Selective H/D Exchange in E–H (E = Si, Ge, Sn) Bonds Catalyzed by 1,2,3-Triazolylidene-Stabilized Nickel Nanoparticles

IF 4.3 2区化学 Q1 CHEMISTRY, INORGANIC & NUCLEAR

Inorganic Chemistry Pub Date : 2025-04-16 DOI:10.1021/acs.inorgchem.5c00216

Pablo Molinillo, Ana Gálvez Del Postigo, Maxime Puyo, Florencia Vattier, Ana M. Beltrán, Nuria Rendón, Patricia Lara, Andrés Suárez

引用次数: 0

Abstract

Nickel nanoparticles (Ni·MIC) stabilized with mesoionic 1,2,3-triazolylidene (MIC) ligands were prepared via decomposition of the [Ni(COD)₂] (COD = 1,5-cyclooctadiene) complex with H₂ (3 bar) in the presence of 0.2 or 0.5 equiv of ligand. The obtained monodisperse and small-sized (3.2–3.8 nm) nanoparticles were characterized by high-resolution transmission electron microscopy (TEM, HRTEM) and inductively coupled plasma (ICP) analysis. Further analysis of the nickel nanoparticles by X-ray photoelectron spectroscopy (XPS) demonstrated the coordination of the MIC ligands to the metal surface. Finally, the Ni·MIC nanoparticles were applied in the isotopic H/D exchange in hydrides of group 14 elements (Si, Ge, Sn) using D₂ gas under relatively mild conditions (1.0–1.8 mol % Ni, 1 bar D₂, 55 °C). High and chemoselective deuterium incorporation at the E–H (E = Si, Ge, Sn) bond in these derivatives was observed.

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1,2,3-三氮酰基稳定镍纳米颗粒催化E - H （E = Si, Ge, Sn）键的选择性H/D交换

在0.2或0.5等量配体的存在下，用H2 （3 bar）分解[Ni(COD)2] （COD = 1,5-环二烯）配合物，制备了以介离子1,2,3-三唑二烯（MIC）配体稳定的镍纳米颗粒（Ni·MIC）。采用高分辨率透射电子显微镜（TEM）、HRTEM和电感耦合等离子体（ICP）对制备的单分散、小尺寸（3.2 ~ 3.8 nm）纳米颗粒进行了表征。通过x射线光电子能谱（XPS）进一步分析镍纳米颗粒，证实了MIC配体与金属表面的配位。最后，在相对温和的条件下（1.0-1.8 mol % Ni, 1 bar D2, 55°C），将Ni·MIC纳米颗粒应用于14族元素（Si, Ge, Sn）氢化物的同位素H/D交换。在这些衍生物的E - h （E = Si, Ge, Sn）键上观察到高度和化学选择性的氘掺入。

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来源期刊

Inorganic Chemistry 化学-无机化学与核化学

CiteScore

7.60

自引率

13.00%

发文量

1960

审稿时长

1.9 months

期刊介绍： Inorganic Chemistry publishes fundamental studies in all phases of inorganic chemistry. Coverage includes experimental and theoretical reports on quantitative studies of structure and thermodynamics, kinetics, mechanisms of inorganic reactions, bioinorganic chemistry, and relevant aspects of organometallic chemistry, solid-state phenomena, and chemical bonding theory. Emphasis is placed on the synthesis, structure, thermodynamics, reactivity, spectroscopy, and bonding properties of significant new and known compounds.