不同吸附条件下生物炭的汞吸附特性研究
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摘要
为了获得汞初始浓度、吸附温度以及气氛(O_2、CO_2、SO_2浓度)等不同吸附条件下生物炭的汞吸附特性,对等温和非等温条件下制备的核桃壳生物炭(分别记为WS_(iso)和WS_(var))进行了研究,并利用比表面积和孔隙度分析仪、傅立叶变换红外光谱仪表征生物炭的孔隙结构和表面官能团等微观特性,探究其影响机理。结果表明:WS_(iso)和WS_(var)孔隙结构及表面化学性质不同,其中WS_(iso)的累积孔体积较大,为0.130 8cm~3/g,WS_(var)的含氧表面官能团数量和种类较多;在相同吸附条件下,WS_(iso)的汞吸附效果整体上优于WS_(var);汞初始浓度、CO_2和O_2浓度的升高会对生物炭汞吸附性能起到促进作用;随着吸附温度和SO_2浓度的升高,生物炭的吸附性能有所下降。
In order to obtain the mercury adsorption characteristics of biochar under different adsorption conditions including initial mercury concentration,adsorption temperature and gas components(concentration of O_2,CO_2and SO_2),the biochar of walnut shells with isothermal(WS_(iso))and variable temperature(WS_(var))preparation conditions were studied.The pore structures and surface functional groups were characterized by specific surface area and porosity analyzer and Fourier transform infrared spectroscopy,and the influence mechanism was investigated.Results showed that the pore structures and surface chemical properties of WS_(iso )and WS_(var )were different.The cumulative pore volume of WS_(iso )was larger,which was 0.130 8cm~3/g.WS_(var)had more oxygen-containing surface functional groups.In the same adsorption condition,the adsorption characteristics of WS_(iso)were better in general.The mercury adsorption ability of biochar increased along with CO_2,O_2and initial mercury concentration.The mercury adsorption ability of biochar decreased with the increase of adsorption temperature and SO_2concentration.
In order to obtain the mercury adsorption characteristics of biochar under different adsorption conditions including initial mercury concentration,adsorption temperature and gas components(concentration of O_2,CO_2and SO_2),the biochar of walnut shells with isothermal(WS_(iso))and variable temperature(WS_(var))preparation conditions were studied.The pore structures and surface functional groups were characterized by specific surface area and porosity analyzer and Fourier transform infrared spectroscopy,and the influence mechanism was investigated.Results showed that the pore structures and surface chemical properties of WS_(iso )and WS_(var )were different.The cumulative pore volume of WS_(iso )was larger,which was 0.130 8cm~3/g.WS_(var)had more oxygen-containing surface functional groups.In the same adsorption condition,the adsorption characteristics of WS_(iso)were better in general.The mercury adsorption ability of biochar increased along with CO_2,O_2and initial mercury concentration.The mercury adsorption ability of biochar decreased with the increase of adsorption temperature and SO_2concentration.
引文
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[27]PRESTO A A,GRANITE E J.Survey of catalysts for oxidation of mercury in flue gas[J].Environmental Science&Technology,2006,40(18):5601-5609.
[28]LIU Y S.Impact of sulfur oxides on mercury capture by activated carbon[J].Environmental Science&Technology,2008,42(3):970-971.
[29]LI Y H,LEE C W,GULLETT B K.The effect of activated carbon surface moisture on low temperature mercury adsorption[J].Carbon,2002,40(1):65-72.
[30]YIN G,LIU Z,LIU Q,et al.The role of different properties of activated carbon in CO2adsorption[J].Chemical Engineering Journal,2013,230(16):133-140.
[2]SYVERSEN T,KAUR P.The toxicology of mercury and its compounds[J].Journal of Trace Elements in Medicine&Biology,2012,26(4):215-226.
[3]CHEN C X,ZHENG B H,JIANG X,et al.Spatial distribution and pollution assessment of mercury in sediments of Lake Taihu,China[J].Journal of Environmental Sciences,2013,25(2):316-325.
[4]修光利,张艳艳,蔡姬,等.大气颗粒物中汞的赋存形态及其依存条件[J].环境科学研究,2013,26(8):807-813.
[5]王亚杰,朱云,王龙.中国区大气汞污染模型模拟初探[J].环境科学研究,2010,23(10):1250-1256.
[6]杨建平,赵永椿,张军营,等.燃煤电站飞灰对汞的氧化和捕获的研究进展[J].动力工程学报,2014,34(5):337-345.
