磷酸改性生物炭-LDHs(Mg-Al-NO3)复合材料对双酚A的吸附
Adsorption of bisphenol a by phosphoric acid modified biochar-LDHs(Mg-Al-NO3) composite
-
摘要: 本研究选取油菜秸秆为原料,在600℃下热解得到生物炭和磷酸改性生物炭,并用共沉淀法制备3种改性生物炭-LDHs (Mg-Al-NO3)复合材料.采用批量吸附法研究不同pH、吸附时间和不同生物炭/LDHs配比条件下复合材料对双酚A的吸附特性,借助XRD、FTIR和BET等测试手段探究了复合材料吸附双酚A的机制.结果表明,改性生物炭-LDHs (Mg-Al-NO3)复合材料吸附双酚A的吸附平衡时间为4 h,符合准二级动力学方程(R2>0.99);复合材料对双酚A的吸附效果稍逊于改性生物炭,改性生物炭在复合材料中所占比重越大,吸附效果越好.当pH值在5.0—9.0范围内变化时,改性生物炭-LDHs (Mg-Al-NO3)复合材料对双酚A的吸附量呈下降趋势,且在pH=9.0时达到最小值.等温吸附模型数据表明,复合材料用Freundlich等温吸附模型效果更好.通过XRD、BET、FTIR测试研究发现,由于LDHs占据了生物炭表面的活性位点,致使生物炭与双酚A之间的相互作用减弱,降低了复合物的吸附能力.本研究结果初步阐释了改性生物炭-LDHs (Mg-Al-NO3)复合材料吸附双酚A的机理,为生物炭-LDHs复合材料处理水体中有机污染物的应用提供了借鉴和参考.Abstract: Biochar and modified biochar were prepared from the rapeseed straw pyrolyzed at 600℃. The modified biochar was complexed with LDHs (Mg-Al-NO3) by the co-precipitation method to obtain modified biochar-LDHs (Mg-Al-NO3) composites. Batch method was used to study the adsorption of bisphenol A on the composite materials with different pH, adsorption time and biochar/LDHs ratios. The mechanism of bisphenol A adsorption by the composite was investigated by means of XRD, FTIR and BET. The results showed that the equilibrum time of bisphenol A adsorption on the modified biochar-LDHs (Mg-Al-NO3) composites was 4 h, and the process was described with the second-order kinetic equation (R2>0.99). The capacity of the composites for the adsorption of bisphenol A was inferior to that of the modified biochar. The larger the proportion of the modified biochar in the composite material, the greater the adsorption was. When the pH varied from 5.0 to 9.0, the adsorption of bisphenol A on the composite showed a decreasing trend, and reached the minimum value when the pH was 9.0. The data of isothermal adsorption model showed that the Freundlich isothermal adsorption model was better than that of Langmuir. Through XRD, BET and FTIR tests, it was found that, LDHs occupied the active sites on the surface of biochar, the interaction between biochar and bisphenol A was weakened, leading to reduced adsorption capacity of the composites. This study revealed the mechanism of bisphenol A adsorption by the modified biochar-LDHs (Mg-Al-NO3) composites and provides a basis for the future application of this material in the treatment of organic pollutants in water.
-
Key words:
- modified biochar /
- LDHs /
- composite materials /
- bisphenol A /
- adsorption
-
[1] FITZGERALD R E, WILKS M.F. Bisphenol A-Why an adverse outcome pathway framework needs to be applied[J]. Toxicology Letters, 2014, 230(2):368-374. [2] 郭丽敏. 关于双酚A奶瓶欧盟遭禁的探讨[J]. 塑料制剂, 2011(2):7-9. GUO L M. Discussion on the ban on bisphenol A milk bottles[J]. Plastic preparation, 2011 (2):7-9(in Chinese).
[3] KUCH H M, BALLSCHMITER K. Determination of endocrine disrupting phenolic compounds and estrogens in surface and drinking water by HRGC-(NCI)-MS in the pictogram per liter range[J]. Environmental Science and Technology, 2001, 35(15):3201-3206. [4] WARDLE D A, NILSSON M C, ZACKRISSON O. Fire-derived charcoal causes loss of forest Humus[J]. Science, 2008, 320(5876):629-629. [5] NGUYEN B T, LEHMANN J, HOCKADAY W C, et al. Temperature sensitivity of black carbon decomposition and oxidation[J]. Environmental Science and Technology, 2010, 44:3324-3331. [6] HALE S E, HANLEY K, LEHMANN J, et al. Effects of chemical, biological, and physical aging as well as soil addition on the sorption of pyrene to activated carbon and biochar[J]. Environmental Science and Technology, 2011, 45:10445-10453. [7] BRUUN S, JENSEN E S, JENSEN L S. Microbial mineralization and assimilation of black carbon, dependency on degree of thermal alteration[J]. Organic Geochemistry, 2008, 39:839-845. [8] 郎印海, 刘伟, 王慧. 生物炭对水中五氯酚的吸附性能研究[J]. 中国环境科学, 2014,34(8):2017-2023. LANG Y H, LIU W, WANG H. Adsorption efficiencies of pentachlorophenol from aqueous solution onto biochars[J]. China Environmental Science, 2014,34(8):2017-2023(in Chinese).
