微波辐照再生活性半焦工艺
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摘要
以甲基橙为吸附质,针对吸附后的活性半焦,利用微波辐照对其进行再生。在不同微波功率和辐照时间下研究活性半焦的再生率和碳损耗率,利用扫描电子显微镜观察半焦的表面形貌,采用氮气吸附仪测定半焦的平均孔径和比表面积。结果表明,微波可以有效脱除活性半焦表面的甲基橙,由于反应器的特殊尺寸,未通气氛条件下活性半焦的再生率较通入氮气条件下活性半焦的再生率高。对于不同甲基橙吸附量的活性半焦,当微波辐照时间为30s时,再生率可保持在98%～99%。过高的微波功率及过长的辐照时间均会增加半焦的碳损耗率,导致再生率增幅缓慢,甚至下降。孔径结构分析表明,微波辐照过程可以优化半焦的孔隙结构。
Based on the methyl orange employed as adsorbate,the activated semi-coke after adsorption was regenerated through microwave irradiation.The regeneration rate and carbon loss rate of activated semi-coke were investigated under the reaction conditions of different microwave powers and irradiation time,the surface appearance was investigated by SEM,and the BET surface area and pore size distribution were analyzed by N_2 adsorption.The results show that the methyl orange can be removed effectively,and the regeneration rate of activated semicoke without the atmosphere of nitrogen is higher than that of activated semi-coke in the atmosphere of nitrogen due to the special size of reactor.Then whatever the adsorbed amounts of activated semi-coke are,the regeneration rate of activated semi-coke can maintain at 98%-99% under the regeneration time of 30 s,and excessive microwave power and inordinately long irradiation time can promote the carbon loss of activated semi-coke,which leads to slow increase of regeneration rate and even decline.In addition,the pore structure can be optimized in microwave irradiation process.
Based on the methyl orange employed as adsorbate,the activated semi-coke after adsorption was regenerated through microwave irradiation.The regeneration rate and carbon loss rate of activated semi-coke were investigated under the reaction conditions of different microwave powers and irradiation time,the surface appearance was investigated by SEM,and the BET surface area and pore size distribution were analyzed by N_2 adsorption.The results show that the methyl orange can be removed effectively,and the regeneration rate of activated semicoke without the atmosphere of nitrogen is higher than that of activated semi-coke in the atmosphere of nitrogen due to the special size of reactor.Then whatever the adsorbed amounts of activated semi-coke are,the regeneration rate of activated semi-coke can maintain at 98%-99% under the regeneration time of 30 s,and excessive microwave power and inordinately long irradiation time can promote the carbon loss of activated semi-coke,which leads to slow increase of regeneration rate and even decline.In addition,the pore structure can be optimized in microwave irradiation process.
引文
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[15]SUN Yanlong,ZHANG Bo,ZHENG Tong,et al.Regeneration of Activated Carbon Saturated with Chloramphenicol by Microwave and Ultraviolet Irradiation[J].Chemical Engineering Journal,2017,320:264-270.
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[19]赵彦博.准东煤微波热解特性的初步实验研究[D].哈尔滨:哈尔滨工业大学,2014.ZHAO Yanbo.Preliminary Experiment Research on Microwave Pyrolysis of Zhundong Coal[D].Harbin:Harbin Institute of Technology,2014.
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[21]姜贤刚,刘洁,冯莉,等.热解温度和脱灰处理对褐煤半焦孔结构的影响及分形分析[J].煤炭转化,2018,41(3):19-26.JIANG Xian’gang,LIU Jie,FENG Li,et al.Effects of Pyrolysis Temperature and De-ashing Treatment on Pore Structure of Lignite Semi-coke and Its Fractal Analysis[J].Coal Conversion,2018,41(3):19-26.
[22]陈红英,谢浩,熊梦瑶,等.Fenton-微波法再生载活性艳红活性炭的研究[J].浙江工业大学学报,2018,46(4):429-434.CHEN Hongying,XIE Hao,XIONG Mengyao,et al.Study on Regeneration of Reactive Brilliant Red Exhausted Activated Carbon by Fenton-microwave[J].Journal of Zhejiang University of Technology,2018,46(4):429-434.