[7]张成,杨永奎,王定勇.重庆大气汞人为排放及其预测[J].环境科学研究,2011,24(8):904-908.
[8]GB 13223-2011,火电厂大气污染物排放标准[S].
[9]PUDASAINEE D,KIM J H,SEO Y C.Mercury emission trend influenced by stringent air pollutants regulation for coal-fired power plants in Korea[J].Atmospheric Environment,2009,43(39):6254-6259.
[10]DABROWSKI J M,ASHTON P J,MURRAY K,et al.Anthropogenic mercury emissions in South Africa:coal combustion in power plants[J].Atmospheric Environment,2008,42(27):6620-6626.
[11]高炜,支国瑞,薛志钢,等.1980-2007年我国燃煤大气汞、铅、砷排放趋势分析[J].环境科学研究,2013,26(8):822-828.
[12]支国瑞,薛志钢,李洋,等.基于国内实测燃煤电厂烟气汞排放估算的不确定度[J].环境科学研究,2013,26(8):814-821.
[13]LIBERTI L,NOTARNICOLA M,AMICARELLI V,et al.Mercury removal with powdered activated carbon from flue gases at the Coriano municipal solid waste incineration plant[J].Waste Management&Research,1998,16(2):183-189.
[14]GRAYDON J W,ZHANG X,KIRK D W,et al.Sorption and stability of mercury on activated carbon for emission control[J].Journal of Hazardous Materials,2009,168(2/3):978-982.
[15]GUO X,ZHENG C G,XU M.Characterization of mercury emissions from a coal-fired power plant[J].Energy&Fuels,2007,21(2):898-902.
[16]董长青,胡笑颖,杨勇平,等.生物质气再燃减少流化床N2O排放的实验研究[J].燃料化学学报,2010,38(2):236-241.
[17]高洪亮,周劲松,骆仲泱,等.燃煤烟气中汞在活性炭上的吸附特性[J].煤炭科学技术,2006,34(5):49-52.
[18]LIU W,VIDIC R D,BROWN T D,et al.Optimization of sulfur impregnation protocol for fixed-bed application of activated carbon-based sorbents for gas-phase mercury removal[J].Environmental Science&Technology,1998,32(4):531-538.
[19]任建莉,陈俊杰,罗誉娅,等.活性炭纤维脱除烟气中气态汞的试验研究[J].中国电机工程学报,2010,30(5):28-34.
[20]王军辉.活性炭吸附脱除燃煤烟气中汞的研究[D].杭州:浙江大学,2006.
[21]JARBSKI A B,LORENC J,ARISTOV Y I,et al.Porous texture characteristics of a homologous series of base-catalyzed silica aerogels[J].Journal of Non-Crystalline Solids,1995,190(3):198-205.
[22]OLSON E S,MILLER S J,SHARMA R K,et al.Catalytic effects of carbon sorbents for mercury capture[J].Journal of Hazardous Materials,2000,74(1/2):61-79.
[23]DIAMANTOPOULOU I,SKODRAS G,SAKELLAROPOU-LOS G P.Sorption of mercury by activated carbon in the presence of flue gas components[J].Fuel Processing Technology,2010,91(2):158-163.
[24]AND D B,LIZZIO A A,DALEY M A.Adsorption of SO2on bituminous coal char and activated carbon fiber[J].Energy&Fuels,1997,11(2):267-271.
[25]KISAMORI S,KURODA K,KAWANO S,et al.Oxidative removal of SO2and recovery of H2SO4over poly(acrylonitrile)-based active carbon fiber[J].Energy&Fuels,1994,8(6):1337-1340.
[26]HALL B,SCHAGER P,WEESMAA J.The homogeneous gas phase reaction of mercury with oxygen,and the corresponding heterogeneous reactions in the presence of activated carbon and fly ash[J].Chemosphere,1995,30(4):611-627.
[27]PRESTO A A,GRANITE E J.Survey of catalysts for oxidation of mercury in flue gas[J].Environmental Science&Technology,2006,40(18):5601-5609.
[28]LIU Y S.Impact of sulfur oxides on mercury capture by activated carbon[J].Environmental Science&Technology,2008,42(3):970-971.
[29]LI Y H,LEE C W,GULLETT B K.The effect of activated carbon surface moisture on low temperature mercury adsorption[J].Carbon,2002,40(1):65-72.
[30]YIN G,LIU Z,LIU Q,et al.The role of different properties of activated carbon in CO2adsorption[J].Chemical Engineering Journal,2013,230(16):133-140.
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