Ni-Zn/玄武岩催化剂生物质催化气化实验
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摘要
采用一步水热法原位合成工艺制备了Ni-Zn/玄武岩复合催化剂,对催化剂微观形貌和表面元素分布进行了表征。以松木颗粒为原料、水蒸气为气化剂,采用下吸式管式气化炉实验平台,研究了Ni-Zn/玄武岩复合材料在不同温度下高温蒸汽的催化气化效果,通过考察气体组分变化,探讨Ni-Zn/玄武岩复合催化剂催化性能随温度变化的规律,并与无催化剂和以白云石为催化剂的催化性能进行实验对比。实验结果表明:水热反应温度为130℃,反应时间为12 h时,Ni、Zn能很好地负载在玄武岩纤维表面;与不加催化剂和加入白云石催化剂相比,Ni-Zn/玄武岩复合催化剂气化温度在950℃时催化效率明显提升,氢气体积分数增加明显,分别由无催化剂时的58. 6%、加入白云石催化剂时的50. 02%升高至63. 28%。
The Ni-Zn/basalt composite catalyst was prepared by the method of in-situ hydrothermal. The microstructure and surface element distribution of the catalyst was characterized. Taking the pine particles as raw materials and water vapor as the gasification agent,and the test system platform of the lower suction tubular gasifier was adopted. Ni-Zn/basalt composite material was studied at different temperatures of high temperature steam catalytic gasification effect. Through investigating the changes in gas composition,the variation laws of the catalytic properties of Ni-Zn/basalt composite catalyst with temperature variation were studied. The result was compared with the contrast experiments with no catalyst and dolomite as catalyst performance. The experimental results showed that Ni and Zn could be well supported on the surface of basalt fiber with the reaction temperature of 130℃ and the reaction time of 12 h. Compared with no catalyst and adding dolomite catalyst,Ni-Zn/basalt composite catalyst gasification temperature at 950℃,the catalytic efficiency was improved significantly and the hydrogen volume fraction was significantly increased. The hydrogen volume fraction was increased to 63. 28% while without catalyst,the hydrogen volume fraction was only 58. 6% and with dolomite catalyst,the hydrogen volume fraction was 50. 02%. It can be seen that Ni-Zn/basalt composite catalyst has high efficiency in the catalytic gasification reaction of pine sawdust. It can provide theoretical and experimental basis for further improving biomass gasification technology.
The Ni-Zn/basalt composite catalyst was prepared by the method of in-situ hydrothermal. The microstructure and surface element distribution of the catalyst was characterized. Taking the pine particles as raw materials and water vapor as the gasification agent,and the test system platform of the lower suction tubular gasifier was adopted. Ni-Zn/basalt composite material was studied at different temperatures of high temperature steam catalytic gasification effect. Through investigating the changes in gas composition,the variation laws of the catalytic properties of Ni-Zn/basalt composite catalyst with temperature variation were studied. The result was compared with the contrast experiments with no catalyst and dolomite as catalyst performance. The experimental results showed that Ni and Zn could be well supported on the surface of basalt fiber with the reaction temperature of 130℃ and the reaction time of 12 h. Compared with no catalyst and adding dolomite catalyst,Ni-Zn/basalt composite catalyst gasification temperature at 950℃,the catalytic efficiency was improved significantly and the hydrogen volume fraction was significantly increased. The hydrogen volume fraction was increased to 63. 28% while without catalyst,the hydrogen volume fraction was only 58. 6% and with dolomite catalyst,the hydrogen volume fraction was 50. 02%. It can be seen that Ni-Zn/basalt composite catalyst has high efficiency in the catalytic gasification reaction of pine sawdust. It can provide theoretical and experimental basis for further improving biomass gasification technology.
引文
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[14]汪靖凯,杭美艳,李可庆,等.玄武岩纤维/Ti O2复合材料的制备及表征[J].材料科学与工艺,2017,25(2):79-84.WANG Jingkai,HANG Meiyan,LI Keqing,et al. Preparation and characterization of basalt fibers/Ti O2composite materials[J]. Material Science and Technology,2017,25(2):79-84.(in Chinese)
[15]牛永红,韩枫涛,陈义胜.高温蒸汽松木颗粒富氢气化试验[J].农业工程学报,2016,32(3):247-252.NIU Yonghong,HAN Fengtao,CHEN Yisheng. Experimental study of high-temperature steam gasification of pine particles for hydrogen-rich gas[J]. Transactions of the CSAE,2016,32(3):247-252.(in Chinese)
[16]吕鹏梅,熊祖鸿,王铁军,等.生物质流化床气化制取富氢燃气的研究[J].太阳能学报,2003,24(6):758-764.LUPengmei,XIONG Zuhong,WANG Tiejun,et al. Biomass gasification in a fluidized bed toproduce hydrogen rich gas[J].Acta Energiae Solaris Sinica,2003,24(6):758-764.(in Chinese)
[17]涂军令.木屑/木屑炭高温水蒸气气化制备合成气研究[D].北京:中国林业科学研究院,2012.TU Junling. Production of synthesis gas by high temperature steam gasification of sawdust/sawdust-derived char[D]. Beijing:Chinese Academy of Forestry,2012.(in Chinese)
[18] AYDIN E S,YUCEL O,SADIKOGLU H. Numerical and experimental investigation of hydrogen-rich syngas production via biomass gasification[J]. International Journal of Hydrogen Energy,2018,43(2):1105-1115.
