Nguyen Tăng Sơn, Tu Le Manh, Nguyen Van Hoang, Pham Thi Lanh, Do Dang Trung, Nguyen Van Hieu
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引用次数: 0
摘要
采用多种技术制备了CeZrO2和H-ZSM-5(80)的双载体体系,包括物理混合、共沉淀和声化学方法,然后通过湿法浸渍沉积双金属Pd和Pt以获得最终的催化剂。催化剂在200和500°C之间的总甲烷氧化中进行了测试,最具活性的是来自声化学合成的材料。该催化剂在300°C的低温和100000 ml g−1 h−1的高气体时空速(GHSV)下实现了84%的显著甲烷转化率。使用x射线衍射(XRD)、Brunauer–Emmett–Teller(BET)、扫描电子显微镜(SEM)、扫描透射电子显微镜(STEM)、能量色散x射线光谱(EDS)进行表征,程序升温还原(TPR)和x射线吸收精细结构(XAFS)技术揭示了催化剂组分的紧密分布以及Pd和CeZrO2组分的容易氧化还原行为。基于声化学CeZrO2的催化剂被证明是相对稳定的,在300°C下连续运行50小时后,甲烷转化损失仅为7%,而商业TiO2基材料的甲烷转化损失为14%。
A bimetallic PdPt catalyst on CeZrO2/H-ZSM-5 dual support with exceptional activity in low temperature methane oxidation
Various techniques were employed to prepare a dual support system of CeZrO2 and H-ZSM-5 (80) including physically mixing, co-precipitation and sonochemical methods, which were followed by the deposition of bimetallic Pd and Pt via wet impregnation to obtain the final catalysts. The catalysts were tested in the total methane oxidation between 200 and 500 °C and the most active is the material derived from sonochemical synthesis. This catalyst achieved a remarkable methane conversion of 84% at a low temperature of 300 °C and high Gas Hourly Space Velocity (GHSV) of 100000 ml g−1 h−1. Characterisation using x-ray diffraction (XRD), Brunauer–Emmett–Teller (BET), scanning electron microscope (SEM), scanning transmission electron microscope (STEM), Energy-dispersive x-ray spectroscopy (EDS), temperature-programmed reduction (TPR) and x-ray absorption fine structure (XAFS) techniques revealed the intimate distribution of catalyst components and facile redox behaviour of both Pd and CeZrO2 components. The catalysts based on sonochemical CeZrO2 was proven to be relatively stable with only 7% methane conversion loss after 50 h continuously on stream at 300 °C compared to the corresponding 14% witnessed with the commercial TiO2-based material.