State Key Laboratory of Coal Combustion, Huazhong University of Science and Technology, 430074 Wuhan, Hubei, China.
State Key Laboratory of Coal Combustion, Huazhong University of Science and Technology, 430074 Wuhan, Hubei, China.
Chemosphere. 2015 Apr;125:16-24. doi: 10.1016/j.chemosphere.2014.12.082. Epub 2015 Feb 2.
A series of novel spinel Fe3-xCuxO4 (0<x<0.71) composites, synthesized by chemical co-precipitation method, are proposed synthesized to use as highly active heterogeneous Fenton-like catalysts to remove elemental mercury (Hg0) from the simulated flue gases. Inductively coupled plasma-Atomic emission spectrometry (ICP-AES), X-ray diffraction patterns (XRD), scanning electron microscopy (SEM), Brunauer-Emmett-Teller (BET) surface area, and X-ray photoelectron spectrometer (XPS) were used to characterize the catalysts. The catalysts were confirmed the presence of the redox pairs Fesurf2+/Fesurf3+ and Cusurf+/Cusurf2+ on the surface of the cubic structure. The performance of heterogeneous Fenton-like reactions for Hg0 removal was evaluated in a lab-scale bubbling reactor at the solution temperature of 50°C. The systematic studies on the effects of different catalysts, H2O2 concentration and solution pH values on Hg0 removal efficiencies were performed. The recycling of the Fe3-xCuxO4 catalysts in Fenton-like solution is stable and Hg0 removal efficiency remain above 90% after 3 cycles. The active hydroxyl radical (OH) generated during heterogeneous Fenton-like reactions was confirmed through electron spin resonance (ESR) spin-trapping technique. The Hg0 removal mechanism has been discussed based on the experimental and analytical results.
一系列新型尖晶石 Fe3-xCuxO4（0<x<0.71）复合材料，通过化学共沉淀法合成，被提议用作高效的非均相类 Fenton 催化剂，以从模拟烟道气中去除元素汞（Hg0）。电感耦合等离子体原子发射光谱法（ICP-AES）、X 射线衍射图（XRD）、扫描电子显微镜（SEM）、BET 比表面积和 X 射线光电子能谱（XPS）用于对催化剂进行表征。催化剂被证实存在于立方结构表面的氧化还原对 Fesurf2+/Fesurf3+和 Cusurf+/Cusurf2+。在 50°C 的溶液温度下，在实验室规模的鼓泡反应器中评估了用于 Hg0 去除的非均相类 Fenton 反应的性能。系统研究了不同催化剂、H2O2 浓度和溶液 pH 值对 Hg0 去除效率的影响。在类 Fenton 溶液中，Fe3-xCuxO4 催化剂的回收是稳定的，经过 3 次循环后，Hg0 去除效率仍保持在 90%以上。通过电子顺磁共振（ESR）自旋捕获技术证实了在非均相类 Fenton 反应中生成的活性羟基自由基（OH）。根据实验和分析结果，讨论了 Hg0 去除机制。
