臭氧加速人造沸石的合成及其对氨氮吸附特性影响
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摘要
通过引入臭氧,加速沸石晶化,从而缩短粉煤灰合成沸石时间,制备出高效且吸附氨氮容量大的人造沸石(Z-CFA-ozone).通过XRD表征结果的分析,可知臭氧加速了沸石的晶化过程,沸石的合成时间缩短了12 h.BET结果可知,Z-CFA-ozone的比表面积为412.67 m~2·g~(-1),是天然沸石的40倍.FTIR结果表明,Z-CFA-ozone对氨氮的吸附是通过离子交换作用,且加入臭氧后Z-CFA-ozone自身表面结构基本保持不变.正交实验结果表明,对Z-CFA-ozone吸附氨氮性能的影响中,臭氧浓度影响最大,温度次之,晶化时间、pH最小.准二级动力学模型和Langmuir等温吸附模型均可较好地拟合其吸附过程.热力学分析表明,Z-CFA-ozone对氨氮的吸附是自发的吸热反应.
Through bubbling with ozone, artificial zeolite with short time and high ammonium adsorption capacity was synthesized from coal fly ash(Z-CFA-ozone). Compared with the normal synthetic product, the corresponding XRD(X-ray Diffraction) patterns indicated the synthetic process of Z-CFA-ozone was accelerated by ozonation, which could save 12 hours. BET(Brunauer-Emmett-Teller) surface area measurement results showed that specific surface area of Z-CFA-ozone was 412.67 m~2·g~(-1), which was almost 40 times larger than that of natural zeolite. Fourier-transformed infrared results revealed that ammonium(NH~+_4-N) was adsorbed on Z-CFA-ozone by ion-exchange, and the structure of Z-CFA-ozone did not change after bubbling with ozone. Orthogonal tests analysis showed that the order of factors affecting the NH~+_4-N adsorption capacity of Z-CFA-ozone was ozone concentration, temperature, crystallization time, and pH. The adsorption process fitted well with the pseudo-second-order kinetics model and the Langmuir isotherm model. Thermodynamic study revealed the adsorption process of NH~+_4-N by Z-CFA-ozone was primarily due to spontaneous endothermic reaction.
Through bubbling with ozone, artificial zeolite with short time and high ammonium adsorption capacity was synthesized from coal fly ash(Z-CFA-ozone). Compared with the normal synthetic product, the corresponding XRD(X-ray Diffraction) patterns indicated the synthetic process of Z-CFA-ozone was accelerated by ozonation, which could save 12 hours. BET(Brunauer-Emmett-Teller) surface area measurement results showed that specific surface area of Z-CFA-ozone was 412.67 m~2·g~(-1), which was almost 40 times larger than that of natural zeolite. Fourier-transformed infrared results revealed that ammonium(NH~+_4-N) was adsorbed on Z-CFA-ozone by ion-exchange, and the structure of Z-CFA-ozone did not change after bubbling with ozone. Orthogonal tests analysis showed that the order of factors affecting the NH~+_4-N adsorption capacity of Z-CFA-ozone was ozone concentration, temperature, crystallization time, and pH. The adsorption process fitted well with the pseudo-second-order kinetics model and the Langmuir isotherm model. Thermodynamic study revealed the adsorption process of NH~+_4-N by Z-CFA-ozone was primarily due to spontaneous endothermic reaction.
引文
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[2] FIGUEROLA E L,ERIJMAN L.Diversity of nitrifyingbacteria in a full-scale petroleum refinery wastewater treatment plant experienci-ng unstable nitrification [J].Journal of Hazardous Materials,2010,181(1-3):281-288.
[3] LIU J Y,LUO J H,ZHOU J Z,et al.Inhibitory effect of high-strength ammonianitrogen on bio-treatment of landfill leachate using EGSB reactor under mesophilic and atmospheric conditions [J].Bioresource Technology,2012,113(4):239-243.
[4] WANG Q H,YANG Y N,LI D W,et al.Treatment of ammonium-rich swine waste in modified porphyritic andesite fixed-bed anaer-obic bioreactor [J].Bioresource Technology,2012,111(1):70-75.
[5] SANTHOSH C,VELMURUGAN V,JACOB G,et al.Role of nanomaterials in water treatment applications:A review [J].Chemical Engineering Journal,2016,306:1116-1137.
[6] 成雪君,王学江,王浩,等.载镁天然沸石复合材料对污水中氮磷的同步回收 [J].环境科学,2017,38(12):5139-5145.CHENG X J,WANG X J,WANG H,et al.Simultaneous recovery of nutrients from wastewater by mesoporous MgO-loaded nature zeolite [J].Environmental Science,2017,38(12):5139-5145 (in Chinese).
[7] 王文华,张晓青,邱金泉,等.磷酸铵镁沉淀与沸石吸附组合工艺处理海水中的氨氮 [J].化工进展,2015,34(7):2060-2064.WANG W H,ZHANG X Q,QIU J Q,et al.Ammonia nitrogen removal from seawater by magnesium ammonium phosphate(MAP) precipitation combined with zeolite adsorption [J].Chemical Industry and Engineering Progress,2015,34(7):2060-2064 (in Chinese).
