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dx.doi.org/10.22093/wwj.2017.62042.2252 1
����� � �� �� Journal of Water and Wastewater ����� ���� ����� ����� Vol.29, No. 2, 2018
Investigation of BTEX Removal from AqueousSolution by Single Wall Carbon Nanotubes Coated
with ZnOM. Zahedniya1, Z. Ghazi Tabatabaei2
1.MScStdudent,DepartmentofChemicalEngineering,AharBranch,IslamicAzadUniversity,Ahar,Iran
2. Assist.Prof.,DepartmentofAppliedChemistry,AharBranch,IslamicAzadUniversityAhar,Iran
(CorrespondingAuthor) [email protected]
(Received Oct. 3, 2016 Accepted Apr. 3, 2017)
To cite this article : Zahedniya, M., Ghazi Tabatabaei, Z., 2018, “Investigation of BTEX removal from aqueous solution by single wall carbon nanotubes decorated with ZnO.” Journal of Water and Wastewater, 29(2), 1-11. Doi:
10.22093/wwj.2017.62042.2252. (In Persian)
Abstract Monoaromatics of Benzene, Toluene, Ethyl Benzene and Xylene which are abbreviated as BTEX, are among the most important environmental pollutants. Due to high solubility of BTEX in water, it is emitted to the aquatic environment with a very high speed. Absorption by carbon nanotubes is be regarded as one new treatment method. The aim of this study was to investigate the removal of BTEX from aqueous solutions through adsorption by single wall carbon nanotubes coated with Zinc oxide nanoparticles. The prepared nanoparticles were characterized by FT IR, XRD, FESEM and EDAX. First, the pHZPC was determined. Then, the effect of different operating parameters such as the amount of sorbent, contact time, pH, temperature and ionic strength were studied through batch method in order to obtain optimal conditions for the absorption process. The optimum conditions for BTEX removal from aqueous solution by ZnO/SWCNTs was obtained as following: pH=6, contact time=20 min, adsorbent concentration=300 mg/L, amount of sorbent=10mg, T=20°C and salt concentration= 2g/L. The results showed that single wall carbon nanotubes coated with zinc oxide effectively absorbs BTEX from water and it has a good potential for treating wastewater contaminated with petroleum
Keywords: BTEX, Single Wall Carbon Nanotubes, Nanoparticles, Adsorption, Water pollution.
dx.doi.org/10.22093/wwj.2017.62042.2252 2
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���9� ��$��%KO�� E�@*+ �� �+��� .L��)% E��@*+ �$��� \�7+ �� 5c��/�������Q������T ���!@ �&!���$ �� �$=!���� ��� � ���' �$�$�!+�!���!Q{�� UV-Vis N� ��' \7 E�@*+ 5(/ ����+��4�'.
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+ f"G���@��� ^�@!J+ a*� �$ 5c/ K�) �� ����' 5(/ K�)��$N+ t�' ���*+
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�@�+ �!��$ 5� ��-���� �?pH ��!���-�� �$��*+ �$��%@1 �� ���-�$+�'�# �� � �K���rs+�@�0+T ������� K�) ��o� ��' ��$ �' �
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0Q'r!�-'N��� [FTIR ��� ��%�������� �#%� ������� �� �������� #% ����0+T � ��' kF7� + �3� ��' ��$��#$.6�;
\����cm-1rqss ���) �!�� �� R���+�!� � ��� ��������L��� .�$ X�N��� $��/� cm-1rrssjuss ��3� 0�+��T $��/� ��� #$
���"������0)C-O( cm-1 rqvt ���"����� 0���+T�@�;)C=O( cm-1t|ss �y|ss # 0����+T�����"�����) 0-OH X����N��� � (
G���cm-1qys 0�+T �� R���+OjZn L��� $ U��� �$ ��� �- ���� �@��$�/��� ��� ��� �����������!��) ����1 ���� .(Atieh et al.
