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Nghiên cứu sự tạo phức đơn phối tử trong hệ lantan (III) - asenazo III

Page 1

phân tích - Khoa Hoá -

-

Vinh, tháng 05/2007.

1


Trang ................................................................................................ 2

............................................. 21

1.6.

.................................................................... 22 ...................................... 27

................................................................................. 7 1.1. Lantan và dãy các

.................................... 27

...................................... 7

...................................................... 27

................................................... 7 .................................................... 29

............................................... 7 .................................................................. 9

.............................................................. 29

.............................................................. 9

.......................................................................................... 29

............................................................................... 9

........................................................................ 29

........................... 10

.................................................................................... 29

.............................................. 11

3+

(10-2M) ................................................................. 29 -3

............................................... 12

M ......................................................... 30

............................................................................ 13

........................................................................... 30

.............................................. 13

................................................................ 30 ............................................................. 30

.................... 14 ....................... 15 .............................. 15

4+

-3

10 M........................................................... 30

2+

10-3M ........................................................... 31

............................................... 16

..................................................................... 31

................................................. 16

......................................................................... 31

................................................ 16 ........ 16 ....................................................... 16

3+

- asenazo III ........................................... 31 ............................................................... 31 .............................................................. 31

...................................... 17

....................... 32

..................................... 17

1.4.2

3+

..................... 32

............................................................... 18

........................................................... 32

............................. 19

..................................................................... 33

................................................................................. 19

....................................... 34

.............. 20

................................ 35

........ 20 2

3


3.1.5. Nghiê ............................................................................. 36 ....... 38 ..................................................................... 38 3.2.1. ......................................................................................... 38 3.2.2

........ 40 3+

- asenazo III ...... 41

4+

................................................................. 42

2+

................................................................ 42

.......................................................................................... 43 ............................................................................... 45 ............................................................................ 46

4

5


- asenazo III

-

- asenazo

III.

1

-

6s2. I2 11,06

1

5,577 0

òa). -

3

-

3+ La /La

)

T0nc

asenazo III. -

= -2,522V. : 6,16 : 9200C

T0s C 0p S

: 34700C : 27,6 : 57,3

Hnc Bán kính (nm)

I3 19,11

: 6,7 La3+ 0,104

La 0,187

La4+ 0,090

0

, 4f7, 4f14

6

7


pK = 10,04

0,1 (LiClO4)

pK = 7,4

Ion La3+

4000

trong không khí

3,0 (LiClO4)

2O3,

LaHal3, LaN, LaC,

LaH3 Oxyt La2O3 (t =20000 C ). La2O3 0

3 2O3

lantan N2

Hydroxyt La(OH)3

t=

1.10-19). {49} Theo dãy các

Do có: E0La3+/La = 3PO4

cacbona La3+ + HOH

La(OH)2+ + H+

La(NO3)3 .6H2O, La(NO3)3 .9H2O, LaBr3.6H2O, La2(SO4)3.8H2 3+ 0

3+

không màu.

T0C 0,3 (NaClO4)

4NO3La(NO3)3 ..4H2O

pK= 9,06

3)2.2La(NO3)3

250C pK = 8,53

0

i 0,05 (0

50% etanol)

pK = 9,06 8,70(25%); 8,17

0,1

pK = 8,14

3,0

pK = 10,04

8

(H2O);

-12. [27, 28]

9


7 trong La(dixet)2.2H2

2O4)4]

5-

, [La(NTA)2]3-

2 2(SO4) 3.9H2O.

+

R3 CH - COO-

R1- NH

[18]

CH - COOH R2 [4] - Antipirin C: C32H28N8S2 axit:

axetic,

xitric,

tactric,

etyldiamintetaaxetic

(EDTA),

dietyltriaminpentaaxetic (DTPA), nitilotriaxetic (NTA), asenazo III, amino -

-3 là 600nm.

735

chúng

=105 .

mg/l), Fe(III) (0.3 mg/l), Zr (0,75 mg/l), Cu(II) (1,5 mg/l), V(IV) (2,5 mg/l), -nbutyl-photphat (TBP) và diankylphotphoric (HDEHP).

