Zuo Shufeng, Yang Peng, Wang Xianqin
Zhejiang Key Laboratory of Alternative Technologies for Fine Chemicals Process, Shaoxing University, Shaoxing 312000, China.
Department of Chemical, Biological and Pharmaceutical Engineering, New Jersey Institute of Technology, Newark, New Jersey 07102, United States.
ACS Omega. 2017 Aug 30;2(8):5179-5186. doi: 10.1021/acsomega.7b00592. eCollection 2017 Aug 31.
An efficient and environmentally friendly synthesis of AlFe-pillared clay (AlFe-PILC)-supported MnCe catalysts was explored. Mixed AlFe pillaring agents were prepared by a one-step method using Locron L and ferric nitrate solutions at a high temperature and high pressure. Montmorillonite was treated with the AlFe pillaring agents to synthesize AlFe-PILC. MnO and CeO with different Mn/Ce atomic ratios were loaded onto the AlFe-PILC support by an impregnation method. The catalysts were characterized using X-ray diffraction, N adsorption, and high-resolution transmission electron microscopy-energy dispersive spectrometry and were tested for the catalytic combustion of benzene and temperature-programmed surface reaction using a microreactor. Compared to conventional methods, this method is simpler and less costly and results in a larger specific surface area, pore volume, and basal spacing, with the ability to control the structure of the catalytic materials. MnCe(6:1)/AlFe-PILC has the highest catalytic activity and can completely degrade benzene (600 ppm in air) at 250 °C. The activity of the catalyst is stable, and no obvious deactivation is observed at 230 °C after 1000 continuous hours. The catalyst is resistant to water and Cl-poisoning. The amount of CeO added is critical to the dispersion of MnO on the support and the creation of optimum number of oxygen vacancy defect sites for the benzene oxidation reaction. The AlFe-PILC-supported MnCe catalyst is a promising porous material; the support structure, proper dispersion of active species, and addition of Ce are essential for achieving complete degradation of organic toxic chemicals at relatively low temperatures.
探索了一种高效且环保的合成AlFe柱撑粘土（AlFe-PILC）负载的MnCe催化剂的方法。使用洛柯龙L和硝酸铁溶液在高温高压下通过一步法制备混合AlFe柱撑剂。用AlFe柱撑剂处理蒙脱石以合成AlFe-PILC。通过浸渍法将具有不同Mn/Ce原子比的MnO和CeO负载到AlFe-PILC载体上。使用X射线衍射、N吸附和高分辨率透射电子显微镜-能量色散光谱对催化剂进行表征，并使用微型反应器对其进行苯的催化燃烧和程序升温表面反应测试。与传统方法相比，该方法更简单、成本更低，并且具有更大的比表面积、孔体积和层间距，能够控制催化材料的结构。MnCe(6:1)/AlFe-PILC具有最高的催化活性，能在250℃下完全降解空气中600 ppm的苯。催化剂的活性稳定，在230℃连续运行1000小时后未观察到明显失活。该催化剂具有抗水和抗氯中毒性能。添加的CeO量对于MnO在载体上的分散以及为苯氧化反应创造最佳数量的氧空位缺陷位点至关重要。AlFe-PILC负载的MnCe催化剂是一种有前途的多孔材料；载体结构、活性物种的适当分散以及Ce的添加对于在相对较低温度下实现有机有毒化学品的完全降解至关重要。
