A Recyclable Magnetic Aminated Lignin Supported Zr-La Dual-Metal Hydroxide for Rapid Separation and Highly Efficient Sequestration of Phosphate

The application of lignin-based adsorbents in the efficient removal of phosphate from wastewater has attracted much attention and been intensively studied in recent years. However, most currently reported lignin-based adsorbents are difficult to recover and recycle. Herein, we have developed a recyc...

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Main Authors: Enmin Zong, Xuanren Wang, Lirong Zhang, Jiayao Yang, Xiaohuan Liu
Format: Article
Language:English
Published: MDPI AG 2023-03-01
Series:Molecules
Subjects:
Online Access:https://www.mdpi.com/1420-3049/28/7/2923
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author Enmin Zong
Xuanren Wang
Lirong Zhang
Jiayao Yang
Xiaohuan Liu
author_facet Enmin Zong
Xuanren Wang
Lirong Zhang
Jiayao Yang
Xiaohuan Liu
author_sort Enmin Zong
collection DOAJ
description The application of lignin-based adsorbents in the efficient removal of phosphate from wastewater has attracted much attention and been intensively studied in recent years. However, most currently reported lignin-based adsorbents are difficult to recover and recycle. Herein, we have developed a recyclable, nanostructured bio-adsorbent, poly(ethyleneimine) (PEI)-modified lignin (LG) integrated with Fe<sub>3</sub>O<sub>4</sub> and Zr-La dual-metal hydroxide (LG-NH<sub>2</sub>@Fe<sub>3</sub>O<sub>4</sub>@Zr-La), by the Mannich reaction followed by the chemical coprecipitation method. Multilayer adsorption existed on the surface of LG-NH<sub>2</sub>@Fe<sub>3</sub>O<sub>4</sub>@Zr-La based on the isotherm fitting curve, and its adsorption capacity reached 57.8 mg P g<sup>−1</sup>, exhibiting a higher phosphate uptake than most reported metallic oxide-based composites. The adsorption process was dominated by inner-sphere complexation of ligand-exchange and electrostatic interactions. Moreover, LG-NH<sub>2</sub>@Fe<sub>3</sub>O<sub>4</sub>@Zr-La exhibited excellent selectivity against coexisting anions, and the adsorption was more efficient under acidic conditions. When the phosphate concentration was 2.0 mg P L<sup>−1</sup>, the removal efficiency of phosphate reached 99.5% and the residual concentration was only 10 μg P L<sup>−1</sup>, which meets the United States Environmental Protection Agency (USEPA) standard for eutrophication prevention. In addition, the LG-NH<sub>2</sub>@Fe<sub>3</sub>O<sub>4</sub>@Zr-La displayed excellent reusability, maintaining 91.8% of removal efficiency after five cycles. Importantly, owing to the magnetic properties of the loaded Fe<sub>3</sub>O<sub>4</sub>, the resulting composite could be separated within 30 s under an external magnetic field. Thus, the separable and recyclable biobased magnetic adsorbent developed in this work exhibited promising application in phosphate capture from real sewage. This research study provides a new perspective for lignin valorization in lignocellulose biorefineries and establishes an approach for developing an economical and efficient bio-adsorbent for phosphate removal from wastewater.
