Brumovský Miroslav, Micić Vesna, Oborná Jana, Filip Jan, Hofmann Thilo, Tunega Daniel
University of Natural Resources and Life Sciences, Vienna, Department of Forest, and Soil Sciences, Institute of Soil Research, Peter-Jordan-Straße 82, 1190 Vienna, Austria; Department of Environmental Geosciences (EDGE), Centre for Microbiology and Environmental Systems Science, University of Vienna, Josef-Holaubek-Platz 2, UZA II, 1090 Vienna, Austria; Regional Centre of Advanced Technologies and Materials, Czech Advanced Technology and Research Institute (CATRIN), Palacký University, Šlechtitelů 27, 779 00 Olomouc, Czech Republic.
Department of Environmental Geosciences (EDGE), Centre for Microbiology and Environmental Systems Science, University of Vienna, Josef-Holaubek-Platz 2, UZA II, 1090 Vienna, Austria.
J Hazard Mater. 2023 Jan 15;442:129988. doi: 10.1016/j.jhazmat.2022.129988. Epub 2022 Sep 15.
Sulfidation and, more recently, nitriding have been recognized as promising modifications to enhance the selectivity of nanoscale zero-valent iron (nZVI) particles for trichloroethene (TCE). Herein, we investigated the performance of iron nitride (FeN) nanoparticles in the removal of a broader range of chlorinated ethenes (CEs), including tetrachloroethene (PCE), cis-1,2-dichloroethene (cis-DCE), and their mixture with TCE, and compared it to the performance of sulfidated nZVI (S-nZVI) prepared from the same precursor nZVI. Two distinct types of iron nitride (FeN) nanoparticles, containing γ'-FeN and ε-FeN phases, exhibited substantially higher PCE and cis-DCE dechlorination rates compared to S-nZVI. A similar effect was observed with a CE mixture, which was completely dechlorinated by both types of FeN nanoparticles within 10 days, whereas S-nZVI was able to remove only about half of the amount, most of which being TCE. Density functional theory calculations further revealed that the cleavage of the first C-Cl bond was the rate-limiting step for all CEs dechlorinated on the γ'-FeN(001) surface, with the reaction barriers of PCE and cis-DCE being 29.9, and 40.8 kJ mol, respectively. FeN nanoparticles proved to be highly effective in the remediation of PCE, cis-DCE, and mixed CE contamination.
硫化以及最近的氮化已被认为是增强纳米级零价铁（nZVI）颗粒对三氯乙烯（TCE）选择性的有前景的改性方法。在此，我们研究了氮化铁（FeN）纳米颗粒在去除更广泛范围的氯代乙烯（CEs）方面的性能，包括四氯乙烯（PCE）、顺式 - 1,2 - 二氯乙烯（cis - DCE）以及它们与TCE的混合物，并将其与由相同前驱体nZVI制备的硫化nZVI（S - nZVI）的性能进行了比较。两种不同类型的氮化铁（FeN）纳米颗粒，包含γ'-FeN和ε - FeN相，与S - nZVI相比，表现出显著更高的PCE和顺式 - DCE脱氯速率。对于CE混合物也观察到了类似的效果，两种类型的FeN纳米颗粒在10天内都能将其完全脱氯，而S - nZVI只能去除大约一半的量，其中大部分是TCE。密度泛函理论计算进一步表明，第一个C - Cl键的断裂是在γ'-FeN(001)表面上所有CEs脱氯的速率限制步骤，PCE和顺式 - DCE的反应势垒分别为29.9和40.8 kJ/mol。事实证明，FeN纳米颗粒在修复PCE、顺式 - DCE和混合CE污染方面非常有效。
