锰氧八面体分子筛用于等离子催化降解乙醛的性能研究
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摘要
分别采用固相法、回流法及水热法制备了锰氧八面体分子筛催化剂(OMS-2),通过XRD、BET、H_2-TPR、TEM等手段对催化剂进行了表征,考察了不同方法制备的锰氧八面体分子筛与低温等离子体耦合去除乙醛的性能。结果表明,OMS-2催化剂可以明显提高等离子降解乙醛的性能,同时提高CO_2选择性并降低等离子副产物O_3的生成。相比于固相法与水热法,回流法制备的OMS-2催化剂具体更高的等离子催化活性,结合催化剂表征结果,可以发现高催化活性的主要原因在于:回流法制备的OMS-2具有较差的结晶度、较大的比表面积及较强的氧物种可移动性。
Manganese oxide octahedral molecular sieves(OMS-2) were prepared by solid-phase method,reflux method and hydrothermal method,respectively.The catalysts were characterized by XRD,BET,H_2-TPR and TEM.This paper investigated the properties of the catalysts by different methods for acetaldehyde degradation with non-thermal plasma. The results showed that OMS-2 catalysts could obviously improve the acetaldehyde removal efficiency and CO_2 selectivity of non-thermal plasma,meanwhile,the byproduct O_3 could also be suppressed.The plasma-catalytic activity of OMS-2 catalyst prepared by reflux method was more significant than those of solid-phase and hydrothermal method. According to the characterization results,the main reason may be that: the high catalytic activity of OMS-2 prepared by reflux has poorer crystallinity, larger specific surface area and stronger mobility of oxygen species.
Manganese oxide octahedral molecular sieves(OMS-2) were prepared by solid-phase method,reflux method and hydrothermal method,respectively.The catalysts were characterized by XRD,BET,H_2-TPR and TEM.This paper investigated the properties of the catalysts by different methods for acetaldehyde degradation with non-thermal plasma. The results showed that OMS-2 catalysts could obviously improve the acetaldehyde removal efficiency and CO_2 selectivity of non-thermal plasma,meanwhile,the byproduct O_3 could also be suppressed.The plasma-catalytic activity of OMS-2 catalyst prepared by reflux method was more significant than those of solid-phase and hydrothermal method. According to the characterization results,the main reason may be that: the high catalytic activity of OMS-2 prepared by reflux has poorer crystallinity, larger specific surface area and stronger mobility of oxygen species.
引文
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[11]HERNANDEZ W,CENTENO M,ROMERO-SARRIA F,et al.Modified cryptomelane-type manganese dioxide nanomaterials for preferential oxidation of CO in the presence of hydrogen[J].Catalysis Today,2010,157(1):160-165.
[12]XU R,WANG X,WANG D,et al.Surface structure effects in nanocrystal MnO2 and Ag/MnO2 catalytic oxidation of CO[J].Journal of Catalysis,2006,237(2):426-430.
[13]KIM S C,SHIM W G.Catalytic combustion of VOCs over a series of manganese oxide catalysts[J].Applied Catalysis B:Environmental,2010,98(3-4):180-185.
[14]LI W,GIBBS G V,OYAMA S T.Mechanism of ozone decomposition on a manganese oxide catalyst.1.in situ raman spectroscopy and Ab initio molecular orbital calculations[J].Journal of the American Chemical Society,1998,120(35):9041-9046.
[15]EINAHA H,HARADA M,FUTAMURA S.Structural changes in alumina-supported manganese oxides during ozone decomposition[J].Chemical Physics Letters,2005,408(4-6):377-380.
[16]GUO Y,LIAO X,HE J,et al.Effect of manganese oxide catalyst on the dielectric barrier discharge decomposition of toluene[J].Catalysis Today,2010,153(3-4):176-183.
[2]陈颖.我国工业源VOCs行业排放特征及未来趋势研究[D].广州:华南理工大学2011.
[3]马召坤,刘善军,仇帅,等.山东省汽车喷涂行业VOCs排放特征研究[J].环境保护科学,2016,42(4):133-138.
[4]沈旻嘉,郝吉明,王丽涛.中国加油站VOC排放污染现状及控制[J].环境科学,2006,27(8):1473-1478.
[5]姜能座,DBE超微雾化吸收法结合纳米技术治理VOCs 的技术研究[J].现代化工,2013,25(6):112-116.
[6]吴芳.滑动弧放电催化协同降解有机污染物的实验研究[D].杭州:浙江大学2008.
[7]CHEN H L,LEE H M,CHEN S H,et al.Removal of volatile organic compounds by single-stage and two-stage plasma catalysis systems:a review of the performance enhancement mechanisms,current status,and suitable applications[J].Environmental Science and Technology,2009,43(7):2216-2227.
[8]YIN Y G,XU W Q,DEGUZMAN R,et al.Studies of stability and reactivity of synthetic cryptomelane-like manganese oxide octahedral molecular sieves[J].Inorganic Chemistry,1994,33 (19):4384-4389.
[9]凌飞,邓丽杰,陈平,等.氧化锰八面体分子筛的合成、表征及其催化燃烧性能[J].浙江大学学报(理学版),2011,38(1):73-77.
[10]刘冀锴,安太成,曾祥英,等.含钛介孔光催化剂的制备研究进展[J].材料导报,2007,21(6):124-129.
[11]HERNANDEZ W,CENTENO M,ROMERO-SARRIA F,et al.Modified cryptomelane-type manganese dioxide nanomaterials for preferential oxidation of CO in the presence of hydrogen[J].Catalysis Today,2010,157(1):160-165.
[12]XU R,WANG X,WANG D,et al.Surface structure effects in nanocrystal MnO2 and Ag/MnO2 catalytic oxidation of CO[J].Journal of Catalysis,2006,237(2):426-430.
[13]KIM S C,SHIM W G.Catalytic combustion of VOCs over a series of manganese oxide catalysts[J].Applied Catalysis B:Environmental,2010,98(3-4):180-185.
[14]LI W,GIBBS G V,OYAMA S T.Mechanism of ozone decomposition on a manganese oxide catalyst.1.in situ raman spectroscopy and Ab initio molecular orbital calculations[J].Journal of the American Chemical Society,1998,120(35):9041-9046.
[15]EINAHA H,HARADA M,FUTAMURA S.Structural changes in alumina-supported manganese oxides during ozone decomposition[J].Chemical Physics Letters,2005,408(4-6):377-380.
[16]GUO Y,LIAO X,HE J,et al.Effect of manganese oxide catalyst on the dielectric barrier discharge decomposition of toluene[J].Catalysis Today,2010,153(3-4):176-183.
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