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77
MnO2 Nanoparticles/Zeolite AgY
**
28/3/91تاريخ پذيرش:12/11/90:دريافتتاريخ : دهيچك
NaYNaNaY
AgNO3AgAgY Ag
AgY AgMn(NO3)2MnKMnO4KM(CSS)
SEM/EDAXXRDXFTIR
)CEES(()CEPS(
15.8 wt% Nano MnO2/Zeolite AgY(GC)
31PNMR(GC-MS)
nano-MnO2/Zeolite AgYna
)CEES(()CEPS(،،)DMMP(
]][[
DS2iiDSHDO2-
]][[
**[email protected] Demetonii Decontaminated solution 2
78
]][[
M2/nO.Al2O3.ySiO2.wH2OMnny y w
-
-YY]][[
-
]][[
AgY
vv
iv Aluminosilicateiv Faujasitev Confined space synthesis(CSS)
د)ج)ب)الف)
79
:هاو دستگاهييايميمواد ش
Mn(NO3)2.6H2OMnARARLoba ChimieLo
Alfa AesarAl
SEM/EDAXSE7353)(LEO 1455
XRDXRSheifert 3003 TT ShX-ray X
Cu kαFTIR FTIRIRSpectrum 100Sp
Perkin ElmerGC GC
Varian Star 3400 CXVaFIDFIOV-101 CW HP 80/100 2m×1.8 in
oCoCoCoCoCominmioCoC
oCo
)CEES(()CEPS((viviGC-MSGCVarian Star 3400
CXDB 5 MS, 101 mic, 30 m× 0.25 mm
ml/minmlNMRNM250 MHz) (Bruker
CAT.NO.1004 CAUniversal
:دروترماليبه روش هNaYت يسنتز زئول
NaYNaNa
vi Demeton
80
pHpH
]][[
ي:ونيبه روش تبادل AgYيات نقرهيه زئوليته
NaYNa
AgNO3Ag
AgYAg
AgY
]].[
: nano-MnO2/Zeolite AgYت يسنتز كامپوز
AgYMn(NO3)2.6H2O
KMnO4KM
]][[
-nanoتيكامپوزلهيد و دمتون به وسيل سولفيل فنيد، كلرو اتيل سولفيل اتيواكنش دسولفوره و حذف كلرو ات
MnO2/Zeolite AgY توسطGC وGC-MS:
GCGC-MS
81
با استفاده از nano-MnO2/Zeolite AgYتيله كامپوزيل فسفونات به وسيل متيمتيذب دواكنش حذف و ج
:1PNMRك يتكن
g/mlg/
rpmrpnano-MnO2/Zeolite AgY
rpmrp
31PNMRNMR
Ag+
))NaY(Si/Al = Na))NaX(Si/Al =
-
AgYAg
82
:FTIRو SEM ،EDAX،XRDله يوسبات سنتز شده بهيتركيو ساختارياخواص ذره،يمورفولوژيبررس
(SEM)
SEM
AgYAgAgYAg
NaY
nano-MnO2/Zeolite AgYEDAXED
(a) (b) (c)
(d) (e) (f)
(g) (h)
SEM(a AgY(1) (b , NaYAgY(2) (c ,(d 9.3 wt% MnO2/ AgY(2)MnO2/ AgY(2) (e 15.8 wt%N Ps (i, h MnO2
83
EDAX(a MnO2/ AgY(2) (b NaY 15.8 wt%
:(XRD)كس يپراش اشعه ايالگو
XRD
NaYNaAgYAgAg
NaYAgYAg
AgYnano-MnO2/Zeolite AgY na
MnO2 AgY
λλXX
θβFWHM
XRD(a AgY(1) (b , NaY
a) b)
(a) (b)
84
(c) (d)
(e) (f)
.AgY(2) (c(d9.3 wt -MnO2/ AgY(2)MnO2/ AgY(2) (e 15.8 wt%f NPs ( MnO2
:(FTIR)ه يل فوريمادون قرمز تبد
FTIRNaYNaAgYAgnano-MnO2/Zeolite AgYna
H2OHcm-1cm
cm-1cmO-H cm-1cmO-H-HH
cm-1cmT-O)T=Si, Al(
cm-1cmT-OTcm-1cm
T-Onano-MnO2/Zeolite AgY
cm-1cmO-H O-H-Hcm-1cm
Mn-O
IRIR(a AgY(1) (b , NaYAgY(2) (c ,(d 9.3 wt% MnO2/Zeolite AgY(2)15.8 wt%MnO2/Zeolite AgY(2) (e
85
د يل سولفيل فنيد و كلرو اتيل سولفيل اتيكلرو اتي تركيبات سولفورهب)ي(جذب و تخرزان دسولفورهيميبررس
:GC-MSو GCيهابا روشnano-MnO2/Zeolite AgYت يله كامپوزيبه وس
nano-MnO2/Zeolite AgYna˚C˚C±±
)GC((
GC GCCEESCEnano-MnO2/Zeolite AgYna
abcde
86
ab
c
d
GC GCnano-MnO2/Zeolite AgY na
(GC-MS)(
2-CEES2(EVS)
(HEES)
))(m/z=(m))(m/z =(m))(m/z=
الف) ب)
ب)الف)
87
m/zm/
