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Chemical Engineering Journal
journal homepage: www.elsevier.com/locate/cej
A mechanistic investigation of highly stable nano ZrO
2
decorated
nitrogen-rich azacytosine tethered graphene oxide-based
dendrimer for the removal of arsenite from water
Subbaiah Muthu Prabhu
a,b
, Radheshyam Rama Pawar
a
, Keiko Sasaki
a,
⁎
, Chang Min Park
b
a
Department of Earth Resources Engineering, Faculty of Engineering, Kyushu University, Fukuoka 819-0395, Japan
b
Department of Environmental Engineering, Kyungpook National University, 80 Daehak-ro, Daegu 41566, South Korea
HIGHLIGHTS
•
ZrO
2
entrapped GO-based Aza-teth-
ered PAMAM dendrimer composite is
prepared.
•
Ligand exchange is likely responsible
for the adsorption of AsO
3
3−
.
•
The lamination/delamination chem-
istry of GO-dendrimer composite are
expressed.
•
Maximum adsorption capacity of
1.075 mmol/g was achieved for
AsO
3
3−
.
•
Selectivity and reusability test (4 cy-
cles) did not afect the efciency of
AsO
3
3−
.
GRAPHICAL ABSTRACT
ARTICLE INFO
Keywords:
Dendrimer
Graphene oxide
Azacytosine
Zirconia
Arsenite
Adsorption
ABSTRACT
We focused to synthesize graphene oxide-polyamidoamine dendrimer, up to 2nd generation, (GO-gen2) via a grafting
method and the tethered groups were further covalently functionalized with a nitrogen-rich of an aromatic triazine
ring of 5-azacytosine (Aza). Zirconia nanoparticles (ZrO
2
) has been identifed as promising material for removal of
AsO
3
3−
from water, however, its practical applicability is hindered due to its nanosize. Hence, ZrO
2
was successfully
decorated through biomolecule assist on GO-gen2-Aza dendrimer. Various amounts of GO-gen2-Aza were used as
stable supports to develop the nanocomposites with ZrO
2
. Then, the adsorption efciency of highly toxic AsO
3
3−
on
developed composites was investigated for water treatment. The synthesized GO-dendrimer composites were char-
acterized well before and after adsorption of AsO
3
3−
using FTIR, PXRD, SEM, XPS, TGA, TEM and BET analysis.
Particle size distribution of ZrO
2
revealed the peak top at 28 nm by zeta potential measurement. During synthesis, the
GO sheets of composite were laminated by incorporation of ZrO
2
nanoparticles. The results of the batch experiments
showed that ZrO
2
@2%GO-gen2-Aza dendrimer had higher adsorption density of AsO
3
3−
than that of other devel-
oped forms of dendrimer composites. Langmuir equation well described the adsorption isotherm with the maximum
adsorption capacity of 1.075 mmol/g. In addition, the enhanced AsO
3
3−
adsorption density on ZrO
2
surface of
ZrO
2
@x%GO-gen2-Aza, in which the GO-sheets were delaminated, resulting more ZrO
2
was dispersed homo-
geneously in the GO-sheets for maximum uptake of AsO
3
3−
from water, confrmed by PXRD patterns. These results
suggested that the developed GO-based dendrimer materials can be utilised for the practical remediation of toxic
AsO
3
3−
and other similar types of toxic ions, selenite, phosphate and fuoride from the contaminated water.
https://doi.org/10.1016/j.cej.2019.03.277
Received 26 December 2018; Received in revised form 15 March 2019; Accepted 29 March 2019
⁎
Corresponding author.
E-mail addresses: muthuprabhu@mine.kyushu-u.ac.jp (S.M. Prabhu), keikos@mine.kyushu-u.ac.jp (K. Sasaki).
Chemical Engineering Journal 370 (2019) 1474–1484
Available online 29 March 2019
1385-8947/ © 2019 Elsevier B.V. All rights reserved.
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