Selective Sulfide Oxidation with Hydrogen Peroxide Catalyzed by a Silica-Supported Polypyridyl-Iron Complex.

IF 3.5 3区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY
Saikat Bera, Ranit Datta, Afsar Ahmed, Arindam Dey, Subhasis Mondal, Tania Mukherjee, Partha Halder, Debajyoti Pramanik, Debobrata Sheet
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Abstract

Inspired by biomimetic models of non-heme iron oxygenase, an iron(II)-complex ligated by a polypyridyl ligand (TPAN) has been covalently anchored onto silica beads to exploit its oxidation capabilities towards sulfide oxidation in the presence of hydrogen peroxide as an oxidant. The prepared catalyst [Fe-TPAN@SiO2] was characterized by Fourier transform infrared spectroscopy (FT-IR), thermogravimetric analysis (TGA), and X-ray photoelectron spectroscopy (XPS). The silica-supported catalyst, measuring under 300 nm in size as observed via transmission electron microscopy (TEM), showed outstanding selectivity in the mono-oxygenation of sulfides, yielding the corresponding sulfoxides with high efficiency. The immobilized catalyst showed far better conversion as compared to the analogous homogeneous complex. The catalyst could be isolated and reused up to six cycles without losing the activity-selectivity profiles. A simultaneous involvement of an iron-oxygen intermediate and a Fenton-type process is proposed, with the former presumed to be the dominant oxidation pathway.

二氧化硅负载的聚吡啶-铁配合物催化过氧化氢选择性硫化物氧化。
受非血红素铁加氧酶的仿生模型的启发,一种由聚吡啶基配体(TPAN)连接的铁(II)-配合物被共价锚定在硅珠上,以利用其在过氧化氢作为氧化剂存在下对硫化物氧化的氧化能力。用傅里叶红外光谱(FT-IR)、热重分析(TGA)和x射线光电子能谱(XPS)对制备的催化剂[Fe-TPAN@SiO2]进行了表征。通过透射电子显微镜(TEM)观察到,二氧化硅负载的催化剂尺寸在300 nm以下,对硫化物的单氧氧化表现出出色的选择性,高效地生成相应的亚砜。与类似的均相配合物相比,固定化催化剂的转化率要好得多。该催化剂可以被分离并重复使用多达6次,而不会失去活性选择性谱。提出了铁氧中间体和fenton型过程的同时参与,前者被认为是主要的氧化途径。
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来源期刊
Chemistry - An Asian Journal
Chemistry - An Asian Journal 化学-化学综合
CiteScore
7.00
自引率
2.40%
发文量
535
审稿时长
1.3 months
期刊介绍: Chemistry—An Asian Journal is an international high-impact journal for chemistry in its broadest sense. The journal covers all aspects of chemistry from biochemistry through organic and inorganic chemistry to physical chemistry, including interdisciplinary topics. Chemistry—An Asian Journal publishes Full Papers, Communications, and Focus Reviews. A professional editorial team headed by Dr. Theresa Kueckmann and an Editorial Board (headed by Professor Susumu Kitagawa) ensure the highest quality of the peer-review process, the contents and the production of the journal. Chemistry—An Asian Journal is published on behalf of the Asian Chemical Editorial Society (ACES), an association of numerous Asian chemical societies, and supported by the Gesellschaft Deutscher Chemiker (GDCh, German Chemical Society), ChemPubSoc Europe, and the Federation of Asian Chemical Societies (FACS).
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