Hoi nghi khoa hoc ki thuat md quoc le zuiu Cong nghiep mo tien tien vi su phat triin bin viing K I E M S O A T A X E N T R O N G C A C N H A M A Y C H E B I E N K H O A N G S A N V A C A C L T N G D y[.]
Trang 1Hoi nghi khoa hoc ki thuat md quoc le - zuiu Cong nghiep mo tien tien vi su phat triin bin viing
K I E M S O A T A X E N T R O N G C A C N H A M A Y C H E B I E N K H O A N G
S A N V A C A C L T N G D y N G T R O N G L A M S A C H C H A T L O N G
V A O N D I N H C H A T T H A I Young II NAM, Sang Yun SEO, Yeon Ho LEE
M y o n g Jun K I M v a Tran T a m
D a i hoc Quoc gia C h o n n a m G w a n g j u , H a n Quoc
Tom tat: Axen tqo ra trong san xudt dupe coi la mot san pham thdi, no dupe tach trong xii ly
va/hodc cdc dung dich thai trong nhieu nha may xir ly khoang Vd>c xir ly thdng thuong bao ham
viec lam ket tua (long) de hinh thanh nen phe thdi dn dinh cho viec loai bd hay tdi che che pham
Axen Bdi viet nay de cap nen tdng cua vi$c ket tua As(V) va gioi thieu mot nghien ciru cy the trong
xu ly tach trong nhd may xir ly nude thdi tai Cdng ty Kwangyang Ferro Alloy (KFA) Han Qudc
Chuong trinh khdi phuc gan day dupe thuc hi$n tqi Md Giant, Canada ciing dupe gidi thieu nham
the hien viec xir ly chat thdi Axen (AS2O3) sau khi ket thuc khai thdc
Cdc khia canh co ban lien quan den su dn dinh vd ket tua Axen, tren cdng trinh thir nghiem
tqi dqi hoc New South Wales bdi Robin dau thap ky 80 ve sau dupe md rdng trong cdc cdng tac
phat trien xir ly cao hon bdi mot nhom nghien ciru tqi Dqi hoc Qudc gia Chonnam Su phat trien
mdi lien quan den xir ly Axen dupe tqo nen tir qua trinh xir ly nude sinh hoat vd khdi chica trong
Mo vd cdc kim loai khac dupe thao ludn trong nghien ciru nay
Chuong trinh md hinh hda Stabcal (dupe phat trien bdi Montana Tech, My) dd dupe sir dung
de khdo sat mire dq dn dinh (Eh-pH, log(ndng dp) so vdi pH) cua nhieu h? thdng As(V) Mire dd
nay cd the du bao vi$c xir ly ket tua tqi nhieu dieu ki?n cua ty I? pH va Fe(III), Ca(II) hay Ba(II)
hoac Mg(II)/As(V) va du bao nong dq can bang Axen cua dung dich con lai sau ket tua
Vi(>c xu ly dupe phat trien tqi Dqi hoc (Duoc gia Chonnam da dupe ung dung tqi mot nha
may xir ly Mo tqi KFA, Kwangyang, Han Qudc Ngay khi bi tach Mg-As(V) trong cdc flowsheet
khac Tac dqng ciia diiu ki$n dung dfch san xudt (dung dich ty I? pH, Fe(III) or Mg(II)/As(V)) dd
dupe khdo sat de tdi uu hda dieu ki$n kit tua Dudi dieu kien tdi uu nay (ty 1$ pH, Fe(IJI) or
Mg(II)/As(V) >3) As(V) cd the dupe tach khdi ddng xir ly den nhd hon 2 mg/L Su ket tua ket tinh
tot va se lam dn djnh cho viec loai trie va tdi che theo yeu cau Ca(II) va Ba(II) la khong thich hpp
ket tua As(V) do cau tqo dn dinh cao ciia cdc chat kit tua CaMo0 4 va BaMo0 4 so vdi chat tuong
ung vdi Axen
Tic khoa: Axen, dn dinh, kit tua, phan img hda hoc, md hinh hda
Gidi thieu
•
A x e n la m o t chat thai t h u o n g gap v a kho x u l y , no k h o n g the b i pha h u y va no chi co
