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李森, 徐思遥, 唐俊杰, 罗勇. La-Co复合氧化物催化降解VOCs[J]. 应用技术学报, 2019, 19(2): 110-118. DOI: 10.3969/j.issn.2096-3424.2019.02.002
引用本文: 李森, 徐思遥, 唐俊杰, 罗勇. La-Co复合氧化物催化降解VOCs[J]. 应用技术学报, 2019, 19(2): 110-118. DOI: 10.3969/j.issn.2096-3424.2019.02.002
LI Sen, XU Siyao, TANG Junjie, LUO Yong. Catalytic Degradation of VOCs over La-Co Composite Oxides[J]. Journal of Technology, 2019, 19(2): 110-118. DOI: 10.3969/j.issn.2096-3424.2019.02.002
Citation: LI Sen, XU Siyao, TANG Junjie, LUO Yong. Catalytic Degradation of VOCs over La-Co Composite Oxides[J]. Journal of Technology, 2019, 19(2): 110-118. DOI: 10.3969/j.issn.2096-3424.2019.02.002

La-Co复合氧化物催化降解VOCs

Catalytic Degradation of VOCs over La-Co Composite Oxides

  • 摘要: 通过共沉淀法制备了一系列的复合La-Co氧化物,以N2吸脱附、X射线衍射、扫描电子显微镜、透射电子显微镜、H2程序升温还原和X射线光电子能谱对其进行表征测试, 并采用密度泛函理论(DFT)模拟计算优化了La-Co催化剂的理论模型。La-Co催化剂活性评价在固定床连续反应器-气相色谱在线检测装置上进行,此时体积空速15 000 h-1、氧气体积分数10%、温度150~275 ℃、作为降解底物的正庚烷和甲苯的体积分数为0.18%。结果表明,La的添加能显著提高Co催化剂物理及化学性能,比表面积最高提高6倍以上,晶面间距减小约24 nm,吸附氧所需能量最多降低0.62 eV。其中LCC4催化剂催化活性最优,其对正庚烷与甲苯转化率达90%时的最低温度分别为152和178 ℃,与Co3O4催化剂相比分别降低69和32 ℃。LCC4催化剂稳定性考察结果显示,其在500 min内对正庚烷及甲苯的降解活性均维持在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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