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Updated: Jun 12, 2025

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周期性趋势和流动性对过渡金属催化硫化作用的影响

Diego Garay-Ruiz¹, Cristiano Zonta^2,3, Silvia Lovat²

¹Institute of Chemical Research of Catalonia (ICIQ), Barcelona Institute of Science & Technology (BIST), Av. Països Catalans, 16, 43007 Tarragona, Spain.

|September 23, 2024

概括

这项研究探讨了d0金属复合物在硫化物氧化中的过氧化物激活. 研究人员阐明了反应机制,揭示了催化剂的周期趋势和独特途径.

科学领域:

有机金属化学有机金属化学
催化剂是一种催化剂.
氧化反应氧化反应

背景情况:

d0金属复合物对过氧化物激活和氧气转移有兴趣.
这些催化过程的微观机械细节仍然不完全理解.

研究的目的:

为了研究硫化物氧化,使用基氧化物与一系列的八个d0金属aminotriphenolate复合物.
为了阐明反应机制,反应性,选择性以及易斯基础对这些催化系统的影响.
为了将实验动力学数据与理论预测和电子属性相关联.

主要方法:

通过Ti (IV),Zr (IV),Hf (IV),V (V),Nb (V),Ta (V),Mo (VI) 和W (VI) 的氨基三酸复合物催化硫化氧化的实验动力学研究.
研究二甲基基-N-氧化物作为易斯基的作用.
反应性与桑德森电子负性值的相关性.
密度函数理论 (DFT) 计算以建模催化循环和过氧物种.

主要成果:

在d0金属复合体系列中观察到反应性和选择性趋势.
测量了易斯基对催化性能的影响.
动力数据与桑德森电子负性相关,表明电子对反应性的影响.
DFT计算提供了有关氧中间体的机制的详细见解.

结论:

由八种不同的d0金属氨基烯酸盐催化硫化物氧化的拟议机械路径.
基于金属身份的反应性和选择性的合理化周期性趋势.
突出了灵活的复合物的独特催化行为.

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相关概念视频

Properties of Transition Metals

Properties of Transition Metals

Transition metals are defined as those elements that have partially filled d orbitals. As shown in Figure 1, the d-block elements in groups 3–12 are transition elements. The f-block elements, also called inner transition metals (the lanthanides and actinides), also meet this criterion because the d orbital is partially occupied before the f orbitals.

Oxidation-Reduction Reactions

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Oxidation–Reduction Reactions

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Sulfides are the sulfur analog of ethers, just as thiols are the sulfur analog of alcohol. Like ethers, sulfides also consist of two hydrocarbon groups bonded to the central sulfur atom. Depending upon the type of groups present, sulfides can be symmetrical or asymmetrical. Symmetrical sulfides can be prepared via an SN2 reaction between 2 equivalents of an alkyl halide and one equivalent of sodium sulfide.

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Alkenes can be dihydroxylated using potassium permanganate. The method encompasses the reaction of an alkene with a cold, dilute solution of potassium permanganate under basic conditions to form a cis-diol along with a brown precipitate of manganese dioxide.

Properties of Organometallic Compounds

Properties of Organometallic Compounds

Organometallic compounds are compounds that contain a carbon–metal bond. Carbon belongs to an organyl group like alkyl, aryl, allyl, or benzyl groups. The metal can be from Group I or Group II of the periodic table, a transition metal, or a semimetal.

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