the b i can bang hoa, bat dong hoa hay each l y de loai thai t r o n g m o t bai rac hoac kho chua
Trong qua k h u , A x e n da duoc su dung trong cac thuoc t r u sau, t r u co va trong san xudt
k i n h n h u n g hien nay no hau n h u b i g i o i han dung trong h 6 n hop bao quan go D o n g - C r o m
- A x e n A x e n dung t r o n g nhirng u n g dung nay bao h a m viec k h o n g k h i can t h i l t trong viec
x u l y chat thai va loai bo, no co the duoc k i e m soat va bo sung m o t each de dang trong cac
hoat dong san xuat
Chat thai tao ra tir cac hoat dong x i r l y khoang v a k h a i k h o a n g la kho x i r l y hon, can
quy m o h o n de loai thai Su t o n tai ciia A x e n sulphua hoa t r o n g t u n h i e n hau n h u la ket hop
Trang 2r r nui ngni icnoa hoc ki thuat md quoc te - 2010 Cong nghiep md tien tien vi su phat trien ben viing
v a i Fe dugc b i l t d i n thong t h u a n g l a arsenopyrite (AsFeS) lien quan d i n khoang san than
va d i n g T r o n g k h i i t p h i b i l n h o n la cac mat hang l i e n k i t v a i c a sa v a cac k i m loai
c h u y l n t i l p n h u cobalt la cobaltite ( C o A s S ) , d i n g n h u enargite ( C u3A s S4) v a nhieu chat khac A x e n sulphide nguyen chat t o n tai n h u realgar (AS4S4 hoac PGS) v a orpiment (AS2S)
N h u n g khoang c h i t gay 6 n h i e m A x e n trong nuac n g a m t r o n g cac qua t r i n h d x y hoa
k h u t u nhien hoac neu tiep xuc v a i k h o n g k h i trong k h a i thac m o dong, than da, va cac k i m loai ca ban pho bien n h u c h i k e m , , m o l y p d e n , w , tao nen n u a c thai axit
Cac k y thuat khac nhau da dugc t h i l t lap d l loai bo A x e n ra k h o i n u a c ngam, n u a c thai va dung d i c h x u l y T i n h c h i t khoa hoc k y thuat dang sau n h u n g k y thuat nay da dugc
de cap m o t each r o n g rai t r o n g nhieu cong t r i n h nghien c u u (Jekel and Seith, 2002; M o h a n and Pitman, 2007; C h o o n g v a n.n.k., 2007; Sharma v a Sohn, 2009) n h u dugc t h i hien trong bang 1
Bang 1 Cdc ky thuat dupe sir dung de tach As(V) vaAs(III) tic cdc dung dich
Dong dac va keo tu McNeil and Edwards, 1995; Gregor, 2001
Han va n.n.k.; 2002 Adsorption on solid substrates Asta va n.n.k., 2009; Genc-Fuhrman va n.n.k., 2004; Dien d$ng Martinez-Villafane va n.n.k., 2009
Mang loc, K h u muoi tham thau ngugc,
IQC na no
Sato va n.n.k., 2002; Shih, 2005;
Geucke va n.n.k., 2009; Qu va n.n.k., 2009
Su k i t tua ciia Fe(III)-Axenat hoac
Fe(HI)-P04-Axen (As(V)
Sato, 2002; Shih, 2005; Geucke va n.n.k., 2009;
Qu va n.n.k., 2009; Nishimura va Robins, 1996;
Fujita va n.n.k., 2008; Meng va n.n.k., 2000 Lenoble va n.n.k., 2005
S\r k i t tua cua Fe(III)- axenit (As(III) Nishimura and Robins, 2008; Jain va n.n.k., 2009
Sy k i t tua cua Ca(II)-As(V) Brown and Bothe, 1999;
Raposo va n.n.k., 2004
Su ket tua cua Ca(II)-As(III) Itakura va n.n.k., 2007
Cac nhan xet quan trong
Mohan va Pittman, 2007 Choong va n.n.k., 2007; Wang va Mulligan, 2009; Sharma va Sohn, 2009
