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Recycled PET as a PDMS-Functionalized Electrospun Fibrous Membrane for Oil-Water Separation

Authors:
Hoan Ngoc Doan at Vietnam National University, Ho Chi Minh City
Hoan Ngoc Doan
Phú Võ Phong at Ho Chi Minh City University of Science
Phú Võ Phong
Kohei Hayashi
Kohei Hayashi
Kohei Hayashi
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Kenji Kinashi at Kyoto Institute of Technology
Kenji Kinashi
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Abstract and Figures

In recent years, low-cost and effective technologies for oil-water separation have been highly desired due to an increase of oily wastewater and frequent oil spill accidents. This study demonstrates a cost-effective and sustainable preparation of flexible fibrous membranes with high oil-water separation performance using recycled polyethylene terephthalate (rPET). The rPET fibrous membrane was prepared via electrospinning; in the following step, the rPET membrane was dip-coated with polydimethylsiloxane (PDMS) to improve the water intrusion pressure and anti-water-fouling property of the rPET fibrous membrane. The effect of PDMS concentration on the membrane morphology, surface chemistry, thermal and mechanical properties, surface wettability and oil-water separation performance was evaluated. The membranes are superoleophilic with an oil contact angle of 0° and exhibit excellent anti-water-fouling properties. The PDMS-functionalized rPET membranes can effectively separate various oil-water mixtures driven by gravity, with a high flux (∼ 20,000 L m⁻² h⁻¹) and a high separation efficiency (> 98%) for up to ten cycles and thus has potential industrial application.
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UNCORRECTED PROOF
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8Master's Program of Innovative Materials, Graduate School of Science and Technology, Kyoto Institute of Technology, Matsugasaki, Sakyo, Kyoto 606-8585, Japan
9Faculty of Materials Science and Engineering, Kyoto Institute of Technology, Matsugasaki, Sakyo, Kyoto 606-8585, Japan
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UNCORRECTED PROOF
H.N. Doan et al. Journal of Environmental Chemical Engineering xxx (xxxx) xxx-xxx
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2. Materials and methods
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;J;H E<  CC ->; :?IJ7D9; 8;JM;;D J>; D;;:B; 7D: ]8;H 9EBB;9
JEH M7I ]N;: 7J  9C  HEJ7J?D= :HKC 9EL;H;: 8O 7 IJ7?DB;IIIJ;;B
C;I> 'E  M7I KI;: 7I 7 ]8;H 9EBB;9JEH M?J> 7 9EDIJ7DJ HEBB?D=
IF;;: E<  HFC ->; H;B7J?L; >KC?:?JO 7D: J;CF;H7JKH; E<  Z 
7D:  Z  X H;IF;9J?L;BO M7I C7?DJ7?D;: 8O CED?JEH?D= M?J> 7 >O
=HEJ>;HCE=H7F> FB79;: ?DI?:; J>; ;B;9JHEIF?DD?D= 9>7C8;H ->; H;IKBJ
?D= ]8HEKI C;C8H7D;I M;H; FB79;: ?D 7 L79KKC EL;D <EH  > 7J  X JE
H;CEL; 7DO H;J7?D;: IEBL;DJI
2.3. PDMS modi=cation
)EBO:?C;J>OBI?BEN7D; )&,<KD9J?ED7B?P;: H)- C;C8H7D;I
H)-)&, M;H; FH;F7H;: KI?D= 7 :?F9E7J?D= C;J>E:  )&, FH;
FEBOC;H M7I 8B;D:;: M?J> 7 9HEIIB?DA;H 7J 7 9EDIJ7DJ M;?=>J H7J?E E<
 ->; 7IFH;F7H;: H)- C;C8H7D;I M;H; 9KJ ?DJE 7 HEKD: I>7F;
M?J> 7 :?7C;J;H E<  CC 7D: M;H; ?CC;HI;: ?D 7 )&,>;N7D; IE
BKJ?ED M?J> L7HO?D= )&, 9ED9;DJH7J?EDI    7D:  MJ 7J  X
<EH  > <J;H J>; :?F9E7J?D= FHE9;II J>; 7H9>?L;: ]8HEKI C;C8H7D;
M7I :H?;: <EH  > ?D 7 L79KKC EL;D 7J  X ->; E8J7?D;: C;C8H7D;I
M;H; :;DEJ;: 7I H)-)&,6 H)-)&,6 H)-)&,6 7D:
H)-)&,6 H;IF;9J?L;BO
2.4. Membrane characterization
&EHF>EBE=O 7D: ;D;H=O :?IF;HI?L; 1H7O IF;9JHEC;JHO 1 <EH J>;
C;C8H7D;I M;H; IJK:?;: 8O 7 ];B:;C?II?ED I97DD?D= ;B;9JHED C?9HE
I9EF; ,& #(% #(% %J: #7F7D ;GK?FF;: M?J> 7D (N
<EH: ;D;H=O :?IF;HI?L; 1H7O IF;9JHEC;J;H ->; C;C8H7D;I M;H; IFKJ
J;H9E7J;: M?J> 7  DC J>?9A B7O;H E< F7BB7:?KC 7D: E8I;HL;: KI?D=
,& 7J 7D 799;B;H7J?D= LEBJ7=; E<  A/ ?8;H :?7C;J;HI M;H; 7D7
BOP;: KI?D= ,& ?C7=;I 7D: ?C7=; FHE9;II?D= IE<JM7H; "C7=;# ->;
IKH<79; HEK=>D;II E< J>; C;C8H7D;I M7I :;J;HC?D;: KI?D= 7 DED9ED
J79J B7I;H FHE]BEC;JHO 7D7BOI?I C;J>E: CEKDJ;: ED 7  B7I;H I97D
D?D= C?9HEI9EF; /$ $;O;D9; E #7F7D "+ IF;9JH7 E< J>; C;C
8H7D;I M;H; H;9EH:;: KI?D= 7D -"+ IF;9JHEF>EJEC;J;H -"+ 
#7I9E E #7F7D M?J> 7 KD?L;HI7B 7JJ;DK7J;: JEJ7B H;^;9J7D9; 799;I
IEHO -+ )+( (' ;GK?FF;: M?J> 7 :?7CED: FH?IC #7I9E E #7F7D
->; 9>;C?97B 9ECFEI?J?EDI E< J>; C;C8H7D; IKH<79;I M;H; ?DL;IJ?
