Tris(2-benzimidazolyl)amine (NTB)-Modified Metal-Organic Framework: Preparation, Characterization, and Mercury Ion Removal Studies

Heavy metal ions (HMIs) are exceedingly hazardous to both humans and the environment, and the necessity to eliminate them from aqueous systems prompted the development of novel materials. In this study, tris(2-benzimidazolylmethyl)amine (NTB) was impregnated into MIL-101-(Cr) metal-organic framework...

Full description

Bibliographic Details
Main Authors: Phani Brahma Somayajulu Rallapalli, Suk Soon Choi, Hiresh Moradi, Jae-Kyu Yang, Jae-Hoon Lee, Jeong Hyub Ha
Format: Article
Language:English
Published: MDPI AG 2023-07-01
Series:Water
Subjects:
Online Access:https://www.mdpi.com/2073-4441/15/14/2559
_version_ 1797587153573642240
author Phani Brahma Somayajulu Rallapalli
Suk Soon Choi
Hiresh Moradi
Jae-Kyu Yang
Jae-Hoon Lee
Jeong Hyub Ha
author_facet Phani Brahma Somayajulu Rallapalli
Suk Soon Choi
Hiresh Moradi
Jae-Kyu Yang
Jae-Hoon Lee
Jeong Hyub Ha
author_sort Phani Brahma Somayajulu Rallapalli
collection DOAJ
description Heavy metal ions (HMIs) are exceedingly hazardous to both humans and the environment, and the necessity to eliminate them from aqueous systems prompted the development of novel materials. In this study, tris(2-benzimidazolylmethyl)amine (NTB) was impregnated into MIL-101-(Cr) metal-organic framework using an incipient wetness impregnation approach, and the ability of the composite material to adsorb Hg<sup>2+</sup> ions from the water was examined. The synthesized materials were analyzed with several physico-chemical techniques such as powder X-ray diffraction, elemental analysis, scanning electron microscopy, thermogravimetric analysis, nitrogen sorption isotherms at 77 K, and X-ray photoelectron spectrometry. MIL-101-NTB quickly adsorbs 93.9% of Hg<sup>2+</sup> ions within 10 min from a 10.0 ppm single ion solution. A better fit of the kinetic data to a pseudo-second-order model validated the chemisorption of Hg<sup>2+</sup> ions on MIL-101-NTB. The experimental data fitted well with the Langmuir isotherm model, and the maximum adsorption capacity obtained at 125 ppm initial concentration was 111.03 mg/g. Despite the presence of other competing ions (Cu<sup>2+</sup>, Pb<sup>2+</sup>, and Cd<sup>2+</sup>), high Hg<sup>2+</sup> ions removal efficiency (99.6%, 1.0 ppm initial concentration) was maintained in the diverse ion batch adsorption studies. A 0.2 M EDTA solution could desorb the Hg<sup>2+</sup> ions, and cyclic Hg<sup>2+</sup> ions sorption studies indicated that MIL-101-NTB might have a high Hg<sup>2+</sup> ions removal efficiency for at least five consecutive cycles. Based on the FTIR and XPS analyses, Hg<sup>2+</sup> ions chelation by NTB molecules and electrostatic interactions between Hg<sup>2+</sup> ions and carboxylate groups in MIL-101-NTB are plausible mechanisms for Hg<sup>2+</sup> ions adsorption.
first_indexed 2024-03-11T00:33:12Z
format Article
id doaj.art-583ea70cbec6479eaf460f82a88d57bd
institution Directory Open Access Journal
issn 2073-4441
language English
last_indexed 2024-03-11T00:33:12Z
publishDate 2023-07-01
publisher MDPI AG
record_format Article
series Water
spelling doaj.art-583ea70cbec6479eaf460f82a88d57bd2023-11-18T21:47:03ZengMDPI AGWater2073-44412023-07-011514255910.3390/w15142559Tris(2-benzimidazolyl)amine (NTB)-Modified Metal-Organic Framework: Preparation, Characterization, and Mercury Ion Removal StudiesPhani Brahma Somayajulu Rallapalli0Suk Soon Choi1Hiresh Moradi2Jae-Kyu Yang3Jae-Hoon Lee4Jeong Hyub Ha5Department of Integrated Environmental Systems, Pyeongtaek University, Pyeongtaek 17869, Republic of KoreaDepartment of Biological and Environmental Engineering, Semyung University, Jecheon 27236, Republic of KoreaDepartment of Environmental Engineering, Kwangwoon University, Seoul 01897, Republic of KoreaDepartment of Environmental Engineering, Kwangwoon University, Seoul 01897, Republic of KoreaENVIONEER Co., Ltd., Jecheon 27116, Republic of KoreaDepartment of Integrated Environmental Systems, Pyeongtaek University, Pyeongtaek 17869, Republic of KoreaHeavy metal