TP CH HA HC T.

50(2) 205-210 THNG 4 NM 2012

NGHIN CU KH NNG S DNG CHT LNG ION TCH

LU HUNH TRONG DU DIESEL
Bi Th L Thy
Trng i hc M a cht, ng Ngc, T Lim, H Ni
n Ta son 29-11-2011

Abstract
The desulfurization potential of free halogen ionic liquid n-butyl pyridine acetate ([BPy][Ac]) was investiated with
Vietnam diesel oil. The results suggested that this ionic liquid might be used as a promising solvent for the extractive
desulfurization of fuel. Phase separation process after extracting is easy because ionic liquid has high density and is not
dissolved in oil. The content of sulfur in desel oil decreases from 498 ppm to 18 ppm after 5 repeatedly extraction
processes (30oC, volume ratio of ionic liquid to oil is 1:1). Extraction yields decrease with decreasing the volume ratio
of ionic liquid to oil. The extraction ability depends on structure of ionic liquid and of sulfur compounds. Ionic liquid
can be reused after regenerating.
Keywords: Ionic liquids, desulfurization, extraction, diesel oil.

1. M U Cht lng ion l mt nhm cht mi nhng

Theo tiu chun Chu u th t nm 2010 gn
nh phi loi b hon ton cc hp cht lu hunh ra
khi nhin liu (< 10 ppm), do hiu qu ca cc
qu trnh tch loi lu hunh l rt quan trng [1, 2].
Cc qu trnh x l vi hidro ang s dng trong
cng nghip lm gim hm lng lu hunh mt
cch hiu qu; Tuy nhin li khng p ng c nhu
cu tch loi su lu hunh v benzothiophen,
dibenzothiophen v cc dn xut ca chng bn vng
vi qu trnh hidro ha nn cn nhiu nng lng v
hidro hn. Ngoi ra, trnh cc phn ng ph lm
gim cht lng nhin liu, cht xc tc phi hot ng
hn, chn lc hn, nn ko theo mt s vn nh gi
u t cao v chi ph vn hnh cao [3].
Do , vic tm ra cc phng php mi loi
b ti a lu hunh v khc phc c cc nhc
im trn ang thu ht rt nhiu s quan tm trn
th gii.
Trn th gii, trong nhng nm gn y, mt s
qu trnh loi lu hunh khng s dng hydro ang
c nghin cu. Qu trnh loi lu hunh s dng
xc tc sinh hc chuyn lu hunh thnh cc hp
cht sunfat c bo co [4]. Phc cht cha
nickel v platin c s dng c hiu qu
ankyl sunfua ha dibenzothiophen [5]. Qu trnh
oxi sunfua ha dng hidropeoxit v axit formic
c nghin cu bi Zhao v cng s [6]. Qu
trnh chit dibenzothiophen vi cht lng ion v oxi
ha benzothiophen thnh sulfon trong pha lng
c bo co [7].
chng ha hn nhiu ng dng nh lm dung mi,
xc tc, ng xc tc cho nhiu phn ng v qu
trnh khc nhau. c tnh u vit ca chng l: tnh
a dng (s kt hp cc anion v cc cation khc
nhau c th to ra mt s lng ln cc cht lng
ion vi cc tnh cht khc nhau), nhit nng chy
thp, p sut hi bo ha rt thp, n nh nhit v
in, phn cc, dn in v dn nhit, c th iu
chnh c cc tnh cht, v d: hot tnh ha hc,
tnh axit, c bit l tnh tan, nht, kh nng cng
kt, phn cc (cn thit cho qu trnh chit) bng
cch thay i cu trc ca cc cation v anion cu
to nn chng.
Cht lng ion c kh nng sonvat ha cao v p
sut hi bo ha thp nn rt thch hp dng lm
dung mi chit. Qu trnh chit da trn c s l cc
hp cht lu hunh d tan trong cht lng ion hn
trong cc hydrocacbon. Mt s nghin cu cho thy
c th s dng chng lm dung mi chit [8-10]
hoc dng phi hp vi tc nhn oxi ha [11-13].
Chit loi b lu hunh bng cht lng ion c
Andreas Jess v cng s c bit quan tm [14-18].
Andreas Jess cho rng vic chit vi cht lng ion l
s la chn tt nht cho giai on tch lu hunh
cui cng sau khi thc hin hydrodesulfua ha
vi xc tc. Qu trnh tch lu hunh bng cht lng
ion c nhiu u im: thc hin iu kin thng;
cht lng ion d tch pha, khng bay hi, c th ti
s dng, c bit c th iu chnh kh nng chit
lu hunh bng cch thay i cu trc cation v
anion ca chng.