D o i v d i x u l y hoac d u n g d i c h thai cd chua i o n A x e n cao (hang t r a m p h i n trieu) v a cac anion n h u sunfat v a clorua, viec su dung hap phu, trao d d i i o n hoac cac k y thuat m a n g
de loai b d A x e n la k h o n g h i e u qua n h u cac i o n nay k i t hop v d i Axenat, c u t h i la A s 0 4 3 -(day g o i la A s ( V ) ) hoac arsenit, A s 0 3 3 - ( h o a c A s ( I I I ) ) anion t r o n g qua t r i n h phan ly K i t hia la lua chon tot nhat ve mat nay v a su x i i l y da dugc su dung r d n g r a i trong thuc t l thuong m a i
N i s h i m u r a v a Robins (1996) lan dau tien de xuat viec su dung cua Fe ( I I I ) de ket h i a
As ( I V ) tir dung d i c h A x e n a t sat dugc c o i la d n d i n h nhat de x u l y ( M e n g v a n.n.k., 2000; Katsoyiannis va Z o u b o u l i s , 2002; Lenoble v a n.n.k., 2005; F u j i t a v a n.n.k., 2008) T r o n g nha may thuc te, m o t l i e u l u g n g cua Fe ( I I I ) clorua hoac sunfat a p H <8,5 se loai b d A x e n ( V ) trong cac h i n h thiic ciia m o t dang bun, m a sau dd dugc lgc v a x i i l y ( H a n va n.n.k., 2002; Choong v a n.n.k., 2007) Cac hop c h i t h y d r o x y l tua s i t cung hoat ddng n h u c h i t hut
Trang 3Hdi nghi khoa hoc kT thuat md quoc re - zuiu Cong nghiep md tien tiin vi sir phat triin bin viing
bam t i t d l san xuat o n d i n h n h i t Fe ( I I I ) , loai A s ( V ) (Katsoyiannis v a Z o u b o u l i s , 2002; Lenoble v a n.n.k., 2005)
Arsenit sat ( A s ( I I I ) ) sunfat hydrat ( 6 F e 2 0 3 5 A s 2 0 3 2 S 0 3 1 2 H 2 0 ) la I n d i n h trong khoang p H 2,0-3,5, v u g t ra ngoai no t r o nen k h o n g o n d i n h ( N i s h i m u r a v a Robins, 2008)
M o t c h i t o x y hoa n h u c l o , clorua sat hoac ferrate ( F e 0 4 2 - ) t h u o n g duoc t h e m vao de o x i hoa A s ( I I I ) hoac he t h i n g A s ( I I I ) / ( V ) h 6 n hop d l duy t r i t i t ca A x e n n h u A s ( V ) truoc
k h i ket hia
Trong thuc t l clorua s i t duoc t i m t h i y d l tao nen m o t viec loai bo h i e u qua h o n so
v o i sulfat s i t ( K a r t i n e n v a M a r t i n , 1995; Z o u b o u l i s v a Katsoziannis, 2002) Cac m u o i clorua cua Fe ( V I ) / A l ( I I I ) la h i e u qua h o n n h o m k h o n g Fe ( V I ) hoac Fe ( V I ) / Fe ( I I I ) trong k i t hia o x y hoa A s ( I I I ) d l tap trung i t h o n gia t r i W H O k h u y e n cao 10 m g / L (Jain
So va n.n.k., 2009)
Viec sir dung h y d r o x i t canxi hay v o i cung da duoc phat h u y r o n g rai de loai bo A x e n tir nudc/nuoc thai ( C h o o n g v a nnk, 2007) la co m o t so loai Ca ( I I ) - A s ( V ) co the duoc ket hia tren dai r o n g cac p H ( B r o w n v a Bothe, 1999; Raposo v a n n k , 2004) 6* nhiet do cao tren 1 0 0 ° C , A s ( I I I ) tang cao d i n 1 g / L cung co t h i duoc tach co h i e u qua v o i thanh phan
bo sung Ca (OH)2 N g o a i ra do su h i n h thanh ciia m o t so chat o n d i n h Ca ( I I ) - A s ( I I I )
c h i n g han n h u C a5( A s 03)3( O H ) 4 H20 v a C a5( A s 03)3O H (Itakura v a nnk, 2007) trong mot