2010; Smith 1999) 0Q'rL9"1 �$a������� #% �����������$ �� �%$�+-�%��D������+ ���3� �� � !��"#���� �$ .���#$����-�� ��� ����'��-
���) �#%#��"������ 0�"�������� 0%/��� h�������������-$O�+$�' �� �/�� � �� L9"1b0Q'r+ ��#3+���' $�'
���6 � #��-L��� ���9� �� L�"� #�M#�� �-����) � ��!� �#%*������9� #-L��� Q � .L�� ��' ��-� N+ ��� f�@�+ 4�\(�G
)$��������D��� ��� �� ��#�C!��"L����� .��� ^FTIR �����9� ��#%0+T "�� � ��' ��$��� �%L9"1 �$c0Q' �$r�+ ��3����#$
*�� EN� 0+T ���"����� � %,��� ��� ��c h�����' ��-5(/��� � L�� ��'-4�$=!�� �� "����� �%+������ ���) #%@+T��/-���� +�����%h�� ������� #% �����-$O � �
�� �� ���-8�!.� .�� �$ *+�,#%^@!J+ ;9� +�9�-�.
Fig. 1. FTIR spectrum curves, a) CNTs, b) Modified carbon nanotubes, c) Functionalized carbon nanotubes
_e�Z)FT IR aj ����-$ ;� � ��� �������bj� ��� �������
��' kF7�cj��' ���@+T � ��� �������
^)[)-��' 39&` Q9� � � "�H; ��'O�� -��&;ZnO/SWCNTS
�:> f�HJ Ae9� B�� 7�&E -�C�)XRD(
0Q'��&��%� �N'� X��6-~QZnO/SWCNTS�$ �� �*+��$�����-#$���6 ��˚���˚��=θ�+ �3��.�#$
a
b
c
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����� � �� �� Journal of Water and Wastewater ����� ���� ����� ����� Vol.29, No. 2, 2018
6���1 � 4�.6 ;%��� �$ $��/�+ �-%θ��� ������˚��/�� ˚��/�� ˚��/�� ˚��/�� ˚��/�� ˚��/�� ˚��/���˚��/��������#�!��� ��� R����+ f%)��� ()���) (��� (
)���) (���) (��� ) � (����� (-�!�������"�ZnO L��������� .6�;�#%��� �$ $��/�+ �-%dF+�� ���' ���c ��&�� ��� l��� +%
$����!����XRD �$�$ ��� ��#%���-) 0JCPDS No. 36-1451(�
+�6 .� '���1 � 4.6 ;%��� �$ $��/�+ �-%��������/��=θ�) K���� ������ ���) �!��� (��� ����)�?&# L����+ � �$��� ����'��4
������� ED�� #% ������ ���� �-E!�" �#%�"����� �%L��� )Chen et al. 2003.( ����$ �������� �� �$=!����� ����%�����' )d � kλ/βcosθ(�#��@� ������ %ZnO $���Gnm�� ����*+
�'.
Fig. 2. X-ray diffraction pattern of ZnO/SWCNTs
_e��)^��XRD L-��{+����ZnO/SWCNTS
�)�)"gH �H��H� - ��&;ZnO/SWCNTS%� ��M' �� � ;
"���C�FESEM � �$-)]�#%-��{+���� ;�- 0Q�' ��Q@� �#�� Y��� �. � ��� L
��� � ������-�� 8� #�+ ?b�VL����� � .-��N��+ 4��-� 4-�)]��#+ �!�� �$�6�Q���Q��� ���� ��a + �-������o ����9� ��!��%
L���� ���D� ���� ���/�� ��� .-�FESEM �!������� �� ����' ���!��)ZnO/SWCNTS 0Q' �$ �����c ���� L��� ���' �>���ZnO
�� ��%������� #% ����������������' L.���
^)b)` H0�0 "&hC. Q:��0� -��&; L9%Hi��ZnO/SWCNTS
�� � ��a +�-��?/� ���G �%��� �a� $��+ 5�@�+�� ?�=��D T%EDX ���� �%9��O�� ����) K�0Q') L���!� .(-��� [��D T ?%
1 Joint Committee of Powder Diffraction Standards
'�6 ���9����G F� �� �����7 T ����G �� C Zn �OL��� �b+ �>�� �7 T ���G K�T-� <��@� ��-6 .L��� ��c ���� 4��;
�$ ��' ��#3+ekv �/�F� �D T �� R���+L���9# . ���� ���+ ��#3+�� $�'��!3-4��� �D T �� R���+ �7�$ 4L�� � ��-4
�$ $�� �+��@�������� M�� �� #% ������6 ��� T-���� �%�"������%���-�� �� ��' 8%��L��.