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TCHH, T. 50(2), 2012 Bi Th L Thy

Vi mc ch s dng cc dung mi khng c nh lng bng phng php ASTM D 545308

halogen, trong nghin cu ny, cht lng ion n-butyl [19].
pyridin axetat ([BPy][Ac]) c tng hp v s Qu trnh chit c th lp li nhiu ln loi
dng lm dung mi chit lu hunh trong du diesel trit lu hunh.
thng phm. T l dung mi v kh nng ti s Hm lng lu hunh trong nguyn liu v
dng cht lng ion cng c nghin cu. trong sn phm phn ng c xc nh trn my
phn tch lu hunh. Hiu sut chit cc hp cht
2. THC NGHM cha lu hunh trong diesel c xc nh nh sau:

Du diesel thng phm c mua t ca hng S S0

X = 100
bn l Vit Nam. S
Pyridin 99,5%, amoni axetat 99%, xyclohexan Trong :
99,5%; etyl axetat 99,5% and metanol 99,5% c X: hiu sut chit lu hunh %.
mua t nh my ha cht Guangdong Guanghua, S: hm lng lu hunh tng ban u (ppm theo
Trung Quc. N-butyl bromua 98% c mua t khi lng).
cng ty ha cht Merck Schuchardt OHG (c). Tt S0: hm lng lu hunh cui (ppm theo khi
c u c s dng khng qua tinh ch thm. lng).
Du diesel trong nghin cu ny c hm lng
2.1. Tng hp cht lng ion (IL) n-butyl pyridin lu hunh l 498 ppm theo khi lng (ppm kl).
axetat [BPy][Ac]
2.3. Ti s dng cht lng ion
Quy trnh tng hp IL [BPy][Ac] gm 2 giai
on: Cho cht lng ion sau khi s dng chit vo
Tng hp cht lng ion n-butyl pyridin bromua bnh cu cha etyl axetat, t l th tch gia cht lng
([BPy][Br]) (phn ng 1) ion v etyl axetat l 1:1. Sau khuy hn hp
Nh t t n-butyl bromua vo bnh cu 500 ml nhit phng trong 2 gi. lng hn hp sau khi
cha pyridin. Sau khuy v gia nhit 70oC khuy, tch lp etyl axetat trn ra. Cht lng ion
trong 48 gi. Hn hp sau phn ng c khuy ra thu c em gia nhit 80oC trong 10 gi loi
3 ln vi etyl axetat loi b cc cht cha phn b dung mi d. Lp li qu trnh 5 ln v s dng
ng sau cho vo bnh khuy, gia nhit trong chn li cht lng ion chit lu hunh trong du. Dung
khng 80oC trong 10 gi loi etyl axetat. Cht mi etyl axetat sau khi chit c th thu hi bng
rn thu c c mu trng c, nng chy nhit cch chng ct n gin (Ts ca etyl axetat l 77oC).
75oC Hp cht lu hunh thu hi c c th l nguyn
Tng hp cht lng ion N-butyl pyridin axetat liu cho cc qu trnh khc.
([BPy][Ac]) (phn ng 2)
Cho lng mol bng nhau ca n-butyl pyridin 3. KT QU V THO LUN
bromua [BPy][Br] v amoni axetat vo bnh cu 500
ml trong c sn 250 ml metanol. Sau gia 3.1. nh hng ca nng cht lng ion
nhit hn hp nhit phng trong 48 gi. [BPy][Ac] n kh nng chit lu hunh
Hn hp phn ng thu c cha kt ta dng
keo mu nu , c lc bng giy lc, thu c Nng cht lng ion [BPy][Ac] trong hn hp
cht lng ion [BPy][Ac] mu c nht tng chit c nh hng quyt nh n hiu sut tch lu
i ln. Sau lm bay hi chn khng loi b hunh ra khi du. Do hng s phn b ca mi hp
dung mi tha. cht cha lu hunh gia mt cht lng ion nht nh
v du l c nh. Nu dng t cht lng ion th hiu
sut chit thp; do , loi b ti a lu hunh cn
+ thc hin qu trnh chit lp li nhiu ln gy tn km
+
Br N
N
Br- (1) thi gian, phc tp ha qu trnh. Nu dng nhiu
cht lng ion th vic thu hi cht lng ion li phc
2.2. Chit loi lu hunh bng cht lng ion tp v tn km. V vy, cn phi nghin cu mc
nh hng ca lng cht lng ion dng chit n
Cho du diesel v cht lng ion vo bnh cu, hiu sut chit. Cc th nghim c thc hin cng
khuy trong 50 pht nhit phng. Sau khi iu kin vi t l th tch ca cht lng ion v du
ngng khuy chuyn hn hp sang ng nghim mu thay i. Kt qu ch ra bng 1.
quay li tm hoc chuyn sang phu chit nh v Kt qu bng 1 cho thy, cht lng ion
lng trong 30 pht, tch ly lp du pha trn. [BPy][Ac] c kh nng chit cc hp cht S trong
Hm lng lu hunh trong du sau khi chit c du, hm lng S trong du gim t 498 ppm xung

