ĈҤI HӐC QUӔC GIA TP. HCM
75ѬӠ1*ĈҤI HӐ&%È&+.+2$
PHҤ0/é'8<7+8<ӂT
1*+,Ç1&ӬU TӘNG HӦ39¬ĈÈ1+*,È+2Ҥ77Ë1+
CӪA MOF-808 KHUYӂT TҰ77521*48È75Î1++ҨP
PHӨ &U 9, 9¬&+ҨT 0¬8+Ӳ8&Ѫ7521*1ѬӞC
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22 WKiQJ01 QăP22
7KjQKSKҫn HӝLÿӗQJÿiQKJLiOXұQYăQWKҥFVƭJӗm:
1. Chӫ tӏch: PGS. TS. Mai HuǤnh Cang
2. Phҧn biӋn 1: TS. %L7ҩQ1JKƭD
3. Phҧn biӋn 2: TS. Phan NguyӉn QuǤnh Anh
4. Ӫ\YLrQ TS. NguyӉQĈăQJ.KRD
5. Ӫ\YLrQWKѭNê TS. PhҥP+RjQJ+X\3Kѭӟc Lӧi
;iFQKұn cӫa Chӫ tӏch HӝLÿӗQJÿiQKJLiOXұQYăQYj7Uѭӣng Khoa quҧQOêFKX\rQ
QJjQKVDXNKLOXұQYăQÿmÿѭӧc sӱa chӳa (nӃXFy
CHӪ TӎCH HӜ,ĈӖNG
75ѬӢNG KHOA
*6763KDQ7KDQK6ѫQ1DP
ĈҤI HӐC QUӔC GIA TP.HCM
CӜ1*+Ñ$;+ӜI CHӪ 1*+Ƭ$9,ӊT NAM
75ѬӠ1*ĈҤI HӐ&%È&+KHOA
Ĉӝc lұp - Tӵ do - HҥQKSK~F
NHIӊM VӨ LUҰ19Ă17+Ҥ&6Ƭ
Hӑ WrQKӑFYLrQ PhҥP/ê'X\7KX\Ӄt
MSHV: 2070268
1Jj\WKiQJQăPVLQK 03/07/1997
1ѫLVLQK %uQKĈӏnh
&KX\rQQJjQK .ӻ thuұW+yD hӑc
0mVӕ: 8520301
,7Ç1Ĉӄ 7¬,
Bҵng tiӃng ViӋt: 1JKLrQFӭu tәng hӧSYjÿiQKJLiKRҥWWtQKFӫa MOF-808 khuyӃt
tұt trong hҩp phө ion Cr(VI) YjFiFFKҩWPjXKӳXFѫ WURQJQѭӟc.
Bҵng tiӃng Anh: Synthesis and application of defective MOF-808 materials for
the adsorption of Cr(VI) and organic dyes in water.
NHIӊM VӨ 9¬1ӜI DUNG:
x Tәng hӧp vұt liӋu MOF-808 khuyӃt tұt bҵng FiFKVӱ dөng hӛn hӧp phӕi tӱ.
x 3KkQWtFKFҩXWU~FFӫa vұt liӋu MOF-808 khuyӃt tұt sau tәng hӧp.
x ĈiQKJLiNKҧ QăQJKҩp phө &U 9, YjFiFchҩt PjXhӳXFѫWURQJQѭӟc cӫa vұt
liӋu MOF-808 khuyӃt tұt.