Fig. 3. FESEM image of ZnO/SWCNTs
_e��)�-�D�FESEM L-��{+� ���ZnO/SWCNTS
Fig. 4. EDX curve of ZnO/SWCNTs
_e�b)��$�9�EDX L-��{+� ��� ZnO/SWCNTS
^)j)&W� -��&; pH pH #��!�� ��%9.+��� �� �� L��-� l�V�:� �!�� �� �-� ��
*�� ������ �$ 5c/-� 5(/ � �V�+ ��0Q�' ��� �/�� � .$��() q+ �aGF+��� $�'pHZPC ���%������� #% �����$=!��� $��+
� �$-4M#�]6 �����v/v� .L��� �-!� 4��$ ��� L�� N+ ����� ��OpH#%�� ��:�v/v*�������������� �= + �#�.L���-�Q���
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����� � �� �� Journal of Water and Wastewater ����� ���� ����� ����� Vol.29, No. 2, 2018
:$-M#�� 0pHZPC �������� �$ �#%0�+T �"��$ ��V� ���' ��$��!�����) ��#%@+��T���"������@����� .L���� ������ ����a +����V�pH
E�@*+ #�-�� pH �$���*+ �$y�� rt�� ����� #���@����-� ;#�"������� �-�&!��$ ;�9� ��� � CpH�$�+� ��!+ �'� �$ .��-4
�@G�+pH ��e!+ . � ��� T�+�� �-+�� � �$�� M-M�$ L�V � #� 4!��) �a�-� #�!+��6 ��:� L�a@_ ���7-��� BTEX yss
+�@�K�)�$��� �!rs+�@���+� ��+ �$ 5c�/ ���� �� K��)ts1$�0Q' �� �/�� � .�' KO�� ��v�J3+L�� �$��� L��V �� ��
La@_BTEX e� ���+ ����?pH ��y�rt+��(�/ h�� ��?��� M#�pH �?��-M-� .L�� �!�-!� 4-$ � [-�&M#�]6 �-�# ���
5c/ �� #�-��� EN� 4��� 0�+%*�� 5(/��� $��+��$=!����$�9� ��� �����J9# ?�)$��$Machado et al. 2011(+�& # .����
pH �?��-+ M�-�� $��+ �� �������) �� �#%�"������@��@ � ����= + �!3���' ���� �-�$ 4pH �#%� ��:����#��%�� ��N��$�4
BTEX �?�� 5c/ ��� �-M-�!�� ��-f/�+ $�� ���� �� $���+ 4*�� 5(/ ����+ M#����� $��+��� ���%�������� �#%� ����
�+�$��' )Li et al. 2002(� ��� ��/�� �� . �- � f���+ 4pH ��� �� �����+ U�!�� E�@*+pH �����v���%�-4M#�]6 .�' �*�
Fig. 5. pHZPC curves for CNTs ([SWCNTs ]0 =0.01g/50mL, T=20±1 ˚C)
_e�k)��$�9� pH )�=7 ����pHZPC� ��� %# ���� ��� %��� (
������� ����� La@_)��/��$ K�)��+$ �!�� �@�+���/�$(W��"@�
^)l)5��J ?��% -��&;
���� M ����� W��9� ��+� ���� T-��Q�$-e!+ �� ���&���#�%��+b�$ �V � +�$ � 5(/ M ���q��|s1$�MO �� $���+ ��� .L���) ����1
�� ���� ��a +�:� \(G �$ 5c/ ��� W9� �+�-��� ���@*+�
a@_ ��Lyss ��@�+ �!��� �$ K�)@J+ ���:� R�- ���.� #���� �' �$�n ��o� �� ~6rs+�@�0+T 5c/ ��� �� K�) �� ��� ���' ��$
�+� �+ �#%q rs rq ts tq ys yq�|s1$��� ��� ���%�?9#� e+�"��$��� \�7 �� ~�6 .�' �$�$ ���1 +��5(�/ ��?
