The Merox process was widely applied in the fine chemical industry to convert mercaptans into disulfides by oxidation with oxygen, including dimethyl disulfide (DMDS). In this paper, a new activated carbon (AC)-supported sulfonated cobalt phthalocyanine (AC-CoPcS) catalyst was prepared through the chemical linkage of ethylenediamine between them. UV−VIS, FT-IR, BET, and XPS were used to characterize the structure of the new catalyst. Then AC-CoPcS was applied to catalyze sodium methylmercaptide (SMM) oxidation for the preparation of DMDS. The effect of process parameters, such as reaction time, catalyst dosage, reaction temperature, and oxygen pressure on SMM conversion per pass (CPPSMM), yield (YieldDMDS), and purity of the DMDS (PurityDMDS) product were investigated to evaluate the catalytic performance of AC-CoPcS. The new supported catalyst exhibits better catalytic performance than the commercial one and can be properly reused four times to obtain CPPSMM and YieldDMDS higher than 90% and 70%. Under the optimum experimental conditions, the CPPSMM and YieldDMDS could reach as high as 98.7% and 86.8%, respectively, and the purity of the DMDS product is as high as 99.8%. This new supported catalyst exhibits good industrial application prospects.
Hybrid complexes with N,N 1 -bis(2-benzimidazolylmethyl)amine and cyclen moieties are novel enzyme mimics and controlled DNA release materials, which could interact with DNA through three models under different conditions. In this paper, the interactions between plasmid DNA and seven different complexes were investigated, and the methods to change the interaction patterns by graphene oxide (GO) or concentrations were also investigated. The cleavage of pUC19 DNA promoted by target complexes were via hydrolytic or oxidative mechanisms at low concentrations ranging from 3.13ˆ10´7 to 6.25ˆ10´5 mol/L. Dinuclear complexes 2a and 2b can promote the cleavage of plasmid pUC19 DNA to a linear form at pH values below 7.0. Furthermore, binuclear hybrid complexes could condense DNA as nanoparticles above 3.13ˆ10´5 mol/L and partly release DNA by graphene oxide with π-π stacking. Meanwhile, the results also reflected that graphene oxide could prevent DNA from breaking down. Cell viability assays showed dinuclear complexes were safe to normal human hepatic cells at relative high concentrations. The present work might help to develop novel strategies for the design and synthesis of DNA controllable releasing agents, which may be applied to gene delivery and also to exploit the new application for GO.
Dimethyl disulfide (DMDS) is an important fine chemical that can be prepared by the refined Merox process of oxidation of sodium methyl mercaptide (SMM) in the presence of a catalyst. In this paper, a novel activated carbon (AC) supported cobalt(II) tetraaminophthalocyanine (AC-CoTAPc) catalyst was prepared by the chemical grafting method. EA, UV-vis, FT-IR, BET and XPS were used to characterize the structure of the new catalyst. The effects of reaction time, catalyst dosage, reaction temperature and oxygen pressure on SMM conversion per pass (CPP[Formula: see text], yield (Yield[Formula: see text] and purity of DMDS product (Purity[Formula: see text] were investigated to evaluate the catalytic performance of new AC-CoTAPc catalyst. The results show that free CoTAPc is easily dissolved in this DMDS product, which needs extra post treatment and cannot be reused. The supported catalyst AC-CoTAPc can easily solve these problems and can be properly reused four times to get Yield[Formula: see text] and CPP[Formula: see text] higher than 70% and 90%. Under optimum conditions, the Yield[Formula: see text] andCPP[Formula: see text] of the AC-CoTAPc catalyst could be as high as 87.4% and 98.1%, with a purity[Formula: see text]of DMDS product of above 99.9%. AC-CoTAPc exhibits better catalytic and reuse performance than the commercial AC-supported sulphonated cobalt(II) phthalocyanine (AC-CoPcS) catalyst and shows broad industrial application prospects.
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