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.)
1. [1]
  Chongjing Liu , Yujian Xia , Pengjun Zhang , Shiqiang Wei , Dengfeng Cao , Beibei Sheng , Yongheng Chu , Shuangming Chen , Li Song , Xiaosong Liu . Understanding Solid-Gas and Solid-Liquid Interfaces through Near Ambient Pressure X-Ray Photoelectron Spectroscopy. Acta Physico-Chimica Sinica, 2025, 41(2): 2309036-0. doi: 10.3866/PKU.WHXB202309036
2. [2]
  Zian Lin , Yingxue Jin . Matrix-Assisted Laser Desorption/Ionization Mass Spectrometry (MALDI-MS) for Disease Marker Screening and Identification: A Comprehensive Experiment Teaching Reform in Instrumental Analysis. University Chemistry, 2024, 39(11): 327-334. doi: 10.12461/PKU.DXHX202403066
3. [3]
  Tao Wang , Qin Dong , Cunpu Li , Zidong Wei . Sulfur Cathode Electrocatalysis in Lithium-Sulfur Batteries: A Comprehensive Understanding. Acta Physico-Chimica Sinica, 2024, 40(2): 2303061-0. doi: 10.3866/PKU.WHXB202303061
4. [4]
  Weihan Zhang , Menglu Wang , Ankang Jia , Wei Deng , Shuxing Bai . Surface Sulfur Species Influence Hydrogenation Performance of Palladium-Sulfur Nanosheets. Acta Physico-Chimica Sinica, 2024, 40(11): 2309043-0. doi: 10.3866/PKU.WHXB202309043
5. [5]
  Ke Qiu , Fengmei Wang , Mochou Liao , Kerun Zhu , Jiawei Chen , Wei Zhang , Yongyao Xia , Xiaoli Dong , Fei Wang . A Fumed SiO₂-based Composite Hydrogel Polymer Electrolyte for Near-Neutral Zinc-Air Batteries. Acta Physico-Chimica Sinica, 2024, 40(3): 2304036-0. doi: 10.3866/PKU.WHXB202304036
6. [6]
  Hongyao Li , Youyan Liu , Luwei Dai , Min Yang , Qihui Wang . The Blessing of Indium Sulfide：Confronting the Narrow Path with Uric Acid. University Chemistry, 2024, 39(5): 325-335. doi: 10.3866/PKU.DXHX202311104
7. [7]
  Hao Wu , Zhen Liu , Dachang Bai . ¹H NMR Spectrum of Amide Compounds. University Chemistry, 2024, 39(3): 231-238. doi: 10.3866/PKU.DXHX202309020
8. [8]
  Hongwei Ma , Hui Li . Three Methods for Structure Determination from Powder Diffraction Data. University Chemistry, 2024, 39(3): 94-102. doi: 10.3866/PKU.DXHX202310035
9. [9]
  Yuqiao Zhou , Weidi Cao , Shunxi Dong , Lili Lin , Xiaohua Liu . Study on the Teaching Reformation of Practical X-ray Crystallography. University Chemistry, 2024, 39(3): 23-28. doi: 10.3866/PKU.DXHX202303003
10. [10]
  Ruiqing LIU , Wenxiu LIU , Kun XIE , Yiran LIU , Hui CHENG , Xiaoyu WANG , Chenxu TIAN , Xiujing LIN , Xiaomiao FENG . Three-dimensional porous titanium nitride as a highly efficient sulfur host. Chinese Journal of Inorganic Chemistry, 2024, 40(5): 867-876. doi: 10.11862/CJIC.20230441
11. [11]
  Jinyao Du , Xingchao Zang , Ningning Xu , Yongjun Liu , Weisi Guo . Electrochemical Thiocyanation of 4-Bromoethylbenzene. University Chemistry, 2024, 39(6): 312-317. doi: 10.3866/PKU.DXHX202310039
12. [12]
  Nan Xiao , Fang Sun . 二芳基硫醚化合物的构建及应用. University Chemistry, 2025, 40(6): 360-363. doi: 10.12461/PKU.DXHX202407099
13. [13]
  Haitao Wang , Lianglang Yu , Jizhou Jiang , Arramel , Jing Zou . S-Doping of the N-Sites of g-C₃N₄ to Enhance Photocatalytic H₂ Evolution Activity. Acta Physico-Chimica Sinica, 2024, 40(5): 2305047-0. doi: 10.3866/PKU.WHXB202305047
14. [14]
  Yue-Zhou Zhu , Kun Wang , Shi-Sheng Zheng , Hong-Jia Wang , Jin-Chao Dong , Jian-Feng Li . Application and Development of Electrochemical Spectroscopy Methods. Acta Physico-Chimica Sinica, 2024, 40(3): 2304040-0. doi: 10.3866/PKU.WHXB202304040
15. [15]
  Weikang Wang , Yadong Wu , Jianjun Zhang , Kai Meng , Jinhe Li , Lele Wang , Qinqin Liu . Green H₂O₂ synthesis via melamine-foam supported S-scheme Cd_0.5Zn_0.5In₂S₄/S-doped carbon nitride heterojunction: synergistic interfacial charge transfer and local photothermal effect. Acta Physico-Chimica Sinica, 2025, 41(8): 100093-0. doi: 10.1016/j.actphy.2025.100093
16. [16]
  Yiming Liang , Ziyan Pan , Kin Shing Chan . One Drink, Two Tears in the Central Nervous System: The Perils of Disulfiram-Like Reactions. University Chemistry, 2025, 40(4): 322-325. doi: 10.12461/PKU.DXHX202406016
17. [17]
  Yingtong Shi , Guotong Xu , Guizeng Liang , Di Lan , Siyuan Zhang , Yanru Wang , Daohao Li , Guanglei Wu . PEG-VN改性PP隔膜用于高稳定性高效率锂硫电池. Acta Physico-Chimica Sinica, 2025, 41(7): 100082-0. doi: 10.1016/j.actphy.2025.100082
18. [18]
  Xue Xiao , Jiachun Li , Xiangtong Meng , Jieshan Qiu . Sulfur-Doped Carbon-Coated Fe_0.95S_1.05 Nanospheres as Anodes for High-Performance Sodium Storage. Acta Physico-Chimica Sinica, 2024, 40(6): 2307006-0. doi: 10.3866/PKU.WHXB202307006
19. [19]
  Yan'e LIU , Shengli JIA , Yifan JIANG , Qinghua ZHAO , Yi LI , Xinshu CHANG . MoO₃/cellulose derived carbon aerogel: Fabrication and performance as cathode for lithium-sulfur battery. Chinese Journal of Inorganic Chemistry, 2025, 41(8): 1565-1573. doi: 10.11862/CJIC.20250054
20. [20]
  Hong CAI , Jiewen WU , Jingyun LI , Lixian CHEN , Siqi XIAO , Dan LI . Synthesis of a zinc-cobalt bimetallic adenine metal-organic framework for the recognition of sulfur-containing amino acids. Chinese Journal of Inorganic Chemistry, 2025, 41(1): 114-122. doi: 10.11862/CJIC.20240382

Get Citation

PDF

XML

Metrics

PDF Downloads(0)
Abstract views(389)
HTML views(10)

通讯作者: 陈斌, bchen63@163.com

1.
沈阳化工大学材料科学与工程学院沈阳 110142