Bhattacharya Saurav, Ma Xiang, Mougharbel Ali S, Haouas Mohamed, Su Pei, Espenship Michael Forrester, Taffa Dereje H, Jaensch Helge, Bons Anton-Jan, Stuerzer Tobias, Wark Michael, Laskin Julia, Cadot Emmanuel, Kortz Ulrich
Department of Life Sciences and Chemistry, Jacobs University, Campus Ring 1, 28759 Bremen, Germany.
Institut Lavoisier de Versailles, UMR 8180 CNRS, UVSQ, Université Paris-Saclay, Versailles 78035, France.
Inorg Chem. 2021 Nov 15;60(22):17339-17347. doi: 10.1021/acs.inorgchem.1c02749. Epub 2021 Oct 27.
We report on the synthesis and structural characterization of a giant, discrete, and neutral molecular disk, [PdO(OH){(CH)AsO}] (), comprising a 40-palladium-oxo core that is capped by 16 dimethylarsinate moieties, resulting in a palladium-oxo cluster (POC) with a diameter of ∼2 nm. , which is the largest known neutral Pd-based oxo cluster, can be isolated either as a discrete species or constituting a 3D H-bonded organic-inorganic framework (HOIF) with a 12-tungstate Keggin ion, [SiWO] or [GeWO]. H and C NMR as well as H-DOSY NMR studies indicate that is stable in aqueous solution, which is also confirmed by ESI-MS studies. was also immobilized on a mesoporous support (SBA15) followed by the generation of size-controlled Pd nanoparticles (diameter ∼2-6 nm, as based on HR-TEM), leading to an effective heterogeneous hydrogenation catalyst for the transformation of various arenes to saturated carbocycles.
我们报道了一种巨大的、离散的中性分子盘[PdO(OH){(CH)AsO}]（）的合成与结构表征，它包含一个由16个二甲基砷酸根部分封顶的40钯氧核心，形成了一个直径约为2 nm的钯氧簇（POC）。作为已知最大的基于钯的中性氧簇，既可以作为离散物种分离出来，也可以与12钨酸盐Keggin离子[SiWO]或[GeWO]构成三维氢键有机-无机框架（HOIF）。氢核磁共振和碳核磁共振以及氢扩散排序核磁共振研究表明，在水溶液中是稳定的，电喷雾电离质谱研究也证实了这一点。还被固定在介孔载体（SBA15）上，随后生成尺寸可控的钯纳米颗粒（基于高分辨透射电子显微镜，直径约为2 - 6 nm），从而得到一种有效的多相氢化催化剂，用于将各种芳烃转化为饱和碳环。
