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随时间推移螺旋桨射流力累积效应下全氟烷基酸的释放响应和机制。

Responses and mechanisms of perfluoroalkyl acid release to the cumulative effects of propeller jet force over time.

机构信息

Ministry of Education Key Laboratory of Integrated Regulation and Resource Development on Shallow Lakes, Hohai University, Nanjing 210098, PR China.

Ministry of Education Key Laboratory of Integrated Regulation and Resource Development on Shallow Lakes, Hohai University, Nanjing 210098, PR China; Yangtze Institute for Conservation and Development, Hohai University, Nanjing 210098, PR China.

出版信息

J Hazard Mater. 2024 Dec 5;480:136345. doi: 10.1016/j.jhazmat.2024.136345. Epub 2024 Oct 28.

Abstract

As the discharge of exogenous perfluoroalkyl acids (PFAAs) is gradually controlled, the secondary release of endogenous PFAAs is poised to become a major challenge. However, the effects of complex hydrodynamic conditions, such as disturbance from ship propeller jets, on PFAA release, are still poorly understood. In the present study, a propeller jet disturbance simulation experiment was carried out using an indoor flume to investigate the responses and mechanisms of PFAA release to the cumulative effects of jet force over time. Although an increase in jet action time (t) increased the total amount of dissolved PFAAs in the overlying water, PFAA dissolution intensity decreased. Conversely, increase in t induced a rise in both total PFAA amount adsorbed and adsorption intensity in suspended particulate matter (SPM). Moreover, differences in functional groups and carbon-fluorine chain lengths resulted in different types of PFAAs exhibiting different sensitivities to changes in t during dissolution and adsorption. During the jet disturbance, there were distinct shear zoning and pressure gradients in the flow field, contributing to the tendency of PFAAs to be distributed in the overlying water. However, after the disturbance, PFAAs tended to distribute in the SPM. Changes in t consistently affected the partition behavior of long-chain PFAAs (C ≥ 7), whereas the effect on the partition behavior of short-chain PFAAs (C < 7) was rather short-lived. In contrast, Perfluoroalkyl carboxylic acids were more readily released from the sediments and porewater than Perfluoroalkyl sulfonic acids; however, the difference decreased with increasing t. Both shear impulse and squeeze impulse showed a significant linear positive correlation with PFAA release (p < 0.05), but the effect of shear impulse was greater. The findings provide perspectives for further understanding of PFAA release under jet disturbance and could facilitate endogenous PFAA contamination control.

摘要

随着外源性全氟烷基酸(PFAAs)的排放逐渐得到控制,内源性 PFAAs 的二次释放将成为一个主要挑战。然而,复杂水动力条件(如船舶螺旋桨射流的干扰)对 PFAAs 释放的影响仍知之甚少。本研究采用室内水槽进行了螺旋桨射流干扰模拟实验,以研究 PFAA 对射流力随时间累积效应的响应和释放机制。尽管射流作用时间(t)的增加增加了上覆水中溶解 PFAAs 的总量,但 PFAA 溶解强度却降低了。相反,t 的增加导致吸附在悬浮颗粒物(SPM)上的总 PFAA 量和吸附强度均升高。此外,不同官能团和碳氟链长度导致不同类型的 PFAAs 在溶解和吸附过程中对 t 的变化表现出不同的敏感性。在射流干扰期间,流场中存在明显的剪切分区和压力梯度,导致 PFAAs 倾向于分布在上覆水中。然而,干扰后,PFAAs 倾向于分布在 SPM 中。t 的变化始终影响长链 PFAAs(C ≥ 7)的分配行为,而对短链 PFAAs(C < 7)的分配行为的影响则较为短暂。相比之下,全氟烷基羧酸比全氟烷基磺酸更容易从沉积物和孔隙水中释放出来;然而,随着 t 的增加,这种差异会减小。剪切脉冲和挤压脉冲均与 PFAA 释放呈显著的线性正相关(p<0.05),但剪切脉冲的影响更大。这些发现为进一步了解射流干扰下 PFAA 的释放提供了新视角,并有助于控制内源性 PFAA 污染。

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