Citation: ZHANG Long-li, WANG Chun-lan, ZHAO Yuan-sheng, YANG Guo-hua, SU Mei, YANG Chao-he. Speciation and quantification of sulfur compounds in petroleum asphaltenes by derivative XANES spectra[J]. Journal of Fuel Chemistry and Technology, ;2013, 41(11): 1328-1335. shu

Speciation and quantification of sulfur compounds in petroleum asphaltenes by derivative XANES spectra

1.
1. State Key Laboratory of Heavy Oil, China University of Petroleum(East china), Qingdao 266580, China;

Corresponding author: ZHANG Long-li,
Received Date: 16 June 2013
Available Online: 9 August 2013
Fund Project: 国家自然科学基金(20776160) (20776160)中国石油大学(华东)"青年教师拔尖人才建设工程"。 (华东)

The XANES spectrum is employed to study the sulfur functional groups in asphaltenes. Since the asphaltenes are complicated mixture, it is difficult to distinguish different classes of sulfur compounds in asphaltenes. Therefore, the higher order derivative spectra of sulfur XANES were introduced in order to improve sulfur XANES resolution and to qualitatively analysis sulfur functional groups in asphaltenes. Sulfur XANES spectra were deconvoluted by using of several Gaussian and arctangent functions to quantify the sulfur species. In order to convert peak area percentages to atomic percentages, the relative 1s→3p transition probabilities of different sulfur classes must be considered. The areas of the different Gaussian peaks were calculated and revised for their oxidation state-dependent absorption cross-section. The contribution of sulfur species to total sulfur was calculated by the corrected peak areas. The result showed that sulfur species in asphaltenes of atmospheric and vacuum residue were mainly in form of thiophene, sulfoxide, thiophene sulfone and sulfate, while hardly contained sulfide.
- asphaltenes,
- sulfur,
- XANES,
- higher order derivative
1. [1]
  [1] 梁文杰, 阙国和, 刘晨光, 杨秋水. 石油化学[M]. 东营: 石油大学出版社, 2008. (LIANG Wen-jie, QUE Guo-he, LIU Chen-guang, YANG Qiu-shui. Petroleum chemistry[M]. Dongying: University of Petroleum Press, 2008.)
2. [2]
  [2] 王宗贤, 阙国和, 梁文杰. 选择性氧化结合红外光谱定量分析减压渣油中的硫醚硫[J]. 石油大学学报: 自然科学版, 1996, 20(4): 83-86. (WANG Zong-xian, QUE Guo-he, LIANG Wen-jie. FTIR-oxidation for quantification of sulfidic sulfur in vacuum residue[J]. Journal of the University of Petroleum, China, 1996, 20(4): 83-86.)
3. [3]
  [3] 王宗贤, 李希方, 阙国和, 梁文杰. 燃料化学学报, 胜利和孤岛减压渣油中的硫醚硫和噻吩硫的测定[J]. 燃料化学学报, 1995, 23(4): 423-428. (WANG Zong-xian, LI Xi-fang, QUE Guo-he, LIANG Wen-jie. Determination of sulfidic and thiophenic sulfur in shengli and gudao vacuum residues[J]. Journal of Fuel Chemistry and Technology, 1995, 23(4): 423-428.)
4. [4]
  [4] 鄢小琳, 史权, 徐春明, 赵锁奇, 柯明. 裂解色谱法研究渣油中硫化物的结构及组成特征[J]. 色谱, 2004, 22(2): 162-165. (YAN Xiao-lin, SHI Quan, XU Chun-ming, ZHAO Suo-qi, KE Ming. Analysis of composition and structure of sulfur compounds inresidual oils by pyrolysis-gas chromatography[J]. Chinese Journal of Chromatography, 2004, 22(2): 162-165.)
5. [5]
  [5] 赵锁奇. 渣油中硫化物类型分布与化学转化性能[J]. 石油学报(石油加工), 2002, 18(1): 18-23. (ZHAO Suo-qi. Distribution of sulfur types in petroleum residue and their chemical conversion[J]. Acta Petrolei Sinica(Petroleum Processing Section), 2002, 18(1): 18-23.)
