Qiangqiang Tao, Yuhe Bai, Li Wang, Tao Feng, Shuai Lu, Aixin Zhang, Kang Li, Ning Hu
{"title":"使用铈基高熵金属氧化物协同催化降解甲氨蝶呤:从 DFT 计算和 CWPO 性能中获得的启示","authors":"Qiangqiang Tao, Yuhe Bai, Li Wang, Tao Feng, Shuai Lu, Aixin Zhang, Kang Li, Ning Hu","doi":"10.1016/j.seppur.2024.130130","DOIUrl":null,"url":null,"abstract":"Methotrexate (MTX), a widely used anticancer drug, is a refractory organic pollutant posing serious threats to ecosystems and human health. This study focuses on the development of a novel catalyst composed of Ce-based high-entropy metal oxides (NHEMO) supported on nepheline for the catalytic wet peroxide oxidation (CWPO) process, targeting MTX degradation in simulated wastewater. The NHEMO catalyst exhibited a unique high-entropy structure that enhances catalytic performance by facilitating diverse electronic interactions, which was confirmed through X-ray diffraction (XRD) and transmission electron microscopy (TEM) analyses showing a well-defined crystal structure and uniform dispersion of metal oxides. Additionally, X-ray photoelectron spectroscopy (XPS) and energy-dispersive X-ray spectroscopy (EDS) revealed a stable metal composition and high oxidation states of active metal sites. At a reaction temperature of 160 °C, with a residence time of 150 s and an oxidation coefficient of 5, the catalyst achieved a MTX removal rate of 93.49 % and a chemical oxygen demand (COD) removal of 99.95 %. Density Functional Theory (DFT) calculations further demonstrated that H<sub>2</sub>O<sub>2</sub> decomposes into both adsorbed (surface-bound) and free (solution-phase) hydroxyl radicals (·OH). These radicals synergistically degrade MTX through both radical and non-radical pathways, ensuring comprehensive pollutant breakdown. The catalyst also showed excellent stability and a very low metal dissolution rate during the reaction, maintaining high catalytic activity after repeated recycling. This catalyst offers high cost-effectiveness, activity, and stability, providing a promising solution for treating refractory organic pollutants in pharmaceutical wastewater.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":null,"pages":null},"PeriodicalIF":8.1000,"publicationDate":"2024-10-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Synergistic catalytic degradation of Methotrexate using Ce-based high-entropy metal oxides: Insights from DFT calculations and CWPO performance\",\"authors\":\"Qiangqiang Tao, Yuhe Bai, Li Wang, Tao Feng, Shuai Lu, Aixin Zhang, Kang Li, Ning Hu\",\"doi\":\"10.1016/j.seppur.2024.130130\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"Methotrexate (MTX), a widely used anticancer drug, is a refractory organic pollutant posing serious threats to ecosystems and human health. This study focuses on the development of a novel catalyst composed of Ce-based high-entropy metal oxides (NHEMO) supported on nepheline for the catalytic wet peroxide oxidation (CWPO) process, targeting MTX degradation in simulated wastewater. The NHEMO catalyst exhibited a unique high-entropy structure that enhances catalytic performance by facilitating diverse electronic interactions, which was confirmed through X-ray diffraction (XRD) and transmission electron microscopy (TEM) analyses showing a well-defined crystal structure and uniform dispersion of metal oxides. Additionally, X-ray photoelectron spectroscopy (XPS) and energy-dispersive X-ray spectroscopy (EDS) revealed a stable metal composition and high oxidation states of active metal sites. At a reaction temperature of 160 °C, with a residence time of 150 s and an oxidation coefficient of 5, the catalyst achieved a MTX removal rate of 93.49 % and a chemical oxygen demand (COD) removal of 99.95 %. Density Functional Theory (DFT) calculations further demonstrated that H<sub>2</sub>O<sub>2</sub> decomposes into both adsorbed (surface-bound) and free (solution-phase) hydroxyl radicals (·OH). These radicals synergistically degrade MTX through both radical and non-radical pathways, ensuring comprehensive pollutant breakdown. The catalyst also showed excellent stability and a very low metal dissolution rate during the reaction, maintaining high catalytic activity after repeated recycling. This catalyst offers high cost-effectiveness, activity, and stability, providing a promising solution for treating refractory organic pollutants in pharmaceutical wastewater.\",\"PeriodicalId\":427,\"journal\":{\"name\":\"Separation and Purification Technology\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":8.1000,\"publicationDate\":\"2024-10-17\",\"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://doi.org/10.1016/j.seppur.2024.130130\",\"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}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Separation and Purification Technology","FirstCategoryId":"5","ListUrlMain":"https://doi.org/10.1016/j.seppur.2024.130130","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}
Synergistic catalytic degradation of Methotrexate using Ce-based high-entropy metal oxides: Insights from DFT calculations and CWPO performance
Methotrexate (MTX), a widely used anticancer drug, is a refractory organic pollutant posing serious threats to ecosystems and human health. This study focuses on the development of a novel catalyst composed of Ce-based high-entropy metal oxides (NHEMO) supported on nepheline for the catalytic wet peroxide oxidation (CWPO) process, targeting MTX degradation in simulated wastewater. The NHEMO catalyst exhibited a unique high-entropy structure that enhances catalytic performance by facilitating diverse electronic interactions, which was confirmed through X-ray diffraction (XRD) and transmission electron microscopy (TEM) analyses showing a well-defined crystal structure and uniform dispersion of metal oxides. Additionally, X-ray photoelectron spectroscopy (XPS) and energy-dispersive X-ray spectroscopy (EDS) revealed a stable metal composition and high oxidation states of active metal sites. At a reaction temperature of 160 °C, with a residence time of 150 s and an oxidation coefficient of 5, the catalyst achieved a MTX removal rate of 93.49 % and a chemical oxygen demand (COD) removal of 99.95 %. Density Functional Theory (DFT) calculations further demonstrated that H2O2 decomposes into both adsorbed (surface-bound) and free (solution-phase) hydroxyl radicals (·OH). These radicals synergistically degrade MTX through both radical and non-radical pathways, ensuring comprehensive pollutant breakdown. The catalyst also showed excellent stability and a very low metal dissolution rate during the reaction, maintaining high catalytic activity after repeated recycling. This catalyst offers high cost-effectiveness, activity, and stability, providing a promising solution for treating refractory organic pollutants in pharmaceutical wastewater.
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.