x u l y t u o n g t u n h u khoang hoa t h u y nhiet Cac i o n k i m l o a i k i e m trai dat t u o n g t u n h u
C a2 + n h u B a2 + v a M g2 + cung h i n h thanh cac hop c h i t I n d i n h v o i A s ( V ) (Raposo va nnk, 2004; Z h u v a nnk, 2005) Swartzbaugh va Sturgill (1998) d l x u i t viec sir dung Ca M g va
m u o i Fe de loai bo A s ( V ) tir cac chat thai ban dan co chua A s , Ga v a cac i o n k i m loai khac
r r r
Su ket tua ciia M g ( I I ) - A s ( V ) duoc san xuat x i r l y chat thai co chua d u l u o n g T u y theo su
b i l n d l i giua 16-18 m g / L A s (pH8.4-8,8), tai m o t t y le M g / A s la 1.5:1 d i n 05:01 D o do, viec lira chon m o t c h i t thir cho ket h i a A x e n p h u thuoc vao trang thai o x i hoa ciing n h u cac loai i o n khac t r o n g dung d i c h
B a i bao nay c h i ra m o t so van de quan t a m den nganh c o n g nghiep k h a i thac m o va khoang san tren khap the g i o i lien quan den su hoat dong ciia chat o n d i n h A x e n va chat co
d i n h hoa de x i r l y Cac v i d u thuc te cua cac hoat dong k h a i thac m a n g den, bao g o m viec xir l y duoc phat t r i e n b o i n h o m nghien c u u ciia chiing t o i de loai bo A x e n tir m o t dung dich dugc x i r l y m o l y p d e n V i e c sir dung phan m l m Stabcal ( H u a n g 2 0 0 8 ) dugc phat t r i i n b d i Montana Tech t r o n g m o h i n h hoa loai A x e n cung dua ra de c h u n g m i n h viec sir dung no trong viec d u doan cac d i e u k i e n can bang cho m o t so he t h o n g thuc te
Su* d u n g m u o i M g ( I I ) de l o a i b d A s ( V ) c h i n g h a n n h u M g } ( A s 0 4 )2 t i r d u n g d i c h
t h a i - M o
Viec sir d u n g M g C l 2 d l loai bo A s ( V ) ( m i i c do d a m dac 0,5-1 g / L ) tir m o t dung
dich-M o la dich-M g 3 ( A s 0 4 ) 2 da dugc c h i i n g m i n h b o i cac nha n g h i e n c u u tai D a i hoc Q u l c gia Chonnam va ap d u n g t a i K w a n g y a n g H g p k i m Sat ( K F A ) T h o n g t i n c h i t i l t cua xir l y dugc phat t r i e n dugc bao cao t r o n g m o t i n p h a m doc lap T r o n g t h o i gian t h i e u ciia mot nguyen lieu M o 03 de san xuat M0S2 de l a m hop k i m s i t - m o l y , N h u k h o i h i n h thanh, hoa tan vao nuoc t r o n g m o t d o n v i tay v a can phai dugc x i i l y N u o c thai A s ( V ) ciing dugc
h i n h thanh do su rira cua C u O tir M o 03 dugc san xuat tir cac 16 t h i e u sir dung acid sulfuric ( A n va nnk, 2009 (a) v a (b))
Trang 4nui nvrii Krioa hoc ki thuat md qudc te - 2010 Cdng nghiep md tien tien vi sic phat trien ben viing
N h u the hien t r o n g cac H i n h 1(a) va 1(b), sir ket hia ciia M g ( I I ) - A s ( V ) la p h u thuoc
vao dung d i c h p H 0 dieu k i e n nghien cuu, Mg3(AsC>4)2 co the d u g c k i t tua trong khoang
p H 6 0 - l l , v o i hliu h i t A s ( V ) d l loai bo i t h o n 0,8 p p m tai pH9.0-9,5 Cac c h i t d i n g k i t
tua cua M g ( O H )2 ciing d u g c d u doan la tang p H tren p H 9 5 , n h u t h i h i e n trong H i n h 1(a)