=7J;: KI?D= 7D 1H7O F>EJE;B;9JHED IF;9JHEC;J;H #(%  #(% E
#7F7D EDJ79J 7D=B; 7D7BOI?I M7I 9ED:K9J;: KI?D= 7 )>E;D?N  9ED
J79J7D=B; IOIJ;C $HECJ;A E &7B7OI?7 7J  X 7D: J>; E8J7?D;:
?C7=;I M;H; 7D7BOP;: M?J> 7D7BOI?I IE<JM7H; "C7=;# EH J>; 7D7BO
I?I J>; H)-)&, C;C8H7D;I M;H; FB79;: ED 7 =B7II IK8IJH7J; M7
J;H M7I KI;: <EH J>; M7J;H 9EDJ79J 7D=B; 0 7D: >;N7D; M7I KI;:
<EH J>; E?B 9EDJ79J 7D=B; &;7IKH;C;DJI M;H; 97HH?;: EKJ ED J>; C;C
8H7D; IKH<79;I 7J HEEC J;CF;H7JKH; ?D 7D EF;D;: 9>7C8;H ->; LEB
KC; E< J>; I;II?B; :HEF M7I C7?DJ7?D;: 7J μ% ->; I7CFB; C;C8H7D;I
M;H; FB79;: ?D 7 >;N7D; 87J> :KH?D= 9EDJ79J 7D=B; C;7IKH;C;DJ JE
;L7BK7J; J>; KD:;HE?B >O:HEF>E8?9?JO ->; 7L;H7=; 9EDJ79J 7D=B; L7B
K;I M;H; E8J7?D;: 8O C;7IKH?D= 7J B;7IJ ]L; :?<<;H;DJ C;7IKH;C;DJ
FE?DJI 79HEII J>; I7CFB; IKH<79; ->; M7J;H ?DJHKI?ED FH;IIKH; L7BK; M7I
C;7IKH;: 8O 7 >EC;C7:; J;IJ?D= IOIJ;C E< EKH EMD :;I?=D 7I I>EMD
?D ?= , ->; J>;HC7B FHEF;HJ?;I E< J>; H;IKBJ?D= ]8;HI M;H; IJK:
?;: KI?D= :?<<;H;DJ?7B I97DD?D= 97BEH?C;JHO , ->;HCE=H7CI M;H;
E8J7?D;: KI?D= 7 - "DIJHKC;DJI * 97BEH?C;J;H - "DIJHKC;DJI
#7F7D "D9 -EAOE #7F7D M?J> 7 >;7J?D= H7J; E<  X C?Da−?D 7 D?
JHE=;D 7JCEIF>;H; ->; J>;HCE=H7L?C;JH?9 7D7BOI?I -  9KHL;I 7D:
J>; ]HIJ :;H?L7J?L; E< J>; -  9KHL; :?<<;H;DJ?7B J>;HCE=H7L?C;JH?9
-  9KHL; M;H; E8J7?D;: 8O 7 -  C79>?D; ?I9EL;HO -  -
"DIJHKC;DJI M?J> 7 >;7J?D= H7J; E<  X C?Da−?D 7 D?JHE=;D 7JCEI
F>;H; ->; C;9>7D?97B FHEF;HJ?;I E< J>; I7CFB;I M;H; 9>7H79J;H?P;:
KI?D= 7 KD?L;HI7B J;DI?B; J;IJ?D= C79>?D; -',"%(' +-– 
E #7F7D 9HEII>;7: IF;;:  CC C?Da− BE7: 9;BB  ' ->; ]
8HEKI I7CFB;I M;H; 9KJ EKJ ?D J>; <EHC E< C?D?7JKH?P;: :E= 8ED;I>7F;:
IF;9?C;DI JOF;  ?D , ",(   KI?D= 7 9KJJ?D=
UNCORRECTED PROOF
H.N. Doan et al. Journal of Environmental Chemical Engineering xxx (xxxx) xxx-xxx
8B7:; ->;D J>; IF;9?C;DI M;H; CEKDJ;: EDJE 7 F7F;H <H7C; KI?D=
:EK8B;I?:;: J7F; ->; J>?9AD;II E< J>; J;IJ?D= IF;9?C;D M7I C;7IKH;:
KI?D= 7 C?9HEC;J;H I9H;M =7K=; &?JKJEOE − &?JKJEOE #7F7D
-;DI?B; J;IJI M;H; F;H<EHC;: ?D 7D 7JCEIF>;H; M?J> 7 J;CF;H7JKH; 7D:
H;B7J?L; >KC?:?JO E<  Z  X 7D:  Z  H;IF;9J?L;BO ->; J;IJI M;H;
F;H<EHC;: KI?D= 7J B;7IJ ]L; IF;9?C;DI <EH ;79> ]8HEKI C;C8H7D;
2.5. Oil-water separation experiment
->; I;F7H7J?ED ;NF;H?C;DJI M;H; F;H<EHC;: KI?D= 7 :;7:;D: ]BJH7
J?ED 7FF7H7JKI ->; E8J7?D;: CE:?];: H)-)&, C;C8H7D; M7I 9KJ
?D 7 HEKD: I>7F; M?J> 7 :?7C;J;H E<  CC 7D: J>;D ]N;: 8;JM;;D J>;
]BJ;H >EB:;H $ , :L7DJ;9 E #7F7D M?J> 7 IJ7?DB;IIIJ;;B IKF
FEHJ;H ;<EH; 9ED:K9J?D= J>; E?BM7J;H I;F7H7J?ED J>; C;C8H7D;I M;H;
FH;M;JJ;: M?J> J>; 9EHH;IFED:?D= E?B ,;F7H7J?ED J;IJI M;H; 9ED:K9J;:
8O FEKH?D=  C% E< J>; E?B M7J;H C?NJKH; LEBKC; H7J?E   ?DJE J>;
KFF;H JK8; 7D: J>; E?B M7I 9EBB;9J;: ?D 7 8;7A;H 7J J>; 8EJJEC E< J>;
]BJ;H >EB:;H ->; ^KN J>HEK=> J>; C;C8H7D; M7I 97B9KB7J;: KI?D= J>;
<EBBEM?D= ;GK7J?ED
M>;H; F?I J>; ^KN V?I J>; LEBKC; E< J>; F;HC;7J; E?B J>HEK=> J>;
C;C8H7D; :KH?D= J?C; t 7D: A?I J>; ;<<;9J?L; 9EDJ79J 7H;7 E< J>; C;C
8H7D; 7D: J>; C?NJKH; ->; I;F7H7J?ED ;<]9?;D9O M7I 97B9KB7J;: KI?D=
J>; <EBBEM?D= ;GK7J?ED
M>;H; η?I J>; I;F7H7J?ED ;<]9?;D9O, M ?I J>; M;?=>J E< J>; E?B 9EBB;9J;:
?D J>; 8;7A;H 7<J;H I;F7H7J?ED 7D: Ma ?I J>; ?D?J?7B M;?=>J 8;<EH; J>;
I;F7H7J?ED ->H;; I7CFB;I E< ;79> ]8HEKI C;C8H7D; M;H; J;IJ;: -E :;
J;HC?D; J>; H;9O9B?D= 78?B?JO E< J>; <KD9J?ED7B?P;: H)- C;C8H7D; J>;
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45
3. Results and discussion
3.1. Morphology and surface chemical composition
)H;L?EKI IJK:?;I :;CEDIJH7J;: J>7J J>; E?BM7J;H I;F7H7J?ED 7D: IKH
<79; M;JJ78?B?JO E< J>; ;B;9JHEIFKD C;C8H7D;I M;H; IJHED=BO :;F;D:;DJ
ED J>; ]8;H :?7C;J;H FEHEI?JO FEH; I?P; IKH<79; 9>;C?IJHO 7D: IKH<79;
HEK=>D;II E< J>; C;C8H7D;I 45 ->;H;<EH; J>; CEHF>EBE=O 7D:
IJHK9JKH; E< J>; 7IIFKD 7D: )&,CE:?];: H)- C;C8H7D;I M;H; ?D
L;IJ?=7J;: ?= 7‒; I>EMI J>; CEHF>EBE=O 7D: IJHK9JKH; E< J>; 7IIFKD
