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

IF 8.9 2区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Environmental Science & Technology Letters Environ. Pub Date : 2024-05-13 DOI:10.1021/acs.estlett.4c0016410.1021/acs.estlett.4c00164
Xing Yan, Baile Wu*, Yanyang Zhang*, Zhichao Yang, Mengjie Zhou, Paul Westerhoff and Bingcai Pan, 
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引用次数: 0

摘要

在磷(P)综合管理的背景下,除了正磷酸盐之外,潜在有害的磷酸酯的环境归宿和监管也是一个新出现的问题。然而,对于磷酸酯与镧基(La)材料(一种广泛应用的磷酸盐清除剂)在环境相关条件下的相互作用,仍然存在明显的知识空白。在本研究中,我们观察到 La(OH)3 和 La2O3 能够在环境相关情景(废水和自然水域)中催化磷酸酯化合物对硝基苯磷酸酯(p-NPP)的水解(比自水解快 20-70 倍)。31P 固态核磁共振显示,最初的表面吸附是通过表面 La 活性位点与磷酸基团之间的路易斯酸碱反应进行的,随后酯键被裂解,磷酸进一步结合成结晶状的 LaPO4。密度泛函理论计算表明,p-NPP 吸附后,P 原子上的电子富集,从而降低了活化能。此外,La(OH)3 还可用于催化水解一系列磷酸单酯、二酯和三酯。这项研究填补了水污染控制过程中磷酸酯在镧基材料存在下的转化方面的知识空白。
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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.

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来源期刊
Environmental Science & Technology Letters Environ.
Environmental Science & Technology Letters Environ. ENGINEERING, ENVIRONMENTALENVIRONMENTAL SC-ENVIRONMENTAL SCIENCES
CiteScore
17.90
自引率
3.70%
发文量
163
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.
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