-

- 560 nm và

3 580 = (22 - 25). 10 .

ion là: pK0 = -3,2; pK1 = 0,66 La3

xLan+3

dãy: photphat < photphonat < photphinat < photphioxyt. [21]

10

pK4 = 8,02

0,10; pK5 = 9,50

0,14; pK2 = 3,50 0,09; pK6 = 10,62

C23H15N5O12S2 -

11

0,26; pK3 = 6,52 0,32; pK7 = 13,2

0,36; 0,08.


xác

- Alizarin S: C14H5(OH)2SO3Na.H2

nóng, không tan

49 1/2

2O3,

La(NO3)2

Asenazo III : C22H18O14N4S2As2 AsO3H2

N

CeO2, Nb2O3 2(màu

vàng chanh), Eu2O3

2O3

OH

N

N

-

xyl naphtalin-3,6-

(2-

12

N

SO 3H

O3SH

dùng

AsO3H2

OH

13

-2,7-bis


-

cto n+ 3

O

2CO3

.

As

O

OH

(n-2) Me

sau: O

+

.

O

.

N

NaCl bão hòa.

O

As

N

. .

N

+

(n-3) Me O

. N .

. (II)

(I)

n+

và hai nhóm

AsO3H2; -

1=660

665nm ;

2=610nm.

nào. O-aseno-oxylazo. Nhóm này có HO

AsO3H2 .

. N

N .

.

- Zr - Hf - U(IV) - Pu4+ - Np4+ - Th m

asenazo III. c

AsO3H2 và -OH.

14

15


[6], [8],[17]

m 3

(10 )

mg/ml 700C,

(nm) Th

665

130

HCl 8N

0.01

U

670

130

HCl 4N

Ce

665

47

PH = 3

0.02

Cu

665

10

PH = 6

0.02

0.05

0.1 xilenol da cam.

A + 24 = 100G/V

= 580 nm. a -

QUANG [12]

16

17


M + qHR M + qHR + pHR '

'

MRq

+ qH+

(1)

KCb

MRqR'P

+ (q+p)H

(2)

Kcb

là các ligan. A

M

(3)

-

(1) 4,

(2)

KNO3 q

MRqR'P

t(phút)

và

MRqvà MRqR'P '

HR

max

1.4.2 A MRqR'p

MRq

-

HR

HR'

4

MR'p

max

trong h

A E C A

F (2)

D B (1)

pH

18

19

hay NH3


4

-

Xร C 4+

; V5+; Zr4+

-5

-4

-3

-

phรกp sau: -

-

(

A=f(C A (1) (2) M

CT .THรถ CM n

20

21

/ CR

R/

CM


M

R

=const; CR R/ CM.

Ai

=const; CM M/ CR.

CR=b2

CM=a2

CR=b1

CM=a1

CM CR

CR CM

)

mRn.

1.6).

M+VR

= const

CM+CR

Dãy 1: CM+CR = a1 Dãy 2: CM+CR = a2 R/CM

hay A=f(CR/(CR+ CM)) MmRn

22

23

); A=f(VR/VR)


Ai CM+ CR =a1 CM+ CR =a2

M(OH)i + qHmR Kp =

M(OH)i(Hm-nR)q +qn H Kp qn

( M (OH ) i ( H m n R) q . H M (OH ) i . H m R

q

(1)

.

M(OH)i(Hm-nR)q ] = CK; [H+] =h CR n ( ) CM m

M + H2O [M(OH) ] =K1

M(OH)

+

H

K1

M(OH)2 + H

K2

-1

M(OH) + H2O [ M(OH)2 ] = K1

-2

2

M(OH)i-1 + H2O

a hai

[M(OH)i ] = K1

2

M(OH)i i

CM = [M] + [M(OH) ] +[ M(OH)2 ]

khรกc nh

CM

[ M] = [M(OH)i]=

(1

-1

h . K 1'

-2

h . K 1 '.K 2 '

CM (1

1

h- . K 1 '

+H

[M(OH)i ] +CK CK .... h- i . K 1 '.K 2 '.....K i ' )

CK

h- 2 . K 1 '.K 2 '

.... h- i . K 1 '.K 2 '.....K i ' )

1.6.

m

Hm+1 R HmR [Hm+1 R ] = [HmR].h/ K0 -

24

+

H

Ko

HmR Hm-1 R + [Hm-1 R ] = K1. [HmR].h-1

H

K1

Hm-2 R + Hm-1R [Hm-2 R ] = K1. K2 [HmR].h-2

H

K2

25

Ki

-i

.