7D: )&,CE:?];: H)- C;C8H7D;I ->; H)- ;B;9JHEIFKD ]8;HI >7L;
7 ICEEJ> IKH<79; 7D: 7 BEM :;=H;; E< ?DJ;H9EDD;9J;: D;JMEHA IJHK9
JKH; M?J> 7 ]8;H :?7C;J;H E<  Z  DC ?= , ->; <EHC7J?ED
E< J>; ?DJ;H9EDD;9J;: D;JMEHA IJHK9JKH; ?D J>; 7IIFKD H)- I7CFB;
9EKB: 8; 7II?=D;: JE J>; ?D9ECFB;J; ;L7FEH7J?ED E< J>; KI;: IEBL;DJI
45 0>;D J>; H)- C;C8H7D; M7I CE:?];: M?J> 7 )&, IEBK
J?ED E<  MJ 7 IB?=>J 9>7D=; ?D J>; CEHF>EBE=O E< J>; C;C8H7D; M?J>
?D9H;7I;: ?DJ;H9EDD;9J;: 8ED:?D= IJHK9JKH; M7I E8I;HL;: 7I I>EMD ?D
?=I 8 7D: ?= , "D J>; 97I; E< 7 )&, 9ED9;DJH7J?ED E< MJ IEC;
7:>;I?L; 7H;7I ?D M>?9> J>; LE?:I 8;JM;;D H)- ]8;HI M;H; ]BB;: 8O
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I?=D?<?97DJBO 0>;D J>; )&, 9ED9;DJH7J?ED M7I <KHJ>;H ?D9H;7I;: JE
MJ J>; 7:>;I?L; 7H;7I 8;97C; B7H=;H J>7D J>7J E< J>; H)-)&
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8;JM;;D J>; ]8;HI M;H; 7BCEIJ ]BB;: M?J> )&,
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L?7 7 DED9EDJ79J B7I;H FHE]BEC;JHO 7D7BOI?I C;J>E: ?= < :;CED
IJH7J;I J>; 9EHH;IFED:?D= Ra7 L7BK;I E< J>; C;C8H7D;I ->; :;J7?B;: EF
J?97B FHE]BEC;JHO ?C7=;I M;H; :;CEDIJH7J;: ?D ?= , ->; 7IIFKD
H)- C;C8H7D; ;N>?8?J;: J>; >?=>;IJ Ra7 L7BK; E<  [C ?D:?97J?D= 7
H;B7J?L;BO HEK=> IKH<79; I ;NF;9J;: J>; 9EHH;IFED:?D= Ra7 L7BK; :;
9H;7I;: JE  [C M>;D J>; C;C8H7D; M7I CE:?];: M?J>  MJ )&,
IEBKJ?ED M>?9> M7I C7?DBO :K; JE J>; ?DJ;H9EDD;9J?ED 8;JM;;D ]8;HI
<EHC;: 8O J>; )&, B7O;H ->; HEK=>D;II =H7:K7BBO :;9H;7I;: M?J>
7 <KHJ>;H ?D9H;7I; ?D J>; 9ED9;DJH7J?ED E< J>; )&, M>?9> H;IKBJ;:
<HEC J>; ?D9H;7I; ?D J>; 7CEKDJ E< 7:>;I?L; 7H;7 <EHC;: 8O )&,
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Fig. 1. ,& ?C7=;I E< 7 7IIFKD H)- 8 H)-)&,6 9 H)-)&,6 : H)-)&,6 7D: ; H)-)&,6 < ->; Ra7 L7BK;I E< J>; C;C8H7D;I ?DI;JI J>; 9EHH;IFED:?D=
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UNCORRECTED PROOF
H.N. Doan et al. Journal of Environmental Chemical Engineering xxx (xxxx) xxx-xxx
7D:  [C H;IF;9J?L;BO M>?9> 9EHH;IFED:;: JE J>; H;IKBJI <HEC J>;
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H)-)&,6
->; FH;I;D9; E< J>; )&, B7O;H ED J>; <KD9J?ED7B?P;: H)- C;C
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?D<H7H;: -+ -"+ C;7IKH;C;DJI ?= 7 I>EMI J>; -+ -"+ IF;9
JH7 E< J>; H)- C;C8H7D;I 8;<EH; 7D: 7<J;H CE:?]97J?ED M?J> :?<<;H;DJ
7CEKDJI E< )&, ->; :?<<;H;D9;I ?D J;HCI E< JH7DIC?JJ7D9; 7J 
     7D:  9Ca−E< J>; H)-)&, C;C
8H7D;I 7H; 7JJH?8KJ;: JE J>; <KD9J?ED7B =HEKFI E< )&, 4–5 ->;I;
87D:I 7H; 7II?=D;: JE ! 7IOCC;JH?9 IJH;J9>?D=  9Ca−  !
IJH;J9>?D=  9Ca− ! 8;D:?D=  9Ca− ,?–(–,? 7IOCC;J
H?9 IJH;J9> ?D=  9Ca− M7==?D= L?8H7J?EDI E< –!a– 9Ca−
! HE9A?D=  9Ca− 7D: ,?– IJH;J9>?D=  9Ca− "J I>EKB: 8;
DEJ;: >;H; J>7J J>; -+ -"+ H;IKBJ E< J>; H)-)&,6 :E;I DEJ
I>EM 7 87D: 7J  9Ca−7IIE9?7J;: M?J> J>; FH;I;D9; E< J>; ,?–!
=HEKF ?D J>; 9HEIIB?DA;H M>?9> ?D:?97J;I J>7J J>; )&, FH;FEBOC;H 7D:
9HEIIB?DA?D= 7=;DJ 7H; 9ECFB;J;BO FEBOC;H?P;: 7I I>EMD ?D ?= 8
->; 9>;C?97B 9ECFEI?J?ED E< J>; )&, B7O;H ED J>; H)- ]8;HI
M7I <KHJ>;H ;L7BK7J;: 8O 1), ?= 7 I>EMI J>; 1), IF;9JH7 E< J>;
H)- C;C8H7D; 7<J;H CE:?]97J?ED M?J> :?<<;H;DJ 7CEKDJI E< )&,
?D M>?9> J>;  I 7D: ( I I?=D7BI 7FF;7H 7J  ;/ 7D: 
;/ H;IF;9J?L;BO "D 7::?J?ED ,? I?=D7BI 7BIE 7FF;7H ?D J>; )&,<KD9
J?ED7B?P;: H)- C;C8H7D;I 7I I;;D 7J 8?D:?D= ;D;H=?;I E<  ;/
7D:  ;/ ->?I H;IKBJ ?D:?97J;I J>7J J>; IKH<79; E< J>; H)- ]8;HI
M7I CE:?];: 8O )&, ->; :;J7?B;: ;B;C;DJ7B 9ECFEI?J?ED E< J>; H)-
C;C8H7D; 8;<EH; 7D: 7<J;H )&, <KD9J?ED7B?P7J?ED M7I 97B9KB7J;: 7I
I>EMD ?D ?= 8 I 7 H;IKBJ J7A?D= J>; H)- ]8;HI J>7J M;H; CE:?];:
8O J>; ),& IEBKJ?ED M?J>  MJ 7I 7D ;N7CFB; J>; H;B7J?L; F;H9;DJ7=;
E< ,? ED J>; C;C8H7D; ?D9H;7I;: I?=D?<?97DJBO <HEC D;7HBO –
!EM;L;H ;L;D ?< J>; JH;7JC;DJ 9ED9;DJH7J?ED E< )&, M7I ?D9H;7I;:
J>; F;H9;DJ7=; E< ,? M7I 7BCEIJ 9EDIJ7DJ 7I I>EMD ?D ?= 8 "D 7::?
