Hong Qiulin, Chen Shiliang
Institute of Environmental Sciences, Qianjiang College, Hangzhou Normal University, Hangzhou 310018, China.
Nanomaterials (Basel). 2020 Aug 26;10(9):1673. doi: 10.3390/nano10091673.
It is generally accepted that the convenient fabrication of a metal phthalocyanine-based heterogeneous catalyst with superior catalytic activity is crucial for its application. Herein, a novel and versatile ultrasonic-assisted biosynthesis approach (conducting ultrasonic treatment during biosynthesis process) was tactfully adopted for the direct immobilization of a sulfonated cobalt phthalocyanine (PcS) catalyst onto a graphene-bacterial cellulose (GBC) substrate without any modification. The prepared phthalocyanine-graphene-bacterial-cellulose nanocomposite, PcS@GBC, was characterized by field emission scanning electron microscope (FESEM) and X-ray photoelectron spectroscopy (XPS). The catalytic activity of the PcS@GBC was evaluated based on its catalytic oxidation performance to dye solution, with HO used as an oxidant. More than a 140% increase of dye removal percentage for the PcS@GBC heterogeneous catalyst was found compared with that of PcS. The unique hierarchical architecture of the GBC substrate and the strong interaction between PcS and graphene, which were verified experimentally by ultraviolet-visible light spectroscopy (UV-vis) and Fourier transform infrared spectroscopy (FT-IR) and theoretically by density functional theory (DFT) calculation, were synergistically responsible for the substantial enhancement of catalytic activity. The accelerated formation of the highly reactive hydroxyl radical (·OH) for PcS@GBC was directly evidenced by the electron paramagnetic resonance (EPR) spin-trapping technique. A possible catalytic oxidation mechanism for the PcS@GBC-HO system was illustrated. This work provides a new insight into the design and construction of a highly reactive metal phthalocyanine-based catalyst, and the practical application of this functional nanomaterial in the field of environmental purification is also promising.
人们普遍认为，制备具有优异催化活性的金属酞菁基多相催化剂对于其应用至关重要。在此，巧妙地采用了一种新颖且通用的超声辅助生物合成方法（在生物合成过程中进行超声处理），将磺化钴酞菁（PcS）催化剂直接固定在未经任何修饰的石墨烯 - 细菌纤维素（GBC）载体上。通过场发射扫描电子显微镜（FESEM）和X射线光电子能谱（XPS）对制备的酞菁 - 石墨烯 - 细菌纤维素纳米复合材料PcS@GBC进行了表征。基于其对染料溶液的催化氧化性能，以H₂O₂作为氧化剂，评估了PcS@GBC的催化活性。与PcS相比，发现PcS@GBC多相催化剂的染料去除率提高了140%以上。通过紫外 - 可见光谱（UV - vis）和傅里叶变换红外光谱（FT - IR）实验验证以及密度泛函理论（DFT）计算理论验证，GBC载体独特的分级结构以及PcS与石墨烯之间的强相互作用共同促成了催化活性的显著增强。电子顺磁共振（EPR）自旋捕获技术直接证明了PcS@GBC中高活性羟基自由基（·OH）的加速形成。阐述了PcS@GBC - H₂O₂体系可能的催化氧化机理。这项工作为高活性金属酞菁基催化剂的设计和构建提供了新的见解，并且这种功能纳米材料在环境净化领域的实际应用也很有前景。