[9] 王林, 徐应明, 梁学峰,等. 生物炭和鸡粪对镉低积累油菜吸收镉的影响[J]. 中国环境科学, 2014,34(11):2851-2858. WANG L, XU Y M, LIANG X F, et al. Effects of biochar and chicken manure on cadmium uptake in pakchoi cultivars with low cadmium accumulation[J]. China Environmental Science, 2014,34(11):2851-2858(in Chinese).
[10] 李广坡, 林伟鑫, 杨美玉,等. 生物炭对水溶液中肉桂酸的吸附机制研究[J]. 环境化学,2018,37(6):1245-1252. LI G P, LIN W X, YANG M Y, et al. Sorption mechanism of cinnamic acid to biochar in aqueous solution[J]. Environmental Chemistry, 2018, 37(6):1245-1252(in Chinese).
[11] MUNHERJEE A, ZIMMERMAN A.R, HARRIS W. Surface chemistry variations among a series of laboratory-produced biochars[J]. Geoderma, 2011, 163(3):247-255. [12] 吴文卫, 周丹丹. 生物炭老化及其对重金属吸附的影响机制[J]. 农业环境科学学报, 2019, 38(1):7-13. WU W W, ZHOU D D. Influence of biochar aging on its physicochemical properties and adsorption of heavymetals[J]. Journal of Agro-Environment Science, 2019, 38(1):7-13(in Chinese).
[13] ZHOU N, CHEN H, XI J. Biochars with excellent Pb(Ⅱ) adsorption property produced from fresh and dehydrated banana peels via hydrothermal carbonization.[J]. Bioresource Technology, 2017, 232:204-210. [14] PENG H B, GAO P. CHU G, et al. Enhanced adsorption of Cu(Ⅱ) and Cd(Ⅱ) by phosphoric acid-modified biochars[J]. Environmental Pollution, 2017, 229:846-853. [15] LI H B, DONG X L, EVANDRO B, et al. Mechanisms of metal sorption by biochars:Biochar characteristics and modifications.[J]. Chemosphere, 2017, 178:466-478. [16] CONSTANTION V R L, PINNAVAIA T J. Basic properties of Mg2+1-x Al3+x layered double hydroxides intercalated by carbonate, hydroxide, chloride, and sulfate anions[J]. Inorganic Chemistry, 1995, 34:883-892. [17] TAN X F, LIU S B, LIU Y G. One-pot synthesis of carbon supported calcined-Mg/Al layered double hydroxides for antibiotic removal by slow pyrolysis of biomass waste[J]. Scientific Reports, 2016, doi:10.1038/srep39691 [18] 王震宇, 刘国成, MONICA XING. 不同热解温度生物炭对Cd(Ⅱ)的吸附特性[J]. 环境科学, 2014, 35(12):4735-4744. WANG Z Y, LIU G C, MONICA X. Different pyrolysis temperatures biochar adsorption properties for Cd (Ⅱ)[J]. Environmental Science, 2014, 35(12):4735-4744(in Chinese).
[19] 钟晓晓, 王涛, 原文丽,等. 生物炭的制备、改性及其环境效应研究进展[J].湖南师范大学自然科学学报, 2017, 40(5):44-50. ZHONG X X, WANG T, YUAN W L, et al. Progresses of preparation, modification and environmental behavior of biochar[J]. Journal of Natural Science of Hunan Normal University, 2017, 40(5):44-50(in Chinese).
[20] 钟晓晓, 王涛, 王凯,等. 磷酸和热解温度对生物炭结构和性质的影响[J].湖南师范大学自然科学学报, 2018, 41(1):48-53. ZHONG X X, WANG T, WANG K, et al. Impacts of phosphorus acid concentration and pyrolysis temperature on structure and property of biochar[J]. Journal of Natural Science of Hunan Normal University, 2018, 41(1):48-53(in Chinese).
[21] 张鑫慧, 张甘霖, 杨金玲. 典型热带土壤时间序列的电荷零点变化特征及其土壤发生意义[J].土壤, 2014, 46(2):347-354. ZHANG X H, ZHANG G L, YANG J L. The characteristics and significance of zero-point change of charge in typical tropical soil time series[J]. Soils, 2014, 46(2):347-354(in Chinese).