[23]牛志睿,董为民.微波辐照活性碳纤维损耗性能的研究[J].山西建筑,2008,34(3):188-189.NIU Zhirui,DONG Weimin.Research on the Loss Function of Activated Carbon Fiber in Microwave Irradiation[J].Shanxi Architecture,2008,34(3):188-189.
[24]张群.微波对活性炭的改性及再生研究[D].杭州:浙江大学,2006.ZHANG Qun.Study on Modification and Regeneration of Activated Carbon by Microwave[D].Zhejiang:Zhejiang University,2006.
[2]张华伟,陈江艳,赵可,等.Mn/Ce掺杂改性半焦对模拟煤气中单质汞的脱除性能研究[J].燃料化学学报,2016,44(4):394-400.ZHANG Huawei,CHEN Jiangyan,ZHAO Ke,et al.Removal of Vapor-phase Elemental Mercury from Simulated Syngas Using Semi-coke Modified by Mn/Ce Doping[J].Journal of Fuel Chemistry and Technology,2016,44(4):394-400.
[3]刘静,杜美利.高吸附性活性半焦的制备工艺研究[J].化工新型材料,2014,42(11):82-84.LIU Jing,DU Meili.Study on Preparation Technology of High Absorption Activated Semicoke[J].New Chemical Materials,2014,42(11):82-84.
[4]LABUS K,GRYGLEWICZ S,MACHNIKOWSKI J.Granular KOH-activated Carbons from Coal-based Cokes and Their CO2Adsorption Capacity[J].Fuel,2014,118(2):9-15.
[5]CHEN Yan,ZHANG Xiangmei,LIU Qianyi,et al.Facile and Economical Synthesis of Porous Activated Semi-cokes for Highly Efficient and Fast Removal of Microcystin-LR[J].Journal of Hazardous Materials,2015,299:325-332.
[6]王力,陈继涛,张华伟,等.改性褐煤半焦的表面性质及对气态HgO的吸附特性[J].环境科学研究,2014,27(8):820-826.WANG Li,CHEN Jitao,ZHANG Huawei,et al.Study on Surface Properties and Adsorption Performance of Modified Semicoke for Gas-phase HgO[J].Research of Environmental Sciences,2014,27(8):820-826.
[7]杨勇贵.活化半焦吸附处理焦化废水性能研究[D].太原:太原理工大学,2013.YANG Yonggui.Adsorption Treatment of Coking Wastewater by Activated Seml-coke[D].Taiyuan:Taiyuan University of Technology,2013.
[8]DING Song,LI Yuran,ZHU Tingyu,et al.Regeneration Performance and Carbon Consumption of Semi-coke and Activated Coke for SO2and NO Removal[J].Journal of Environmental Sciences,2015,34(8):37-43.
[9]MI Jie,YU Meng,YUAN Fenyun,et al.Regeneration Characteristics and Kinetics of Modified Semi-coke Supported(Fe,Zn,Ce)Desulfurization Sorbents[J].Energy and Fuels,2012,26(11):6551-6558.
[10]张肖阳.Zn-Mn-Cu半焦吸附剂的超声辅助加压浸渍法制备及其脱硫与再生性能的研究[D].太原:太原理工大学,2015.ZHANG Xiaoyang.Researches on Zn-Mn-Cu Sorbent Loaded on Semi-coke Prepared by Ultrasound-assisted High-pressure Impregnation Method and Its Desulfurization and Regeneration[D].Taiyuan:Taiyuan University of Technology,2015.
[11]于英民,郭瑞莉,李春虎.半焦吸附剂烟气脱硫脱硝性能[J].燃料化学学报,2011,39(5):385-389.YU Yingmin,GUO Ruili,LI Chunhu.Flue Gas Desulfurization and Denitrification Performance of the Semi-coke Adsorbents[J].Journal of Fuel Chemistry and Technology,2011,39(5):385-389.