m/zm/
و GCيهابا روشnano-MnO2/Zeolite AgYت يله كامپوزيوسب دمتون بهيتخرزان جذب و يميريگاندازه
GC-MS:
-
GC-MSGC
)methyl ethane sulfenate(
––––
O-ethyl-O-merhyle Vinyl Phosphorothioate
ب)الف)
88
GC GCDemetonDenano-MnO2/Zeolite AgY na
هاي مختلفو در زمانها در حلالهاي استخراج شده از كروماتوگرام. داده3جدول% جذب/تخريب
ab
c
d
methyl ethane sulfenateme(o –ethyl o – methyl s –vinyl phosphorothiate)(o
ب)الف)
89
:PNMR31ل فسفونات با استفاده از روش يمتليمتيزان جذب و حذف ديميبررس
nano-MnO2/Zeolite AgY
(DMMP)(DPNMR3131..
δ = 0 ppmδ δ = 33ppmδ
DMMP
DMMPDM
31PNMRDMMPDM
PNMR3131DMMPDMnano-MnO2/Zeolite AgYna
90
PNMR3131DMMPDMnano-MnO2/Zeolite AgYna
NaYNa
wt% MnO2wt
nano-MnO2/Zeolite AgY wt%wt
nano-MnO2/Zeolite AgY wt%wt
91
The Desulfurization and Removal of Sulfurous and Organo-phosphurous
Compounds via Using MnO2 Nanoparticles/Zeolite AgY Composite
Catalyst
Meysam Sadeghi**, Mohammad Reza Shahdadi, Hussein Toolabi and Mir Hassan Husseini
Department of chemistry, Faculty of Basic Sciences, Imam Hussein Comprehensive University, Tehran, Iran
Received: 31 January 2012 Accepted: 17June 2012
AbstractIn this research, zeolite NaY molecular sieve was prepared by a hydrothermal method. Then, silver
ions were replaced in the zeolite NaY with silver nitrate (AgNO3) solution via using ion exchange (IE) method
for the preparation of zeolite AgY. In the next step, the Manganese dioxide (MnO2) nanoparticles (9.3 and 15.8
wt %) as guest were deposited in the zeolite AgY (as host) structure with Mn(NO3)2 aqueous and KMnO4
solutions via confined space synthesis (CSS) method. Synthesized samples were studied and characterized via
SEM/EDAX, XRD and FTIR techniques. The desulfurization and removal reactions of sulfurous compounds of
chloroethyl ethyl sulfide (CEES), chloroethyl phenyl sulfide (CEPS) and organo-phosphurous compounds of
demeton and dimethyl methyl phosphonate (DMMP) have been investigated by 15.8 wt% Nano MnO2/Zeolite
AgY composite via the influences of various parameters such as solvent and time by using gas chromatography
(GC) and 31PNMR. Then, products of the elimination and destruction reactions were identificated via gas
chromatography-mass spectrometry (GC-MS). These products have less toxic to compare sulfurous and organo-
phosphurous compounds under reaction.
Keywords: Nano MnO2/Zeolite AgY, Chloroethyl ethyl sulfide, Chloroethyl phenyl sulfide, Demeton, Dimethyl methyl phosphonate, Desulfurization.
*. Corresponding author: Department of chemistry, Faculty of Basic Sciences, Imam Hussein Comprehensive University,E-mail address: [email protected]
92
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