Yi Yang, Xintong You, Shuo Tang, Ying Li, Minyi Liu, Ying Mei, Wei Shu
{"title":"创新型 La-Fe-CNT 膜对磷酸盐的吸收:结构-活性相关性与机理研究","authors":"Yi Yang, Xintong You, Shuo Tang, Ying Li, Minyi Liu, Ying Mei, Wei Shu","doi":"10.1021/acsestengg.4c00321","DOIUrl":null,"url":null,"abstract":"Eutrophication caused by excessive phosphorus pollution not only brings a series of environmental problems but also threatens biological safety. The adsorption method has been widely used for preventing eutrophication due to its high selectivity, environmental friendliness, easy operation, and cost-effectiveness. In this study, an easily separated magnetic lanthanum and iron-fabricated carbon nanotube (La–Fe–CNT) membrane was synthesized by a simple combined impregnation and vacuum filtration method for highly effective phosphate uptake. Characterization results show that metallic (hydr)oxide species were successfully fabricated on the CNT membrane, and phosphate was absorbed on it. The structure-activity correlation of La–Fe–CNT was quantitatively investigated by the Box–Behnken design model, and the following optimized conditions were obtained: a reaction temperature of 44 °C, synthesis time of 14.3 h, and La molar ratio of 0.53, with an adsorption capacity of 127 mg/g. La–Fe–CNT performs well over a wide pH range (142 mg/g at pH 2) with high stability (less than 2 mg/L metal leaching). Three interactions exist during the adsorption process, including electrostatic interactions, ligand exchange, and Lewis acid–base interactions. A kinetic study shows that the phosphate adsorption process is a physical-chemical process with combined intraparticle and surface film diffusion. The equilibrium phosphate adsorption capacity of La–Fe–CNT in the isotherm study is 120.2 mg/g, and the phosphate uptake process involves a complex process including both Langmuir and Freundlich adsorption. The adsorbent still retains nearly 70% of its original capacity after 5 cycles of operation, depicting its stability and sustainability for potential industrial applications.","PeriodicalId":7008,"journal":{"name":"ACS ES&T engineering","volume":null,"pages":null},"PeriodicalIF":7.4000,"publicationDate":"2024-09-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Phosphate Uptake over the Innovative La–Fe–CNT Membrane: Structure-Activity Correlation and Mechanism Investigation\",\"authors\":\"Yi Yang, Xintong You, Shuo Tang, Ying Li, Minyi Liu, Ying Mei, Wei Shu\",\"doi\":\"10.1021/acsestengg.4c00321\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"Eutrophication caused by excessive phosphorus pollution not only brings a series of environmental problems but also threatens biological safety. The adsorption method has been widely used for preventing eutrophication due to its high selectivity, environmental friendliness, easy operation, and cost-effectiveness. In this study, an easily separated magnetic lanthanum and iron-fabricated carbon nanotube (La–Fe–CNT) membrane was synthesized by a simple combined impregnation and vacuum filtration method for highly effective phosphate uptake. Characterization results show that metallic (hydr)oxide species were successfully fabricated on the CNT membrane, and phosphate was absorbed on it. The structure-activity correlation of La–Fe–CNT was quantitatively investigated by the Box–Behnken design model, and the following optimized conditions were obtained: a reaction temperature of 44 °C, synthesis time of 14.3 h, and La molar ratio of 0.53, with an adsorption capacity of 127 mg/g. La–Fe–CNT performs well over a wide pH range (142 mg/g at pH 2) with high stability (less than 2 mg/L metal leaching). Three interactions exist during the adsorption process, including electrostatic interactions, ligand exchange, and Lewis acid–base interactions. A kinetic study shows that the phosphate adsorption process is a physical-chemical process with combined intraparticle and surface film diffusion. The equilibrium phosphate adsorption capacity of La–Fe–CNT in the isotherm study is 120.2 mg/g, and the phosphate uptake process involves a complex process including both Langmuir and Freundlich adsorption. The adsorbent still retains nearly 70% of its original capacity after 5 cycles of operation, depicting its stability and sustainability for potential industrial applications.\",\"PeriodicalId\":7008,\"journal\":{\"name\":\"ACS ES&T engineering\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":7.4000,\"publicationDate\":\"2024-09-13\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"ACS ES&T engineering\",\"FirstCategoryId\":\"1085\",\"ListUrlMain\":\"https://doi.org/10.1021/acsestengg.4c00321\",\"RegionNum\":0,\"RegionCategory\":null,\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"ENGINEERING, ENVIRONMENTAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"ACS ES&T engineering","FirstCategoryId":"1085","ListUrlMain":"https://doi.org/10.1021/acsestengg.4c00321","RegionNum":0,"RegionCategory":null,"ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"ENGINEERING, ENVIRONMENTAL","Score":null,"Total":0}
Phosphate Uptake over the Innovative La–Fe–CNT Membrane: Structure-Activity Correlation and Mechanism Investigation
Eutrophication caused by excessive phosphorus pollution not only brings a series of environmental problems but also threatens biological safety. The adsorption method has been widely used for preventing eutrophication due to its high selectivity, environmental friendliness, easy operation, and cost-effectiveness. In this study, an easily separated magnetic lanthanum and iron-fabricated carbon nanotube (La–Fe–CNT) membrane was synthesized by a simple combined impregnation and vacuum filtration method for highly effective phosphate uptake. Characterization results show that metallic (hydr)oxide species were successfully fabricated on the CNT membrane, and phosphate was absorbed on it. The structure-activity correlation of La–Fe–CNT was quantitatively investigated by the Box–Behnken design model, and the following optimized conditions were obtained: a reaction temperature of 44 °C, synthesis time of 14.3 h, and La molar ratio of 0.53, with an adsorption capacity of 127 mg/g. La–Fe–CNT performs well over a wide pH range (142 mg/g at pH 2) with high stability (less than 2 mg/L metal leaching). Three interactions exist during the adsorption process, including electrostatic interactions, ligand exchange, and Lewis acid–base interactions. A kinetic study shows that the phosphate adsorption process is a physical-chemical process with combined intraparticle and surface film diffusion. The equilibrium phosphate adsorption capacity of La–Fe–CNT in the isotherm study is 120.2 mg/g, and the phosphate uptake process involves a complex process including both Langmuir and Freundlich adsorption. The adsorbent still retains nearly 70% of its original capacity after 5 cycles of operation, depicting its stability and sustainability for potential industrial applications.
期刊介绍:
ACS ES&T Engineering publishes impactful research and review articles across all realms of environmental technology and engineering, employing a rigorous peer-review process. As a specialized journal, it aims to provide an international platform for research and innovation, inviting contributions on materials technologies, processes, data analytics, and engineering systems that can effectively manage, protect, and remediate air, water, and soil quality, as well as treat wastes and recover resources.
The journal encourages research that supports informed decision-making within complex engineered systems and is grounded in mechanistic science and analytics, describing intricate environmental engineering systems. It considers papers presenting novel advancements, spanning from laboratory discovery to field-based application. However, case or demonstration studies lacking significant scientific advancements and technological innovations are not within its scope.
Contributions containing experimental and/or theoretical methods, rooted in engineering principles and integrated with knowledge from other disciplines, are welcomed.