J?ED J>; F;H9;DJ7=; E< ,? M7I 7BCEIJ J>; I7C; 7I J>; ;B;C;DJ7B H7J?E E<
7 8KBA )&, ,?   799EH:?D=BO 7BB E< J>; ,? F;H9;DJ7=;I <EH J>;
H)- ]8;HI <KD9J?ED7B?P;: M?J> )&, 9ED9;DJH7J?EDI E<   7D:  MJ
I>EM 7FFHEN?C7J;BO – 
->; 9>7D=?D= ]8;H IKH<79; 9>;C?97B 9ECFEI?J?ED M7I <KHJ>;H ?DL;I
J?=7J;: 8O 7D 1), D7HHEM IF;9JHKC 7J  I <EH J>; 7IIFKD 7D: CE:?];:
H)- C;C8H7D;I I I>EMD ?D ?=  7 8HE7:  I IF;9JH7 9;DJ;H;: 7J
 ;/ 9EKB: 8; :;9ECFEI;: ?DJE  ;/  ;/ 7D:  ;/
7D: J>;I; F;7AI 9EHH;IFED:;: JE J>; –!– –( 7D: (–=( 8?D:
?D= ;D;H=?;I H;IF;9J?L;BO ->; H)- C;C8H7D; 9E7J;: M?J> J>;  MJ
)&, IEBKJ?ED H)-)&,6 :;CEDIJH7J;: J>7J J>; F;7A ?DJ;DI?JO E<
–( 7D: (–=( 8?D:?D= ;D;H=?;I =H;7JBO :;9H;7I;: ?D 9ECF7H?IED M?J>
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?D9H;7I; ?D )&, 9ED9;DJH7J?ED J>; I?=D7BI 9EHH;IFED:?D= JE J>;  (
7D: ( =( 8?D:?D= ;D;H=?;I :?I7FF;7H ?D 7BB J>; 1), D7HHEM IF;9JH7
?D:?97J?D= J>7J J>; IKH<79;I E< J>; H)- C;C8H7D;I M;H; <KBBO 9EL;H;:
M?J> )&,
Fig. 2. 7 -+ -"+ IF;9JH7 E< J>; H)-)&, D7DE]8HEKI C;C8H7D;I E8J7?D;: M?J> L7H?EKI )&, 9ED9;DJH7J?EDI 8 -+ "-"+ IF;9JH7 E< J>; H)-)&,6 )&,6KBA )&
,6)H;FEBOC;H 7D: )&,6HEIIB?DA;H
Fig. 3. 7 ,KHL;OI97D 1), IF;9JH7 E< H)-)&, D7DE]8HEKI C;C8H7D;I E8J7?D;: <HEC L7H?EKI )&, 9ED9;DJH7J?EDI 7D: 8 :;J7?B;: ;B;C;DJ7B 9ECFEI?J?ED E< J>; H)- C;C8H7D;
8;<EH; 7D: 7<J;H )&, <KD9J?ED7B?P7J?ED
UNCORRECTED PROOF
H.N. Doan et al. Journal of Environmental Chemical Engineering xxx (xxxx) xxx-xxx
Fig. 4.  I IF;9JH7 7D7BOI?I E< J>; 7IIFKD H)- 8KBA )&, 7D: H)-)&, ]8HEKI C;C8H7D;I E8J7?D;: M?J> L7H?EKI )&, 9ED9;DJH7J?EDI
->; :?IJH?8KJ?ED E< )&, ED J>; C;C8H7D; M7I ;L7BK7J;: 8O KI?D=
1 ,? C7FF?D= 7I I>EMD ?D ?= , I 7 H;IKBJ 7 >ECE=;D;EKIBO :?I
F;HI;: ,? 9EDJ;DJ ED J>; ]8;HI M7I E8I;HL;:
3.2. Thermal properties
->; ;<<;9J E< )&, 9ED9;DJH7J?ED ED J>; J>;HC7B FHEF;HJ?;I E< J>;
H)- C;C8H7D;I M7I ?DL;IJ?=7J;: 8O KI?D= , 7D: -  7D7BOI?I 7I
I>EMD ?D ?=  "D J>; , J>;HCE=H7CI 7D ;D:EJ>;HC?9 F;7A 9EHH;
IFED:;: JE 7D ;DJ>7BFO H;B7N7J?ED J>7J 7FF;7H;: 7J 7FFHEN?C7J;BO  X
<EH ;79> I7CFB; M>?9> M7I 7JJH?8KJ;: JE J>; FH;I;D9; E< 7 C;IECEHF>?9
F>7I; EH?;DJ;: 7CEHF>EKI F>7I; ?D J>; ]8;HI 45 ->; C;IECEH
F>?9 F>7I; MEKB: 8; <EHC;: M>;D J>; ]8;HI M;H; IJH;J9>;: :KH?D= J>;
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J>; H)- ]8;HI 9EKB: FH;L;DJ J>; >;7J?D= ;<<;9J ED J>; H)- 97KI?D= 7D
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?=I 8 7D: , ->; H;IKBJI I>EM J>7J J>; FOHEBOI?I E< J>; 7IIFKD
H)- I7CFB; IJ7HJ;: 7J 7FFHEN?C7J;BO  X ->; I7CFB; M7I 9EC
FB;J;BO :;=H7:;: 7J  X M?J> 7 F;7A 7J  X 7D: FHE:K9?D= H;I?:K;
M?J> 7D 7CEKDJ E<  MJ &;7DM>?B; J>; H)-)&, I7CFB;I I>EM
7 >?=>;H J>;HC7B IJ78?B?JO M?J> JME CEH; F;7AI 7J  X 7D:  X ?D
J>; - 9KHL;I ?D:?97J?D= J>; FH;I;D9; E< )&, ED J>; I7CFB; M?J>
7 >?=>;H :;=H7:7J?ED J;CF;H7JKH; ->; -  7D: - 9KHL;I E< J>;
7IIFKD H)- 7D: H)-)&, C;C8H7D;I I>EM :?<<;H;DJ I>7F;I M?J>
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- F;7A 7J  X 7D: ?DIJ;7: 7D ?D9H;7I; E< - F;7AI 7J  X 7D:
 X M;H; C;7IKH;: ->; H)-)&, I7CFB;I M;H; 9ECFB;J;BO :;
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3.3. Wettability
