Citation: Luo Ying, Qi Jibing, Guo Fang. Research Progress in the Regeneration Mechanism of Chelated Iron Desulfurization Solution[J]. Chemistry, ;2016, 79(7): 597-603. shu

Research Progress in the Regeneration Mechanism of Chelated Iron Desulfurization Solution

1.
Shanxi Province Key Laboratory of Higee-Oriented Chemical Engineering, North University of China, Taiyuan 030051

Received Date: 8 October 2015
Available Online: 16 February 2016
Fund Project:

The chelated iron desulfurization has realized the catalyst recycling, in which ferrous ion regeneration is the core of the whole technology. In the regeneration process, researchers found the reaction to be first order, second order in Fe²⁺, and even found a transition in reaction order from 1 to 2, due to the different reaction rate constant ratio. The ferrous ion can be oxidized by molecular oxygen (O₂) and its derivatives (such as superoxide (H_n⁺O₂^·), hydrogen peroxide (H₂O₂), hydroxyl radical (OH·)) or high valence state of iron containing oxygen intermediates (such as (L)Fe⁴⁺=O, (L^·+) Fe⁴⁺=O and (L)_nFe⁴⁺(OH)(OOH)). The oxidation mechanism of ferrous NTA appeared to be similar to that of ferrous chelates of EDTA and HEDTA. In the regeneration process, there was a suitable pH range for the ligand. When ligand NTA was excessive, its activity depends on the pH and the concentration of NTA, and the differences of the NTA concentration lead to different reaction pathways. In the oxidation reactions, the chelate degradation occurred due to the excess oxygen consumption by the ligand, which leads to the deviation of the stoichiometry.
- Chelating Ferrous,
- Hydrogen sulfide,
- Regeneration,
- Hydroxyl radical,
- Stoichiometry
1. [1]
  [1] 杜灿屏, 麻生明. 有机化学学科前沿与展望. 北京:科学出版社, 2011.
2. [2]
  [2] S Piche, F Larachi. Chem. Eng. Sci., 2006, 61:3452~3462.
3. [3]
  [3] S Piché F Larachi. Chem. Eng. Sci., 2006, 61:7171~7176.
4. [4]
  [4] H J Wubs, A A C M Beenackers. Ind. Eng. Chem. Res., 1993, 32:2580~2594.
5. [5]
  [5] 胡尧良. 石油炼制与化工, 2008, 39:14~20.
6. [6]
  [6] 王开岳. 石油与天然气化工, 1995, 24:178~184.
7. [7]
  [7] J F Demmink, I C F Van Gils, A Beenackers. Ind. Eng. Chem. Res., 1997, 36:4914~4927.
8. [8]
  [8] T Kaden, S Fallab. Advances in the Chemistry of Coordination Compounds. New York:MacMillan Co., 1961, 196:654~663.
9. [9]
  [9] Y Kurimura, R Ochiai, N Matsuura. Bull. Chem. Soc. Jpn. 1968, 41:2234~2239.
10. [10]
  [10] S O Travin, Y I Skurlatov. Russ. J. Phys. Chem., 1981, 55:815.
11. [11]
  [11] C Bull, G J McClune, J A Fee. J. Am. Chem. Soc., 1983, 105:5290~5300.
12. [12]
  [12] E Sada, H Kumazawa, H Machida. Ind. Eng. Chem. Res., 1987, 26:1468~1472.
13. [13]
  [13] E R Brown, J D Mazzarella. Electroanal. Chem., 1987, 222:173~192.
14. [14]
  [14] V Zang, R Van Eldik. Inorg. Chem., 1990, 29:1705~1711.
15. [15]
  [15] S Sabine, V E Rudi. Inorg. Chem., 1997, 36:4115~4120.
16. [16]
  [16] A P Purmal, Y I Skurlatov, S O Travin. Bull. Acad. USSR Div. Chem. Sci. (Engl. Transl.), 1980, 29:315~320.
17. [17]
  [17] X Liu, D T Sawyer, S A Bedell et al. Ligand degradation in the iron/dioxygen-induced dehydrogenation of H₂S. Seventh Sulfur Recovery Conference, Austin, TX. 1995, 24.
18. [18]
  [18] C Kang, A Sobkowiak, D T Sawyer. Inorg. Chem., 1994, 33:79~82.
19. [19]
  [19] H Sugimoto, D T Sawyer. J. Am. Chem. Soc., 1984, 106):4283~4285.
20. [20]
  [20] А А Неяглов, Н. Г Дигуров, Г. В.В. Бухаркина. Очистка широкои фракции легких угпёъоаороаов газового конаёнсата месторожаения от сернистых соединении. лр. Кцнет. Кат., 1991, 32:541~547.
21. [21]
  [21] C Walling, M Kurz, H J Schugar. Inorg. Chem., 1970, 9:931~937.
22. [22]
  [22] C Walling. Acc. Chem. Res., 1975, 8:125~131.
23. [23]
  [23] J M C Gutteridge. Free Radical Res., 1990, 9:119~125.
24. [24]
  [24] J D Rush, W H Koppenol. J. Am. Chem. Soc., 1988, 110:4957~4963.
25. [25]
  [25] W H Koppenol. Free Radical. Biol. Med., 1985, 1:281~285.
26. [26]
  [26] D T Sawyer, C Kang, A Llobet et al. J. Am. Chem. Soc., 1993, 115:5817~5818.
27. [27]
  [27] E Luzzatto, H Cohen, C Stockheim et al. Free Radical Res., 1995, 23:453~463.
28. [28]
  [28] J D Rush, W H Koppenol. J. Biol. Chem., 1986, 261:6730~6733.
29. [29]
  [29] I Yamazaki, L H Piette. J. Biol. Chem., 1990, 265:13589~13594.
30. [30]
  [30] I Yamazaki, L H Piette. J. Am. Chem. Soc., 1991, 113:7588~7593.
31. [31]
  [31] S Rahhal, H W Richter. J. Am. Chem. Soc., 1988, 110:3126~3133.
32. [32]
  [32] J T Groves. Structure, Mechanism and Biochemistry. 1985.
33. [33]
  [33] J T Groves, Y Watanabe. J. Am. Chem. Soc., 1986, 108:7834~7836.
34. [34]
  [34] H C Tung, C Kang, D T Sawyer. J. Am. Chem. Soc., 1992, 114:3445~3455.
35. [35]
  [35] H Bamnolker, H Cohen, D Meyerstein. Free Radical Res., 1991, 15:231~241.
36. [36]
  [36] H J Wubs, A A C M Beenackers. AIChE J., 1994, 40:433~444.
37. [37]
  [37] J F Demmink, A Beenackers. Ind. Eng. Chem. Res., 1997, 36:1989~2005.
38. [38]
  [38] J F Demmink, A Beenackers. Ind. Eng. Chem. Res., 1998, 37(4):1444~1453.
39. [39]
  [39] A E Martell, R J Motekaitis. Determination and use of stability constraints. VCH Publishers:New York, 1988.
40. [40]
  [40] M J Burkitt, B C Gilbert. Free Radical Res., 1991, 14:107~123.
41. [41]
  [41] N H Clark, A E Martell. Inorg. Chem., 1988, 27:1297~1298.
42. [42]
  [42] G C Blytas, Z Diaz. USP:4356155, 1982.
43. [43]
  [43] Z Diaz. USP:4515764, 1985.
44. [44]
  [44] D McManus, F R Kin. USP:4622212, 1986.
45. [45]
  [45] R J Motekaitis, A E Martell. J. Coord. Chem., 1994, 31:67~78.
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沈阳化工大学材料科学与工程学院沈阳 110142