Efficient entrapment and separation of anionic pollutants from aqueous solutions by sequential combination of cellulose nanofibrils and halloysite nanotubes

Tuula Selkälä, Terhi Suopajärvi, Juho Antti Sirviö, Tero Luukkonen, Paivo Kinnunen, Kirsten Inga Kling, Jakob Birkedal Wagner, Henrikki Liimatainen*

*Corresponding author for this work

Research output: Contribution to journalJournal articleResearchpeer-review

Abstract

The synergistic combination of different nanomaterials for improved performance in environmental applications such as the removal of aqueous micropollutants has attracted increasing interest in recent years. This study demonstrates a novel sequential adsorption–aggregation concept that harnesses tubular halloysite nanotubes (HNTs) and flexible cellulose nanofibrils (CNFs) for the removal of a small, anionic dye molecule, chrome azurol S, from water. Hollow HNTs were first allowed to interact with the aqueous dye solution, after which the dye-loaded colloidal nanotubes were aggregated and separated from the water phase with cationized CNFs. The combination of 25 mg CNFs with 1 g HNTs at pH 7 resulted in efficient removal of dye (80%) and turbidity (~100%) and the removal of dye was further promoted in more acidic conditions (within the pH range of 6–8.5) because of the attractive electrostatic interactions. Cationic CNFs not only enabled the separation of dye-loaded clay particles from the water phase through a rapid aggregation but also participated in dye removal through adsorption (~20%). In comparison with nano-sized HNTs, the dye removal performance of micro-sized and chemically similar kaolin was poor (43%). Given the good availability of both HNTs and CNFs and the low consumption of the more expensive component (i.e., CNFs) in the process, the concept is straightforward, readily applicable, environmentally benign, and potentially cost-effective.
Original languageEnglish
JournalChemical Engineering Journal
Volume374
Pages (from-to)1013-1024
ISSN1369-703X
DOIs
Publication statusPublished - 2019

Keywords

  • Deep eutectic solvent
  • Kaolin
  • Mordant blue 29
  • Nanocellulose
  • Nanoclay
  • Wastewater treatment

Cite this

Selkälä, Tuula ; Suopajärvi, Terhi ; Sirviö, Juho Antti ; Luukkonen, Tero ; Kinnunen, Paivo ; Kling, Kirsten Inga ; Wagner, Jakob Birkedal ; Liimatainen, Henrikki. / Efficient entrapment and separation of anionic pollutants from aqueous solutions by sequential combination of cellulose nanofibrils and halloysite nanotubes. In: Chemical Engineering Journal. 2019 ; Vol. 374. pp. 1013-1024.
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title = "Efficient entrapment and separation of anionic pollutants from aqueous solutions by sequential combination of cellulose nanofibrils and halloysite nanotubes",
abstract = "The synergistic combination of different nanomaterials for improved performance in environmental applications such as the removal of aqueous micropollutants has attracted increasing interest in recent years. This study demonstrates a novel sequential adsorption–aggregation concept that harnesses tubular halloysite nanotubes (HNTs) and flexible cellulose nanofibrils (CNFs) for the removal of a small, anionic dye molecule, chrome azurol S, from water. Hollow HNTs were first allowed to interact with the aqueous dye solution, after which the dye-loaded colloidal nanotubes were aggregated and separated from the water phase with cationized CNFs. The combination of 25 mg CNFs with 1 g HNTs at pH 7 resulted in efficient removal of dye (80{\%}) and turbidity (~100{\%}) and the removal of dye was further promoted in more acidic conditions (within the pH range of 6–8.5) because of the attractive electrostatic interactions. Cationic CNFs not only enabled the separation of dye-loaded clay particles from the water phase through a rapid aggregation but also participated in dye removal through adsorption (~20{\%}). In comparison with nano-sized HNTs, the dye removal performance of micro-sized and chemically similar kaolin was poor (43{\%}). Given the good availability of both HNTs and CNFs and the low consumption of the more expensive component (i.e., CNFs) in the process, the concept is straightforward, readily applicable, environmentally benign, and potentially cost-effective.",
keywords = "Deep eutectic solvent, Kaolin, Mordant blue 29, Nanocellulose, Nanoclay, Wastewater treatment",
author = "Tuula Selk{\"a}l{\"a} and Terhi Suopaj{\"a}rvi and Sirvi{\"o}, {Juho Antti} and Tero Luukkonen and Paivo Kinnunen and Kling, {Kirsten Inga} and Wagner, {Jakob Birkedal} and Henrikki Liimatainen",
year = "2019",
doi = "10.1016/j.cej.2019.06.008",
language = "English",
volume = "374",
pages = "1013--1024",
journal = "Biochemical Engineering Journal",
issn = "1369-703X",
publisher = "Elsevier",