 >?=>BO I;B;9J?L; M;JJ78?B?JO ?I 7 9HK9?7B <79JEH J>7J I?=D?<?97DJBO
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Fig. 5. 7 , J>;HCE=H7CI 7D: 8 -  9KHL;I E< J>; 7IIFKD H)- 7D: H)-)&, C;C8H7D;I E8J7?D;: M?J> L7H?EKI )&, 9ED9;DJH7J?EDI
UNCORRECTED PROOF
H.N. Doan et al. Journal of Environmental Chemical Engineering xxx (xxxx) xxx-xxx
Fig. 6. 7 0 7D: ?DJHKI?ED FH;IIKH; E< J>; H)-)&, C;C8H7D; 8 E?B 9EDJ79J 7D=B; 7D: KD:;HE?B 0 E< J>; H)-)&, C;C8H7D; 9 :OD7C?9 C;7IKH;C;DJ E< M7J;H 7:>;
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M7J;H ?D 7?H r?I J>; 9KHL7JKH; H7:?KI E< C;D?I9KI θw?I J>; 9EDJ79J 7D
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H.N. Doan et al. Journal of Environmental Chemical Engineering xxx (xxxx) xxx-xxx
3.4. Mechanical properties
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UNCORRECTED PROOF
H.N. Doan et al. Journal of Environmental Chemical Engineering xxx (xxxx) xxx-xxx
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C?NJKH; I I>EMD ?D ?= ; 7D: /?:;E , J>; H)-)&,6 C;C
8H7D; M7I ]N;: JE 7 C;C8H7D; >EB:;H 9EDD;9J;: JE 7 L79KKC FKCF
JE O?;B: 7 FH;IIKH;:H?L;D ^EM <EH E?BM7J;H I;F7H7J?ED 0?J> IKF;H
E;B;EF>?B?9 FHEF;HJ?;I J>; E?B 97D H7F?:BO F;HC;7J; J>HEK=> J>; C;C
8H7D; (D J>; EJ>;H >7D: J>; KD:;HE?B IKF;H>O:HEF>E8?9?JO FH;L;DJI
J>; M7J;H <HEC F;HC;7J?D= J>HEK=> J>; C;C8H7D; B;7:?D= JE J>; >?=>
E?BM7J;H I;F7H7J?ED ;<]9?;D9O E< J>; IOIJ;C ;97KI; E< ?JI ;N9;BB;DJ
I;F7H7J?ED FHEF;HJ?;I J>; H)-)&,6 C;C8H7D; ?I 78B; JE I;F7H7J;
:?<<;H;DJ E?BM7J;H C?NJKH;I 7D: J>KI >7I FEJ;DJ?7B ?D:KIJH?7B 7FFB?97
J?EDI
4. Conclusion
 BEM9EIJ 7D: ;DL?HEDC;DJ7BBO <H?;D:BO ]8HEKI C;C8H7D; <EH
E?BM7J;H I;F7H7J?ED M7I IK99;II<KBBO <78H?97J;: ->; )&,<KD9J?ED
7B?P;: H)- C;C8H7D;I M?J> IKF;HEB;EF>?B?9 7D: KD:;HE?B IKF;H>O
:HEF>E8?9 FHEF;HJ?;I M;H; C7:; KI?D= ;B;9JHEIF?DD?D= 7D: :?F9E7J?D=
C;J>E:I ->; CEHF>EBE=O 9>;C?97B 9ECFEI?J?ED J>;HC7B 7D: C;9>7D
?97B FHEF;HJ?;I IKH<79; M;JJ78?B?JO 7D: E?BM7J;H I;F7H7J?ED F;H<EHC7D9;
E< J>; H)- C;C8H7D; 97D 8; 9EDJHEBB;: 8O C7D?FKB7J?D= J>; )&,
9ED9;DJH7J?ED ?D J>; :?F9E7J?D= IEBKJ?ED ->; H)-)&, C;C8H7D;
I>EMI 7 >?=> E?BM7J;H I;F7H7J?ED F;H<EHC7D9; M?J> ;N9;BB;DJ 7DJ?M7
J;H <EKB?D= 8;>7L?EH ;97KI; E< ?JI EKJIJ7D:?D= 7DJ?M7J;H <EKB?D= FHEF
;HJ?;I J>; H)-)&, C;C8H7D; ?I 78B; JE A;;F 7 >?=> I;F7H7J?ED F;H
<EHC7D9; 7<J;H J;D 9O9B;I J>KI FEII;II?D= =H;7J FEJ;DJ?7B <EH E?BM7J;H
I;F7H7J?ED FHE9;:KH;I
UNCORRECTED PROOF
H.N. Doan et al. Journal of Environmental Chemical Engineering xxx (xxxx) xxx-xxx
+;:?- 7KJ>EHI>?F 9EDJH?8KJ?ED IJ7J;C;DJ
Hoan Ngoc Doan: ED9;FJK7B?P7J?ED "DL;IJ?=7J?ED 0H?J?D=  EH?=?D7B
:H7<J Phu Phong Vo: "DL;IJ?=7J?ED Kohei Hayashi: "DL;IJ?=7J?ED
Kenji Kinashi: ,KF;HL?I?ED 0H?J?D=  H;L?;M  ;:?J?D= Wataru Sakai:
0H?J?D=  H;L?;M  ;:?J?D= Naoto Tsutsumi: 0H?J?D=  H;L?;M 
;:?J?D=
Declaration of Competing Interest
->; 7KJ>EHI :;9B7H; J>7J J>;O >7L; DE ADEMD 9ECF;J?D= ]D7D9?7B
?DJ;H;IJI EH F;HIED7B H;B7J?EDI>?FI J>7J 9EKB: >7L; 7FF;7H;: JE ?D^K;D9;
J>; MEHA H;FEHJ;: ?D J>?I F7F;H
Acknowledgements
->?I IJK:O M7I F7HJ?7BBO IKFFEHJ;: 8O H7DJI?D?: <HEC #,),
EH;JEEH; )HE=H7C  I?7<H?97 ,9?;D9; )B7J<EHCI #7F7D !'
