实验参数对Ag/BiOI光催化剂湿法脱除气态单质汞的影响
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摘要
采用沉淀-光还原法制备了不同Ag负载量的碘氧化铋(Ag/BiOI)可见光催化剂,在小型湿法光催化脱汞装置上考察了Ag负载量、反应溶液温度、pH、阴离子(Cl~-,NO_3~-,SO_4~(2-)和CO_3~(2-))、烟气成分(O_2,SO_2和NO)、光催化剂剂量和循环次数等对单质汞(Hg~0)脱除效率的影响。结果表明:与BiOI相比,Ag负载可以大幅提高其脱汞活性,Ag负载量为2 wt%时,其脱汞效率高达98%;Cl-和NO_3~-对Hg0的脱除效率几乎没有影响,而SO_4~(2-)和CO_3~(2-)会对脱汞效率有一定的抑制作用,其中CO_3~(2-)对脱汞效率的影响尤为严重。循环脱汞实验表明Ag(2%)/BiOI光催化剂的稳定性良好。
The Ag/BiOI photocatalysts with different silver loadings were synthesized by using precipitationphotoreduction method. Influences of Ag content,reaction temperature,solution pH,common anions(NO-3,CO_3~(2-),Cl-and SO_4~(2-)),flue gas components(O_2,SO_2 and NO),photocatalyst dosage and cyclic utilization on elemental mercury(Hg0) removal efficiency were investigated in a laboratory-scale wet bubbling Hg0 photocatalytic reactor. The results show that in comparison to BiOI,Hg0 removal efficiency of Ag/BiOI was greatly improved when a small amount of metallic silver were added. In particular,when the Ag content is 2 % in Ag(2%)/BiOI material,the Hg0 removal efficiency reaches 98 %. Cl-and NO-3 show no influences on Hg0 removal,while SO_4~(2-) and CO_3~(2-) exhibit inhibitory effects on Hg0 removal,particular for CO_3~(2-). The cyclic mercury removal test indicats that the Ag(2 %)/BiOI photocatalyst is much stable in the process of Hg0 photocatalytic oxidation.
The Ag/BiOI photocatalysts with different silver loadings were synthesized by using precipitationphotoreduction method. Influences of Ag content,reaction temperature,solution pH,common anions(NO-3,CO_3~(2-),Cl-and SO_4~(2-)),flue gas components(O_2,SO_2 and NO),photocatalyst dosage and cyclic utilization on elemental mercury(Hg0) removal efficiency were investigated in a laboratory-scale wet bubbling Hg0 photocatalytic reactor. The results show that in comparison to BiOI,Hg0 removal efficiency of Ag/BiOI was greatly improved when a small amount of metallic silver were added. In particular,when the Ag content is 2 % in Ag(2%)/BiOI material,the Hg0 removal efficiency reaches 98 %. Cl-and NO-3 show no influences on Hg0 removal,while SO_4~(2-) and CO_3~(2-) exhibit inhibitory effects on Hg0 removal,particular for CO_3~(2-). The cyclic mercury removal test indicats that the Ag(2 %)/BiOI photocatalyst is much stable in the process of Hg0 photocatalytic oxidation.
引文
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[2]SABRI Y M,IPPPLITO S J,ATANACIO A J,et al.Mercury vapor sensor enhancement by nanostructured gold deposited on nickel surfaces using galvanic replacement reactions[J].Journal of Materials Chemistry,2012,22:21395-21404.
[3]汤顺林,王利娜,冯朝晖,等.河南省主要聚煤期煤中总汞及有机结合态汞的研究[J].河南理工大学学报(自然科学版),2015,34(4):562-567.TANG S L,WANG L N,FENG C H,et al.Syudy on THg and orginic combined mercury in the main coal accumulating period in Henan province[J].Journal of Henan Polytechnic University(Natural Science),2015,34(4):562-567.
[4]谭增强,牛国平,陈晓文,等.椰壳碳基吸附剂的脱汞特性[J].环境工程学报,2015,9(12):5992-5996.TAN Z Q,NIU G P,CHEN X W,et al.Removal of elemental mercury by coconut shell carbon[J].Chinese Journal of Environmental Engineering,2015,9(12):5992-5996.
[5]CAO Y,CHENG C M,CHEN C W,et al.Abatement ofmercury emissions in the coal combustion process equipped with a fabricfilter baghouse[J].Fuel,2008,87:3322-3330.
[6]徐丽梅玫,许飘,李彩,等.稻壳活性炭对单质汞吸附性能的实验研究[J].环境工程学报,2010,4(9):2065-2068.XU LI M M,XU P,LI C,et al.Anexperimental study on adsorptive performance of rice husk activated carbon to mercury[J].Chinese Journal of Environmental Engineering,2010,4(9):2065-2068.
[7]HUTSON N D,KRZYZYNSKA R,SRIVASTAVA R K.Simultaneous removal of SO2,NOx,and Hg0from coal flue gas using a Na Cl O2-enhanced wet scrubber[J].Industrial and Engineering Chemistry Research,2008,47(16):5825-5831.
[8]ZHOU C S,SUN L S,ZHANG A C,et al.Elemental mercury(Hg0)removal from containing SO2/NO flue gas by magnetically separable Fe2.45Ti0.55O4/H2O2advanced oxidation processes[J].Chemical Engineering Journal,2015,273:381-389.