206
TCHH, T. 50(2), 2012 Nghin cu kh nng s dng
cn 234 ppm (H = 43%) sau mt ln chit. Khi dng 3.2. Hiu sut chit lu hunh qua cc ln chit
cht lng ion th khng cn dng H2 nn c th thc lp li
hin p sut thp, nhit thng. Khi gim 2
hoc 3 ln th tch cht lng ion dng chit th Kt qu loi lu hunh trong du diesel thng
hiu sut gim t 43% xung cn 28% v 23% phm bng [BPy][Ac] c thc hin qua 6 giai
tng ng. S gim ny c th khc phc khi thc on c th hin qua bng 3 v hnh 1. C th
hin vi quy m ln gim chi ph. Khi , qu thy rng nng lu hunh ca du mu gim t
trnh chit cn lp li nhiu ln hn hoc l chit lin 498 ppm n 18 ppm sau 6 ln chit lp li. Hiu
tc. Mt s nghin cu trc [20] v chit lu hunh sut chit t 96,4%. T c th thy rng t
trong du s dng mt s cht lng ion gc c hm lng lu hunh thp hn na cn thc
tetrafloborat cng cho kt qu ha hn tng t, hin thm mt s ln chit ty theo yu cu.
ngha l hiu sut chit tng i cao (bng 2).
Bng 3: Qu trnh chit lp li lu hunh trong du
Bng 1: nh hng ca t l du/IL n kh nng diesel (30oC, t l th tch cht lng ion/du = 1:1)
chit S ca IL [BPy][Ac] (30oC, 50 pht, chit 1 ln) Hm lng lu Hiu sut chit
S ln chit hunh cn li t c sau cc
Hm lng lu Hiu sut chit (ppm kl) ln chit (% kl)
T l ca
hunh sau khi lu hunh
du/IL (V) 1 283 43,2
chit (ppm kl) (H, % kl) 2 160 68
1:1 283 43 3 91 81,7
2:1 358 28 4 51 89,8
5 29 94,2
3:1 383 23 6 18 96,4

Bng 2: Kh nng chit lu hunh ca mt s cht Kt qu nghin cu cho thy cht lng ion l
lng ion trong du Dongying (25oC, 20 pht, hm dung mi tim nng tch loi hiu qu lu hunh
lng lu hunh trong du ban u l 711 ppm kl) trong du. Kh nng chit lu hunh ca cht lng
ion c gii thch do hai loi tng tc chnh gia
T l du / IL Hiu sut cht lng ion v cc hp cht lu hunh:
Cht lng ion Tng tc dng lin kt hidro xy ra gia
(khi lng) chit (% kl)
nguyn t hydro ca hp cht cha lu hunh vi
[OMIM]/BF4 1:1 29,96
cc d nguyn t ca cht lng ion. Dng tng tc
[OMIM]/BF4 5:1 10,13 ny lin quan n vic tch cc hp cht mch h
[OPy]/ BF4 1:1 16,17 cha lu hunh.
[OPy]/ BF4 5:1 8,16
Hm lng S lu hunh sau khi chit, ppm kl)

Vic chit mt ln nh th nghim trn (hm 500 100

lng lu hunh trong du t 283 ppm) (bng 1)

hm luong luu huynh ocn lai

400 80
cha t yu cu qui nh v hm lng lu hunh
Hiu sut chit, % kl

nh tiu chun quc t. Theo l thuyt ca qu trnh

Hieu suat chiet

300 60
chit th mc tch cng cao nu thc hin chit Ham luong S con lai
Hieu suat chiet
lp li cng nhiu ln. Vic chia nh mt lng
200 40
dung mi chit nhiu ln cho hiu sut tch cao
hn vic chit 1 ln vi chnh lng dung mi .
100 20
Do chng ti tin hnh chit lp li mt mu
du vi cht lng ion [BPy][Ac] vi iu kin:
0 0
0 1 2 3 4 5 6
vi = V / i Sso
ln
lanchit
chiet
Trong :
Hnh 1: Qu trnh chit lp li lu hunh trong du
V = th tch ca cht lng ion
diesel (30oC, t l th tch cht lng ion/du = 1:1)
i: s ln chit
vi: th tch cht lng ion mi ln chit Hiu ng vng thm l tng tc - trong
(v1 = v2 = v3 = = vi nhng hp cht c cu trc vng thm ging nhau.
v vi = V. Tc l tng tc - gia vng thm ca cht lng
ion v vng thm ca hp cht cha lu hunh.

