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関連する概念動画

Crystal Field Theory - Octahedral Complexes02:58

Crystal Field Theory - Octahedral Complexes

31.8K
Crystal Field Theory
To explain the observed behavior of transition metal complexes (such as colors), a model involving electrostatic interactions between the electrons from the ligands and the electrons in the unhybridized d orbitals of the central metal atom has been developed. This electrostatic model is crystal field theory (CFT). It helps to understand, interpret, and predict the colors, magnetic behavior, and some structures of coordination compounds of transition metals.
CFT focuses on...
31.8K
Ladder Diagrams: Complexation Equilibria01:07

Ladder Diagrams: Complexation Equilibria

676
Ladder diagrams are useful for evaluating equilibria involving metal-ligand complexes. The vertical scale of the ladder diagram represents the concentration of unreacted or free ligand, pL. The horizontal lines on the scale depict the log of stepwise formation constants for metal-ligand complexes and indicate the dominant species in all the regions.
The formation constant, K1, for the formation of Cd(NH3)2+ complex from cadmium and ammonia is 3.55 × 102. Log K1 (i.e. pNH3) is 2.55, and...
676
Metal-Ligand Bonds02:51

Metal-Ligand Bonds

25.6K
The hemoglobin in the blood, the chlorophyll in green plants, vitamin B-12, and the catalyst used in the manufacture of polyethylene all contain coordination compounds. Ions of the metals, especially the transition metals, are likely to form complexes.
In these complexes, transition metals form coordinate covalent bonds, a kind of Lewis acid-base interaction in which both of the electrons in the bond are contributed by a donor (Lewis base) to an electron acceptor (Lewis acid). The Lewis acid in...
25.6K
Extraction: Advanced Methods00:56

Extraction: Advanced Methods

1.3K
Metal ions can be separated from one another by complexation with organic ligands–the chelating agent– to form uncharged chelates. Here, the chelating agent must contain hydrophobic groups and behave as a weak acid, losing a proton to bind with the metal. Since most organic ligands used in this process are insoluble or undergo oxidation in the aqueous phase, the chelating agent is initially added to the organic phase and extracted into the aqueous phase. The metal-ligand complex is...
1.3K
Structural Isomerism02:34

Structural Isomerism

22.4K
Isomerism in Complexes
Isomers are different chemical species that have the same chemical formula. Structural isomerism of coordination compounds can be divided into two subcategories, the linkage isomers and coordination-sphere isomers.
Linkage isomers occur when the coordination compound contains a ligand that can bind to the transition metal center through two different atoms. For example, the CN− ligand can bind through the carbon atom or through the nitrogen atom. Similarly, SCN− can...
22.4K
Valence Bond Theory02:42

Valence Bond Theory

11.7K
Coordination compounds and complexes exhibit different colors, geometries, and magnetic behavior, depending on the metal atom/ion and ligands from which they are composed. In an attempt to explain the bonding and structure of coordination complexes, Linus Pauling proposed the valence bond theory, or VBT, using the concepts of hybridization and the overlapping of the atomic orbitals. According to VBT, the central metal atom or ion (Lewis acid) hybridizes to provide empty orbitals of suitable...
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Ion Mobility-Mass Spectrometry Techniques for Determining the Structure and Mechanisms of Metal Ion Recognition and Redox Activity of Metal Binding Oligopeptides
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銅 (III) 酸化物単位をリガンド構造変異によって混乱させる

Debanjan Dhar1, Gereon M Yee1, Andrew D Spaeth1

  • 1Department of Chemistry, Center for Metals in Biocatalysis, Chemical Theory Center, and Minnesota Supercomputing Institute, University of Minnesota , 207 Pleasant Street Southeast, Minneapolis, Minnesota 55455, United States.

Journal of the American Chemical Society
|December 24, 2015
PubMed
まとめ

改造されたリガンドを持つ新しい銅複合体は,水素原子抽象 (HAT) 反応に影響を与えます. 電子調節は熱力学と運動学に影響を与え,反応エンタルピーと速度の間の線形傾向を明らかにし,バリアとトンネリングによる微妙な変動がある.

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Quantifying the Binding Interactions Between CuII and Peptide Residues in the Presence and Absence of Chromophores
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Structure and Coordination Determination of Peptide-metal Complexes Using 1D and 2D 1H NMR
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Ion Mobility-Mass Spectrometry Techniques for Determining the Structure and Mechanisms of Metal Ion Recognition and Redox Activity of Metal Binding Oligopeptides
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Structure and Coordination Determination of Peptide-metal Complexes Using 1D and 2D 1H NMR
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Structure and Coordination Determination of Peptide-metal Complexes Using 1D and 2D 1H NMR

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科学分野:

  • 有機金属化学
  • カタリシス
  • 反応メカニズム

背景:

  • 銅複合体は触媒に不可欠です
  • 金属中心の反応性に対するリガンド効果を理解することが鍵となる.
  • 水素原子抽象 (HAT) は基本的な反応経路である.

研究 の 目的:

  • 合わせた電子特性を有する新しい銅 (III) 水酸化物複合体を合成し,特徴づけること.
  • HAT反応に対するリガンド改変の熱力学および運動学的効果を調査する.
  • 銅酸化物種の反応性を支配する要因を解明する.

主な方法:

  • 新しいリガンドセットの合成: (pipMe) LH2と (NO2) LH2.
  • Cu (II) -OH2複合体のO−H結合解離エネルギー (BDE) の測定
  • 異なるC−H結合強度の基質を用いたCu (III) 酸化物複合体によるHAT反応の運動研究.
  • 運動同位体効果 (KIEs) の分析と移行状態理論の計算.

主要な成果:

  • リガンドの修正により,O-H債券のBDEがわずかに違っていた.
  • 二次速度定数 (log k) と反応エンタルピー (ΔH) の間の線形相関が観察された.
  • 反応速度の微妙な変動は,HATバリアの高さの変化と,低温 (-80〜-20 °C) で量子トンネルの効率に起因する.

結論:

  • リガンド設計による銅複合体の電子調節は,HAT反応の熱力学と運動学に大きな影響を及ぼします.
  • 観測された線形傾向は反応エンタルピーの支配的な役割を果たしますが,トンネリングなどの他の要因も役割を果たします.
  • この研究は,触媒用途の銅酸化物複合体の反応性を制御するための貴重な洞察を提供します.