[22] 王俊超, 郑凯琪, 俞筱妍,等. 垫料生物炭对Cd2+的吸附性能[J].环境工程学报, 2016, 10(11):6655-6661. WANG J C, ZHENG K Q, YU X Y, et al. Adsorption properties of Cd2+ by bedding materials derived-biochar[J]. Chinese Journal of Environmental Engineering, 2016, 10(11):6655-6661(in Chinese).
[23] AMIT B, IOANNIS A, Adsorptive removal of bisphenol A (BPA) from aqueous solution:A review[J]. Chemosphere, 2017, 168:885-902. [24] 李健. 类水滑石(LDHs)结构的合成及吸附、光催化、腐蚀性能研究[D]. 青岛:山东科技大学,2017. LI J. Prepation and adsorption, photocatalysis and corrosion of LDHs materials structure[D]. Qingdao:Shandong University of Science and Technology, 2017(in Chinese). [25] 牛红梅, 徐莉. 镁铝水滑石及其插层组装化合物的合成与表征[J]. 西安科技大学学报, 2010, 30(6):731-733. NIU H M, XU L. Synthesis and characterization of magnesia-aluminum hydrotalcite and its intercalated assembly compounds[J]. Journal of XI'AN University of Science and Technology, 2010, 30(6):731-733(in Chinese).
[26] 程春艳, 赵洪晨, 赵双双,等.Mg-Al层状双金属氢氧化物的合成及表征[J].科技视界,2018(19):70-71. CHENG C Y, ZHAO H C, ZHAO S S, et al. Synthesis and characterization of mg-al layered double hydroxides[J]. Science and Technology Vision, 2018 (19):70-71(in Chinese).
[27] 王璐, 赵保卫, 马锋锋,等. 马铃薯秸秆生物炭对黄土吸附Cd(Ⅱ)的影响[J]. 环境化学, 2016, 35(7):1422-1430. WANG L, ZHAO B W, MA F F, et al. Effects of biochar derived from potato straw on adsorption of Cd(Ⅱ) onto loess[J]. Environmental Chemistry, 2016, 35(7):1422-1430(in Chinese).
[28] PETROVIC J T, STOJANVIC M D, MILOKOVIC J V, et al. Alkali modified hydrochar of grapepomace as a perspective adsorbent of Pb2+ from aqueous solution[J]. Journal of Environmental Management, 2016, 182:292-300. [29] 王彤彤, 马江波, 曲东,等. 两种木材生物炭对铜离子的吸附特性及其机制[J]. 环境科学, 2017, 38(5):2161-2171. WANG T T, MA J B, QU D, et al. Adsorption characteristics and mechanism of copper ions on two kinds of wood biochar[J]. Environmental Science,2017, 38(5):2161-2171(in Chinese).
[30] 朱银涛, 李业东, 王明玉,等. 玉米秸秆碱化处理制备的生物炭吸附锌的特性研究[J]. 农业环境科学学报, 2018, 37(1):179-185. ZHU Y T, LI Y D, WANG M Y, et al. Adsorption characteristics of biochar prepared by corn stalk alkalization on zinc[J]. Journal of Agro-Environment Science, 2018, 37(1):179-185(in Chinese).
[31] ZHAO Y F, ZHANG B, ZHANG X, et al. Preparation of highly orderedcubic NaA zeolite from halloysite mineral for adsorption of ammonium ions[J]. Journal of Hazardous Materials, 2010, 178(1-3):658-664. [32] SUN L, CHEN D, WAN S, et al. Performance, kinetics, and equilibrium of methylene blue adsorption on biochar derived from eucalyptus saw dust modified with citric, tartaric, and acetic acids[J]. Bioresource Technology, 2015, 198:300-308. [33] 徐楠楠, 林大松, 徐应明,等. 玉米秸秆生物炭对Cd2+的吸附特性及影响因素[J]. 农业环境科学学报. 2014, 33(5):958-964. XU N N, LIN D S, XU Y M, et al. Adsorption characteristics and influencing factors of Cd2+ on corn straw biochar[J]. Journal of Agro-Environment Science, 2014, 33(5):958-964(in Chinese).
[34] 吴鸿伟, 陈萌, 黄贤金,等. 改性生物炭对水体中头孢噻肟的吸附机制[J]. 中国环境科学, 2018, 38(7):2527-2534. WU H W, CHEN M, HUANG X J, et al. Preparation of modified biochar for adsorption of cefotaxime in solution[J].China Environmental Science, 2018,38(7):2527-2534(in Chinese).
计量
- 文章访问数: 1933
- HTML全文浏览数: 1933
- PDF下载数: 81
- 施引文献: 0