������ E�@*+ )��%.�'!�-���� �� 07G [���V���� W9� �+� ��+���� \(GBTEX �+� ��� �$��� �=7|s0Q�' �$z��3�
+��+� �$ \(G LT�� �� �#$ ts���1$"� E����� �-� �$��� 8��� ��-� L@T .L�� ��' � � [�-����� 4L��� 4��9+ � $���N� �- $
/-�& #%��!�� �$ 5c/ h�� �$ $�/�+ EN�%���-��� ��'� � �� �� 5(/ LT�� �� E��$ ��%�?�� �+/ h��-+ M�-� +� .��
� �+� L'()-/ 4-�& Ee'� #�+� $�' #$��� M#� �� �O +�+ 5(/��� $�' )Hyung & Kim 2008.( 0Q'z H9#�3� 4��� �
+�#$��� �� �#$�5(�/BTEX ��+� �$ �#%�� ��N�ts����1$e����aGF+ 0�1 �� �%� .L�� �!'���-�'� L�� 4Q9+ L�G 4�
��m ��' 0+� ���5(/ LSWNATs-ZnO � �� .�'� �-4W������%���-5(/ � M#�]6 4-� �$ E$�N� ��+� ts����1$ ��a� �$
.�' �!��)
Fig. 6. Effect of pH on BTEX removal by CNTs ([BTEX]=300mg/l, [ZnO/SWCNTs ]0 =0.01g/250mL,
T=20±1 ˚C) _e�l)�V�pH \(G �$ � ��� %# ���� ��� �*�� 5(/ ��?�+ ��
BTEX )����� La@_BTEX yss �!�� �$ K�) �@�+ ����+ 5c/ �$sr/s�$ K�)tqs +$ �!�� �@�+ts�/�$W��"@��(
^)m)�6�N H0�0 LT< &W� -��&; ���� ��a + ���:� \(G �$ 5c/ ��� La@_ �V�-�� ���@*+ #�
La@_ �yss ���@�+ �!�� �$ K��):� R�@J+ ��-�� .� #�����' �
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1 2 3 4 5 6 7 8 9 10 11 12
Fina
lpH
Initial pH
0
10
20
30
40
50
60
2 3 4 5 6 7 8 9 10 11 12 13
q(m
g/g
CN
T)
pH
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����� � �� �� Journal of Water and Wastewater ����� ���� ����� ����� Vol.29, No. 2, 2018
Fig. 7. Effect of contact time on BTEX removal ([BTEX]=300mg/L, [ZnO/SWCNTs ]0 =0.01g/250mL,
T=20±1 ˚C ,pH=6) _e�m)�� -:� \(G �$ ��+ �+� �����BTEX
)����� La@_BTEX yss �@�+ �!�� �$ K�) ����+ 5c/ �$sr/sK�) �$tqs +$ �!�� �@�+ts� W��"@� �/�$ pH�����v(
Fig. 8. Effect of nano-sorbent concentration on BTEX removal ([BTEX]=300mg/L, pH=6, T=20±1 ˚C , Contact
Time=20 min) _e�n)\(G �$ 5c/ ��� La@_ �V� ����� BTEX
����� La@_)BTEX ��� �@�+ +$ �!�� �$ K�)���/�$ W9� �+� W��"@���� ���1$ pH������(
$�+-�rs rq�ts+�@�0�+T � ��' kF7� 5c/ ��� �� K�) ��$��' ��o� �� ���-$�) �� ~6 �ts1$��� ��� �$� C�# ��%�?�9#
� e+�"�+�E�@*+ 5(/ ��? #%������� ��' \7 )���%�'��� ���!�-0Q��' �$ 0��7G [p.L���� ����' �$�$ ���3� ��!�-�� 0��7G [
��������e������L���a@_ �� ���#%^���@!J+SWNATs-ZnO �SWNATs :� \(G �$-�� �� �BTEX 0Q�' l���+ p�� ���%
���-� \(GBTEX ��� �&�-�?��� ��� L�� Y�o�+ 4-L�a@_ M�� �� 5c/%$�+-#$�� � 5(/ ��L��� �!'�$ L��+ �V� \(G}
�-�?�� ��-�Q+ M#%5(/ $���BTEX ����%�� � 5c/ h��
�?��-��!�$ M�E�Q��+ #%BTEX / ��-�& �#%$��/�+ E�N��$ 5c��/ h���� �$���@��7� 0��?����-#$���� M�0����+ �$ \(��G
�?����-$���+ M-L���� 5c��/ L��a@_ �)Cheng et al. 2012.(
H9#�� 4-� ��$�9� 4�� �&�-0�+T �� �� L�� Y�o�+ 4�$��9� ��$������� #% ����"�� ��c ,������ �%�?��� \(�G ��7�$-M
./�� 0�1�$��$.