C» tren p H 1 0 8 , k h o n g co k i t hia cua M g ( I I ) - A s ( V ) d u k i l n n h u t h i h i e n trong ca hai so
do cac H i n h 1 (a) v a (b)
1 2 4 6 S 10 12 H
pH
PH
Hinh 1 Nong dp so vdi pH cua (a) Mg(II va (b) As(V) nhu dd du bao trong mo hinh kit tua sic
dung Stabcal Cdc dieu kUfn kit tua: 469 mg/L (hope 0.0063 MAs(V)), 0.0188 MMg(H)
vd 0.74 MMofVD tai 25 °C
5»| 1 500* ,
6 7 8 9 10 11 12
As(T)
Hinh 2 (a) Hinh thdi cua As(V) dupe xac dinh bdi cdc xet nghiem ngung tu tqipH khac
nhau, cho chat long tong hpp cua As(V) va As(III) (nhu cdc diim die lieu md) vd cho chat long
Mo thuc (diim die li$u dupe dien) dtyl$ moi Mg/As khac nhau
(b) So sanh cdc hinh thai AS so vdipH dupe do va du bao tie Stabcal, cho thay co chi
hap phu cho viing pH thap (do H3M0O4 kit tua) vd khu pH cao (do Mn(OH) 2 kit tua)
Cac chat ding kit tua ciia hydroxit Mg (II) nhu thi giai thich thuc tl la hon As (V)
co t h i dugc ra ra tir d u n g dich, hoac bang each h i p p h u hoac d i n g k i t tua, h o n nua, no d u
bao tir m o h i n h h i n h thanh Stabcal D i r lieu t h u dugc tir t h i n g h i e m k i t tua tai cac d i l u k i e n
tuong t u , sir dung A s ( V ) t i n g hgp hoac dung dich thai M o co chua 0 0 0 6 3 M A s ( V ) d u g c
Trang 5Hoi nghi khoa hoc ki thuat mo quui, < e - u Cong nghiep md tien tien vi su phat triin bin viing
t h i hien trong h i n h 2, cho thay A s ( V ) dugc lay ra nhieu h o n tir ca hai loai c h i t long hon nhung d u bao t u m o h i n h Stabcal trong khoang p H cao ( p H > 9) D o i v o i cac loai chat long tong hgp, khoang p H thap cho thay su giong nhau cua ca hai h i n h thai n o n g do, tuc la M o t trong n h u n g d u doan tir Stabcal va no xac d i n h bang t h u n g h i e m T u y nhien d o i v o i chat long that, viec loai bo cac A s ( V ) tai m o t p H <7 co the la do hap p h u cua A s ( V ) vao ket tua H2M0O4 d u k i e n cho khoang p H thap
Su tach A s ( I I I ) tir d u n g dich b d i M g ( I I ) la k h o n g h i e u qua n h u tren hinh.2 Tai pH>8.5, A s ( I I I ) co the d u g c tach k h o i dung d i c h b d i m o t chat hap p h u hoac co che dong
k i t hia ( b d i n g u n g t u M g ( O H )2)
Viec lira chon M g ( I I ) de ket tua A s ( V ) n h u ma gie axenat, Mg3(AsC>4)2 co dugc sau
k h i x e m xet cac he t h o n g khac, dugc biet den de tao nen cac chat ket tua o n d i n h h o n do do hoa tan thap h o n san p h a m A x e n a t nay Co FeAsC»4, C a 3 ( A s 0 4 )2 va B a 3 ( A s 0 4 )2 v d i gia tri
Ks p la 5 7 x l 0 -2 1' 6 8 x l 0- 1 9, 1.0xlO"2 3 5 3t u o n g ung, so v d i 2.1 x 1 0- 2 0 cho M g3( A s 04)2
So s a n h cac he t h o n g F e ( I I I ) - A s ( V ) , C a ( I I ) - A s ( V ) , B a ( I I ) - A s ( V ) v a M g ( I I ) - A s ( V )
a
I
'•Vl
-V \
g
a
Al (T, HA«04
\
-A
10 12 II
10 13 14
pH
Hinh 4 Cdc sff do on dinh cho cdc h$ thong khac nhau: Fe(IH)-As(V), Ca(II)-As(III)
va Ba(II)-As(V)
Tuy nhien, trong su h i e n dien cua i o n M0O42