[8] MAGRIOTIS Z M,LEAL PVB,SALES PFD,et al.A comparative study for the removal of mining wastewater by kaolinite,activate-d carbon and beta zeolite [J].Applied Clay Sciences,2014,91(2):55-62.
[9] 崔凯.改性沸石处理废水中氨氮的研究 [D].沈阳:沈阳工业大学,2016.CUI K.Study on the treatment of ammonia-nitrogen from wastewater with modified zeolite [D].Shenyang:Shenyang University of Technolo-gy,2016 (in Chinese).
[10] JUNICHI M,KIM Y J,YAMADA H,et al.alkali-hydrothermal modification of air-classified korean natural zeolite and their ammonium adsorption behaviors [J].Separation Science & Technology,2004,39 (16):3739-3752.
[11] JUSOH N,YEONG Y F,MOHAMAD M,et al.Rapid-synthesis of zeolite T via sonochemical-assisted hydrothermal growth method[J].Ultrasonic Sonochemistry,2017,34:273-280.
[12] HOLLER H,WIRSCHING U.Zeolite formation from fly ash [J].Fortschritte Der Min.1985,63(1):21-43.
[13] 程鹏.通过不同方法产生羟基自由基加速沸石分子筛合成的研究 [D].长春:吉林大学,2016.CHENG P.Accelerated synthesis of zeolites via hydroxyl radicals generated by different methods [D].Changchun:Jilin University,2016 (in Chinese).
[14] MERENYI G,LIND J,NAUMOV S,et al.Reaction of ozone with hydrogen peroxide (peroxone process):A revision of current mechanistic concepts based on thermokinetic and quantum-chemical considerations [J].Environmental Science & Technology,2010,44(9):3505-3507.
[15] MAKI H,OKAMURA H,AOYAMA I,et al.Halogenation and toxicity of the biodegradtion products of a nonionic surfactant,nony-l phenolethoxylate [J].Environ Taxicol Chem,1998,17(4):650-654.
[16] 宋淦.MgO吸附剂制备及其CO2吸附性能研究 [D].重庆:重庆大学,2016.SONG G.The research of preparation and CO2 adsorption performance of MgO [D].Chongqing:Chongqing University,2016 (in Chinese).
[17] VISA M.Synthesis and characterization of new zeolite materials obtained from fly ash for heavy metals removal in advanced waste-water treatment [J].Powder Technology,2016,294:338-347.
[18] HUANG H M,XIAO D,PANG R,et al.Simultaneous removal of nutrients from simulated swine wastewater by adsorption of mod-ified zeolite combined with struvite crystallization [J].Chemical Engineering Journal,2014,256.(6):431-438.
[19] 许育新,喻曼,陈喜靖,等.天然沸石对水中氨氮吸附特性的研究[J].农业资源与环境学报,2015,32(3):250-256.XU Y X,MAN Y,CHEN X J,et al.Characteristics of ammonia nitrogen adsorption on natural zeolite in water [J].Journal of Agricultural Resources and Environment,2015,32(3):250-256 (in Chinese).
[20] 李圣品,刘菲,陈鸿汉,等.法库沸石对氨氮的吸附特性和阳离子交互过程 [J].环境工程学报,2015,9(1):157-163.LI S P,LIU F,CHEN H H,et al.Adsorption characters of ammonium by Faku zeolite and cation exchanges in ammonium removalprocess [J].Chinese Journal of Environmental Engineering 2015,9(1):157-165 (in Chinese).
[21] 霍汉鑫,林海,董颖博,等.盐酸改性对天然斜发沸石孔道特征、成分、表面电位及阳离子交换性能的影响 [J].工程科学学报,2015,37(6):746-750.HUO H X,LIN H,DONG Y F,et al.Effects of hydrochloric acid modification on the channel characteristics,composition,surface potential and cation exchange behavior of natural clinoptilolite [J].Chinese Journal of Engineering 2015,37(6):746-750 (in Chinese).
[22] 陈婧,谢水波,曾涛涛,等.羟基铁插层膨润土的制备及其对铀(VI)的吸附特性与机制 [J].复合材料学报,2016,33(11):2649-2656..CHEN J,XIE S B,ZENG T T,et al.Preparation of hydroxy—Fe intercalated bentonite and its adsorption characteristics and mechanism of ura-nium(VI) [J].Acta Materiae Compositae Sinica,2016,33(11):2649-2656 (in Chinese).
[23] HAERIFAR,MONIREH,AZIZIAN S.An exponential kinetic model for adsorption at solid/solution interface [J].Chemical Engineering Journal,2013,215-216:65-71.
[24] LI R M,CHE R,LIU Q,et al.Hierarchically structured layered-double-hydroxides derived by ZIF-67 for uranium recovery from si-mulated seawater [J].Journal of Hazardous Materials,2017,338:167-176.
[25] 张新颖,余杨波,王美银,等.天然斜发沸石的氨氮改性吸附与化学再生 [J].环境化学,2016,35(5):1058-1066.ZHANG X Y,YU Y B,WANG M Y,et al.Modification and chemical regeneration of natural clinoptilolite for ammonium nitrogrn adsorption [J].Environmental Chemistry,2016,35(5):1058-1066 (in Chinese).