6. [6]
  [6] GEORGE G N, GORBATY M L J. Sulfur K-edge x-ray absorption spectroscopy of petroleum asphaltenes and model compounds[J]. J Am Chem Soc, 1989, 111(9): 3182-3186.
7. [7]
  [7] WALDO G S, MULLINS O C, PENNER-HAHN J E, CRAMER S P. Determination of the chemical environment of sulphur in petroleum asphaltenes by X-ray absorption spectroscopy[J]. Fuel, 1992, 71(1): 53-57.
8. [8]
  [8] MULLINS O C. Asphaltenes: Fundamentals and applications[M]. New York: Plenum Press, 2005: 53-56.
9. [9]
  [9] VAIRAVAMURTHY M A, MALETIC D, WANG S, MANOWITZ B, EGLINTON T, LYONS T. Characterization of sulfur-containing functional groups in sedimentary humic substances by X-ray absorption near-edge structure spectroscopy[J]. Energy Fuels, 1997, 11(3): 546-553.
10. [10]
  [10] RAVEL B, NEWVILLE M. ATHENA, ARTEMIS, HEPHAESTUS: Data analysis for X-ray absorption spectroscopy using IFEFFIT[J]. J Synchrotron Radiat, 2005, 12(4): 537-541.
11. [11]
  [11] 张龙力, 王春岚, 赵元生, 杨国华, 杨朝合. 塔河常压渣油沥青质含硫官能团形态与其性质的关系研究[J]. 燃料化学学报, 2012, 40(9): 1081-1086. (ZHANG Long-li, WANG Chun-lan, ZHAO Yuan-sheng, YANG Guo-hua, YANG Chao-he. Study on the relationship between sulfur functionalities and the characteristics of THAR asphaltene[J]. Journal of Fuel Chemistry and Technology, 2012, 40(9): 1081-1086.)
12. [12]
  [12] WALDO G S, CARLSON R M K, MOLDOWAN J M, PETERS K E, PENNER-HAHN J E. Sulfur speciation in heavy petroleums: Information from X-ray absorption near-edge structure[J]. Geochim Cosmochim Acta, 1991, 55(3): 801-814.
13. [13]
  [13] XIA K, WEESNER F, BLEAM W, HELMKE P, BLOOM P, SKYLLBERG U. XANES studies of oxidation states of sulfur in aquatic and soil humic substances[J]. Soil Sci Soc Am J, 1998, 62(5): 1240-1246.
14. [14]
  [14] HUFFMAN G, MITRA S, HUGGINS F, SHAH N, VAIDYA S, LU F. Quantitative analysis of all major forms of sulfur in coal by X-ray absorption fine structure spectroscopy[J]. Energy Fuels, 1991, 5(4): 574-581.
15. [15]
  [15] PRIETZEL J, BOTZAKI A, TYUFEKCHIEVA N, BRETTHOLLE M, THIEME J, KLYSUBUN W. Sulfur speciation in soil by S K-edge XANES spectroscopy: Comparison of spectral deconvolution and linear combination fitting[J]. Environ Sci Technol, 2011, 45(7): 2878-2886.
16. [16]
  [16] 苏红军, 杜培军, 盛业华. 高光谱遥感数据光谱特征提取算法与分类研究[J]. 计算机应用研究, 2008, 25(2): 390-394. (SU Hong-jun, DU Pei-jun, SHENG Ye-hua. Study on feature extraction and experiment of hyperspectral data[J]. Application Research of Computers, 2008, 25(2): 390-394.)
17. [17]
  [17] TALSKY G. Derivative spectrophotometry of first and higher orders[M]. New York: VCH Publishers, 1994.
18. [18]
  [18] VAIRAVAMURTHY A. Using X-ray absorption to probe sulfur oxidation states in complex molecules[J]. Spectrochimica Acta A, 1998, 54(12): 2009-2017.
19. [19]
  [19] RESSLER T, WONG J, ROOS J, SMITH I L. Quantitative speciation of Mn-bearing particulates emitted from autos burning (methylcyclopentadienyl) manganese tricarbonyl-added gasolines using XANES spectroscopy[J]. Environ Sci Technol, 2000, 34(6): 950-958.)
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