[9]ZHAO Y,HAO R L,ZHANG P,et al.An integrative process for Hg0removal using vaporized H2O2/Na2S2O8[J].Fuel,2014,136:113-121.
[10]LIU Y X,ZHANG J,PAN J F.Photochemical oxidation removal of Hg0from flue gas containing SO2/NO by an ultraviolet irradiation/hydrogen peroxide(UV/H2O2)process[J].Energy and Fuels,2014,28:2135-2143.
[11]ZHAN F M,LI C T,ZENG G M,et al.Experimental study on oxidation of elemental mercury by UV/Fenton system[J].Chemical Engineering Journal,2013,232:81-88.
[12]CHANG X F,HUANG J,CHENG C,et al.Bi OX(X=Cl,Br,I)photocatalyst prepared using Na Bi O3as Bi source:Characterization and catalytic performance[J].Catalysis Communications,2010,11:460-464.
[13]ZHANG X,AI Z H,JIA F L,et al.Generalized onepot Synthesis,characterization,and photocatalytic activity of hierarchical Bi OX(X=Cl,Br,I)Nanoplate Microspheres[J].The Journal of Physical Chemistry C,2008,112(3):747-753.
[14]姬燕培,陈西良.纳米Bi OI的制备及其对溴甲酚绿的光催化降解[J].环境科学与技术,2016,39(10):31-35.JI Y P,CHEN X L.Synthesis of Bi OI nanomaterials and its light driven photocatalytic degradation towards Bromocresol Green[J].Environmental Science and Technology,2016,39(10):31-35.
[15]ZHANG A C,XING W B,et al.A novel low-cost method for Hg0removal from flue gas by visible-lightdriven Bi OX(X=Cl,Br,I)photocatalysts[J].Catalysis Communications,2016,87:57-61.
[16]王欢,崔文权,韩炳旭,等.Ag/Ag X(X=Cl,Br,I)等离子共振光催化剂的研究进展[J].化工进展,2013,3(2):346-351.WANG H,CUI W Q,HAN B X,et al.Research progress of plasmonic Ag/Ag X(X=Cl,Br,I)photocatalysts[J].Chemical Industry and Engineering Progress,2013,3(2):346-351.
[17]GAO Y P,WANG L B,LI Z Y,et al.Microwave-assisted synthesis of flower-like Ag-Bi OCl nanocomposite with enhanced visible-light photocatalytic activity[J].Materials Letters,2014,136:295-297.
[18]DUTTA D P,TYAGI A K.Facile sonochemical synthesis of Ag modified Bi4Ti3O12nanoparticles with enhanced photocatalytic activity under visible light[J].Materials Research Bulletin,2016,74:397-407.
[19]ZHENG Y H,CHEN C Q,ZHAN Y Y,et al.Photocatalytic activity of Ag/Zn O heterostructure nanocatalyst:correlation between structure and property[J].The Journal of Physical Chemistry C,2008,112:10773-10777.
[20]李成伟,张安超,宋军,等.Ag/Bi OI光催化剂湿法脱除烟气中单质汞性能及机理[J].化工进展,2018,37(4):1442-1451.LI C W,ZHANG A C,SONG J,et al.Mechanism and performance of wet process to remove gaseous elemental mercury from flue gas using Ag/Bi OI photocatalyst[J].Chemical Industry and Engineering Progress,2018,37(4):1442-1451.
[21]ZHANG A C,ZHANG L X,et al.Facile synthesis of ternary Ag/Ag Br-Ag2CO3hybrids with enhanced photocatalytic removal of elemental mercury driven by visible light[J].Journal of Hazardous Materials,2016,314:78-87.
[22]CAO J,LI X,LIN H L,et al.Low temperature synthesis of novel rodlike Bi5O7I with visible light photocatalytic performance[J].Materials Letters 2012,76(6):181-183.
[23]余长林,操芳芳,等.Ag/Bi OX(X=Cl,Br,I)复合光催化剂的制备、表征及其光催化性能[J].物理化学学报,2012,28(3):647-653.YU C L,CAO F F,et al.Preparation,Characterization and photocatalytic performance of Ag/Bi OX(X=Cl,Br,I)composite photocatalysts[J].Acta PhysicoChimica Sinica,2012,28(3):647-653.
[24]LIU Y X,ZHANG J,SHENG C D,et al.Preliminary study on a new technique for wet removal of nitric oxide from simulated flue gas with an ultraviolet(UV)/H2O2process[J].Energy and Fuels,2010,24(90):4925-4930.
[25]SANTIAGAO D E,ARANA J,CONZALEZ-DIAZ,et al.Effect of inorganic ions on the photocatalytic treatment of agro-industrial waste waters containing imazalil[J].Applied Catalysis B:Environmental,2014,156-157(3):284-292.
[26]KIM J,LEE W,CHOI W.Platinized WO3as an environmental photocatalyst that generates OH radicals under visible light[J].Environmental Science and Technology,2010,44:6849-6854.
[27]LIU Y X,ZHANG J,PAN J F,et al.Investigation on removal of NO from SO2-containing simulated flue gas by an ultraviolet/Fenton-like reaction[J].Energy and Fuels,2012,26(9):5430-5436.
[28]LI G T,WONG K H,ZHANG X W,et al.Degradation of acid orange 7 using magnetic Ag Br under visible light:The roles of oxidizing species[J].Chemosphere,2009,76(9):1185-1191.
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