温和条件下在PNP [= 2,6-双（二叔丁基-膦基甲基）吡啶]螯合Mo（N-2）（3）上的生物NH3合成，这归因于催化循环，其中只有赤道N-2减少了。目前的计算表明，轴向N-2配体的减少是产生23当量后循环终止的原因。 NH3。 NH3从轴向NNH3的脱离通过在Mo上留下轴向氮基氮N来启动末端反应途径。强轴向氮化物键的反式作用导致第二轴向N-2从Mo脱离，N-Mo-N-2保留为非催化，钳制螯合基团。

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《Comments on Inorganic Chemistry: A Journal of Critical Discussion of the Current Literature》 |2014年第2期|共14页
作者
Feibelman Peter J.;
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正文语种 eng
中图分类无机化学;有机化学;
关键词
ammonia; mild; pincer; synthesis; turnover;

机译：氨;温和;钳子;合成;周转;

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1. What Limits Turnover Number in NH3 Synthesis on a PNP Pincer Molecule? [J] . Feibelman Peter J. Comments on Inorganic Chemistry: A Journal of Critical Discussion of the Current Literature . 2014,第1a2期

机译：什么限制PNP钳分子上NH3合成中的周转数？
2. Catalytic Mechanisms of Direct Pyrrole Synthesis via Dehydrogenative Coupling Mediated by PNP-lr or PNN-Ru Pincer Complexes: Crucial Role of Proton-Transfer Shuttles in the PNP-lr System [J] . Shuanglin Qu, Yanfeng Dang, Chunyu Song, Journal of the American Chemical Society . 2014,第13期

机译：通过PNP-lr或PNN-Ru夹杂物介导的脱氢偶联直接合成吡咯的催化机理：质子转移穿梭在PNP-lr系统中的关键作用
3. Synthesis, X-ray crystal structure and thermal decomposition of two peroxovanadium complexes with coordinated ammonia molecules: [{VO(O-2)2(NH3)}(2){[mu-Cu(NH3)(4)}] and [Zn(NH3)(4)][VO(O-2)(2)(NH3)](2) [J] . Chrappova J, Schwendt P, Dudasova D, Polyhedron: The International Journal for Inorganic and Organometallic Chemistry . 2008,第2期

机译：两种具有配位氨分子的过氧钒钛配合物的合成，X射线晶体结构和热分解：[{VO（O-2）2（NH3）}（2）{[mu-Cu（NH3）（4）}]和[ Zn（NH3）（4）] [VO（O-2）（2）（NH3）]（2）
4. Catalytic Nitrogen Fixation Using Rhenium-Dinitrogen ComplexBearing PNP Pincer Ligands [C] . Fanqiang Meng, Shogo Kuriyama, Kazunari Nakajima 日本化学会春季年会 . 2020

机译：催化氮固定采用铼 - 二硝基复合PNP钳子配体
5. Studies of PNP and PCP pincer complexes: Synthesis and carbon-hydrogen activation potential of PNP pincer complexes and a PCP pincer complex applied to alkene hydrogenation [D] . Pelczar, Elizabeth Marie 2008

机译：PNP和PCP钳形复合物的研究：PNP钳形复合物和PCP钳形复合物的合成及其碳氢活化潜力，用于烯烃加氢
6. Synthesis and Structural Dynamics of Five-CoordinateRh(III) and Ir(III) PNP and PONOP Pincer Complexes [O] . Thomas M. Hood, Baptiste Leforestier, Matthew R. Gyton, -1

机译：五坐标的合成及其结构动力学Rh（III）和Ir（III）PNP和PONOP钳形配合物
7. Synthesis and reactivity of iridium complexes of a macrocyclic PNP pincer ligand [O] . Thomas M. Hood, Adrian B. Chaplin 2021

机译：大环PNP钳子配体铱络合物的合成与反应性

What Limits Turnover Number in NH3 Synthesis on a PNP Pincer Molecule?

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