[19] NIPATTUMMAKUL N,AHMED I I,KERDSUWAN S,et al. Hydrogen and syngas production from sewage sludge via steam gasification[J]. International Journal of Hydrogen Energy,2010,35(21):11738-11745.
[20]李琳娜.生物质高温水蒸气气化制备富氢燃气的研究[D].北京:中国林业科学研究院,2011.LI Linna. Preparation of hydrogen rich gas high temperature steam gasification biomass research[D]. Beijing:Chinese Academy of Forestry,2011.(in Chinese)
[21] DEVI L,PTASINSKI K J,JANSSEN F J J G. A review of the primary measures for tar elimination in biomass gasification processes[J]. Biomass&Bioenergy,2003,24(2):125-140.
[22]徐恒泳,孙希贤,范业梅,等.甲烷,二氧化碳转化制合成气的研究:Ⅰ.催化剂及其催化性能[J].石油化工,1992(3):147-153.XU Hengyong,SUN Xixian,FAN Yemei,et al. Studies of reforming methane with carbon dioxide to produce synthesis gas:Ⅰ. catalyst and its catalytic property[J]. Petrochemical Technology,1992(3):147-153.(in Chinese)
[2]阴秀丽,吴创之,徐冰嬿,等.生物质气化对减少CO2排放的作用[J].太阳能学报,2000,21(1):40-44.YIN Xiuli,WU Chuangzhi,XU Bingyan,et al. The effect of biomass gasification on reducing CO2emission[J]. Acta Energiae Solaris Sinica,2000,21(1):40-44.(in Chinese)
[3]周明,许庆利,蓝平,等.生物质制氢研究进展[J].吉林化工学院学报,2009,26(4):35-39.ZHOU Ming,XU Qingli,LAN Ping,et al. Progress inbiomass hydrogen production[J]. Journal of Jilin Institute of Chemical Technology,2009,26(4):35-39.(in Chinese)
[4]俞元元,肖军,沈来宏,等.不同催化剂对生物质半焦低温气化效果的影响[J].农业工程技术(新能源产业),2013,29(2):190-197.YU Yuanyuan,XIAO Jun,SHEN Laihong,et al. Effects of different catalysts on steam gasification of biomass char at low temperature[J]. Agricultural Engineering Technology(New Energy Industry),2013,29(2):190-197.(in Chinese)
[5]裴爱霞,郭烈锦,金辉.超临界水中花生壳气化制氢的实验及机理研究[J].西安交通大学学报,2006,40(11):1263-1267.PEI Aixia,GUO Liejin,JIN Hui. Experimental research on catalysts and their catalytic mechanism for hydrogen production by gasification of peanut shell in supercritical water[J]. Journal of Xi'an Jiaotong University,2006,40(11):1263-1267.(in Chinese)
[6]牛永红,韩枫涛,张雪峰,等.白云石催化松木燃料棒水蒸气气化试验[J/OL].农业机械学报,2016,47(12):246-252.NIU Yonghong,HAN Fengtao,ZHANG Xuefeng,et al. Steam gasification of pine fuel rods catalyzed by dolomite[J/OL].Transactions of the Chinese Society for Agricultural Machinery,2016,47(12):246-252. http:∥www. j-csam. org/jcsam/ch/reader/view_abstract. aspx? flag=1&file_no=20161230&journal_id=jcsam. DOI:10. 6041/j. issn. 1000-1298. 2016. 12. 030.(in Chinese)
[7]谢大幸,肖军,谢玉荣,等.基于生物质稻秸气化的催化剂研究[J].太阳能学报,2011,32(1):8-13.XIE Daxing,XIAO Jun,XIE Yurong,et al. Study on catalysts for rice straw gasification[J]. Acta Energiae Solaris Sinica,2011,32(1):8-13.(in Chinese)
[8]王欣,罗学刚,张盼盼,等.玄武岩催化甲烷裂解制C2烃[J].精细化工,2016,33(10):1099-1104.WANG Xin,LUO Xuegang,ZHANG Panpan,et al. Catalytic pyrolysis of methane to C2hydrocarbons over basalt[J]. Fine Chemicals,2016,33(10):1099-1104.(in Chinese)
[9]汪大千,姚丁丁,杨海平,等. Ni/C催化剂对生物质气化制氢的影响[J].中国电机工程学报,2017,37(19):5682-5687.WANG Daqian,YAO Dingding,YANG Haiping,et al. Influence of Ni/C catalysts in hydrogen production from biomass gasification[J]. Proceedings of the CSEE,2017,37(19):5682-5687.(in Chinese)
