Featured by abundant derivation and powerful catalytic activities, chiral catalysts and ligands with oxazolinyl ferrocenes core play a vital role in the area of enantioselective transformations. Despite great researches on phosphine ligands with oxazolinyl ferrocene silyl ether core have been broadly explored, the example of N,O -ferrocene compounds with identical core is rare. We herein disclosed the practical approaches to the preparation of planar chiral oxazolinyl hydroxyl ferrocene silyl ethers. Several available methods were employed for the establishment of the configuration on planar chirality , which considered as key parameter for the subsequent relative products. Furthermore, an array of N,O,O- tridentate ferrocenes was obtained through desilylation treated with TBAF. The absolute stereochemical configuration of the synthesized ferrocene derivatives was determined by X-ray diffraction.
Xinjie Wang,Juntian Li,Juan Li,Binghua Jing,Yun Sun,Teng Wang,Didi Li,Haibo Huang,Zhimin Ao
Ligands play an important role in the dispersion of metal and catalytic activity in single-atom transition metal-doped catalysts (SATMCs). In this work, a series of oxygen-ligand (O-ligand)-single-atom-Ni/2-dimensional reduced graphene oxide (RGO) materials (SANiX-O-2DRGO (X = 0.5–5)) were fabricated by a simple one-step co-reduction method. The single Ni atom on SANi5-O-2DRGO is embedded into the RGO and ligated by four O-ligand atoms. A systematic study confirms that the O-ligand is conducive to the dispersion of Ni and the formation of SATMCs with high metal loading. Density functional theory (DFT) calculation results demonstrate that the d-band center value of O-ligand-single-atom-Ni is closer to the Fermi level than that of the conventional N coordination, which is beneficial for electronic transition and enhances catalytic activity, i.e., the O-ligand accelerates the electron transfer between the carrier and the single metal atom, thus improving the catalytic oxidation capacity of volatile organic compounds (VOCs) on SANi5-O-2DRGO. As a demonstration, SANi5-O-2DRGO exhibits excellent reusability, water resistance, and stability for ethyl acetate oxidation. The degradation of ethyl acetate remained at 100% over 150 hours of continuous onstream operation. The catalytic oxidation mechanism of ethyl acetate on SANi5-O-2DRGO was also investigated. The O-ligand atoms provide the key electron transfer in the activation of adsorbed oxygen and catalytic oxidation process of reaction intermediates.
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