,,1*¬<*,$21+,ӊM VӨ: 06/09/2021
,,,1*¬<+2¬17+¬1+1+,ӊM VӨ: 20/12/2021
,9&È1%Ӝ +ѬӞNG DҮN: 76/r9NJ+j761JX\ӉQĈăQJ.KRD
NӝLGXQJYj\rXcҫX/971ÿmÿѭӧFWK{QJTXDEӝ P{Q
1Jj\
WKiQJ
QăP
1Jj\ WKiQJ
QăP
1Jj\ WKiQJ QăP
75ѬӢNG KHOA
CHӪ NHIӊM BӜ 0Ð1
CBHD &+Ë1+
GS. TS. 3+$17+$1+6Ѫ11$0
3*676/Ç7+ӎ HӖNG NHAN
76/Ç9lj+¬
LӠI CҦ0Ѫ1
LӡLÿҫXWLrQW{L[LQJӱi lӡi cҧPѫQÿӃQJLDÿuQKQKӳng QJѭӡi WKkQOX{Q \rX WKѭѫQJ
ÿӝng YLrQ Yj hӛ trӧ W{LQKӳng l~FNKy NKăQ trong cuӝc sӕng. Nhӡ vұy W{L FythӇ
KRjQWKjQKTXiWUuQKKӑc tұp tҥLWUѭӡQJĈҥi hӑF%iFK.KRD
7{L[LQFҧPѫQFiFWKҫ\F{WURQJEӝ P{Q.ӻ thuұW+yDKӳXFѫFiFDQKFKӏ phө
WUiFKSKzQJWKtQJKLӋm Kӻ thuұW+yDKӳXFѫÿmWҥRÿLӅu kiӋn tӕt nhҩt vӅ FѫVӣ vұt
chҩt, sҳp xӃp thӡLJLDQÿӇ W{LFyWKӇ thӵc hiӋQWKtQJKLӋm vӟLÿLӅu kiӋn tӕt nhҩt.
Ĉһc biӋt, W{L muӕn gӱi lӡi cҧm ѫQ VkX sҳc ÿӃn 76/r9NJ+j Yj76 NguyӉQĈăQJ
Khoa, nhӳng QJѭӡi thҫy ÿmWұQWuQKFKӍ dҥ\ÿӝQJYLrQYjOX{QWKHRViWW{LWURQJ
TXiWUuQKOjPWKtQJKLӋPTXDQWkPJL~Sÿӥ W{LWURQJVXӕt thӡLJLDQOjPOXұQYăQ
Thҫ\ÿmWUX\ӅQÿҥWFKRW{LQKLӅu kiӃn thӭc, kinh nghiӋPTXêEiX YjSKѭѫQJSKiS
QJKLrQFӭu, sҳp xӃSF{QJYLӋc mӝWFiFK khoa hӑc.
ĈӇ KRjQWKjQKluұQYăQ Qj\QJRjLQKӳng nӛ lӵc cӫa bҧQWKkQW{LFNJQJ[LQFҧm
ѫQ sӵ hӛ trӧ nhiӋWWuQKFӫa nhӳQJQJѭӡi bҥn, WKjQKYLrQQJKLrQFӭXOjPWKtQJKLӋm
tҥi 3KzQJWKtQJKLӋm 209B2 WURQJTXiWUuQKWKӵc hiӋn luұQYăQ.
%iFK.KRDQJjy 08 thing 01 QăP2022
+ӑFYLrQWKӵc hiӋn
3KҥP/ê'X\7KX\ӃW
7Ï07ҲT LUҰ19Ă1
Trong luұQ YăQ Qj\ FiF Yұt liӋu Zr-MOF khuyӃt tұt (MOF-B2+ Yj 02)808_NH2 ÿm ÿѭӧc tәng hӧS WKjQK F{QJ sӱ dөng mӝt hӛn hӧp chӭa benzene
WULFDUER[\OLFDFLGYjGүn xuҩt benzene dicarboxylic acid bҩWÿӕi xӭng3KkQWtFKQKLӉu
xҥ tia X dҥng bӝW 3;5' ÿm[iFQKұn FiFvұt liӋu khuyӃt tұt FyFҩXWU~FWLQKWKӇ
WѭѫQJWӵ QKѭ02)-808 gӕc. DӵDWUrQNӃt quҧ SKkQWtFK1H-NMR, tӍ lӋ khuyӃt tұt cӫa
FiFYұt liӋu MOF-B2+Yj02)-808_NH2 ÿѭӧF[iFÿӏnh lҫQOѭӧWOjYj
Sӵ xuҩt hiӋn cӫDFiFNKX\Ӄt tұt trong mҥng tinh thӇ JL~SFҧi thiӋn ÿiQJNӇ FiFÿһc
WtQKmao quҧn YjNtFKWKѭӟc tinh thӇ cӫa MOF-808. Vӟi cҩu WU~FYӟi FiFWkPDFLG
sҹQFyYjFiFWkPKҩp phө mӟLÿѭӧc bә VXQJWK{QJTXDFiFNKX\Ӄt tұt, FiFMOF-808
khuyӃt tұt thӇ hiӋQiLOӵc mҥnh vӟi FiFDQLRQQKѭLRQ&U 9, YjFiFFKҩWPjXDQLRQ