?I I?D9;H;BO =H7J;<KB JE )HE<;IIEH ,EDE ,7I7A? $"- <EH 9EDJ79J 7D=B;
9>7H79J;H?P7J?ED 7D: )HE<;IIEH -7A;I>? ,>?EDE $"- <EH ,& 9>7H
79J;H?P7J?ED !' =H;7JBO 79ADEMB;:=;I J>; &?D?IJHO E< :K97J?ED
,FEHJI 7D: KBJKH; E< #7F7D &1- I9>EB7HI>?F FHEL?:;: 8O J>; #7F7D
;I; EL;HDC;DJ <EH >?I IJK:?;I 7J $OEJE "DIJ?JKJ; E< -;9>DEBE=O
Appendix A. Supplementary data
,KFFB;C;DJ7HO C7J;H?7B H;B7J;: JE J>?I 7HJ?9B; 97D 8; <EKD: ?D J>;
EDB?D; L;HI?ED 7J :E?>JJFI:E?EH=@@;9;
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45 # ;O;H ! -H7DDKC - 7AA; )/ !E:IED -$ EBB?;H DL?HEDC;DJ7B ;<<;9JI
E< J>; ;;FM7J;H !EH?PED E?B IF?BB 7 H;L?;M &7H )EBBKJ KBB   –
>JJFI:E?EH=@C7HFEB8KB
45  #;HD;BVL !EM JE :;<;D: 7=7?DIJ <KJKH; E?B IF?BBI '7JKH;   –
>JJFI:E?EH=7
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+;:CED: 7J; E< :?IF;HI7DJI 7IIE9?7J;: M?J> J>; ;;FM7J;H !EH?PED E?B IF?BB DL
?HED ,9? -;9>DEB   – >JJFI:E?EH=;IF
45 2 >;D  %?K 0 %;?  )EHJ;>7KBJ , *?D )EHEKI 8EHED D?JH?:; D7DEI>;;JI <EH
;<<;9J?L; M7J;H 9B;7D?D= '7J ECCKD    >JJFI:E?EH=
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IFED=;I M?J> ;D>7D9;: I;B;9J?L; 97F?BB7H?JO <EH ;<]9?;DJ E?B IF?BB 9B;7DKF , FFB
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IF?BBI M;7J>;H;: KD:;H H9J?9 9ED:?J?EDI <HEC B78EH7JEHO IJK:?;I JE B7H=;I97B;
];B: ;NF;H?C;DJI &7H )EBBKJ KBB   – >JJFI:E?EH=
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78?B?JO L?7 ?DJ;H<79?7B IJ;H;E9ECFB;N 9HOIJ7BB?P7J?ED # &7J;H >;C   
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7H: &7J;H   – >JJFI:E?EH=@@>7PC7J
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@@>7PC7J
45 "' ,JH7?D * 0K & )EKHH7>?C? &, !;:;DGL?IJ +- (BIIED +% D:;HIIED
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-!
45 ' 37D:;H & ?BB7D  ,M;;JI;H +;9O9B;: )- D7DE]8;HI <EH M7J;H ]BJH7J?ED
7FFB?97J?EDI &7J;H?7BI 7I;B   – >JJFI:E?EH=
C7
45 & 3>7D= 0 &7 # K? , 0K # !7D 2 3EK  !K7D= !O:HEJ>;HC7B IODJ>;
I?P;: ./H;I?IJ7D9; 7D: JH7DIF7H;DJ 9E7J?D= 9ECFEI?J;: IKF;HEBE;F>?B?9 ;B;9JHE
IFKD C;C8H7D; <EH >?=> ;<]9?;D9O E?BO M7IJ;M7J;H JH;7JC;DJ # !7P7H: &7J;H
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45 # ; # 3>7D=  07D= 3 %? # 2K  ?D= ,KF;H>O:HEF>?B?9 7D: KD:;HM7J;H
IKF;HEB;EF>E8?9 D7DE]8HEKI C;C8H7D; M?J> >?;H7H9>?97B IJHK9JKH;: IA?D <EH ;<<;9
J?L; E?B?DM7J;H ;CKBI?ED I;F7H7J?ED # &7J;H >;C    – >JJFI
:E?EH=9J77
45 # ;  3ED= * #?D # 2K  ?D= ?EC?C;J?9 7D: IKF;HM;JJ78B; D7DE]8HEKI
IA?DI <EH >?=>BO ;<]9?;DJ I;F7H7J?ED E< E?B?D07J;H ;CKBI?EDI :L KD9J &7J;H
  – >JJFI:E?EH=7:<C
45 3 3>K 0 07D=  *? 2 %KE 2 %?K 2 1K  K?  07D= 1 >;D 7B9?D78B;
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45 2 %? 3 3>K # 2K  ?D= 7H8ED D7DEJK8;I ;D>7D9;: ^KEH?D7J;: FEBOKH;J>7D;
C79HEFEHEKI C;C8H7D;I <EH M7J;HFHEE< 7D: 8H;7J>78B; 7FFB?97J?ED , FFB
&7J;H "DJ;H<79;I   – >JJFI:E?EH=79I7C?
8
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7D; D;JMEHAI )EBOC;H  K?B:<   – >JJFI:E?EH=
@FEBOC;H
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CE7D7BOJ?97B 9>7H79J;H?P7J?ED E<  FEHEKI )&, <E7C C7J;H?7BI ->; ;<<;9J E< ?C
FKH?J?;I :;H?L;: <HEC 7 IK=7H J;CFB7J?D= FHE9;II )EBOC;HI 7I;B   –
>JJFI:E?EH=FEBOC
45 $ ]C;DAE 0 07BB79; # ;DP;H ,KH<79; CE:?]97J?ED E< ,OB=7H: FEBO:?
C;J>OB I?BEN7D; D;JMEHAI 8O KBJH7L?EB;J 7D: KBJH7L?EB;JEPED; JH;7JC;DJ # EB
BE?: "DJ;H<79; ,9?   – >JJFI:E?EH=@9?I
45 )) /E !' E7D $ $?D7I>? 0 ,7A7? ' -IKJIKC? ) !KOD> ;DJH?<K=7BBO
IFKD H;9O9B;: )- FHE9;II?D= 7D: 9>7H79J;H?P7J?ED )EBOC;HI 7I;B  
>JJFI:E?EH=FEBOC
45 $ $EJ7 $MED 0 >E? #& &78HO  -KJ;@7 !O=HEH;IFEDI?L; C;C8H7D;I
<EH ;<<;9J?L; E?B–M7J;H I;F7H7J?ED '7J ECCKD    >JJFI:E?EH=
D9ECCI
45 # ; # 3>7D=  07D= 3 %? # 2K  ?D= ,KF;H>O:HEF>?B?9 7D: KD:;HM7J;H
IKF;HEB;EF>E8?9 D7DE]8HEKI C;C8H7D; M?J> >?;H7H9>?97B IJHK9JKH;: IA?D <EH ;<<;9
J?L; E?B?DM7J;H ;CKBI?ED I;F7H7J?ED # &7J;H >;C    – >JJFI
:E?EH=9J77
45  >;D  0;D=  &7>CEE: , >;D # 07D= ,;F7H7J?ED C;9>7D?IC 7D: 9ED
IJHK9J?ED E< IKH<79;I M?J> IF;9?7B M;JJ78?B?JO <EH (?B07J;H I;F7H7J?ED , FFB
&7J;H "DJ;H<79;I   – >JJFI:E?EH=79I7C?
8
UNCORRECTED PROOF
H.N. Doan et al. Journal of Environmental Chemical Engineering xxx (xxxx) xxx-xxx
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8;H= ?E?DIF?H;: I;B<H;F7?H?D= IB?FF;HO IKH<79;I M?J> FH;IIKH;IJ78B; ECD?F>E8?9
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45 & -;D@?C87O7I>? #2 )7HA # &KJE 2 $E87O7I>? + 2EI>?A7M7 2 &EDD7? ,
,>?H7JEH? "D I?JK <EHC7J?ED E< IB?FF;HOB?GK?:"D<KI;: D7DE]8HEKI IKH<79; <EH
7 JH7DIF7H;DJ 7DJ?<EKB?D= ;D:EI9EF; %;DI 79I 8?EC7J;H ,9? D=   >JJFI
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45 - "I\A && ;C?H -7?BEH;: ;B;9JHEIFKD ]8;HI <HEC M7IJ; FEBOIJOH;D; <EH >?=> E?B
7:IEHFJ?ED ,KIJ7?D &7J;H -;9>DEB  ;>JJFI:E?EH=@
IKIC7J;
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... There are relatively few studies on the modification of PET super-hydrophilic/super-oleophobic membranes [16,17]. PET membranes are typically modified by altering the surface hydrophobic groups, specifically the ester groups. ...