ions (HMIs) are exceedingly hazardous to both humans and the environment, and the necessity to eliminate them from aqueous systems prompted the development of novel materials. In this study, tris(2-benzimidazolylmethyl)amine (NTB) was impregnated into MIL-101-(Cr) metal-organic framework using an incipient wetness impregnation approach, and the ability of the composite material to adsorb Hg<sup>2+</sup> ions from the water was examined. The synthesized materials were analyzed with several physico-chemical techniques such as powder X-ray diffraction, elemental analysis, scanning electron microscopy, thermogravimetric analysis, nitrogen sorption isotherms at 77 K, and X-ray photoelectron spectrometry. MIL-101-NTB quickly adsorbs 93.9% of Hg<sup>2+</sup> ions within 10 min from a 10.0 ppm single ion solution. A better fit of the kinetic data to a pseudo-second-order model validated the chemisorption of Hg<sup>2+</sup> ions on MIL-101-NTB. The experimental data fitted well with the Langmuir isotherm model, and the maximum adsorption capacity obtained at 125 ppm initial concentration was 111.03 mg/g. Despite the presence of other competing ions (Cu<sup>2+</sup>, Pb<sup>2+</sup>, and Cd<sup>2+</sup>), high Hg<sup>2+</sup> ions removal efficiency (99.6%, 1.0 ppm initial concentration) was maintained in the diverse ion batch adsorption studies. A 0.2 M EDTA solution could desorb the Hg<sup>2+</sup> ions, and cyclic Hg<sup>2+</sup> ions sorption studies indicated that MIL-101-NTB might have a high Hg<sup>2+</sup> ions removal efficiency for at least five consecutive cycles. Based on the FTIR and XPS analyses, Hg<sup>2+</sup> ions chelation by NTB molecules and electrostatic interactions between Hg<sup>2+</sup> ions and carboxylate groups in MIL-101-NTB are plausible mechanisms for Hg<sup>2+</sup> ions adsorption.https://www.mdpi.com/2073-4441/15/14/2559heavy metal ionadsorptionmetal-organic frameworktris(2-benzimidazolylmethyl)aminewater treatment
spellingShingle Phani Brahma Somayajulu Rallapalli
Suk Soon Choi
Hiresh Moradi
Jae-Kyu Yang
Jae-Hoon Lee
Jeong Hyub Ha
Tris(2-benzimidazolyl)amine (NTB)-Modified Metal-Organic Framework: Preparation, Characterization, and Mercury Ion Removal Studies
Water
heavy metal ion
adsorption
metal-organic framework
tris(2-benzimidazolylmethyl)amine
water treatment
title Tris(2-benzimidazolyl)amine (NTB)-Modified Metal-Organic Framework: Preparation, Characterization, and Mercury Ion Removal Studies
title_full Tris(2-benzimidazolyl)amine (NTB)-Modified Metal-Organic Framework: Preparation, Characterization, and Mercury Ion Removal Studies
title_fullStr Tris(2-benzimidazolyl)amine (NTB)-Modified Metal-Organic Framework: Preparation, Characterization, and Mercury Ion Removal Studies
title_full_unstemmed Tris(2-benzimidazolyl)amine (NTB)-Modified Metal-Organic Framework: Preparation, Characterization, and Mercury Ion Removal Studies
title_short Tris(2-benzimidazolyl)amine (NTB)-Modified Metal-Organic Framework: Preparation, Characterization, and Mercury Ion Removal Studies
title_sort tris 2 benzimidazolyl amine ntb modified metal organic framework preparation characterization and mercury ion removal studies
topic heavy metal ion
adsorption
metal-organic framework
tris(2-benzimidazolylmethyl)amine
water treatment
url https://www.mdpi.com/2073-4441/15/14/2559
work_keys_str_mv AT phanibrahmasomayajulurallapalli tris2benzimidazolylaminentbmodifiedmetalorganicframeworkpreparationcharacterizationandmercuryionremovalstudies
AT suksoonchoi tris2benzimidazolylaminentbmodifiedmetalorganicframeworkpreparationcharacterizationandmercuryionremovalstudies
AT hireshmoradi tris2benzimidazolylaminentbmodifiedmetalorganicframeworkpreparationcharacterizationandmercuryionremovalstudies
AT jaekyuyang tris2benzimidazolylaminentbmodifiedmetalorganicframeworkpreparationcharacterizationandmercuryionremovalstudies
AT jaehoonlee tris2benzimidazolylaminentbmodifiedmetalorganicframeworkpreparationcharacterizationandmercuryionremovalstudies
AT jeonghyubha tris2benzimidazolylaminentbmodifiedmetalorganicframeworkpreparationcharacterizationandmercuryionremovalstudies