QKѭsunset yellow (SY) Yjquinoline yellow 4< YjPHWK\ORUDQJH 02 . %rQFҥnh
ÿyFiFYұt liӋXQj\FNJQJWKӇ hiӋn khҧ QăQJKҩp phө ÿiQJNӇ ÿӕi vӟLFiFFKҩWPjX
cation trong dung dӏch. .KL VR ViQK Yӟi vұt liӋu MOF-808 gӕc, hiӋu quҧ cӫD FiF
khuyӃt tұWÿѭӧc tҥRWKjQKÿѭӧc chӭQJPLQKWK{QJTXDYLӋc cҧi thiӋn khҧ QăQJKҩp
phө cӫa vұt liӋXÿӕi vӟi ion Cr(VI) (60 ± FiFchҩWPjXDQLRQ ± Yj
FiFFKҩWPjXFDWLRQ ± 20%). CiFYұt liӋu MOF-808 Qj\ ӣ dҥQJQJX\rQEҧn hay
khuyӃt tұt) ÿӅXFyKRҥWWtQKWӕWKѫQQKLӅu vұt liӋX02)NKiF.
i
ABSTRACT
In this thesis, defective Zr-based metal-organic framework materials, namely, MOF808_OH and MOF-808_NH2, were successfully synthesized in the presence of a
mixture containing benzene tricarboxylic acid and asymmetric benzene dicarboxylic
acid derivatives. X-ray powder diffraction measurements (PXRD) indicated that the
highly crystalline structure of the defective materials was in good agreement with the
pristine MOF-808. The quantity of defective sites in MOF-808-NH2 and MOF808_OH structures, which was determined via 1H-NMR analysis of the digested
materials, was found to be about 3% and 7%, respectively, of the total number of
linkers. The presence of the structural defects in the material framework led to
significant improvements in crystal size and porosity of MOF-808. The defective
MOF structure with more active sites due to such defects had a strong affinity with
dichromate anion and anionic dyes, e.g. sunset yellow, quinoline yellow, and methyl
orange (MO). Besides, MOF-808_OH and MOF-808_NH2 exhibited comparable
performances in trapping cation dyes, e.g methylene blue and malachite green. As
compared with the pristine MOF-808, defect-containing MOF-808 showed
considerable enhancements of adsorption capacities for Cr(VI) (60 ± 70%), anionic
dyes (25 ± 60%) and cationic ones (10 ± 20%). Among metal-organic framework
materials applied in the adsorptive removal of Cr(VI) and anionic dyes, defective
MOF-808 materials were proved as competitive and potential adsorbents.