A novel chemical crosslinking enabled special wettability coating for higher efficiency oil–water separation
Article
Full-text available
  • Apr 2024
  • APPL PHYS A-MATER
The environmental destruction caused by oil pollution has been an inescapable fact, and there is an urgent need for efficient separation materials to solve this problem. Generally speaking, Polyethylene terephthalate (PET) is relatively easy to modify into super-hydrophobic/super-oleophilic membranes due to its hydrophobic ester groups. However, there are some challenges in preparing them as underwater super-oleophobic films. Herein, this paper proposes a two-step coating method for the preparation of underwater super-oleophobic PET films by coating the surface of PET films with silicone to form a cross-linked layer through polymerization (Cross-linking), followed by coating the surface of the cross-linked layer with a fluorinated compound/SiO2 (Coating-F@SiO2). Experiments have shown that the new filter membrane exhibits excellent corrosion resistance and special wettability (> 150°). After 30 filtration cycles, it still maintains excellent oil–water separation efficiency (> 99.9%). This simple method for preparing oil–water separation membrane enriches the treatment process of oil pollution. The large-area and low-cost preparation route also provides a prospect for scalable applications.
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... Oil/water separation was done using a membrane made of cellulose and ionic liquids [31]. Doan et al. [32] employed functionalized PDMS as a membrane for the oil/ water separation. Cellulose-based membrane was used for NaCl rejection from the water [33]. ...
Azadirachta indica seed powder–reinforced and nano sand–filled USPER membrane for oil/seawater separation
Article
Full-text available
  • Feb 2024
In situ methyl ethyl ketone peroxide–mediated free radial curing was used to synthesize a traditional Azadirachta indica seed (AIS) powder–reinforced and nano sand–filled unsaturated polyester resin (USPER) composite under various experimental settings. Different thermal characteristics (such as differential scanning calorimetry and thermogravimetric analysis), scanning electron microscopy, energy-dispersive X-ray spectroscopy, colour mapping, Fourier transform infrared spectrum, antimicrobial activities and water contact angle measurements were used to characterize the prepared USPER composite. The USPER composite’s various mechanical and physico-chemical characteristics were also studied. The usage of the USPER composite–based membrane for oil/seawater separation was studied. The USPER composite’s tensile strength revealed a 0.17 order of dependence at different percentage weight loadings of nano sand. The mechanical characteristics grew gradually as the concentration of nano sand rose. The highest water flux was calculated to be 62.5 L/m²/h with a 100% oil rejection efficiency. The outcomes were contrasted with the values from the literature.
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Preparation and application of stimuli-responsive PET TeMs: RAFT graft block copolymerisation of styrene and acrylic acid for the separation of water–oil emulsions
Article
Full-text available
  • May 2024
Stimuli-responsive membranes play an important role in the fields of biomedicine, food and chemical industries, and environmental applications, including separation of water–oil emulsions. In this study, we present a method to fabricate pH-sensitive membranes using UV-initiated RAFT graft copolymerization of styrene (ST) and acrylic acid (AA) on poly(ethylene terephthalate) (PET) track-etched membranes (TeMs). The optimization of polymerization conditions led to successful grafting of polystyrene (PS) and poly(acrylic acid) (PAA) onto PET TeMs, resulting in membranes with stable hydrophobicity and pH change responsiveness. The membranes show a contact angle of 65° in basic environments (pH 9) and 97° in acidic environments (pH 2). The membranes were characterized by atomic force microscopy (AFM), scanning electron microscopy with energy dispersive X-ray spectroscopy (SEM-EDX), thermogravimetric analyses (TGA), Fourier transform infrared spectroscopy (FTIR), contact angle (CA) methods. The PET TeMs-g-PS-g-PAA exhibited good performance in separating water–oil emulsions with a high efficiency of more than 90% and flux for direct chloroform–water 2500 L m⁻² h⁻¹ and reverse emulsions of benzene–water 1700 L m⁻² h⁻¹. This method of preparing stimuli-responsive membranes with controlled wettability and responsiveness to environmental pH provides versatility in their use in separating two types of emulsions: direct and reverse.
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The global risks of increasing reliance on bottled water
Article
Full-text available
  • Jul 2018
The rapid growth of bottled water use in low- and middle-income countries, and its normalization as a daily source of drinking water, does not provide a pathway for universal access. Generous and sustained investment in centralized and community utilities remains the most viable means for achieving safe water access for all. OPEN-ACCESS LINK TO PAPER https://rdcu.be/234K
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Centrifugally Spun Recycled PET: Processing and Characterization
Article
Full-text available
  • Jun 2018
Centrifugal spinning, which is a high-productivity fiber fabrication technique, was used to produce a value-added product from recycled poly(ethylene terephthalate) (rPET). In the present study, rPET fibers, with fiber diameters ranging from submicron to micrometer in scale, were fabricated by spinning a solution of rPET in a mixture of dichloromethane and trifluoroacetic acid. The influence of the polymer solution concentration (the viscosity), the rotational speed of the spinneret, and the inner diameter of the needles on the formation and morphology and mechanical properties of the fibers were examined through scanning electron microscopy and using a tensile testing machine. The thermal behaviors of fibrous mats with various average diameters were also investigated through differential scanning calorimetry. The smoothest and smallest fibers, with an average diameter of 619 nm, were generated using an rPET solution of 10 wt % under a rotation speed of 15,000 rpm using needles having an inner diameter of 160 µm. The fibrous mats have an average tensile strength and modulus of 4.3 MPa and 34.4 MPa, respectively. The productivity and the mechanical properties indicate that centrifugal spinning is an effective technique to fabricate high-value product from rPET.
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Hydrothermal synthesized UV-resistance and transparent coating composited superoloephilic electrospun membrane for high efficiency oily wastewater treatment
Article
  • Sep 2019
  • J HAZARD MATER
As oily wastewater issues continue to grow, the treatment of oily wastewater has become urgent an emergency. However, present solutions are restricted by the limited performance of materials. An UV-resist and transparent coating consisting of PDMS and ZnO decorated on a highly stable and self-standing polyimide is reported in this work as a potential solution. The obtained fibrous membranes not only allow high-efficiency (higher than 99%) oily wastewater separation but also show superior UV-resistant activity. Moreover, the superoleophilicity and hydrophobicity of the composite membrane were confirmed to be stable under harsh conditions, and the transparent coating layer has the potential to be applied in other fields. The design of the UV-resistant, transparent and superoleophilic nanofibrous membrane is very practical, and will be quite promising for reducing oily environmental contaminations from waters.
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Electrospun flexible nanofibrous membranes for oil/water separation
Article
  • Aug 2019
Frequent oil spills and ever-growing discharge of industrial oily wastewater seriously threaten the ecosystem and human safety, and result in huge economic loss, which has stimulated researchers to explore advanced oil/water separation materials. Electrospun nanofibrous membranes, featuring tunable wettability, good flexibility, high porosity, and outstanding pore connectivity, have received increasing attention. In this review, we aim to present the design and fabrication of electrospun flexible nanofibrous membranes with special wettability for oil/water separation. This review focuses on the discussion of various electrospun flexible membranes, assorted into three categories, including polymer-based membranes, ceramic-based membranes, and carbon-based membranes. In each type, the representative works, fabrication techniques, and the synergistic effect among membrane structure, selective wettability, and oil/water separation performance are discussed in detail. Finally, future perspectives and challenges in the promising field are highlighted.