^)n)IC`�� "��� &W� ��V�#+$ �%��� �� ^@!J+-5(/ � BTEX ��' �$-.� ,�� ��' �
�$ 0Q'u�?�� �� $�$ �3�-�� �=7 �� +$ MtsW���"@� ��/�$�?�� �� \(G �+����-+ M�� .�#$-�?�� 4-��� M�-� L��� 4�Q9+
���$�!� �$ � 5c/ R"��� 0��?��� ��O-0�*+ M�#%� E�N���!�3�����%\(��GBTEX �?���� ��+� .���'�-�� ��+$ Mts��� |q���/�$
W��"@� f�� + ��� \(�G �+���� M#� �� ��?y/q��7�$ .��'�?�� � \(G �+���� M#�-+ �3� +$ M�5(/ �#$BTEX ���
��%SWNTCs-ZnO ��-��� ;-+���?)� ��� ��� �$���� (����+�)) ;� .L��-����&3#�]6 ���$ ?M#�]6 %�# �$��� ���+�) ��� $���
���-��� 5(/ � ��+��� ��Q��� ��%5c/ #�-a���! � ���L�$��� ��'� EN� 4��� ����� .(Rao et al. 2009 & Saeedi et al.
2011)
Fig. 9. Impact of temperature on BTEX removal ([BTEX]=300mg/L, [ZnO/SWCNTs ]0 =0.01g/250mL,
pH=6) _e�o)\(G �$ M ��� %+$ ����� BTEX)����� La@_BTEX
yss �@�+ �!�� �$ K�) ����+ 5c/ �$sr/s�$ K�)tqs �!�� �@�+
pH �����v(
^)o)-0H9 p�#= &W�
���%�����V����1 �-����� �� E�@*+%����-�������� �#%' ?! ��\(G �$ ��BTEX ��-�� ��-� C��� =��� ��7- C
84868890929496
0 10 20 30 40
Rem
oval
(%)
Contact time (min)
61.3866.99
75.37
94.47 94.59 95.01
10 15 20
Rem
oval
(%)
Nanotubes (mg)
SWCNTs SWCNTs/ ZnO
50
60
70
80
90
100
0 10 20 30 40 50
Perc
enta
geof
rem
oval
(%)
Temperature (˚C)
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����� � �� �� Journal of Water and Wastewater ����� ���� ����� ����� Vol.29, No. 2, 2018
��#NZ)\(G �-��� �7�$BTEX 5c/ �� �$=!�� � ��� E�@*+ ��
� ��� �������j;9� La@_ �$ %�� ��"�� ^@!J+ %#)����� La@_BTEX yss �@�+ �!�� �$ K�) ����+ 5c/ �$sr/s�$ K�)tqs +$ �!�� �@�+
tsW��"@� �/�$ �pH�����v(Table 1. Percentage of BTEX removal from aqueous solution
using ZnO/SWCNTs in different salt concentrations ([BTEX]=300mg/L, [ZnO/SWCNTS ] 0 =0.01g/250mL, T=20±1 ˚C , pH=6)
Na₂SO₄Na₂CO₃K2CO3NaCl CaCl₂Salt
Concentration (mg/l)
74.0596.6798.7597.8188.1650076.3496.7399.3598.1391.67100077.9196.8399.5698.3292.03150078.8296.4399.8398.4695.562000
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