煤矸石微波辅助合成沸石分子筛的研究
|
摘要
为探究煤矸石合成沸石分子筛的最优工艺,以煤矸石为主要原料,采用传统水浴加热与微波辅助加热的方法,合成4A型沸石分子筛与P型沸石分子筛,利用电子显微镜和X射线衍射,对其形貌和结构进行分析表征。实验通过制备相同的沸石分子筛,得出制备沸石分子筛的煤矸石需要高岭石含量较高、有害杂质含量较低及较为合适的粒径(3μm～50μm)。相较于传统水浴加热,微波辅助加热得到的沸石分子筛纯度低,但加热时间仅需30 min～40 min,而传统水浴加热合成需要24 h,同时微波辅助加热还提高了沸石分子筛反应速率和分散度。
In order to explore the optimal process for the synthesis of zeolite molecular sieve from coal gangue,with coal gangue as the main raw material,4 A zeolite molecular sieve and P zeolite molecular sieve were synthesized by the traditional water bath heating method and the microwave-assisted heating method.The morphology and structure were characterized by electron microscopy and X-ray diffraction.By preparing the same zeolite molecular sieve,it was concluded that coal gangue prepared for the zeolite molecular sieve required higher kaolinite content,lower harmful impurity content,and suitable particle size(3 μm-50 μm).Compared with the traditional water bath heating method,the microwave-assisted heating method of the zeolite molecular sieve was low in purity,but the microwave-assisted heating time was very short,only about 30 min-40 min,while the traditional water bath heating synthesis took 24 h.At the same time,the reaction rate and dispersion of the zeolite molecular sieve were also improved.
In order to explore the optimal process for the synthesis of zeolite molecular sieve from coal gangue,with coal gangue as the main raw material,4 A zeolite molecular sieve and P zeolite molecular sieve were synthesized by the traditional water bath heating method and the microwave-assisted heating method.The morphology and structure were characterized by electron microscopy and X-ray diffraction.By preparing the same zeolite molecular sieve,it was concluded that coal gangue prepared for the zeolite molecular sieve required higher kaolinite content,lower harmful impurity content,and suitable particle size(3 μm-50 μm).Compared with the traditional water bath heating method,the microwave-assisted heating method of the zeolite molecular sieve was low in purity,but the microwave-assisted heating time was very short,only about 30 min-40 min,while the traditional water bath heating synthesis took 24 h.At the same time,the reaction rate and dispersion of the zeolite molecular sieve were also improved.
引文
[1]刘思琴,陈政江,槐苑楠,等.粉煤灰和煤矸石合成沸石分子筛的研究进展[J].煤化工,2015,43(4):43-47.LIU S Q,CHEN Z J,HUAI Y N,et al.Research Progress on Synthesis of Zeolite Molecular Sieves from Coal Fly Ash and Coal Refuse[J].Coal Chemical Industry,2015,43(4):43-47.
[2]孔德顺,李志,艾德春,等.高铁高砂煤矸石合成4A沸石分子筛[J].光谱实验室,2011,28(2):787-791.KONG D S,LI Z,AI D C,et al.Synthesis of 4A Zeolites Molecular Sieve from Coal Gangue with High Contents of Iron and Silica[J].Chinese Journal of Spectroscopy Laboratory,2011,28(2):787-791.
[3]李平,马平,田红丽,等.高铝煤矸石合成4A分子筛研究[J].石油化工应用,2014,33(3):89-91.LI P,MA P,TIAN H L,et al.Synthesis of 4A-Zeolite from Coal Gangue with High Silica[J].Petrochemical Industry Application,2014,33(3):89-91.
[4]陈建龙.煤矸石合成NaA和NaX型分子筛及其对重金属废水的吸附研究[D].西安:陕西师范大学,2014.
[5]朱明,金国林.煤矸石合成NaX分子筛的研究[J].化学世界,2003,44(1):8-10.ZHU M,JIN G L.Synthesis of Zeolite NaX from Coal Gangue[J].Chemical World,2003,44(1):8-10.