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Efficient entrapment and separation of anionic pollutants from aqueous solutions by sequential combination of cellulose nanofibrils and halloysite nanotubes. / Selkälä, Tuula; Suopajärvi, Terhi; Sirviö, Juho Antti; Luukkonen, Tero; Kinnunen, Paivo; Kling, Kirsten Inga; Wagner, Jakob Birkedal; Liimatainen, Henrikki.

In: Chemical Engineering Journal, Vol. 374, 2019, p. 1013-1024.

Research output: Contribution to journalJournal articleResearchpeer-review

TY - JOUR

T1 - Efficient entrapment and separation of anionic pollutants from aqueous solutions by sequential combination of cellulose nanofibrils and halloysite nanotubes

AU - Selkälä, Tuula

AU - Suopajärvi, Terhi

AU - Sirviö, Juho Antti

AU - Luukkonen, Tero

AU - Kinnunen, Paivo

AU - Kling, Kirsten Inga

AU - Wagner, Jakob Birkedal

AU - Liimatainen, Henrikki

PY - 2019

Y1 - 2019

N2 - The synergistic combination of different nanomaterials for improved performance in environmental applications such as the removal of aqueous micropollutants has attracted increasing interest in recent years. This study demonstrates a novel sequential adsorption–aggregation concept that harnesses tubular halloysite nanotubes (HNTs) and flexible cellulose nanofibrils (CNFs) for the removal of a small, anionic dye molecule, chrome azurol S, from water. Hollow HNTs were first allowed to interact with the aqueous dye solution, after which the dye-loaded colloidal nanotubes were aggregated and separated from the water phase with cationized CNFs. The combination of 25 mg CNFs with 1 g HNTs at pH 7 resulted in efficient removal of dye (80%) and turbidity (~100%) and the removal of dye was further promoted in more acidic conditions (within the pH range of 6–8.5) because of the attractive electrostatic interactions. Cationic CNFs not only enabled the separation of dye-loaded clay particles from the water phase through a rapid aggregation but also participated in dye removal through adsorption (~20%). In comparison with nano-sized HNTs, the dye removal performance of micro-sized and chemically similar kaolin was poor (43%). Given the good availability of both HNTs and CNFs and the low consumption of the more expensive component (i.e., CNFs) in the process, the concept is straightforward, readily applicable, environmentally benign, and potentially cost-effective.

AB - The synergistic combination of different nanomaterials for improved performance in environmental applications such as the removal of aqueous micropollutants has attracted increasing interest in recent years. This study demonstrates a novel sequential adsorption–aggregation concept that harnesses tubular halloysite nanotubes (HNTs) and flexible cellulose nanofibrils (CNFs) for the removal of a small, anionic dye molecule, chrome azurol S, from water. Hollow HNTs were first allowed to interact with the aqueous dye solution, after which the dye-loaded colloidal nanotubes were aggregated and separated from the water phase with cationized CNFs. The combination of 25 mg CNFs with 1 g HNTs at pH 7 resulted in efficient removal of dye (80%) and turbidity (~100%) and the removal of dye was further promoted in more acidic conditions (within the pH range of 6–8.5) because of the attractive electrostatic interactions. Cationic CNFs not only enabled the separation of dye-loaded clay particles from the water phase through a rapid aggregation but also participated in dye removal through adsorption (~20%). In comparison with nano-sized HNTs, the dye removal performance of micro-sized and chemically similar kaolin was poor (43%). Given the good availability of both HNTs and CNFs and the low consumption of the more expensive component (i.e., CNFs) in the process, the concept is straightforward, readily applicable, environmentally benign, and potentially cost-effective.

KW - Deep eutectic solvent

KW - Kaolin

KW - Mordant blue 29

KW - Nanocellulose

KW - Nanoclay

KW - Wastewater treatment

U2 - 10.1016/j.cej.2019.06.008

DO - 10.1016/j.cej.2019.06.008

M3 - Journal article

VL - 374

SP - 1013

EP - 1024

JO - Biochemical Engineering Journal

JF - Biochemical Engineering Journal

SN - 1369-703X

ER -