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氧化石墨烯负载的氧化钒配位化合物作为苯甲醇绿色氧化的高效催化剂。

Graphene oxide supported oxidovanadium coordination compound as an efficient catalyst for the green oxidation of benzyl alcohol.

作者信息

Aliniya Mohammadreza, Bikas Rahman, Heydari Neda, Krawczyk Marta S, Lis Tadeusz

机构信息

Department of Chemistry, Faculty of Science, Imam Khomeini International University, Qazvin, 34148-96818, Iran.

Department of Basic Chemical Sciences, Faculty of Pharmacy, Wroclaw Medical University, Borowska 211A St, 50-556, Wroclaw, Poland.

出版信息

Sci Rep. 2025 Jul 2;15(1):23027. doi: 10.1038/s41598-025-07345-3.

DOI:10.1038/s41598-025-07345-3
PMID:40596244
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC12217261/
Abstract

In this research, a green method for the oxidation of benzyl alcohol to its oxidized products has been reported. Firstly, (E)-4-amino-N'-(phenyl(pyridin-2-yl)methylene)benzohydrazide (HL) as an NNO-donor ligand was synthesized by the reaction of 2-benzoylpyridine and 4-aminobenzohydrazide in a molar ratio of 1:1 under reflux condition. HL was used for the synthesis of a V(V) coordination compound, [VO(µ-O)L], through its reaction with NHVO in methanol under reflux condition and the orange crystals of dinuclear oxidovanadium(V) coordination compound, [VO(µ-O)L], were obtained by partial evaporation of the solvent during four days. HL and [VO(µ-O)L] were characterized by spectroscopic methods and the structure of [VO(µ-O)L] was determined by single crystal X-ray analysis which showed that it is a neutral binuclear oxidovanadium(V) coordination compound and is crystallized in triclinic system (P-1 space group). In the unit cell there are two kinds of independent centrosymmetric dinuclear [VO(µ-O)L] molecules and the V(V) ions in both molecules are six coordinated. Due to the presence of free amine functional group in the structure, [VO(µ-O)L] was supported on the surface of graphene oxide, and a heterogeneous catalyst (GO-V) was provided. GO-V was characterized by FT-IR, UV-DRS, TGA, XRD, FE-SEM, EDX/map and BET analyses. The obtained heterogeneous catalyst was used in the oxidation of benzyl alcohol, and during this process, the effect of influencing parameters was investigated. The catalyst was recovered after the catalytic process and characterized by FT-IR, XRD, FE-SEM and EDX/map analyses. The results indicated that GO-V has high stability and activity in the catalytic conversion of benzyl alcohol to its oxidized products.

摘要

在本研究中,报道了一种将苯甲醇氧化为其氧化产物的绿色方法。首先,通过2-苯甲酰基吡啶与4-氨基苯甲酰肼在回流条件下以1:1的摩尔比反应合成了作为NNO供体配体的(E)-4-氨基-N'-(苯基(吡啶-2-基)亚甲基)苯甲酰肼(HL)。HL通过在回流条件下于甲醇中与NHVO反应用于合成V(V)配位化合物[VO(µ-O)L],通过在四天内部分蒸发溶剂获得了双核氧化钒(V)配位化合物[VO(µ-O)L]的橙色晶体。通过光谱方法对HL和[VO(µ-O)L]进行了表征,并通过单晶X射线分析确定了[VO(µ-O)L]的结构,结果表明它是一种中性双核氧化钒(V)配位化合物,结晶于三斜晶系(P-1空间群)。在晶胞中有两种独立的中心对称双核[VO(µ-O)L]分子,且两个分子中的V(V)离子均为六配位。由于结构中存在游离胺官能团,[VO(µ-O)L]负载在氧化石墨烯表面,从而得到了一种多相催化剂(GO-V)。通过傅里叶变换红外光谱(FT-IR)、紫外可见漫反射光谱(UV-DRS)、热重分析(TGA)、X射线衍射(XRD)、场发射扫描电子显微镜(FE-SEM)、能谱分析/图谱(EDX/map)和比表面积分析(BET)对GO-V进行了表征。将所得的多相催化剂用于苯甲醇的氧化反应,并在此过程中研究了影响参数的作用。催化反应后回收催化剂,并通过FT-IR、XRD、FE-SEM和EDX/map分析对其进行表征。结果表明,GO-V在将苯甲醇催化转化为其氧化产物的过程中具有高稳定性和活性。

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