K 1 '.K 2 '....K i ' hi


[ M (OH)i ].( CHm R Hm-(n-1)R [Hm-n R ] =

Hm-n R + H

K1.K2

Kn

CK ( 1

[HmR].h-n

n

Q = ( K1.K2

CHR = [Hm+1 R ] + [HmR] + [Hm-1

[HmR] =

[Hm-nR ] =

(CHmR (1

h . Ko

-1

-1

h . K1

(CHm R (1

h .Ko

-1

m-nR],

m-n

n)

q

R ] +q.CK

qCK ) .... h- n . K 1 .K 2 .....K n )

qCK )(K 1 .K 2 ....K n ) -1

h . K1

.... h- n . K 1.K 2 .....K n ).hn

[ M(OH)i(Hm-nR)q ] = CK; [H+] =h

( M (OH) i (H m n R) q . H

Kp =

-1

h .Ko

M (OH) i . H mR

q

qn

.

1

=

CK .hqn.(1 h.K o h 1.K 1 .... h n .K 1.K 2 .K n )q [ M (OH)i ]( CHmR q.CK )q

M(OH)i(Hm-nR)q

M(OH)i + q Hm-nR

KH

H

q

KH

M (OH) i . H m n R ( M (OH) i (H m n R) q m-n

R ] vào (2) ta có:

[ M (OH)i ].( CHm R

KH =

CK ( 1

h

(2)

-1 .Ko

-1

h . K1

26

qCK )q (K 1.K 2 ....K n )q -n

q

.... h . K 1.K 2 .....K n ) .h

qn

=

1

27

h-1. K 1

qCK )q

.... h- n . K 1.K 2 .....K n )q


KH =

B.Q. h qn

lgB =f(pH): -lgB

K - lg B = qn. pH - lg H (3) Q. tg

M(OH)i(Hm-nR)q

1

n tg

2

pH

lgB vào pH

Hình 1.8: HR,

CK= CM.

q, Ko, K1, K2

n

Ai . A gh

-

lgB =f(pH ) có tg < 0 và không

pH

Ai

CK

(CHmR - qCK)

M

M(OH) M(OH)2

M(OH)3

i=o

i=1

i=3

i=2

lgB =f(pH ) có tg i

pH1 pH2

i

lgB= f(pH) PH

-lgBM

-lgBM(OH)

-lgBM(OH)

2

-lgBM(OH)3

Kp

KH

pH1

- lg

-

pH2

[ M (OH)i ].( CHm R

= KP

KH

(1 và Q= ( K1.K2

28

T Q.

h . Ko n)

q

-1

h-1. K 1

. 29

qCK )q

.... h- n . K 1.K 2 .....K n ) q


S2 n

nh SX

[15]

=tp;k. SX

-

-

p;k

Ai = (a

a)

+ (b

b)

Ci

X-

-

X+

a

X 2

Ci . A i Ci Ci A i 2 n. Ci ( Ci )2

a=

-

n Ci . A i Ci A i b= = 2 n. Ci ( Ci )2

a

= tp,k.Sa

b

= tp,k.Sb

a

a t p,k .Sa

b

b

b t p,k .Sb

1, n

X

-

C i 1

-

2

=

So sánh ttn

p;k

tn

(x i

X2, X3

X

i

yi n

X )2

n 1

30

=

< tp;k thì X

-

a a b

tn

31

X a SX a là d

.100

t p; k .SX X

.100


th

3) 3 .6H2 -3

M)

Trong C22H18O14N4S2As2Na2

-

. asenazo III 10-3M. -3

M)

C

-3

ác

M.

0,01mg. 3

-

ch

3

3

-

4+ 3+

-2

(10 M)

(10-3M)

Cân chính xác trên cân phân tích 0,13053 gam Th(NO3)4 4H2O theo

Cân chính xác 0,81226 gam La(NO 3)3.6H2

4+ 3+

32

33


trình Data -

3)4 4H2 3(10

-3

MS-Excel

M)

Pascal.

it HNO3 (1 : 5).