[6]QIAN T T,LI J H.Synthesis of Na-A Zeolite from Coal Gangue with the In-situ Crystallization Technique[J].Advanced Powder Technology,2015,26(1):98-104.
[7]李萍,杨效益,赵慧贤,等.煤矸石加碱熔融法制备亚微米4A沸石[J].石油化工,2010,39(10):1 162-1 165.LI P,YANG X Y,ZHAO H X,et al.Prepration of Submicron 4A Zeolite from Coal Gangue by Alkali-Melting Method[J].Petrochemical Technology,2010,39(10):1 162-1 165.
[8]晋晓彤.煤矸石和粉煤灰制备分子筛的研究[D].武汉:武汉工程大学,2016.
[9]岳虎,郁钟铭,任青山.煤矸石制备PAFS与P型分子筛的实验研究[J].煤炭技术,2017,36(9):318-320.YUE H,YU Z M,REN Q S.Study of PAFS and P Zeolite Prepared by Coal Gangue[J].Coal Technology,2017,36(9):318-320.
[10]腾庭庭,卢新卫.以煤矸石为原料合成Y型沸石及其吸附性能的探究[J].合成化学,2017,25(9):763-768.TENG T T,LU X W.Synthesis and Adsorption Perfor mance of Mesoporous Zeolite-Y[J].Chinese Journal of Synthetic Chemistry,2017,25(9):763-768.
[11]于存贞,王延玲,常升.以煤矸石为原料固体-蒸汽相转化合成4A型沸石[J].轻金属,2011(8):15-18.YU C Z,WANG Y L,CHANG S.Synthesis of 4A Zeolite with Solid-vapor Phase Inversion Process with Coal Gangue as Material[J].Light Metals,2011(8):15-18.
[12]INADA M,TSUJIMOTO H,EGUCHI Y,et al.Microwaveassisted Zeolite Synthesis from Coal Fly Ash in Hydrothermal Process[J].Fuel,2005,84(12-13):1 482-1 486.
[13]郭永龙,王焰新,蔡鹤生,等.水热条件下利用微波加热从粉煤灰合成沸石研究[J].地球科学:中国地质大学学报,2003,28(5):517-521.GUO Y L,WANG Y X,CAI H S,et al.Synthesis of Zeolites from Fly Ash by Microwave Assisted Hydrothermal Alkaline Activation[J].Earth Science(Journal of China University of Geosciences),2003,28(5):517-521.
[14]CARDOSOA A M,HORNB M B,FERRETC L S,et al.Integrated Synthesis of Zeolites 4A and Na-P1 Using Coal Fly Ash for Application in the Formulation of Detergents and Swine Wastewater Treatment[J].Journal of Hazardous Materials,2015,287:69-77.
[15]JIANG Z Q,YANG J,MA H W,et al.Reaction Behaviour of Al2O3and SiO2in High Alumina Coal Fly Ash During Alkali Hydrothermal Process[J].Trans Nonferrous Met Soc China,2015,25(6):2 065-2 072.
[16]陈彦广,徐婷婷,韩洪晶,等.粉煤灰微波-水热合成法制备分子筛的研究进展[J].化工进展,2015,34(8):2 922-2 923.CHEN Y G,XU T T,HAN H J,et al.Research Development of Zeolites Preparation from Coal Fly Ash by Microwave-hydrothermal Synthesis[J].Chemical Industry and Engineering Progress,2015,34(8):2 922-2 923.
[2]孔德顺,李志,艾德春,等.高铁高砂煤矸石合成4A沸石分子筛[J].光谱实验室,2011,28(2):787-791.KONG D S,LI Z,AI D C,et al.Synthesis of 4A Zeolites Molecular Sieve from Coal Gangue with High Contents of Iron and Silica[J].Chinese Journal of Spectroscopy Laboratory,2011,28(2):787-791.
