School of Environmental Engineering, Wuhan Textile University, Wuhan 430073, China.
School of Environmental Engineering, Wuhan Textile University, Wuhan 430073, China; Engineering Research Center for Clean Production of Textile Dyeing and Printing, Ministry of Education, Wuhan 430073, China.
J Environ Sci (China). 2019 Oct;84:1-12. doi: 10.1016/j.jes.2019.04.009. Epub 2019 Apr 19.
A series of functional organic-metal AgCl-decorated graphitic carbon nitride (AgCl-CN) composites were synthesized and applied for the degradation of oxalic acid (OA) under visible light. The highest photocatalytic activity was achieved with AgCl decoration ratio of 1.0 (denoted as AgCl-CN). The pseudo-first-order constant for OA degradation was 0.0722 min with the mineralization efficiency of 90.80% after 60 min reaction in the photocatalytic process with AgCl-CN. A variety of characterization techniques including Brunauer-Emmett-Teller, X-ray diffraction, scanning electron microscope, transmission electron microscopy, X-ray photoelectron spectroscopy, Fourier transform infrared spectra, ultraviolet-visible diffuse reflectance spectra, photoluminescence, and Mott-Schottky were utilized to elucidate the physicochemical, microstructure, and optical properties contributing to the improvement of the photocatalytic performance. The results showed that AgCl-CN had an oblate flaky erythrocyte-like structure with a moderate band gap energy of ~3.00 eV. In addition, the effects of the key parameters (i.e., AgCl-CN dosage, initial OA concentration, solution pH, and presence of natural organic matter) on OA degradation were systematically investigated. Radical scavenger experiments indicated that photogenerated holes, electrons, superoxide anion radicals, and hydroxyl radicals were the dominant reactive species. Moreover, AgCl-CN exhibited excellent stability and reusability for OA degradation without detectable Ag release in the solution over multiple reaction cycles. The efficient OA mineralization could be mainly ascribed to the moderate specific surface area, increased numbers of active sites, and effective interfacial charge transfer of AgCl-CN. Overall, the AgCl-CN composite was demonstrated to be a highly efficient, stable, and recoverable photocatalyst.
一系列功能有机金属 AgCl 修饰的石墨相氮化碳(AgCl-CN)复合材料被合成,并应用于可见光下草酸(OA)的降解。AgCl 修饰比例为 1.0(表示为 AgCl-CN)时,具有最高的光催化活性。在光催化过程中,OA 的降解的假一级动力学常数为 0.0722 min,60 min 后矿化效率达到 90.80%。采用比表面积仪、X 射线衍射仪、扫描电子显微镜、透射电子显微镜、X 射线光电子能谱仪、傅里叶变换红外光谱仪、紫外-可见漫反射光谱仪、光致发光光谱仪和 Mott-Schottky 等多种表征技术,阐明了促进光催化性能提高的物理化学、微观结构和光学性质。结果表明,AgCl-CN 具有适度的带隙能(~3.00 eV)的扁片状红细胞样结构。此外,系统研究了关键参数(即 AgCl-CN 用量、初始 OA 浓度、溶液 pH 值和天然有机物的存在)对 OA 降解的影响。自由基捕获实验表明,光生空穴、电子、超氧阴离子自由基和羟基自由基是主要的活性物质。此外,AgCl-CN 在多次反应循环中,在溶液中没有检测到 Ag 释放的情况下,对 OA 降解表现出优异的稳定性和可重复使用性。高效的 OA 矿化主要归因于 AgCl-CN 的适度比表面积、增加的活性位点数量和有效的界面电荷转移。总的来说,AgCl-CN 复合材料是一种高效、稳定、可回收的光催化剂。