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双功能催化降解双氯芬酸过 Cu-Pd 共改性海绵铁基三金属:参数优化。

Bifunctional catalytic degradation of diclofenac over Cu-Pd co-modified sponge iron-based trimetal: Parameter optimization.

机构信息

School of Civil Engineering, Southeast University, Nanjing, 210096, PR China.

School of Civil Engineering, Southeast University, Nanjing, 210096, PR China; Ecological Environment Monitoring Center of Eastern China, Nanjing Institute of Environmental Sciences, Ministry of Ecology and Environment (MEE), Nanjing, 210042, PR China.

出版信息

Environ Res. 2023 Jun 15;227:115640. doi: 10.1016/j.envres.2023.115640. Epub 2023 Mar 17.

DOI:10.1016/j.envres.2023.115640
PMID:36933636
Abstract

Currently, the pharmaceutical and personal care products (PPCPs) have posed great challenge to advanced oxidation techniques (AOTs). In this study, we decorated sponge iron (s-Fe) with Cu and Pd (s-Fe-Cu-Pd) and further optimized the synthesis parameters with a response surface method (RSM) to rapidly degrade diclofenac sodium (DCF). Under the RSM-optimized conditions of Fe: Cu: Pd = 100: 4.23: 0.10, initial solution pH of 5.13, and input dosage of 38.8 g/L, 99% removal of DCF could be obtained after 60 min of reaction. Moreover, the morphological structure of trimetal was characterized with high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM), X-ray diffraction (XRD), X-ray photoelectron spectra (XPS). Electron spin resonance (ESR) signals have also been applied to capture reactive hydrogen atoms (H*), superoxygen anions, hydroxyl radicals, and single state oxygen (O). Furthermore, the variations of DCF and its selective degradation products over a series of s-Fe-based bi(tri)metals have been compared. Additionally, the degradation mechanism of DCF has also been explored. To our best knowledge, this is the first report revealing the selective dechlorination of DCF with low toxicity over Pd-Cu co-doped s-Fe trimetal.

摘要

目前,药物和个人护理产品(PPCPs)对高级氧化技术(AOTs)构成了巨大挑战。在这项研究中,我们用铜和钯修饰了海绵铁(s-Fe),并用响应面法(RSM)进一步优化了合成参数,以快速降解双氯芬酸钠(DCF)。在 RSM 优化条件下,Fe:Cu:Pd = 100:4.23:0.10,初始溶液 pH 值为 5.13,输入剂量为 38.8 g/L,反应 60 min 后可获得 99%的 DCF 去除率。此外,还采用高角度环形暗场扫描透射电子显微镜(HAADF-STEM)、X 射线衍射(XRD)、X 射线光电子能谱(XPS)对三元体的形态结构进行了表征。电子顺磁共振(ESR)信号也被用来捕获反应性氢原子(H*)、超氧阴离子、羟基自由基和单重态氧(O)。此外,还比较了一系列基于 s-Fe 的双(三)金属对 DCF 及其选择性降解产物的变化。此外,还探讨了 DCF 的降解机制。据我们所知,这是首次报道 Pd-Cu 共掺杂 s-Fe 三元体对低毒性 DCF 具有选择性脱氯作用。

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