{"title":"One-step self-assembled ZIF-derived flower-like carbon enhances reactivity of zero-valent iron during persulfate activation","authors":"","doi":"10.1016/j.seppur.2024.129844","DOIUrl":null,"url":null,"abstract":"<div><div>The sintering aggregation of carbon material (ZIF-N-C-600), as well as the tendency towards agglomeration and oxidation of zero-valent iron nanoparticles (Fe<sup>0</sup>) limit their applications in advanced oxidation processes. Hence, a flower-like Fe<sup>0</sup>@ZIF-N-C-600 was rationally constructed by facile one-step self-assembly to ameliorate peroxydisulfate (PDS) activation. The polyhedral ZIF-N-C-600 aggregates were exfoliated into thinner porous nanosheets and Fe<sup>0</sup> nanoparticles were effectively dispersed and anchored onto ZIF-N-C-600. 96.7 % of metronidazole (MNZ) was eliminated by the Fe<sup>0</sup>@ZIF-N-C-600/PDS system, and the removal reaction rate constant k values were 2 and 2.55 times as high as Fe<sup>0</sup>@ZIF/PDS and Fe<sup>0</sup>/PDS, respectively. Fe<sup>0</sup>, defective sites, C=O and pyridinic N were identified as the active sites promoting PDS activation to produce ·OH, SO<sub>4</sub>·<sup>-</sup>, ·O<sub>2</sub><sup>–</sup> and <sup>1</sup>O<sub>2</sub> for synergistic oxidative elimination of MNZ. The formation rate of ·OH was calculated to be 4.62 times higher than that of the SO<sub>4</sub>·<sup>-</sup> by multivariate nonlinear fitting, and the ·OH contributes up to 63.5 %. Fe<sup>0</sup>@ZIF-N-C-600/PDS system possesses excellent tolerance and selectivity to complicated water bodies, and the effective continuous degradation was achieved in a self-made catalytic reactor. Moreover, DFT calculations and LC-MS analysis were applied to deduce possible pathways for MNZ degradation. This work offers an effective strategy to regulate the morphology of sintered carbon materials and improve the application of metal nanoparticles in advanced oxidation processes.</div></div>","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":null,"pages":null},"PeriodicalIF":8.1000,"publicationDate":"2024-09-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Separation and Purification Technology","FirstCategoryId":"5","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S1383586624035834","RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"ENGINEERING, CHEMICAL","Score":null,"Total":0}
引用次数: 0
Abstract
The sintering aggregation of carbon material (ZIF-N-C-600), as well as the tendency towards agglomeration and oxidation of zero-valent iron nanoparticles (Fe0) limit their applications in advanced oxidation processes. Hence, a flower-like Fe0@ZIF-N-C-600 was rationally constructed by facile one-step self-assembly to ameliorate peroxydisulfate (PDS) activation. The polyhedral ZIF-N-C-600 aggregates were exfoliated into thinner porous nanosheets and Fe0 nanoparticles were effectively dispersed and anchored onto ZIF-N-C-600. 96.7 % of metronidazole (MNZ) was eliminated by the Fe0@ZIF-N-C-600/PDS system, and the removal reaction rate constant k values were 2 and 2.55 times as high as Fe0@ZIF/PDS and Fe0/PDS, respectively. Fe0, defective sites, C=O and pyridinic N were identified as the active sites promoting PDS activation to produce ·OH, SO4·-, ·O2– and 1O2 for synergistic oxidative elimination of MNZ. The formation rate of ·OH was calculated to be 4.62 times higher than that of the SO4·- by multivariate nonlinear fitting, and the ·OH contributes up to 63.5 %. Fe0@ZIF-N-C-600/PDS system possesses excellent tolerance and selectivity to complicated water bodies, and the effective continuous degradation was achieved in a self-made catalytic reactor. Moreover, DFT calculations and LC-MS analysis were applied to deduce possible pathways for MNZ degradation. This work offers an effective strategy to regulate the morphology of sintered carbon materials and improve the application of metal nanoparticles in advanced oxidation processes.
期刊介绍:
Separation and Purification Technology is a premier journal committed to sharing innovative methods for separation and purification in chemical and environmental engineering, encompassing both homogeneous solutions and heterogeneous mixtures. Our scope includes the separation and/or purification of liquids, vapors, and gases, as well as carbon capture and separation techniques. However, it's important to note that methods solely intended for analytical purposes are not within the scope of the journal. Additionally, disciplines such as soil science, polymer science, and metallurgy fall outside the purview of Separation and Purification Technology. Join us in advancing the field of separation and purification methods for sustainable solutions in chemical and environmental engineering.