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La-Co復合氧化物催化降解VOCs

Catalytic Degradation of VOCs over La-Co Composite Oxides

  • 摘要: 通過共沉澱法製備了一系列的復合La-Co氧化物,以N2吸脫附、X射線衍射、掃描電子顯微鏡、透射電子顯微鏡、H2程序升溫還原和X射線光電子能譜對其進行表征測試, 並采用密度泛函理論(DFT)模擬計算優化了La-Co催化劑的理論模型。La-Co催化劑活性評價在固定床連續反應器-氣相色譜在線檢測裝置上進行,此時體積空速15 000 h-1、氧氣體積分數10%、溫度150~275 ℃、作為降解底物的正庚烷和甲苯的體積分數為0.18%。結果表明,La的添加能顯著提高Co催化劑物理及化學性能,比表面積最高提高6倍以上,晶面間距減小約24 nm,吸附氧所需能量最多降低0.62 eV。其中LCC4催化劑催化活性最優,其對正庚烷與甲苯轉化率達90%時的最低溫度分別為152和178 ℃,與Co3O4催化劑相比分別降低69和32 ℃。LCC4催化劑穩定性考察結果顯示,其在500 min內對正庚烷及甲苯的降解活性均維持在99%±0.5%。

     

    Abstract: A series of La-Co composite oxides were prepared via co-precipitation method, and were characterized by N2 adsorption&desorption, X-ray diffraction, scanning electron microscopy, Transmission electron microscope, H2 temperature programmed reduction and X-ray photoelectron spectroscopy, respectively. Furthermore, the theoretical model of La-Co composite oxides were simulated using Density Function Theory (DFT). And then, the catalytic activity of the catalysts for degradation of 0.18% n-heptane and 0.18% toluene was respectively investigated in a continuous fixed bed reactor with GHSV of 15 000 h-1, oxygen concentration of 10% and temperature from 150 to 275 ℃. The results showed that lanthanum significantly improves the physical and chemical properties of Co catalysts. It was observed that specific surface area is increased by 6 times, crystal space is reduced by 24 nm, and the energy required to adsorb oxygen is reduced by 0.62 eV. The catalyst named LCC4 performed best activity and obtained 90% conversion of n-heptane and toluene at 152 and 178 ℃, which dropped by 69 and 32 ℃ compared with that of the Co catalysts. Finally, the stability test of LCC4 catalyst was carried out over 500 minutes, and the loss of degradation activity of n-heptane and toluene was only 0.5%.

     

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