ii
LӠ,&$0Ĉ2$1
7{L[LQFaPÿRaQÿk\OjF{QJWUuQKQJKLrQFӭu cӫDW{LFiFVӕ liӋXYjNӃt quҧ QrX
trong luұQYăQQj\OjWUXQJWKӵFYjFKѭDÿѭӧFF{QJEӕ trong luұQYăQFQJFҩp NKiF
NӃXNK{QJÿ~QJQKѭÿmQrXWUrQW{L[LQKRjQWRjQFKӏXWUiFKQJKLӋm vӅ ÿӅ WjLFӫa
PuQK
PhҥP/ê'X\7KuyӃt
iii
MӨC LӨC
DANH MӨ&+Î1+ҦNH ...................................................................................... vi
DANH MӨC BҦNG .............................................................................................. ix
DANH MӨC VIӂT TҲT ......................................................................................... x
LӠI MӢ ĈҪU ......................................................................................................... 1
&+ѬѪ1*
1.1
: TӘNG QUAN ..................................................................... 2
Vұt liӋu khung hӳXFѫ± kim loҥi (Metal-organic frameworks ± MOFs) ..... 2
1.1.1 Giӟi thiӋu vӅ MOFs.................................................................................. 2
1.1.2 CҩXWU~FFӫa MOFs .................................................................................. 2
&iFSKѭѫQJSKiSWәng hӧSYjKRҥWKyD02)V ......................................... 4
1.1.4 Mӝt sӕ WtQKFKҩWÿһFWUѭQJFӫa MOFs....................................................... 7
1.2
Kӻ thuұt tҥo khuyӃt tұt (defect-engineering) cho vұt liӋu MOFs ............... 12
&iFSKѭѫQJSKiSWҥo khuyӃt tұt cho MOFs ............................................ 13
1.2.2 ҦQKKѭӣng cӫDFiFNKX\Ӄt tұWÿӃQWtQKFKҩWYjӭng dөng cӫa MOFs ...... 19
1.3
Ӭng dөng vұt liӋu MOF trong hҩp phө xӱ OêFiFLRQNLPORҥi nһQJYjFiF
chҩWPjX hӳXFѫ ................................................................................................. 23
1.4
MөFWLrXFӫa luұQYăQ............................................................................... 27
&+ѬѪ1*
: THӴC NGHIӊM ............................................................... 28
2.1
NӝLGXQJQJKLrQFӭu ................................................................................ 28
2.2
3KѭѫQJSKiSQJKLrQFӭu .......................................................................... 28
2.3
+ya chҩWYjWKLӃt bӏ SKkQWtFK ................................................................... 29
2.3.1
+yDFKҩt ............................................................................................ 29
2.3.2
ThiӃt bӏ SKkQWtFK ............................................................................... 30
2.4
Quy WUuQKWәng hӧp MOF-808 khuyӃt tұWYjFiF=U-02)NKiF ................. 31
iv
2.4.1
Tәng hӧp MOF-808, MOF-BYj02)-808 khuyӃt tұt ............ 31
2.4.2
Tәng hӧp UiO-66 .............................................................................. 32
2.5
7KtQJKLӋPÿiQKJLiNKҧ QăQJKҩp phө LRQ&U 9, YjFKҩWPjXKӳXFѫ .... 33
2.5.1
7KtQJKLӋm hҩp phө ion Cr(VI) .......................................................... 33
2.5.2
7KtQJKLӋm hҩp phө chҩWPjX ............................................................ 35
&+ѬѪ1*
KӂT QUҦ 9¬%¬1/8ҰN ................................................ 37
3.1.
Tәng hӧp vұt liӋu MOF-808 khuyӃt tұt (defective MOF-808) .................. 37
3.2.
ĈһFWUѭQJcҩXWU~FFӫDFiFYұt liӋu MOF-808 khuyӃt tұt .......................... 38
3.2.1
CҩXWU~FYjKuQKWKiLFӫa tinh thӇ MOF-808 ...................................... 38
3.2.2
TӍ lӋ khuyӃt tұt trong cҩXWU~FYұt liӋu ................................................ 41
3.2.3
ĈһFWtQKPDRTXҧn cӫa vұt liӋu .......................................................... 44
3.2.4
Ĉӝ bӅn nhiӋt cӫa vұt liӋu.................................................................... 46
3.3.
ĈiQKJLiNKҧ QăQJKҩp phө cӫa cӫDFiFPүu vұt liӋu khuyӃt tұWÿӕi vӟi ion
&U 9, YjFiFFKҩWPjXKӳXFѫ ........................................................................... 48
3.3.1.
Khҧ QăQJKҩp phө ion Cr(VI) cӫDFiFPүu vұt liӋu khuyӃt tұt ............ 49
3.3.2.
Khҧ QăQJKҩp phө FiFFKҩWPjXDQLRQFӫDFiFPүu vұt liӋu ............... 52
3.3.3.
Khҧ QăQJKҩp phө FiFFKҩWPjXFDWLRQFӫDFiFPүu vұt liӋu .............. 59
3.3.4.
