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关于颗粒性质和环境条件对钯和硫化纳米零价铁的电子效率影响的定量研究。

A quantitative study of the effects of particle' properties and environmental conditions on the electron efficiency of Pd and sulfidated nanoscale zero-valent irons.

机构信息

College of Environment, Zhejiang University of Technology, Hangzhou 310014, China.

School of Environmental Science and Engineering, Qilu University of Technology, Jinan, 250353, China.

出版信息

Sci Total Environ. 2022 Dec 20;853:158469. doi: 10.1016/j.scitotenv.2022.158469. Epub 2022 Sep 2.

Abstract

Electron efficiency (or electron selectivity, ɛ) is an important quantitative criterion for zero-valent iron treatment of organohalide contaminated groundwater. The aim of this quantitative study was the systematic exploration and comparison of the effects of the Pd/Fe and S/Fe molar ratios (i.e., [Pd/Fe] and [S/Fe]), trichloroethylene (TCE) concentrations ([TCE]), pH solution, aging time, and water matrices on the ɛ of Pd-nZVI and S-nZVI. To this end, we used TCE as a probe contaminant. The ɛ of Pd-nZVI increased and then decreased with [Pd/Fe], while that of S-nZVI increased with [S/Fe], as more hydrophobic FeS was formed on S-nZVI at higher [S/Fe]. The ε of S-nZVI and Pd-nZVI increased with increasing [TCE]. Specifically, the ε of S-nZVI and Pd-nZVI at [TCE] of 200 ppm increased by 24.9 % and 79.3 %, respectively, compared with that at [TCE] of 10 ppm. As the H evolution reaction (HER) was more sensitive to surface passivation than TCE dechlorination, the ε of S-nZVI and Pd-nZVI under alkaline conditions was higher than that under basic conditions, and increased by 11.7 % and 37.8 %, respectively, at pH 10 relative to that at pH 6. The ε also increased with the aging time of the S-nZVI and Pd-nZVI particles; the increase was by 27.2 % and 59.6 %, respectively, at aging time of 30 d compared with that of the fresh ones. The ɛ of both particles were higher in artificial groundwater (AGW) than in real groundwater (RGW). For all batch experiments, the ε of S-nZVI increased over the reaction time and tended to outperform that of Pd-nZVI, even though the ε of Pd-nZVI was higher than that of S-nZVI at the initial stage of TCE dechlorination, thereby justifying the longevity of S-nZVI.

摘要

电子效率(或电子选择性,ɛ)是零价铁处理有机卤代物污染地下水的重要定量标准。本定量研究的目的是系统地探索和比较 Pd/Fe 和 S/Fe 摩尔比(即 [Pd/Fe] 和 [S/Fe])、三氯乙烯(TCE)浓度 ([TCE])、溶液 pH 值、老化时间和水基质对 Pd-nZVI 和 S-nZVI 的电子效率的影响。为此,我们使用 TCE 作为探针污染物。随着 [Pd/Fe] 的增加,Pd-nZVI 的电子效率先增加后降低,而 S-nZVI 的电子效率随着 [S/Fe] 的增加而增加,因为在较高的 [S/Fe] 下,更多疏水性的 FeS 在 S-nZVI 上形成。S-nZVI 和 Pd-nZVI 的电子效率随着 [TCE] 的增加而增加。具体而言,与 [TCE] 为 10 ppm 相比,[TCE] 为 200 ppm 时,S-nZVI 和 Pd-nZVI 的电子效率分别增加了 24.9%和 79.3%。由于析氢反应(HER)比 TCE 脱氯对表面钝化更敏感,因此碱性条件下 S-nZVI 和 Pd-nZVI 的电子效率高于碱性条件下的电子效率,在 pH 值为 10 时,分别比在 pH 值为 6 时增加了 11.7%和 37.8%。电子效率也随着 S-nZVI 和 Pd-nZVI 颗粒的老化时间而增加;与新鲜颗粒相比,老化 30 天时,分别增加了 27.2%和 59.6%。两种颗粒在人工地下水(AGW)中的电子效率均高于实际地下水(RGW)。对于所有批次实验,S-nZVI 的电子效率随反应时间增加,并趋于优于 Pd-nZVI 的电子效率,尽管在 TCE 脱氯的初始阶段,Pd-nZVI 的电子效率高于 S-nZVI,但 S-nZVI 的电子效率仍具有更长的使用寿命。

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