原位合成分子筛修饰石煤提钒尾渣表面制备低温NH_(3)-SCR催化剂  

In situ synthesis of molecular sieve to modify the surface of vanadium tailings extracted from stone coal to prepare a low-temperature NH_(3)-SCR catalyst

作　　者：刘真 刘浩[1] 张爱红 陶长元[1] 杜军[1] LIU Zhen;LIU Hao;ZHANG Ai-hong;TAO Chang-yuan;DU Jun(College of Chemistry and Chemical Engineering,Chongqing University,Chongqing 401331,China)

机构地区：[1]重庆大学化学化工学院,重庆401331

出　　处：《化学研究与应用》2024年第11期2543-2550,共8页Chemical Research and Application

基　　金：科技部国家重点研发计划项目(2020YFC1909705-3)资助。

摘　　要：石煤是我国的主要钒资源之一,经过提钒工艺后产生大量钒渣(FZ)。本文通过在其表面原位合成分子筛SSZ-13后将其用作脱硝催化剂载体SSZ-13/FZ而实现钒渣全量化资源利用。对钒渣表面原位合成分子筛的实验条件进行了优化,通过浸渍法制备了以V、Mn为活性组分、CeO_(2)为助剂的VMnCeO_(x)-SSZ-13(n)/FZ脱硝催化剂。采用固定床反应装置评价催化剂的脱硝活性,结果表明:催化剂VMnCeO_(x)-SSZ-13(0.5)/FZ在温度130~350℃内具有优异的脱硝活性,其中170~330℃内NO转化率(ηNO)超过90%,表现出良好的低温脱硝性能和宽温程脱硝活性。载体及催化剂的结构和性能表征结果显示,SSZ-13(n)/FZ相较于FZ有更大的比表面积,催化剂同时存在B酸和L酸双活性位点,且酸量显著增加,提高了活性组分的分散和反应物的吸附活化,从而促进NH3-Selective Catalytic Reduction(NH_(3)-SCR)反应。Stone coal is one of the main vanadium resources in China,and a large amount of vanadium tailing(FZ)is produced after the vanadium extraction process.In this paper,the full quantitative resource utilization of vanadium slag was realized by in situ synthesizing zeolite SSZ-13 on its surface and applying the as-formed SSZ-13/FZ a denitrification catalyst carrier.The experimental conditions for in-situ synthesis of zeolite on the surface of vanadium slag were optimized,and the denitrification catalysts VMnCeOSSZ-13(n)/FZ with V and Mn as active components and CeO_(2)as additives were prepared by the impregnation method.The results showed that the catalyst VMnCeO_(x)-SSZ-13(0.5)/FZ had excellent denitrification activity at 130~350℃,and the NO conversion rate(nno)was more than 90%at 170~330℃,showing good low-temperature denitrification performance and wide temperature range denitrification activity.The results of the structure and properties of the support and catalyst showed that SSZ-13(n)/FZ had a larger specific surface area than that of FZ,the dual active sites of both B acid and L acid sites,and the acid content increased significantly,which improved the dispersion of active components and the adsorption activation of reactants,thereby promoting the NH_(3)-Selective Catalytic Reduction(NH_(3)-SCR)reaction.

关 键 词：NH_(3)-SCR 提钒尾渣 SSZ-13 低温活性 

分 类 号：O614.5[理学—无机化学]