6RViQKNKҧ QăQJKҩp phө cӫa vұt liӋu khuyӃt tұt vӟi MOF-YjFiF
vұt liӋXNKiF .................................................................................................... 61
&+ѬѪ1*
: KӂT LUҰ19¬.,ӂN NGHӎ............................................ 68
4.1
KӃt luұn .................................................................................................... 68
4.2
KiӃn nghӏ.................................................................................................. 69
7¬,/,ӊU THAM KHҦO ..................................................................................... 70
PHӨ LӨC ............................................................................................................. 80
v
DANH MӨ&+Î1+ҦNH
+uQK Minh hӑa sӵ KuQKWKjQKFӫa cҩXWU~F02)V>@ ................................................. 3
+uQK DҥQJKuQKKӑc cӫDFiFORҥi phӕi tӱ hӳXFѫ OLQNHU FѫEҧQÿѭӧc sӱ dөng trong tәng
hӧp MOFs [6].................................................................................................................... 3
+uQK Mӝt sӕ dҥng cҩXWU~F6%8cӫa MOFs [6]. .......................................................... 4
+uQK4XiWUuQKWәng hӧp MOFs bҵQJSKѭѫQJSKiSQKLӋWGXQJP{L ............................ 5
+uQK Ҧnh SEM cӫa tinh thӇ MOF-ÿѭӧc tәng hӧp bҵQJSKѭѫQJSKiSJLDQKLӋWWK{QJ
WKѭӡQJ D YjJLDQKLӋt bҵQJYLVyQJ E >@ .................................................................... 6
+uQK 4Xi WUuQK Wәng hӧp UiO-66 khuyӃt tұW Fy Pһt chҩW ÿLӅu chӍnh (modulator)
WULIOXRURDFHWLFDFHWLF D YjELӃQÿәi cҩXWU~FGR[ӱ OêQKLӋt sau tәng hӧp (b) [22]............. 9
+uQK &ѫFKӃ ÿӅ xuҩt cho sӵ SKiYӥ cҩXWU~FFӫa Zr-02)VNKLFyPһWQѭӟc (lӓng) hoһc
KѫLQѭӟc [27]................................................................................................................... 10
+uQK &iFSKѭѫQJWKӭc tҥo MOFs bӅQQѭӟc dӵDWUrQWKX\Ӄt HSAB [26]. ................... 10
+uQK &ѫFKӃ ÿӅ xuҩt cho sӵ SKiYӥ cҩXWU~FFӫa Zr-MOFs trong dung dӏFKDFLG D Yj
trong dung dӏch base (b). ................................................................................................. 11
+uQK Sӵ NKiFELӋt vӅ cҩXWU~FFӫD02)VWK{QJWKѭӡQJYj02)VFyNKX\Ӄt tұt trong
khung mҥng [37]. ............................................................................................................ 13
+uQK 0{Wҧ biӃQÿәi cҩXWU~FFӫa vұt liӋu MIL-100 (Fe) qua xӱ OêDFLG>@ .......... 14
+uQK Minh hoҥ FKRTXiWUuQKÿѭDFiFSKӕi tӱ mҥFKGjLYjRFҩXWU~F02)VWK{QJTXD
TXiWUuQKWUDRÿәLOLQNHUFyVӵ hӛ trӧ cӫDGXQJP{L 6$/( VROYHQW-assisted linker exchange)
[40]. ................................................................................................................................ 15
+uQK Tәng hӧp vұt liӋu UiO-66 khuyӃt tұWGѭӟi sӵ hӛ trӧ cӫa argon plasma [42]. ... 15
+uQK Tәng hӧp MOF-5 gӕFYj02)-5 khuyӃt tұt bҵQJTXiWUuQKNӃWWLQKQKDQKYjVӱ
dөng hӛn hӧp phӕi tӱ [43]. .............................................................................................. 16