3+

3.1. NGHIÊN

Cd(NO)3 10-3.

Casenazo III = 8.10-5

-

3

h. 3+

khác nhau (l = 1.001 cm,

- asenazo III

(nm)

3+ 3

= 0.1M). A

(nm)

450

0.145

570

0.400

470

0.205

580

0.305

520

0.475

590

0.200

540

0.520

600

0.115

560

0.460

710

0.015

M

Pascal MS-Excel Matlab.

34

A

35


0.6

0.6

0.5 0.4

A

0.4 0.3 0.2

0.2

0.1 0 0

200

400

600

800

0 610

620

630

640

650

660

670

680

690

700

710(nm)

La3+ - asenazo III

max

3+

= 540 nm.

-

-3

asenazo III 10-3

3

1M,

3+ 3+

-

max

max

max 3+ 3+

khác nhau (l = 1.001 cm,

.

-

3+

-

= 0.1M).

625

630

640

645

650

655

680

700

0.026

0.076

0.221

0.299

0.380

0.429

0.128

0.041

(nm) 3+

Ai

4.10 M ; Casenazo III = 8.10 M, CNaNO3 -5

-5

Ai La3+ hình 3.3.

36

37

3+

là


3+

- asenazo III vào

t (phút) 0.55 0.5

t(phút)

5

10

15

20

30

60

90

120

150

180 0.45

Ai

0,424 0,424 0,423 0,424 0,424 0,422 0,422 0,421 0,421 0,421

0.4 0.35 0.3 0

50

100

150

200

i

ôi 3+

3+

-

-

La3+

= 4.10-5M, Casenazo III = 8.10-5M,

CNaNO3 3+

3.4 và hình 3.4. 3+

- asenazo

III vào pH pH 1,50 1,71 2,00

2,20

2,52 3,00 3,20 3,50

4,00 4,51 5,06

A 0,210 0,345 0,420 0,422 0,425 0,430 0,400 0,351 0,301 0,240 0,200

38

39


Ai 0.5

0.4 0.3

STT

VLa(III) (ml)

VasenazoIII (ml)

CasenazoIII.10-5M

Ai

0.2

1

1.0

1,00

1,60

0,170

0.1

2

1,0

2,00

3,20

0,210

0

3

1,0

3,00

4,80

0,257

4

1,0

4,00

6,40

0,320

5

1,0

5,00

8,00

0,425

6

1,0

6,00

9,60

0,425

7

1,0

7,00

11,20

0,424

8

1,0

8,00

12,80

0,425

9

1,0

10,00

16,00

0,425

10 1,0 asenazo III và o

12,00

19,20

0,425

1.5

2.03

3+

2.52

3.2

4

5.06

pH

-

10-5 -3

-3 -4

40

Ai 0.45 0.4 0.35

41


C AsenazoIII C La 3

-5

asenazo III asenazo III

C AsenazoIII C La 3

8,00.10 4,00.10

= 5,00

= 8,00.10-5

C AsenazoIII ( l =1,001 cm, C AsenazoIII C La 3

5 5

2 -4

M trong các

3

DD1

DD2

DD3

DD4

DD5

DD6

DD7

La3+.10-3 M(ml)

1,0

1,0

1,0

1,0

1,0

1,0

1,0

-3

2,0

2,0

2,0

2,0

2,0

2,0

2,0

1,25

2,5

3,75

5,0

7,5

10,0

11,25

Asenazo III. 10 M(ml)

NaNO3 1M(ml)

Ai

3+

0,423 0,424 0,425 0,424 0,425

= 0,1M, pH = 3,0,

= 655nm)

C La3+ . 10-5

CAsenazoIII.10-

9,00

0,32

2,88

0,9

0,309

2,00

8,00

0,64

2,56

0,8

0,600

3,00

7,00

0,96

2,24

0,7

0,950

3,50

6,50

1,12

2,08

0,65

1,021

4,00

6,00

1,28

1,92

0,6

0,920

5,00

5,00

1,60

1,60

0,5

0,681

6,00

4,00

1,92

1,28

0,4

0,520

7,00

3,00

2,24

0,96

0,3

0,345

8,00

2,00

2,56

0,64

0,2

0,220

9,00

1,00

2,88

0,32

0,1

0,113

V La3+ (ml)

VAsenazoIII(ml)

1,00

5

Ai

0,424 0,424

= 0,1.