[10]边岳,徐宝山,王本水,等.胜利褐煤负载镍生物质气化催化剂实验研究[J].洁净煤技术,2014,20(6):13-18.BIAN Yue,XU Baoshan,WANG Benshui,et al. Preparation of nickel-loaded on Shengli lignite catalysts for catalytic gasification of biomass[J]. Clean Coal Technology,2014,20(6):13-18.(in Chinese)
[11]丁鼎.金属元素在生物质一体化制氢中的催化作用研究[D].上海:华东理工大学,2017.DING Ding. Study on the effect of metal elements with integrated process for hydrogen production[D]. Shanghai:East China University of Science and Technology,2017.(in Chinese)
[12] XUE A J,PAN J H,TIAN M C,et al. Experimental study on catalytic pyrolysis of biomass pellet[J]. Applied Mechanics and Materials,2013,291-294:320-323.
[13] ZHAO B F,ZHANG X D,CHEN L,et al. High quality fuel gas from biomass pyrolysis with calcium oxide[J]. Bioresource Technology,2014,156:78-83.
[14]汪靖凯,杭美艳,李可庆,等.玄武岩纤维/Ti O2复合材料的制备及表征[J].材料科学与工艺,2017,25(2):79-84.WANG Jingkai,HANG Meiyan,LI Keqing,et al. Preparation and characterization of basalt fibers/Ti O2composite materials[J]. Material Science and Technology,2017,25(2):79-84.(in Chinese)
[15]牛永红,韩枫涛,陈义胜.高温蒸汽松木颗粒富氢气化试验[J].农业工程学报,2016,32(3):247-252.NIU Yonghong,HAN Fengtao,CHEN Yisheng. Experimental study of high-temperature steam gasification of pine particles for hydrogen-rich gas[J]. Transactions of the CSAE,2016,32(3):247-252.(in Chinese)
[16]吕鹏梅,熊祖鸿,王铁军,等.生物质流化床气化制取富氢燃气的研究[J].太阳能学报,2003,24(6):758-764.LUPengmei,XIONG Zuhong,WANG Tiejun,et al. Biomass gasification in a fluidized bed toproduce hydrogen rich gas[J].Acta Energiae Solaris Sinica,2003,24(6):758-764.(in Chinese)
[17]涂军令.木屑/木屑炭高温水蒸气气化制备合成气研究[D].北京:中国林业科学研究院,2012.TU Junling. Production of synthesis gas by high temperature steam gasification of sawdust/sawdust-derived char[D]. Beijing:Chinese Academy of Forestry,2012.(in Chinese)
[18] AYDIN E S,YUCEL O,SADIKOGLU H. Numerical and experimental investigation of hydrogen-rich syngas production via biomass gasification[J]. International Journal of Hydrogen Energy,2018,43(2):1105-1115.
[19] NIPATTUMMAKUL N,AHMED I I,KERDSUWAN S,et al. Hydrogen and syngas production from sewage sludge via steam gasification[J]. International Journal of Hydrogen Energy,2010,35(21):11738-11745.
[20]李琳娜.生物质高温水蒸气气化制备富氢燃气的研究[D].北京:中国林业科学研究院,2011.LI Linna. Preparation of hydrogen rich gas high temperature steam gasification biomass research[D]. Beijing:Chinese Academy of Forestry,2011.(in Chinese)
[21] DEVI L,PTASINSKI K J,JANSSEN F J J G. A review of the primary measures for tar elimination in biomass gasification processes[J]. Biomass&Bioenergy,2003,24(2):125-140.
[22]徐恒泳,孙希贤,范业梅,等.甲烷,二氧化碳转化制合成气的研究:Ⅰ.催化剂及其催化性能[J].石油化工,1992(3):147-153.XU Hengyong,SUN Xixian,FAN Yemei,et al. Studies of reforming methane with carbon dioxide to produce synthesis gas:Ⅰ. catalyst and its catalytic property[J]. Petrochemical Technology,1992(3):147-153.(in Chinese)
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