+uQK Minh hoҥ TXiWUuQKWәng hӧSFiF+3-UiO-66 vӟLNtFKWKѭӟc mao quҧQFyWKӇ ÿLӅu
chӍnh [45]. ....................................................................................................................... 17
+uQK Tәng hӧp Ru-MOFs khuyӃt tұt bҵQJFiFKVӱ dөng hӛn hӧp linker [46]. ......... 18
vi
+uQK &iFKѭӟng tiӃp cұQFKXQJÿӇ tҥRUDFiFWkPKRҥWWtQKÿyQJYDLWUz[~FWiFFӫa
MOFs [47]...................................................................................................................... 19
+uQK 0{Wҧ cҩXWU~F Fӫa UiO-66 khuyӃt tұW D [~FWiF &X8L2- E Yj [~F WiF
Cu/UiO-66 sau khi hoҥWKRiEҵQJNKt+2 (c) [51]. ........................................................... 21
+uQK 0{Wҧ TXiWUuQKWәng hӧp vұt liӋu UiO-66-D-NH2 bҵng p-arsanilic acid [54] ... 22
+uQK4X\WUuQKWәng hӧSFiFYұt liӋu MOF-808. ....................................................... 31
+uQK 4X\WUuQKWәng hӧp vұt liӋu UiO-66. ................................................................. 33
+uQK 0{Wҧ WKtQJKLӋPÿiQKJLiNKҧ QăQJKҩp phө K2Cr2O7 YjFKҩWPjX ................. 34
+uQK Tәng hӧSFiFYұt liӋu MOF-808. ...................................................................... 37
+uQK KӃt quҧ SKkQWtFK3;'FӫDFiFPүu vұt liӋu MOF-808 tәng hӧp. .................... 39
+uQK Ҧnh SEM cӫa vұt liӋu MOF-808 gӕc (a), MOF-B2+ E Yj02)-808_NH2 (c)
........................................................................................................................................ 40
+uQK Phә 1H NMR cӫa mүu MOF-808 gӕFÿmSKkQUm ............................................. 42
+uQK Phә 1H NMR cӫa mүu MOF-808_OH gӕFÿmSKkQUm ...................................... 43
+uQK Phә 1H NMR cӫa mүu MOF-808_NH2 gӕFÿmSKkQUm .................................... 44
+uQK Ĉѭӡng hҩp phө/giҧi hҩSÿҷng nhiӋt N2 cӫDFiFYұt liӋu tәng hӧp ӣ 77K. .......... 45
+uQK 3KkQEӕ NtFKWKѭӟc mao quҧn cӫDFiFYұt liӋu tәng hӧp. .................................. 46
+uQK KӃt quҧ SKkQWtFK7*$FӫDFiFPүu vұt liӋu tәng hӧp...................................... 47
+uQK CҩXWU~F=U-cluster cӫa UiO-66 vӟLFiFWkPDFLGÿѭӧFKuQKWKjQKEӣi khuyӃt tұt
trong mҥng tinh thӇ (a), DUT-67 vӟLOLrQNӃt phӕLWUt E 02)-808 vӟi 6 OLrQNӃt phӕLWUt
(c) [90] ........................................................................................................................... 48
+uQK Ҧnh Kѭӣng cӫa thӡLJLDQÿӃn khҧ QăQJKҩp phө ion Cr(VI) cӫa vұt liӋu MOFB2+YjMOF-808_NH2. ............................................................................................ 50
+uQK ҦQKKѭӣng cӫa nӗQJÿӝ dung dӏFKEDQÿҫXÿӃn khҧ QăQJKҩp phө ion Cr(VI) cӫa
vұt liӋu MOF-B2+YjMOF-808_NH2. ...................................................................... 51
+uQK ҦQKKѭӣng cӫa thӡLJLDQÿӃn khҧ QăQJKҩp phө SY cӫa vұt liӋu MOF-808_OH
YjMOF-808_NH2. .......................................................................................................... 53
vii
+uQK ҦQKKѭӣng cӫa thӡLJLDQÿӃn khҧ QăQJKҩp phө QY cӫa vұt liӋu MOF-808_OH