[3]李平,马平,田红丽,等.高铝煤矸石合成4A分子筛研究[J].石油化工应用,2014,33(3):89-91.LI P,MA P,TIAN H L,et al.Synthesis of 4A-Zeolite from Coal Gangue with High Silica[J].Petrochemical Industry Application,2014,33(3):89-91.
[4]陈建龙.煤矸石合成NaA和NaX型分子筛及其对重金属废水的吸附研究[D].西安:陕西师范大学,2014.
[5]朱明,金国林.煤矸石合成NaX分子筛的研究[J].化学世界,2003,44(1):8-10.ZHU M,JIN G L.Synthesis of Zeolite NaX from Coal Gangue[J].Chemical World,2003,44(1):8-10.
[6]QIAN T T,LI J H.Synthesis of Na-A Zeolite from Coal Gangue with the In-situ Crystallization Technique[J].Advanced Powder Technology,2015,26(1):98-104.
[7]李萍,杨效益,赵慧贤,等.煤矸石加碱熔融法制备亚微米4A沸石[J].石油化工,2010,39(10):1 162-1 165.LI P,YANG X Y,ZHAO H X,et al.Prepration of Submicron 4A Zeolite from Coal Gangue by Alkali-Melting Method[J].Petrochemical Technology,2010,39(10):1 162-1 165.
[8]晋晓彤.煤矸石和粉煤灰制备分子筛的研究[D].武汉:武汉工程大学,2016.
[9]岳虎,郁钟铭,任青山.煤矸石制备PAFS与P型分子筛的实验研究[J].煤炭技术,2017,36(9):318-320.YUE H,YU Z M,REN Q S.Study of PAFS and P Zeolite Prepared by Coal Gangue[J].Coal Technology,2017,36(9):318-320.
[10]腾庭庭,卢新卫.以煤矸石为原料合成Y型沸石及其吸附性能的探究[J].合成化学,2017,25(9):763-768.TENG T T,LU X W.Synthesis and Adsorption Perfor mance of Mesoporous Zeolite-Y[J].Chinese Journal of Synthetic Chemistry,2017,25(9):763-768.
[11]于存贞,王延玲,常升.以煤矸石为原料固体-蒸汽相转化合成4A型沸石[J].轻金属,2011(8):15-18.YU C Z,WANG Y L,CHANG S.Synthesis of 4A Zeolite with Solid-vapor Phase Inversion Process with Coal Gangue as Material[J].Light Metals,2011(8):15-18.
[12]INADA M,TSUJIMOTO H,EGUCHI Y,et al.Microwaveassisted Zeolite Synthesis from Coal Fly Ash in Hydrothermal Process[J].Fuel,2005,84(12-13):1 482-1 486.
[13]郭永龙,王焰新,蔡鹤生,等.水热条件下利用微波加热从粉煤灰合成沸石研究[J].地球科学:中国地质大学学报,2003,28(5):517-521.GUO Y L,WANG Y X,CAI H S,et al.Synthesis of Zeolites from Fly Ash by Microwave Assisted Hydrothermal Alkaline Activation[J].Earth Science(Journal of China University of Geosciences),2003,28(5):517-521.
[14]CARDOSOA A M,HORNB M B,FERRETC L S,et al.Integrated Synthesis of Zeolites 4A and Na-P1 Using Coal Fly Ash for Application in the Formulation of Detergents and Swine Wastewater Treatment[J].Journal of Hazardous Materials,2015,287:69-77.
[15]JIANG Z Q,YANG J,MA H W,et al.Reaction Behaviour of Al2O3and SiO2in High Alumina Coal Fly Ash During Alkali Hydrothermal Process[J].Trans Nonferrous Met Soc China,2015,25(6):2 065-2 072.
[16]陈彦广,徐婷婷,韩洪晶,等.粉煤灰微波-水热合成法制备分子筛的研究进展[J].化工进展,2015,34(8):2 922-2 923.CHEN Y G,XU T T,HAN H J,et al.Research Development of Zeolites Preparation from Coal Fly Ash by Microwave-hydrothermal Synthesis[J].Chemical Industry and Engineering Progress,2015,34(8):2 922-2 923.