207
TCHH, T. 50(2), 2012 Bi Th L Thy
Tng tc ny ph hp tch cc hp cht vng Trong nghin cu ny, cht lng ion sau khi
thm cha lu hunh nh: thiophen, benzothiophen, dng chit cc hp cht lu hunh trong du
dibenzothiophen v cc dn xut [21]. c ti sinh bng dung mi thch hp. Sau khi ti
Do , h s phn b ca cc hp cht lu hunh sinh cht lng ion li c dng chit S trong du
trong cht lng ion ph thuc vo bn cht ha hc diesel.
ca cht lng ion v hp cht lu hunh. Thng
thng, h s phn b ca cc hp cht thm cha 3.3 S ti sinh cht lng ion [BPy]Ac
lu hunh cao hn ca cc hp cht bo (bng 4)
[17]. V th khi chit lu hunh trong du mu (pha Kt qu tch loi lu hunh bng cht lng ion
thiophen, benzothiophen, dibenzothiophen vi nng sau khi ti sinh c th hin trong bng 5.
cho trc vo hydrocacbon nh n-octan), hiu sut
chit thng cao hn chit vi xng v diesel thc. Bng 5: Hiu sut chit S trong diesel ca IL trc
Qu trnh chit vi cht lng ion s hiu qu hn nu v sau khi ti sinh (30oC, t l th tch cht lng
thc hin sau bc hidrodesunfua ha. Cc hp cht ion/du = 1:1, chit 5 ln lin tc)
bo cha lu hunh d dng b loi trong qu trnh
hydrodesunfua ha. Cc hp cht thm nh: Hiu sut chit S (% kl)
T l th tch
thiophen, benzothiophen, dibenzothiophen v cc dn du mu/IL Cht lng ion Cht lng ion
xut ca chng kh tch cn li s c tch bng sch ti sinh
cch chit vi cht lng ion. 1 94,2 88,8

Bng 4: H s phn b ca mt s hp cht cha lu 2 92,6 87

hunh trong [BMIM]/OcSO4 [17] (a du mu, hp
cht lu hunh ha tan trong i-octan/1-octen, t l So vi hiu sut chit ca cht lng ion sch th
khi lng cht lng ion/du = 1:1, 15 pht; b du hiu sut chit ca cht lng ion sau khi ti sinh thp
mu, hp cht lu hunh ha tan trong n-dodecan, t hn mt cht. Kt qu tng t cng t c khi
l khi lng cht lng ion/du = 1:1, 15 pht) thay i t l th tch ca du/cht lng ion. Vi cc
qu trnh lin tc ngi ta c th tnh ton ti sinh
H s phn b (KN,
cht lng ion mt cch hp l tit kim chi ph.
Hp cht lu hunh (mg S. kg-1 IL/mg S. kg-1
Trong cng nghip qu trnh chit gin on lp
du)
li nh trong nghin cu ny c th thay bng mt
Dodecanethiola 0,1
qu trnh lin tc s dng phng php chit nhiu
Tetrahydrothiophena 0,4
bc ngc chiu [20]. C th tin hnh trong cc
Thiophena 0,7
thit b khuy mc ni tip nhau hoc trong mt thp
BTb 1,6
(thp a, thp m, thp a hnh vnh khn c cnh
DBTb 1,9
khuy, v.v..). Du diesel (F) i vo u ny, cht
4-MDBTb 1,3
lng ion (G) i vo u kia ca h thng c m
4,6-DMDBTb 0,9
phng trn hnh 2.
Pha du ang chit (R) v cht lng ion ha tan
Kh nng ti sinh v ti s dng ca xc tc
lu hunh (E) i ngc chiu v tip xc trc tip
cng nh dung mi trong cc qu trnh ha hc l
vi nhau. Nh vy khi cht lng ion ha tan t lu
mt tnh cht quan trng ch ng sau hot tnh.
hunh nht li tip xc vi du c nng lu
Tnh cht ny quyt nh xc tc hay dung mi
hunh b nht nn c kh nng tch c trit
c c dng trong cng nghip hay khng. Xc tc
lu hunh trong du. Ngc li, khi cho cht lng
hay dung mi c kh nng ti sinh v ti s dng s
ion c nng lu hunh m c tip xc vi du
tit kim chi ph tng hp chng. Ngoi ra, vic
c hm lng lu hunh cao th cht lng ion thu
ti sinh xc tc v dung mi cn trnh c vic thi
c c nng cng cao. Qu trnh ny c th tit
ra mi trng mt lng ln cht thi lm nh
kim dung mi, thi gian v chi ph.
hng n mi trng.

Hnh 2: S nguyn tc chit nhiu bc ngc chiu [20]

208
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Hydrocarbons, Spark Ignition Engine Fuel, Diesel 18. Phm Vn Ton. Cc qu trnh thit b trong cng
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Lin h: Bi Th L Thy
Trng i hc M-a cht H Ni
ng Ngc, T Lim, H ni
Email: thuykhai2001@yahoo.com.

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