用于湿式甲烷燃烧的高活性、高稳定性钯沸石催化剂

Xuechao Tan, Suk Bong Hong
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摘要

天然气发动机是柴油和汽油发动机最可行的替代品。然而,目前用于消除发动机尾气中未燃烧甲烷的最先进催化剂--氧化铝上的钯(Pd)--存在着点火温度高(> 400 °C)和耐水性差的问题。在此,我们系统地研究了沸石结构和硅/铝比例、催化剂煅烧温度和框架外阳离子类型对湿法甲烷燃烧沸石支撑钯催化剂催化性能的影响,以克服这些局限性。我们发现,在 Si/Al 比率为 45 的 Na 后置换 500 °C 煅烧 IWV 沸石上支撑的 3.0 wt% Pd 催化剂,在 10% 水蒸汽存在下燃烧甲烷的熄灭温度低至 290 °C,同时在 330 °C 下 100 小时内保持约 85% 的甲烷转化率。这项研究为使支撑钯催化剂接近实际应用提供了新的方向。
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A highly active and stable palladium zeolite catalyst for wet methane combustion
Natural gas engines are the most viable alternative to diesel and gasoline ones. However, the current state-of-art catalyst, palladium (Pd) on alumina, for eliminating unburnt methane from engine exhaust suffers from high light-off temperature (> 400 °C) and poor water tolerance. Here we systematically investigated the effects of zeolite structure and Si/Al ratio, catalyst calcination temperature and extra-framework cation type on catalytic performance of zeolite-supported Pd catalysts for wet methane combustion to overcome these limitations. We found that a 3.0 wt% Pd catalyst supported on Na-post-exchanged 500 °C-calcined IWV zeolite with a Si/Al ratio of 45 has a light-off temperature as low as 290 °C for methane combustion in the presence of 10 % water vapor while maintaining ca. 85 % methane conversion at 330 °C for 100 h. This study provides a new direction for bringing supported Pd catalysts close to real-world applications.
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