Nie Yulun, Hu Chun, Qu Jiuhui, Hu Xuexiang
State Key Laboratory of Environmental Aquatic Chemistry, Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences, Beijing 100085, China.
J Hazard Mater. 2008 Jun 15;154(1-3):146-52. doi: 10.1016/j.jhazmat.2007.10.005. Epub 2007 Oct 7.
SiO2-C2H4-ferrocene (SiCFe) was synthesized by covalent grafting of ferrocene on functionalized silica gel with a -C2H4- linkage. On the basis of characterization by diffuse reflectance UV-vis spectra (DRS) and Fourier transform infrared spectra (FT-IR), ferrocene has been successfully anchored on the silica gel. Under UVA (lambdamax=365 nm) irradiation, the catalyst exhibited high photocatalytic activity in the degradation of Acid Red B (ARB), especially in the presence of H2O2. Meanwhile, the catalytic activity of SiCFe was maintained effectively even after reused for 4 times without any significant destruction of ferrocene. The influence of initial solution pH and wavelength of UV light on the catalyst's activity was also investigated. Electron spin resonance (ESR) studies revealed that both OH and HO2/O2- radicals were involved as the active species in the ARB degradation process. Furthermore, results of total organic carbon (TOC) and FT-IR analysis indicated that ARB degradation proceeded by the cleavage of NN, followed by hydroxylation and opening of phenyl rings to form aliphatic acids and further oxidization of the aliphatic acids to produce carbon dioxide and water. A possible reaction mechanism was proposed on the basis of all the information obtained under various experimental conditions.
通过将二茂铁以 -C2H4- 键共价接枝到功能化硅胶上合成了SiO2-C2H4-二茂铁（SiCFe）。基于漫反射紫外可见光谱（DRS）和傅里叶变换红外光谱（FT-IR）的表征，二茂铁已成功锚定在硅胶上。在UVA（λmax = 365 nm）照射下，该催化剂在酸性红B（ARB）的降解中表现出高光催化活性，尤其是在H2O2存在的情况下。同时，即使重复使用4次后，SiCFe的催化活性也能有效保持，且二茂铁没有任何明显破坏。还研究了初始溶液pH值和紫外光波长对催化剂活性的影响。电子自旋共振（ESR）研究表明，OH和HO2/O2- 自由基均作为活性物种参与了ARB降解过程。此外，总有机碳（TOC）和FT-IR分析结果表明，ARB的降解是通过NN键的断裂进行的，随后是苯环的羟基化和开环，形成脂肪酸，并进一步氧化脂肪酸以产生二氧化碳和水。基于在各种实验条件下获得的所有信息，提出了一种可能的反应机理。