YjMOF-808_NH2. .......................................................................................................... 54
+uQK ҦQKKѭӣng cӫa thӡLJLDQÿӃn khҧ QăQJKҩp phө MO cӫa vұt liӋu MOF-808_OH
YjMOF-808_NH2. .......................................................................................................... 55
+uQK ҦQKKѭӣng cӫa nӗQJÿӝ dung dӏcKÿӃn khҧ QăQJKҩp phө SY cӫa MOF-808_OH
YjMOF-808_NH2 ........................................................................................................... 56
+uQK ҦQKKѭӣng cӫa nӗQJÿӝ dung dӏFKÿӃn khҧ QăQJKҩp phө QY cӫa MOF-808_OH
YjMOF-808_NH2 ........................................................................................................... 57
+uQK ҦQKKѭӣng cӫa nӗQJÿӝ dung dӏFKÿӃn khҧ QăQJKҩp phө MO cӫa MOF-808_OH
YjMOF-808_NH2 ........................................................................................................... 58
+uQK Khҧ QăQJ Kҩp phө chҩW PjX FDWLRQ 0% Yj 0* Fӫa MOF-B2+ Yj 02)808_NH2 ......................................................................................................................... 60
+uQK 6RViQKNKҧ QăQJKҩp phө cӫa vұt liӋu khuyӃt tұt vӟi MOF-808 gӕc. .............. 62
+uQK 6RViQKNKҧ QăQJKҩp phө cӫa vұt liӋu khuyӃt tұt vӟi MOF-808 gӕc. .............. 64
+uQK 6RViQKNKҧ Qăng hҩp phө cӫa vұt liӋu khuyӃt tұt vӟi UiO-66 tәng hӧp. ......... 66
+uQK$ Phә cӝQJKѭӣng tӱ hҥWQKkQSURWRQFӫa phӕi tӱ BDC_OH ............................ 80
viii
DANH MӨC BҦNG
Bҧng 1.1 Ӭng dөng cӫDFiFYұt liӋu MOFs trong hҩp phө ion Cr(VI). ............................. 24
Bҧng 1.2 Ӭng dөng cӫDFiFYұt liӋu MOFs trong hҩp phө chҩWPjXKӳXFѫ.................... 25
Bҧng 2.1 Danh mөFKyDFKҩt sӱ dөng ............................................................................. 29
Bҧng 2.2 7KjQKSKҫn tәng hӧp cӫa FiFYұt liӋu MOF-808. ............................................. 32
Bҧng 2.3 7K{QJWLQFӫDFiFFKҩWPjXÿѭӧc sӱ dөng trong luұQYăQ ................................. 36
Bҧng 3.1 DiӋQWtFKEӅ mһWULrQJYjNtFKWKѭӟc mao quҧn cӫDFiFYұt MOF-808. ............. 46
Bҧng 3.2 6RViQKÿһFWtQKPDRTXҧQYjWӍ lӋ khuyӃt tұt cӫa hai vұt liӋu khuyӃt tұt ........... 61
ix
DANH MӨC VIӂT TҲT
Tӯ viӃt tҳt
7rQÿҫ\ÿӫ
GiҧLWKtFK
MOF
Metal Organic Framework
Khung hӳXFѫ± kim loҥi
SBU
Secondary building unit
ĈѫQYӏ cҩXWU~FWKӭ cҩp
DMF
N,N-Dimethyl formamide
DEF
N,N-Diethyl formamide
DMSO
Dimethyl sulfoxide
mCUS
Modified coordinatively unsaturated
&iFWkPNLPORҥLNK{QJ
metal sites
EmRKRjSKӕLWUt
BTC
Benzene-1,3,5-tricarboxylic acid
BDC_OH
5-Hydroxyisophthalic acid
BDC_NH2
5-Aminoisophthalic acid
x
LӠI MӢ ĈҪU
Vұt liӋu khung hӳXFѫ-kim loҥL 02)V ÿѭӧc tҥRWKjQKWӯ FiFFҫu nӕi hӳXFѫYjFiF
WkPNLPORҥL02)VFyQKӳQJWtQKchҩWÿӝFÿiRQKѭFyFҩXWU~FWLQKWKӇ, diӋQWtFKEӅ
mһWULrQJOӟn Yj khung cҩXWU~FOLQKÿӝng. Nhӡ nhӳQJÿһFWtQKQәi bұt ҩ\Pj02)V
ÿѭӧFQJKLrQFӭu ӭng dөng trong nhiӅXOƭQKYӵFNKiFQKDXQKѭhҩp phөWiFKOѭXWUӳ
NKtWURQJSKkQWiFKKyDKӑF\VLQKYj[~FWiF.