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Electrospun frogspawn structured membrane for gravity-driven oil-water separation
Article
  • Mar 2019
The aim of this study is to prepare a fibrous membrane scaffold that possesses a frogspawn structure for high-efficiency oil-water separation. Polyamic acid was first electrospun onto a rotating wheel-collector to obtain the fibrous membrane. Subsequently, post-processing by immersion in a polydimethylsiloxane solution and a silica nanoparticles suspension, followed by a thermal treatment generated a frogspawn-structured fibrous membrane. The obtained membrane achieved superhydrophobicity and superoleophilicity, with the water contact angle as high as 155.75° and the oil contact angle lower than 10°. The separation efficiencies of the membrane were higher than 99.55% and the permeate flux was maintained at greater than 4400 L/m ² ∙h after 20 separation cycles. Additionally, the wettability studies suggested the membrane exhibits high stability because it can resist damages due to high temperature (150 °C), acid/basic conditions and organic/inorganic solvents. These findings indicated that this composite membrane has great potential for use in gravity-driven oil-water separation and can extend the range of its application for treatments of oil spills incident, oily wastewater and spent liquor.
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Separation Mechanism and Construction of Surfaces with Special Wettability for Oil/Water Separation
Article
  • Feb 2019
Oil leakage and the discharge of oil/water mixtures by domestic and industrial consumers have caused not only severe environmental pollution and a threat to all species in the ecosystem but also a huge waste of precious resources. Therefore, the separation of oil/water mixtures, especially stable emulsion, has become an urgent global issue. Recently, materials containing special wettability feature for oil and water have drawn immense attention due to their potential applications for oil/water separation application. In this paper, we systematically summarize the fundamental theories, separation mechanism, design strategies, and recent developments in materials with special wettability for separating stratified and emulsified oil/water mixtures. The related wetting theories that unveil the physical underlying mechanism of the oil/water separation mechanism are proposed and the practical design criteria for oil/water separation materials are provided. Guided by the fundamental design criteria, various porous materials with special wettability characteristics, including those which are superhydrophilic-underwater superoleophobic, superhydrophobic-superoleophilic, and superhydrophilic-in air superoleophobic are systemically analyzed. These superwetting materials are widely employed to separate oil/water mixtures: from stratified oil/water to emulsified ones. In addition, the materials that implement the demulsification of emulsified oil/water mixtures via the ingenious design of multiscale surface morphology and the construction of special wettability are also discussed. In each section, we introduce the design ideas, base materials, preparation methods, and representative works in detail. Finally, the conclusions and challenges for the oil/water separation research field are discussed in depth. Keywords: oil/water mixture, emulsion, special wettability, oil/water separation, demulsification
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Sustainable approach to recycle waste polystyrene to high-value submicron fibers using solution blow spinning and application towards oil-water separation
Article
  • Nov 2018
Polystyrene waste disposal is an environmental challenge and transforming it into value-added products such as submicron fibers is an attractive paradigm. In this work, we have reported a sustainable approach to deal with the twin issues of handling low-density polystyrene waste and its re-utilization. Using ethyl acetate as a costefficient environmentally preferable solvent, we have successfully demonstrated conversion of waste expanded polystyrene (WPS) into hydrophobic fibers via solution blow spinning technique and its application towards oilwater separation. The macroscale spray pattern analysis in combination with microscale analysis is reported as a facile tool for evaluating the effect of polymer solution properties and operating parameters on the spray morphology. Additionally, the fiber spinnability limits are identified that provide the operational parameters in which fibers without any undesirable structural features are obtained. Here, the lower fiber spinnability limits were identified as 6 wt% polymer concentration, 3 kg cm⁻² gas pressure and 10 cm nozzle-to-target distance, below which excessive beads or film formation was observed. The upper fiber spinnability limits were 14 wt% polymer concentration and 5 kg cm⁻² gas pressure beyond which the solution blow spinning was not feasible. Moreover, wettability studies showed the enhanced hydrophobic and superoleophilic behavior of the synthesized WPS fibrous mats with water contact angle as ~138° and oil contact angle as ~0°. The WPS fiber-coated membrane demonstrated a maximum separation efficiency of 97% for free oil (diesel)-water mixtures, indicating potential applications in oil recovery and treatment of oily wastewater.
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Tailored electrospun fibers from waste polystyrene for high oil adsorption
Article
  • Nov 2018
Recent ship accidents that resulted catastrophic oil spills necessitate producing environmentally friendly, cost-effective, and large-scale fabrication technology for oil- sorbent materials. Various material systems have been employed to fabricate sorbent materials; however, using fresh material components as adsorbent can lead to a secondary pollution. Therefore, recycling of plastics wastes for the fabrication of adsorbent material could be a wise approach to handle this environmental issue. In this study, foam-expanded polystyrene (f-PS), a commodity polymer used for insulation and packing materials, was electrospun from solution mixture of THF and DMF. Surface and interior porosity were achieved from individual fibers electrospun from a composition of DMF:THF (1:3) at 20-wt% of solid f-PS content. The resulting adsorbents exhibited a considerable hydrophobicity (WCA ≈ 120°) and oleophilicity (CA ≈ 10°), which can selectively adsorb both vegetable and engine oils from polluted waters. The porosity of the fibers has significant effect on the sorption capacity and separation efficiency up to 124 g/g and 99%, respectively. Thus, electrospun mats of the polystyrene wastes offer a promising adsorbent for the remediation of oily wastewaters.
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Polybenzoxazine Functionalized Melamine Sponges with Enhanced Selective Capillarity for Efficient Oil Spill Cleanup
Article
  • Oct 2018
Severe environmental and ecological issues arising from the frequent oil spill accidents have been great worldwide concerns. Considering the abruptness, complex condition, and long-term perniciousness of the spilled oil, the development of economic and versatile materials to quickly remove oil contaminants, especially for oil with high viscosity from a large water body is of significant importance, but remain a big challenge. Herein, we demonstrated a facile strategy to fabricate a versatile hierarchical structured sponge with superhydrophobicity and powerful oil capillarity via the in situ polymerization of a novel phenolic resin (polybenzoxazine) composite open-cell sponges. The tuneable hierarchical structures of the as-prepared sponge significantly improved its water repellence and oil capillarity; meanwhile, a plausible mechanism is also proposed. With the merits of high porosity, excellent water repellence, enhanced oil capillarity, and robust mechanical stability, the obtained sponge exhibited an intriguing oil spill clean-up performance with fast oil absorption speed, good recyclability, and high absorption capacity. Besides that, the modified sponge could also be utilized for the separation of oil/water mixture with individual phase and the surfactant-stabilized emulsion solely under the driven of gravity. The robust oil/water separation performance, low cost, and facile synthesis strategy make the resultant sponges a competitive material for the large scale oil spill emergency remediation.
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