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非稳态菲克扩散模型降低了薄膜型被动采样器中扩散梯度法估计胶层扩散系数的不确定性。

Non-Steady-State Fickian Diffusion Models Decrease the Estimated Gel Layer Diffusion Coefficient Uncertainty for Diffusive Gradients in Thin-Films Passive Samplers.

机构信息

Department of Civil Engineering, University of Arkansas, Fayetteville, Arkansas 72701, United States.

U.S. Environmental Protection Agency, Cincinnati, Ohio 45268, United States.

出版信息

Environ Sci Technol. 2023 Jul 4;57(26):9793-9801. doi: 10.1021/acs.est.3c01861. Epub 2023 Jun 21.


DOI:10.1021/acs.est.3c01861
PMID:37342010
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC10324599/
Abstract

Mass transport in diffusive gradients in thin-film passive samplers is restricted to diffusion through a gel layer of agarose or agarose cross-linked polyacrylamide (APA). The gel layer diffusion coefficient, , is typically determined using a standard analysis (SA) based on Fick's first law from two-compartment diffusion cell (D-Cell) tests. The SA assumes pseudo-steady-state flux, characterized by linear sink mass accumulation-time profiles with a typical threshold ≥ 0.97. In 72 D-Cell tests with nitrate, 63 met this threshold, but the SA-determined ranged from 10.1 to 15.8 × 10 cm·s (agarose) and 9.5 to 14.7 × 10 cm·s (APA). A regression model developed with the SA to account for the diffusive boundary layer had 95% confidence intervals (CIs) on of 13 to 18 × 10 cm·s (agarose) and 12 to 19 × 10 cm·s (APA) at 500 rpm. A finite difference model (FDM) developed based on Fick's second law with non-steady-state (N-SS) flux decreased uncertainty in tenfold. The FDM-captured decreasing source compartment concentrations and N-SS flux in the D-Cell tests and, at 500 rpm, the FDM-determined ± 95% CIs were 14.5 ± 0.2 × 10 cm·s (agarose) and 14.0 ± 0.3 × 10 cm·s (APA), respectively.

摘要

在薄层层析扩散采样器中,质量传递仅限于通过琼脂或琼脂交联聚丙烯酰胺 (APA) 的凝胶层扩散。凝胶层扩散系数 ,通常使用基于双室扩散池 (D-Cell) 测试中菲克第一定律的标准分析 (SA) 来确定。SA 假设假稳态通量,其特征是具有典型阈值 ≥ 0.97 的线性汇质量积累时间曲线。在 72 个硝酸盐 D-Cell 测试中,有 63 个符合此阈值,但 SA 确定的 范围为 10.1 到 15.8 × 10 cm·s(琼脂)和 9.5 到 14.7 × 10 cm·s(APA)。使用 SA 开发的回归模型来解释扩散边界层,在 500 rpm 时,琼脂的 置信区间 (CI) 为 13 到 18 × 10 cm·s,APA 的 置信区间 (CI) 为 12 到 19 × 10 cm·s。基于菲克第二定律和非稳态 (N-SS) 通量的有限差分模型 (FDM) 可将不确定性降低十倍。FDM 捕获了 D-Cell 测试中源隔室浓度和 N-SS 通量的下降,并在 500 rpm 时,FDM 确定的 ± 95% CI 分别为 14.5 ± 0.2 × 10 cm·s(琼脂)和 14.0 ± 0.3 × 10 cm·s(APA)。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/ae0d/10324599/dbd5c9488a2d/es3c01861_0006.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/ae0d/10324599/75ce92f2e07a/es3c01861_0002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/ae0d/10324599/705f62a9ff75/es3c01861_0003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/ae0d/10324599/78ea1a731d2a/es3c01861_0004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/ae0d/10324599/0ecaf707af93/es3c01861_0005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/ae0d/10324599/dbd5c9488a2d/es3c01861_0006.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/ae0d/10324599/75ce92f2e07a/es3c01861_0002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/ae0d/10324599/705f62a9ff75/es3c01861_0003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/ae0d/10324599/78ea1a731d2a/es3c01861_0004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/ae0d/10324599/0ecaf707af93/es3c01861_0005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/ae0d/10324599/dbd5c9488a2d/es3c01861_0006.jpg

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[4]
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[5]
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[6]
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[7]
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[8]
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[9]
Development and Calibration of an Organic-Diffusive Gradients in Thin Films Aquatic Passive Sampler for a Diverse Suite of Polar Organic Contaminants.

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