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spelling doaj.art-298c3d8093554308b97a971dbb0628032023-11-17T17:11:03ZengMDPI AGMolecules1420-30492023-03-01287292310.3390/molecules28072923A Recyclable Magnetic Aminated Lignin Supported Zr-La Dual-Metal Hydroxide for Rapid Separation and Highly Efficient Sequestration of PhosphateEnmin Zong0Xuanren Wang1Lirong Zhang2Jiayao Yang3Xiaohuan Liu4College of Life Science, Zhejiang Provincial Key Laboratory of Plant Evolutionary Ecology and Conservation, Taizhou University, 1139 Shifu Street, Taizhou 318000, ChinaCollege of Life Science, Zhejiang Provincial Key Laboratory of Plant Evolutionary Ecology and Conservation, Taizhou University, 1139 Shifu Street, Taizhou 318000, ChinaCollege of Life Science, Zhejiang Provincial Key Laboratory of Plant Evolutionary Ecology and Conservation, Taizhou University, 1139 Shifu Street, Taizhou 318000, ChinaSchool of Biological and Chemical Engineering, Zhejiang University of Science and Technology, Hangzhou 310023, ChinaCollege of Life Science, Zhejiang Provincial Key Laboratory of Plant Evolutionary Ecology and Conservation, Taizhou University, 1139 Shifu Street, Taizhou 318000, ChinaThe application of lignin-based adsorbents in the efficient removal of phosphate from wastewater has attracted much attention and been intensively studied in recent years. However, most currently reported lignin-based adsorbents are difficult to recover and recycle. Herein, we have developed a recyclable, nanostructured bio-adsorbent, poly(ethyleneimine) (PEI)-modified lignin (LG) integrated with Fe<sub>3</sub>O<sub>4</sub> and Zr-La dual-metal hydroxide (LG-NH<sub>2</sub>@Fe<sub>3</sub>O<sub>4</sub>@Zr-La), by the Mannich reaction followed by the chemical coprecipitation method. Multilayer adsorption existed on the surface of LG-NH<sub>2</sub>@Fe<sub>3</sub>O<sub>4</sub>@Zr-La based on the isotherm fitting curve, and its adsorption capacity reached 57.8 mg P g<sup>−1</sup>, exhibiting a higher phosphate uptake than most reported metallic oxide-based composites. The adsorption process was dominated by inner-sphere complexation of ligand-exchange and electrostatic interactions. Moreover, LG-NH<sub>2</sub>@Fe<sub>3</sub>O<sub>4</sub>@Zr-La exhibited excellent selectivity against coexisting anions, and the adsorption was more efficient under acidic conditions. When the phosphate concentration was 2.0 mg P L<sup>−1</sup>, the removal efficiency of phosphate reached 99.5% and the residual concentration was only 10 μg P L<sup>−1</sup>, which meets the United States Environmental Protection Agency (USEPA) standard for eutrophication prevention. In addition, the LG-NH<sub>2</sub>@Fe<sub>3</sub>O<sub>4</sub>@Zr-La displayed excellent reusability, maintaining 91.8% of removal efficiency after five cycles. Importantly, owing to the magnetic properties of the loaded Fe<sub>3</sub>O<sub>4</sub>, the resulting composite could be separated within 30 s under an external magnetic field. Thus, the separable and recyclable biobased magnetic adsorbent developed in this work exhibited promising application in phosphate capture from real sewage. This research study provides a new perspective for lignin valorization in lignocellulose biorefineries and establishes an approach for developing an economical and efficient bio-adsorbent for phosphate removal from wastewater.https://www.mdpi.com/1420-3049/28/7/2923ligninmagnetic adsorbentZr hydroxidesLa hydroxidesphosphaterecycle
spellingShingle Enmin Zong
Xuanren Wang
Lirong Zhang
Jiayao Yang
Xiaohuan Liu
A Recyclable Magnetic Aminated Lignin Supported Zr-La Dual-Metal Hydroxide for Rapid Separation and Highly Efficient Sequestration of Phosphate
Molecules
lignin
magnetic adsorbent
Zr hydroxides
La hydroxides
phosphate
recycle
title A Recyclable Magnetic Aminated Lignin Supported Zr-La Dual-Metal Hydroxide for Rapid Separation and Highly Efficient Sequestration of Phosphate
title_full A Recyclable Magnetic Aminated Lignin Supported Zr-La Dual-Metal Hydroxide for Rapid Separation and Highly Efficient Sequestration of Phosphate
title_fullStr A Recyclable Magnetic Aminated Lignin Supported Zr-La Dual-Metal Hydroxide for Rapid Separation and Highly Efficient Sequestration of Phosphate
title_full_unstemmed A Recyclable Magnetic Aminated Lignin Supported Zr-La Dual-Metal Hydroxide for Rapid Separation and Highly Efficient Sequestration of Phosphate
title_short A Recyclable Magnetic Aminated Lignin Supported Zr-La Dual-Metal Hydroxide for Rapid Separation and Highly Efficient Sequestration of Phosphate
title_sort recyclable magnetic aminated lignin supported zr la dual metal hydroxide for rapid separation and highly efficient sequestration of phosphate
topic lignin
magnetic adsorbent
Zr hydroxides
La hydroxides
phosphate
recycle
url https://www.mdpi.com/1420-3049/28/7/2923
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