摘要
采用溶胶凝胶法和浸渍法制备了负载于蜂窝陶瓷上的Co/Fe/Al_2O_3/cordierite催化剂,在陶瓷管流动反应器上对其催化C_3H_6选择性还原NO的性能进行了测试。结果表明,该催化剂表现出最优脱硝性能,在模拟烟气条件下,当反应温度为550℃时可实现97%的脱硝效率。Co的引入可显著增强Fe/Al_2O_3/cordierite催化剂抗SO_2和H_2O的能力。在模拟烟气中同时引入0.02%SO_2和3%H_2O后,1.5Co/Fe/Al_2O_3/cordierite的脱硝性能受影响甚微,当反应温度高于500℃时1.5Co/Fe/Al_2O_3/cordierite催化C_3H_6还原NO的效率均可达到90%以上;相比之下,未经Co修饰的催化剂Fe/Al_2O_3/cordierite脱硝性能受到了严重的抑制,在整个反应温度区间(200-700℃)内,其催化C_3H_6还原NO的效率最高不足50%。XRD和SEM表征结果表明,经过适量的Co修饰后的1.5Co/Fe/Al_2O_3/cordierite表面变得更疏松,且形成了以钴铁和钴铝双金属氧化物为主要成分的球状晶粒。H_2-TPR结果表明,相比于Fe/Al_2O_3/cordierite,1.5Co/Fe/Al_2O_3/cordierite有更好的低温还原性能。PyFTIR结果表明,Co的引入可使催化剂表面的Lewis酸明显增加,且生成了Brnsted酸。N2吸附-脱附表征结果表明,Co可增大催化剂的比表面积。
The Co/Fe/Al2O3/cordierite catalysts with different Co loadings were prepared by sol-gel and impregnation methods,and their performance in the selective catalytic reduction of NO with C3H6 over catalytic were experimentally studied in a ceramic tubular reactor. The results indicated that 1. 5 Co/Fe/Al2O3/cordierite showed the highest C3H6-SCR activity with 97% NO reduction in the simulated flue gas at 550 ℃. Cobalt was able to effectively improve the ability of Fe/Al2O3/cordierite catalysts to resist SO2 and H2O in flue gas. When 0.02% SO2 and 3% water vapor were added to the simulated flue gas,the NO reduction efficiency of 1.5 Co/Fe/Al2O3/cordierite was almost unaffected, the NO reduction by 1. 5 Co/Fe/Al2O3/cordierite with C3H6 all surpassed 90%. In contrast, the catalytic activity of Fe/Al2O3/cordierite without cobalt modification was seriously suppressed by SO2 and H2O,the highest NO reduction efficiency of Fe/Al2O3/cordierite was less than50% within the entire reaction temperature range（ 200-700 ℃）.XRD and SEMresults showed that the surface of1.5 Co/Fe/Al2O3/cordierite after the modification by cobalt became loose,and formed by the cobalt iron and cobalt aluminum metal oxide-based spherical grains.H2-TPR results showed that 1.5 Co/Fe/Al2O3/cordierite had better lowtemperature reduction performance than Fe/Al2O3/cordierite. Py-FTIR results confirmed that Co can dramatically increased the Lewis acid and produced Brnsted acid on the catalyst surface. N2 adsorption/desorption characterization results proved that Co can increase the specific surface area of the catalyst.
作者
刘欣
苏亚欣
董士林
周皞
邓文义
赵兵涛
LIU Xin1, SU Ya-xin1 , DONG Shi-lin1 , ZHOU Hao2 , DENG Wen-yi1, ZHAO Bing-tao3(1. School of Environmental Science and Engineering, Donghua University, Shanghai 201620, China; 2. Changzhou Vocational Institute of Engineering, Changzhou 213164, China; School of Energy and Power Engineering, University of Shanghai Science and Technology, Shanghai 200093, Chin)
出处
《燃料化学学报》
EI
CAS
CSCD
北大核心
2018年第6期743-753,共11页
Journal of Fuel Chemistry and Technology
基金
国家自然科学基金(51278095)
江苏省前瞻性联合研究项目(BY2015032-02)
上海市自然科学基金(17ZR1419300)资助~~
