Xing Yan, Baile Wu*, Yanyang Zhang*, Zhichao Yang, Mengjie Zhou, Paul Westerhoff and Bingcai Pan,
{"title":"镧材料可催化水解磷酸酯:对水处理和富营养化控制的影响","authors":"Xing Yan, Baile Wu*, Yanyang Zhang*, Zhichao Yang, Mengjie Zhou, Paul Westerhoff and Bingcai Pan, ","doi":"10.1021/acs.estlett.4c0016410.1021/acs.estlett.4c00164","DOIUrl":null,"url":null,"abstract":"<p >In the context of comprehensive phosphorus (P) management, in addition to orthophosphate, the environmental fate and regulation of potentially harmful phosphate esters are an emerging concern. However, there is still a discernible knowledge gap on the interaction between phosphate esters and Lanthanum (La) based materials, a widely applicable phosphate scavenger, under environmentally relevant conditions. In this study, we observed that La(OH)<sub>3</sub> and La<sub>2</sub>O<sub>3</sub> enable catalytic hydrolysis of a model phosphate ester compound, <i>para</i>-nitrophenyl phosphate (<i>p</i>-NPP) (20–70 times faster than self-hydrolysis), in environmentally relevant scenarios (wastewater and natural waters). <sup>31</sup>P solid-state NMR reveals an initial surface adsorption via a Lewis acid–base reaction between the surface La active sites and the phosphate groups, followed by the cleavage of the ester bond and the progressive transformation of phosphate further bound into crystalline LaPO<sub>4</sub>. Density functional theory computation suggested the electron enrichment on the P atom after <i>p</i>-NPP adsorption, resulting in the reduction of activation energy. Also, La(OH)<sub>3</sub> is extendable to catalytic hydrolysis of a suite of phosphate mono-, di-, and triesters. This study bridges the knowledge gap on the transformation of phosphate esters in the presence of lanthanum-based materials during water pollution control.</p>","PeriodicalId":37,"journal":{"name":"Environmental Science & Technology Letters Environ.","volume":"11 8","pages":"878–885 878–885"},"PeriodicalIF":8.9000,"publicationDate":"2024-05-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Lanthanum Materials Enable Catalytic Hydrolysis of Phosphate Esters: Implications for Water Treatment and Eutrophication Control\",\"authors\":\"Xing Yan, Baile Wu*, Yanyang Zhang*, Zhichao Yang, Mengjie Zhou, Paul Westerhoff and Bingcai Pan, \",\"doi\":\"10.1021/acs.estlett.4c0016410.1021/acs.estlett.4c00164\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p >In the context of comprehensive phosphorus (P) management, in addition to orthophosphate, the environmental fate and regulation of potentially harmful phosphate esters are an emerging concern. However, there is still a discernible knowledge gap on the interaction between phosphate esters and Lanthanum (La) based materials, a widely applicable phosphate scavenger, under environmentally relevant conditions. In this study, we observed that La(OH)<sub>3</sub> and La<sub>2</sub>O<sub>3</sub> enable catalytic hydrolysis of a model phosphate ester compound, <i>para</i>-nitrophenyl phosphate (<i>p</i>-NPP) (20–70 times faster than self-hydrolysis), in environmentally relevant scenarios (wastewater and natural waters). <sup>31</sup>P solid-state NMR reveals an initial surface adsorption via a Lewis acid–base reaction between the surface La active sites and the phosphate groups, followed by the cleavage of the ester bond and the progressive transformation of phosphate further bound into crystalline LaPO<sub>4</sub>. Density functional theory computation suggested the electron enrichment on the P atom after <i>p</i>-NPP adsorption, resulting in the reduction of activation energy. Also, La(OH)<sub>3</sub> is extendable to catalytic hydrolysis of a suite of phosphate mono-, di-, and triesters. This study bridges the knowledge gap on the transformation of phosphate esters in the presence of lanthanum-based materials during water pollution control.</p>\",\"PeriodicalId\":37,\"journal\":{\"name\":\"Environmental Science & Technology Letters Environ.\",\"volume\":\"11 8\",\"pages\":\"878–885 878–885\"},\"PeriodicalIF\":8.9000,\"publicationDate\":\"2024-05-13\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Environmental Science & Technology Letters Environ.\",\"FirstCategoryId\":\"1\",\"ListUrlMain\":\"https://pubs.acs.org/doi/10.1021/acs.estlett.4c00164\",\"RegionNum\":2,\"RegionCategory\":\"环境科学与生态学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"ENGINEERING, ENVIRONMENTAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Environmental Science & Technology Letters Environ.","FirstCategoryId":"1","ListUrlMain":"https://pubs.acs.org/doi/10.1021/acs.estlett.4c00164","RegionNum":2,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"ENGINEERING, ENVIRONMENTAL","Score":null,"Total":0}
Lanthanum Materials Enable Catalytic Hydrolysis of Phosphate Esters: Implications for Water Treatment and Eutrophication Control
In the context of comprehensive phosphorus (P) management, in addition to orthophosphate, the environmental fate and regulation of potentially harmful phosphate esters are an emerging concern. However, there is still a discernible knowledge gap on the interaction between phosphate esters and Lanthanum (La) based materials, a widely applicable phosphate scavenger, under environmentally relevant conditions. In this study, we observed that La(OH)3 and La2O3 enable catalytic hydrolysis of a model phosphate ester compound, para-nitrophenyl phosphate (p-NPP) (20–70 times faster than self-hydrolysis), in environmentally relevant scenarios (wastewater and natural waters). 31P solid-state NMR reveals an initial surface adsorption via a Lewis acid–base reaction between the surface La active sites and the phosphate groups, followed by the cleavage of the ester bond and the progressive transformation of phosphate further bound into crystalline LaPO4. Density functional theory computation suggested the electron enrichment on the P atom after p-NPP adsorption, resulting in the reduction of activation energy. Also, La(OH)3 is extendable to catalytic hydrolysis of a suite of phosphate mono-, di-, and triesters. This study bridges the knowledge gap on the transformation of phosphate esters in the presence of lanthanum-based materials during water pollution control.
期刊介绍:
Environmental Science & Technology Letters serves as an international forum for brief communications on experimental or theoretical results of exceptional timeliness in all aspects of environmental science, both pure and applied. Published as soon as accepted, these communications are summarized in monthly issues. Additionally, the journal features short reviews on emerging topics in environmental science and technology.