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采用负载纳米 Fe/Pd 双金属沸石高效修复地下水同时污染的 Cr(VI)和硝酸盐:工艺产物与相互作用机制。

Highly efficient remediation of groundwater co-contaminated with Cr(VI) and nitrate by using nano-Fe/Pd bimetal-loaded zeolite: Process product and interaction mechanism.

机构信息

School of Energy and Environmental Engineering, University of Science and Technology Beijing, Beijing 100083, China; Beijing Key Laboratory on Resource-oriented Treatment of Industrial Pollutants, Beijing 100083, China.

School of Energy and Environmental Engineering, University of Science and Technology Beijing, Beijing 100083, China; Beijing Key Laboratory on Resource-oriented Treatment of Industrial Pollutants, Beijing 100083, China.

出版信息

Environ Pollut. 2020 Aug;263(Pt A):114479. doi: 10.1016/j.envpol.2020.114479. Epub 2020 Apr 1.

Abstract

Hexavalent chromium and nitrate co-contaminated groundwater remediation are attracting extensive attention worldwide. However, the transformation pathways of chromium and nitrate and the interplay mechanism between them remain unclear. In this work, zeolite-supported nanoscale zero-valent iron/palladium (Z-Fe/Pd) was synthesized and used for the first time to simultaneously remediate Cr(VI) and nitrate. Transmission electron microscopy, X-ray diffraction, and X-ray photoelectron spectroscopy analyses confirmed that nanoscale zero-valent iron/palladium was successfully loaded onto zeolite and it exhibited good dispersibility and oxidation resistance. Results of batch experiments showed that the Cr(VI) and nitrate removal efficiencies decreased from 95.5% to 91.5% to 45% and 73%, respectively, with the initial solution pH increasing from 3.0 to 8.0. The removal rates and efficiencies of Cr(VI) and nitrate under anoxic conditions were higher than those under open atmosphere because the dissolved oxygen diminished the electron selectivity toward the target pollutants. Moreover, the presence of Cr(VI) inhibited nitrate reduction by forming Fe(III)-Cr(III) hydroxide to impede electron transfer. Cr(VI) removal was promoted by nitrate, within limits, by balancing the consumption and generation rate of FeO, which enhanced electron migration from the Fe(0) core to the external surface. The removal capacities of Cr(VI) and nitrate reached 121 and 95.5 mg g, respectively, which were superior to the removal capacities of similar materials. Results of product identification, XRD, and XPS analyses of spent Z-Fe/Pd indicated that the reduction of Cr(VI) was accompanied by adsorption and co-precipitation, whereas the reduction of nitrate was catalyzed by the synergism of Fe(0) and Pd(0). An alternative to the simultaneous remediation of Cr(VI) and nitrate from groundwater under anoxic conditions is provided.

摘要

六价铬和硝酸盐的地下水共污染修复正引起全世界的广泛关注。然而,铬和硝酸盐的转化途径及其相互作用机制仍不清楚。在这项工作中,沸石负载纳米零价铁/钯(Z-Fe/Pd)被首次合成并用于同时修复 Cr(VI)和硝酸盐。透射电子显微镜、X 射线衍射和 X 射线光电子能谱分析证实,纳米零价铁/钯成功负载到沸石上,具有良好的分散性和抗氧化性。批实验结果表明,Cr(VI)和硝酸盐的去除效率分别从 95.5%降至 91.5%至 45%和 73%,初始溶液 pH 值从 3.0 增至 8.0。缺氧条件下 Cr(VI)和硝酸盐的去除速率和效率均高于开放大气条件下的,因为溶解氧降低了电子对目标污染物的选择性。此外,Cr(VI)的存在通过形成 Fe(III)-Cr(III)氢氧化物来抑制硝酸盐还原,从而阻碍电子转移,从而抑制硝酸盐还原。在一定范围内,Cr(VI)的去除促进了硝酸盐的还原,通过平衡 FeO 的消耗和生成速率,增强了电子从 Fe(0)核向外部表面的迁移。Cr(VI)和硝酸盐的去除容量分别达到 121 和 95.5mg/g,优于类似材料的去除容量。对使用后的 Z-Fe/Pd 的产物鉴定、XRD 和 XPS 分析结果表明,Cr(VI)的还原伴随着吸附和共沉淀,而硝酸盐的还原则是由 Fe(0)和 Pd(0)的协同作用催化的。为缺氧条件下地下水同时修复 Cr(VI)和硝酸盐提供了一种替代方法。

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