[12]张伟.活性半焦烟气脱硫动力学与再生工艺的研究与设计[D].青岛:中国海洋大学,2007.ZHANG Wei.The Study on the Kinetics and Regeneration for FGD by Using Modified Semi-coke[D].Qingdao:Ocean University of China,2007.
[13]张立强,崔琳,王志强,等.微波再生对活性炭循环吸附SO2的影响[J].燃料化学学报,2014,42(7):890-895.ZHANG Liqiang,CUI Lin,WANG Zhiqiang,et al.Effects of Microwave Regeneration of Activated Carbon on Its SO2Adsorption[J].Journal of Fuel Chemistry and Technology,2014,42(7):890-895.
[14]王晴东.基于多物理场的褐煤微波热解制气特性及机理研究[D].武汉:武汉科技大学,2016.WANG Qingdong.Microwave Pyrolysis Gasification Characteristics and Mechanism Study of Lignite Based on the Multiphysics Field[D].Wuhan:Wuhan University of Science and Technology,2016.
[15]SUN Yanlong,ZHANG Bo,ZHENG Tong,et al.Regeneration of Activated Carbon Saturated with Chloramphenicol by Microwave and Ultraviolet Irradiation[J].Chemical Engineering Journal,2017,320:264-270.
[16]CUI Chunyue,ZHENG Qingzhu,HAN Yanhe,et al.Rapid Microwave-assisted Regeneration of Magnetic Carbon Nanotubes Loaded with p-nitrophenol[J].Applied Surface Science,2015,346:99-106.
[17]MAO Haiyan,ZHOU Dingguo,HASHISHO Z,et al.Constant Power and Constant Temperature Microwave Regeneration of Toluene and Acetone Loaded on Microporous Activated Carbon from Agricultural Residue[J].Journal of Industrial and Engineering Chemistry,2015,21(1):516-525.
[18]NOR N M,SUKRI M F F,MOHAMED A R.Development of High Porosity Structures of Activated Carbon via Microwaveassisted Regeneration for H2S Removal[J].Journal of Environmental Chemical Engineering,2016,4(4):4839-4845.
[19]赵彦博.准东煤微波热解特性的初步实验研究[D].哈尔滨:哈尔滨工业大学,2014.ZHAO Yanbo.Preliminary Experiment Research on Microwave Pyrolysis of Zhundong Coal[D].Harbin:Harbin Institute of Technology,2014.
[20]何秋香,陈祖亮.柚子皮制备生物炭吸附苯酚的特性和动力学[J].环境工程学报,2014,8(9):3853-3859.HE Qiuxiang,CHEN Zuliang.Characterization and Kinetics of Biochar Prepared from Pomelo Peel for Adsorption of Phenol[J].Chinese Journal of Environmental Engineering,2014,8(9):3853-3859.
[21]姜贤刚,刘洁,冯莉,等.热解温度和脱灰处理对褐煤半焦孔结构的影响及分形分析[J].煤炭转化,2018,41(3):19-26.JIANG Xian’gang,LIU Jie,FENG Li,et al.Effects of Pyrolysis Temperature and De-ashing Treatment on Pore Structure of Lignite Semi-coke and Its Fractal Analysis[J].Coal Conversion,2018,41(3):19-26.
[22]陈红英,谢浩,熊梦瑶,等.Fenton-微波法再生载活性艳红活性炭的研究[J].浙江工业大学学报,2018,46(4):429-434.CHEN Hongying,XIE Hao,XIONG Mengyao,et al.Study on Regeneration of Reactive Brilliant Red Exhausted Activated Carbon by Fenton-microwave[J].Journal of Zhejiang University of Technology,2018,46(4):429-434.
[23]牛志睿,董为民.微波辐照活性碳纤维损耗性能的研究[J].山西建筑,2008,34(3):188-189.NIU Zhirui,DONG Weimin.Research on the Loss Function of Activated Carbon Fiber in Microwave Irradiation[J].Shanxi Architecture,2008,34(3):188-189.
[24]张群.微波对活性炭的改性及再生研究[D].杭州:浙江大学,2006.ZHANG Qun.Study on Modification and Regeneration of Activated Carbon by Microwave[D].Zhejiang:Zhejiang University,2006.