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作 者:李春全[1] 宁晓田 杨珊珊 尚海灵 袁方 孙志明[1] LI Chunquan;NING Xiaotian;YANG Shanshan;SHANG Hailing;YUAN Fang;SUN Zhiming(School of Chemical and Environmental Engineering,China University of Mining and Technology(Beijing),Beijing 100083,China;School of Water Resources and Environment,China University of Geosciences(Beijing),Beijing 100083,China;Water Conservancy Science Research Institute of Inner Mongolia,Hohhot 010018,China)
机构地区:[1]中国矿业大学(北京)化学与环境工程学院,北京100083 [2]中国地质大学(北京)水资源与环境学院,北京100083 [3]内蒙古自治区水利科学研究院,呼和浩特010052
出 处:《硅酸盐学报》2024年第10期3093-3105,共13页Journal of The Chinese Ceramic Society
基 金:国家自然科学基金项目(52304310)。
摘 要:苯并芘(B[a]p)作为典型多环芳烃化合物之一,具有强致癌、致畸及致突变作用,广泛分布在土壤、大气以及水体环境。基于过硫酸盐的高级氧化技术因其快速、简便以及高效等优点在环境治理领域一直是研究热点。尤其是铁基催化材料,因其环保、成本低和反应活性高等特性被广泛应用在过硫酸盐活化领域,但其在应用过程中存在易氧化、易团聚以及Fe(Ⅱ)再生能力差等缺陷。因此,本工作采用一步水热法制备了FeS_(2)/高岭石复合材料,用于高效活化过一硫酸盐(PMS)降解B[a]P。其在投加量为2.0 g/L,初始B[a]p浓度为20 mg/L,PMS剂量为2 mmol/L的条件下,15 min内对B[a]p的去除率达到93%,并证实了体系中^(1)O_(2)和O_(2)^(·-)起主导作用。此外,在土壤体系中,随着复合材料和PMS用量的增加,B[a]p的降解率逐渐增加;随着水土比(质量比)的增加,呈现出先增加后降低的趋势;而随着pH值的增加,降解效率反而呈现降低的趋势,选取催化剂用量50 mg/g,PMS用量80 mg/g,水土比3:1以及pH值为3的条件下进行实验,60 min内对B[a]p的去除率达到69.02%。Introduction Polycyclic aromatic hydrocarbons(PAHs)are hydrophobic aromatic compounds consisting of two or more condensed benzene rings,having greater teratogenicity,carcinogenicity,mutagenicity and toxicity.The most representative PAHs is benzo(a)pyrene(B[a]p),which is composed of five benzene rings,and is classified as a Group I carcinogen.The treatment technologies for B[a]p removal include bioremediation,physical remediation and chemical remediation.The advanced oxidation technology based on sulfate radicals becomes a recent research hotspot because of its high redox potential,high reactivity and environmental friendliness.Nevertheless,persulfate needs to be activated through various approaches to produce a series of reactive species,and iron-based materials are widely used due to the abundant reserves,environmental friendliness and excellent activation performance.In this paper,pyrite(FeS_(2))was used as a cheap and non-toxic sulfide mineral,allowing for a slow release of Fe^(2+)as well as the cycling of Fe^(2+)and Fe3+.Kaolinite was chosen as a suitable carrier to solve the agglomeration of FeS_(2) nanoparticles.A composite with FeS_(2) and kaolinite was prepared to obtain efficient persulfate activation and B[a]p degradation.Methods Ferrous sulfate heptahydrate(FeSO4·7H2O),sodium thiosulfate(Na2S2O3),cetyltrimethylammonium bromide and kaolinite were ultrasonically mixed and stirred for 30 min,and then the solution was transferred to a reactor for the hydrothermal reaction.At the end of the reaction,the solution was centrifuged and washed for three times,and then put into a vacuum oven for 12 h to obtain the composite catalyst.The B[a]p solution,desired dosage of catalysts and peroxymonosulfate(PMS)solution were added in a centrifuge tube of 50.00 mL,and then conducted in a rotating mixer at room temperature.Before adding PMS solution,the adsorption-desorption equilibrium process was carried out under 30 min continuous stirring.Moreover,1.00 mL of the mixture was taken at the setting time points and quench
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