7X\QKLrQ FiFWLQKWKӇ vұt liӋu MOFs thӇ hiӋn mӝt sӕ hҥn chӃ nhҩWÿӏnh WURQJTXi
WUuQK[~FWiFFNJQJQKѭKҩp phө do FiFlӛ mao quҧn nhӓ (micropore) cҧn trӣ sӵ di
chuyӇn cӫDFiFSKkQWӱ lӟn tro
11QJFiFNrQKPDRTXҧn. 7UrQWKӵc tӃ viӋc mӣ rӝng ÿѭӡQJNtQKPDRTXҧn MOFs Fy
thӇ thӵc hiӋn bҵQJFiFKlӵa chӑQFiF phӕi tӱ hӳXFѫ (linker) mҥch GjLKѫQ7X\QKLrQ
FiFYұt liӋu MOFs mao quҧn lӟQWKѭӡQJNpPEӅn thӫy nhiӋWYjFyJLiWKjQKFDR. Vҩn
ÿӅ quan trӑQJÿһt ra trong viӋc tәng hӧS02)VOjWҥRUDFiFYұt liӋu vӟLFiFPDRTXҧn
rӝQJKѫQQKѭQJYүQÿҧm bҧRÿѭӧFÿӝ bӅn cӫa vұt liӋX&KtQKYuYұy, nhiӅu QJKLrQ
cӭu ÿmFKRWKҩ\Kѭӟng tiӃp cұn mӟLOjtҥo khuyӃt tұt cho khung mҥng tinh thӇ cӫa
vұt liӋu. &iFNKuyӃt tұt tҥRWKjQKNK{QJQKӳQJOjPWăQJÿӝ rӝng mao quҧQPjFzQ
tҥRUDFiFWkPKRҥWWtQKÿһc biӋt cӫa vұt liӋu.
%rQFҥQKÿyVӵ xuҩt hiӋn cӫa Zr-MOFs vӟi ÿӝ bӅn caoYѭӧt trӝi so vӟLFiFQJKLrQ
cӭXWUѭӟFÿk\OjPӝWEѭӟc nhҧy vӑWWURQJOƭQKYӵc tәng hӧp MOFs. Trong sӕ FiF=rMOFs, MOF-808 ÿѭӧFFK~êÿӃn vӟi nhiӅu ÿһFWtQKQәi trӝi. Ĉһc biӋWOjWURQJFҩu
WU~F 02)- FiF Fөm kim loҥi zirconium chӍ cҫQ OLrQ NӃt vӟi 6 phӕi tӱ hӳX Fѫ
(WK{QJWKѭӡQJOjKRһc 8 ӣ FiF=U-MOFs ÿӇ GX\WUuNKXQJWLQKWKӇ) YjFzQOҥLFiF
vӏ WUtWUӕQJWKtFKKӧp cho viӋc hҩp phө anions. 1JRjLUDYiӋc tҥo khuyӃt tұt cho mҥng
tinh thӇ cӫa MOF-OjPӝt giҧLSKiS tiӅPQăQJJL~S mӣ rӝQJNtFKWKѭӟc mao quҧn,
QkQJFDRNKҧ QăQJKҩp thө so vӟi trҥQJWKiL gӕc. 'Rÿy, luұQYăQÿmOӵa chӑn thӵc
hiӋn QJKLrQFӭu vӅ tәng hӧSYjÿiQKJLiKRҥWWtQKFӫa MOF-808 khuyӃt tұt trong hҩp
phө &U 9, YjFKҩWPjXKӳXFѫWURQJQѭӟc.
1
&+ѬѪ1* : TӘNG QUAN
1.1
Vұt liӋu khung hӳXFѫ ± kim loҥi (Metal-organic frameworks ± MOFs)
1.1.1 Giӟi thiӋu vӅ MOFs
Tӯ F{QJWUuQKQJKLrQFӭu ÿҫXWLrQvӅ vұt liӋu khung kim loҥi-hӳXFѫ 0HWDO-Organic
Frameworks - MOFs) cӫDJLiRVѭ
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