42

- asenazo III vào

43

C AsenazoIII C AsenazoIII C La 3

Ai


5

4,00

8,00

2,00

0,425

6

4,00

8,60

2,15

0,425

7

4,00

10,00

2,50

0,425

8

4,00

12,00

3,00

0,425

9

4,00

14,00

3,50

0,425

10

4,00

16,00

4,00

0,425

1.2 1 0.8 0.6 0.4 0.2 0 0

0.1 0.2 0.3 0.4 0.5 0.6 0.7 0.8 0.9

1

C AsenazoIII C AsenazoIII C La 3

C AsenazoIII C AsenazoIII C La 3

La3+ : asenazo III = 1 : 2. C 3+

La 16.10-5M, CNaNO3

-5

-5

3+

- asenazo III và o

C AsenazoIII ( = 655 nm, l = 1,001 cm, = 0,1M) C La 3

STT

C La3+ . 10-5

CAsenazoIII.10-5

C AsenazoIII C La 3

1

4,00

1,60

0,40

0,105

2

4,00

3,20

0,80

0,180

3

4,00

4,80

1,20

0,258

4

4,00

6,40

1,60

0,335

44

Ai

45


Ai

4+

0.45 3+

0.4 -5

0.35

-5

4.10

4+

0.3

3

100.10-5

0.25 0.2 0.15 0.1

4+

khác nha

0.05 0.4

0.8

1.2

1.6

2

2.15

2.5

3

3.5

C AsenazoIII C La 3

4

= 655 nm).

4

4

4

4

4

4

4

CTh4+.10-5

0

10

20

40

60

80

100

0,428

0,315

0,301

0,273

0,213

0,182

0,068

CLa3+.10

0

(l = 1,001 cm,

-5

Ai

C AsenazoIII C La 3

4+

3+

:

ion Th4+ 2+

y hoàn toàn phù 3+ 3+

-

-5

-5

4.10

2+

ASENAZO III

3+

4+

âsenazo III

= 2.C La3+

(l = 1,001 cm,

= 655 nm)

CLa3+.10-5

4

4

4

4

4

4

4

CCd2+.10-5

0

10

20

40

60

80

100

0,428

0,428

0,427

0,428

0,576

0,620

0,698

Ai

46

100.10

và Cd2+. 2+

3+

3 -5

47


10

- Ion Cd2+ asenazo III.

1.056

AI 1.2 2+

CCd 2

là :

40 4

C La3 - Ion Th asenazo III.

5,0

1 0.8

10

0.6

4+

0.4 0.2 0 0

1

2

3

4

5

6

CLA3+.10-5

4,0). 10-5M. asenazo III

= 2.CLa3+. Ai = (1,9189

cm,

= 0,1, pH = 3,0,

= 655 nm).

= (1,9189

STT

CLa3+.10-5

1

0,5

0,125

2

1,0

0,210

3

1,5

0,308

4

2,0

0,390

5

2,5

0,481

6

3,0

0,550

7

3,5

0,621

8

4,0

0,702

9

4,5

0.910

48

0,2780) .104 . CLa3+ + (0,0076

0,2780) .104.

Ai

49

0,0863).


1. 2. 3. max

= 655 nm;

- Hà

4.

pH = 3,0; t = 30 phút,

= 0,1. 3+

- asenazo III là:

5.

3+

La : asenazo III = 1: 2 6. 3+

Ai = (1,9189

3+

-

:

0,2780) .104 . CLa3+ + (0,0076

0,0863).

7.

2+

La(III) là:

CCd 2 C La 3

40 4

8.

-

10 9.

(2-Pyridilazo)-Rezoxin (PAR) và HX (HX: CH3COOH, CH2ClCOOH,

Còn ion Th4+

CHCl2COOH, CCl3

La(III). 10. 11.

0

1.tr. 80-82 (1982).

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