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用新型 TiO2 基杂化纳米复合材料降解水体、土壤和河底沉积物中的三环多环芳烃。

Degradation of tricyclic polyaromatic hydrocarbons in water, soil and river sediment with a novel TiO based heterogeneous nanocomposite.

机构信息

Department of Chemistry Dr B R Ambedkar National Institute of Technology Jalandhar, Punjab, 144011, India.

Department of Chemistry Malaviya National Institute of Technology Jaipur Jaipur, Rajasthan, 302017, India.

出版信息

J Environ Manage. 2019 Oct 15;248:109340. doi: 10.1016/j.jenvman.2019.109340. Epub 2019 Aug 3.

Abstract

Polycyclic aromatic hydrocarbons (PAHs), pervasive and precedence pollutants have potential to decimate the bionetwork and human health. Therefore, photocatalytic degradation of toxic three membered PAHs, namely acenaphthene (ACN), phenanthrene (PHN) and fluorene (FLU) was explored in water and soil. Titanium dioxide based zinc hexacyanoferrate framework (TiO@ZnHCF) nanocomposite was synthesized via a two step A. indica mediated co-precipitation method. Under sunlight, fall in concentration of PAHs (Water- 93%-96%, soil- 82%-86% and river sediment- 81.63%-85.43%) with time revealed superior activity of nanocomposite (TiO@ZnHCF) as compared to the bared one. Slower degradation in soil and sediment could be attributed to the reduced diffusion caused by the interaction between the organic content of soil/sediment with PAHs. Doping caused an increase in surface area (118.15 mg) with decrease in band gap energy (1.65 eV) and photoluminescence intensity. PAHs removal (X = 9.48 mg g of ACN, 9.35 mg g of PHN and 8.96 mg g of FLU) involved role of "cation- π" interaction with nanocomposite. Besides, it reduced t values of ACN (1.88 h), PHN (2.09 h) and FLU (2.86 h) and resulted into smaller by-products. Smaller by-products like (Z)-prop-1-ene-1,2,3-triol (m/z = 91) and (E)-3-hydroxyacrylaldehyde (m/z = 71) identified in GC-MS, evidently braced e excitement from encapsulated nanocatalyst followed by OH (active species) based oxidation of PAHs. Lower photoluminescence intensity indicates the least charge carrier recombination with highest photocatalytic activity of nanocomposites. Inclusive of the present study provides promising photocatalyst with greater surface activity, low quantum yield with charge separation, reusable up to ten cycles deprived of substantial loss of its action and suppressing the cost of process.

摘要

多环芳烃(PAHs)是普遍存在且具有优先污染性的污染物,有可能破坏生物网络和人类健康。因此,本文探索了在水和土壤中用光催化降解有毒的三元 PAHs,即苊(ACN)、菲(PHN)和芴(FLU)。通过两步 A. indica 介导共沉淀法合成了基于二氧化钛的锌六氰合铁酸盐框架(TiO@ZnHCF)纳米复合材料。在阳光下,PAHs 浓度随时间的下降(水-93%-96%,土壤-82%-86%和河流沉积物-81.63%-85.43%)表明纳米复合材料(TiO@ZnHCF)的活性优于裸露的纳米复合材料。土壤和沉积物中降解速度较慢可能是由于有机物质与 PAHs 之间的相互作用导致扩散减少所致。掺杂导致表面积增加(118.15mg),带隙能降低(1.65eV),光致发光强度降低。PAHs 的去除(X=9.48mg/g 的 ACN、9.35mg/g 的 PHN 和 8.96mg/g 的 FLU)涉及与纳米复合材料的“阳离子-π”相互作用。此外,它还降低了 ACN(1.88h)、PHN(2.09h)和 FLU(2.86h)的 t 值,并产生了更小的副产物。GC-MS 鉴定出更小的副产物,如(Z)-丙烯-1,2,3-三醇(m/z=91)和(E)-3-羟基丙烯醛(m/z=71),这显然支持了被包裹的纳米催化剂激发后,基于 OH(活性物质)的 PAHs 氧化。较低的光致发光强度表明电荷载流子复合最少,纳米复合材料的光催化活性最高。本研究提供了一种有前途的光催化剂,具有更大的表面活性、低量子产率和电荷分离,可重复使用十次以上,且其作用没有明显损失,并降低了工艺成本。

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