", c h i l m u u t h i trong d i l u k i e n x i i ly ( p H > 4) Ca ( I I ) v a B a ( I I ) se h i n h thanh C a M o 04 k h o n g hoa tan v a t h i m o l i p d a t B a M o 04
tren m o t dai p H r o n g , n h u t h i hien tren H i n h 4 D i l u nay se p h u nhan viec sir dung cac ion
d l loai bo A s ( V ) tir cac l o a i c h i t long x i r l y M o D 6 i v d i Fe no cung la cung dugc b i l t d i n
v d i viec loai bo cua A s ( V ) b d i Fe ( I I I ) la chu y l u la do h i p thu, va su h i n h thanh cua
Trang 6r r noi ngni Knoa hoc kT thuat md quoc te - 2010 Cong nghiep mo tien tiin vi su phat trien ben vung
scorodite o n d i n h h o n d l xu* l y c h i co the dugc thuc h i e n d nhiet do cao h o n ( F u j i t a va nnk, 2008) Cac chat Fe I n d i n h ( I I I ) dugc m o h i n h hoa v a dugc the h i e n tren hinh.4 la Fe203
D i l u k i e n : 0 0 0 6 M A s ( V ) - 0 0 1 8 M F e ( I I I ) hoac C a ( I I ) hoac B a ( I I ) - 0 7 4 M M o ( V I ) Xu* l y A x e n t a i M d G i a n t , C a n a d a - M o t c h u o n g t r i n h k h d i p h u c c h a t t h a i r a n ( h t t p : / / e n w i k i p e d i a o r g / w i k i / G i a n t M i n e )
M d Giant la m o t m d vang l d n nam gan Y e l l o w k n i f e , Northwest Territories, Canada, b i t dau san x u i t vao nam 1948 v a ngirng hoat ddng vao nam 2004 N d dugc san x u i t tren 7.000.000 oz (220.000 k g ) vang tren 4 thap k y hoat ddng T u y nhien hoat ddng khai thac tao ra mot trach nhiem to I o n v l m d i trudng, nd cd t h i van d nhiem A s la l d n n h i t tren t h i gidi, m a cac chu sd h u u m d trudc day d l lai cho chinh q u y l n Canada va Tay B i c d l giai q u y l t Cac m d
k h l n g Id da phai x u l y 237.000t ciia tridxit A x e n ( A s203) b u i sinh ra do nung arsenopyrite B u i nay tan trong nude v a chua khoang 6 0 % A x e n 950ha cdng t r u d n g bao g d m 8 m d Id thien, 4 hao khai thac quang dudi, 325.000m3 d i t b i d nhiem va khoang 100 toa nha bao g d m ca t l hop nha nung/ddng gdi b i d nhiem r i t cao do b i nhiem A x e n va sgi amiang M o t d u an k h d i phuc
$400,000,000 dugc tai t r g cua chinh p h i i dang dugc t i l n hanh d l giai q u y l t van d l nay (http://www.ainc-inac.gc.ca/ai/scr/nt/cnt/gm/ab/abp/index-eng.asp)
Cac tridxit Axen, m a trudc do da dugc ddng cung trong h i m m d d u d i long d i t va dudi ldp bang vinh cuu t u nhien Tuy nhien do hoat ddng khai thac lien tuc, cac ldp bang vihh cuu b i t dau tan Nude m d chua A s ro r i ra khdi l u u t r u dudi long d i t , d nhiem nude n g i m ciia k h u vuc
Trong D e an khac phuc hau qua
ft
Thermosyphons
t",
(hinh 3, sao chep tir trang web d tren), 15
ham m d va g i l n g diing dang dugc ddng
ciing b d i mot he t h i n g nhan tao, sir dung
CO2 n h u la c h i t l a m lanh D u n g dich
C 02 dugc dua xudng thdng qua m o t ong
de lam lanh viing d u d i ngam va cac k h i
nong sau dd tang len den b l mat thdng
qua xi-phdng nhiet hoat ddng, dugc cd
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