Citation: ZHAO Peng, LI Jun-fang, WU Yan, MAO Xue-feng, ZHANG Xiao-jing, CHANG Qiu-lian. Reaction and hydrogen transfer in complex multi-phase system during coal hydro-liquefaction[J]. Journal of Fuel Chemistry and Technology, ;2018, 46(12): 1423-1429. shu

Reaction and hydrogen transfer in complex multi-phase system during coal hydro-liquefaction

ZHAO Peng ^1,2,, ,
LI Jun-fang ^1,2 ,
WU Yan ^1,2 ,
MAO Xue-feng ^1,2 ,
ZHANG Xiao-jing ^1,2 ,
CHANG Qiu-lian ^1,2

1.
Coal Chemistry Branch of China Coal Research Institute, Beijing 100013, China
2.
State Key Laboratory of Coal Mining and Clean Utilization, China Coal Research Institute, Beijing 100013, China

Corresponding author: ZHAO Peng, 411296849@qq.com
Received Date: 12 June 2018
Revised Date: 10 August 2018

Fund Project: NSFC-Joint Funds for Coal Base Low Carbon of Shanxi Province of China U1610221the National Key R & D Program of China 2016YFB0600303The project was supported by the National Key R & D Program of China (2016YFB0600303) and NSFC-Joint Funds for Coal Base Low Carbon of Shanxi Province of China(U1610221)

Figures(7)

Reaction behavior of Naomaohu (NMH) coal in tetralin was carried out under atmosphere of H₂. Hydrogen transfer in complex multi-phase system of direct coal liquefaction were discussed. The influence of phase transition process of iron-based catalyst on liquefaction performance was investigated using X-ray diffraction, saturate magnetization and scanning electron microscope. The results show that NMH coal presents good liquefaction performance at 420℃ and 17 MPa. Active phase Fe₇S₈ plays catalytic role during initial reaction and changes into nonactive phase-Fe₉S₁₀ and FeS later. High hydrogenation activity of catalyst and long residence time are beneficial to hydrogenation of preasphaltene and asphaltene into light oil. Catalyst promotes the activation of H₂ transferring to coal pyrolysis products and solvent. Catalyst promotes the hydrogen in solvent to transfer to coal pyrolysis products as well. The contribution to activated hydrogen from solvent is twice as that from H₂ in the condition of the experiment. Hydrogen transferring from H₂ to solvent changes little with temperature, pressure and time. Activated hydrogen from H₂ and solvent is proportional to the conversion of coal and asphaltene to oil and gas.
- low rank coal,
- hydroliquefaction,
- hydrogen transfer process,
- catalysis activity
1. [1]
  LIU Zhen-yu. Principal chemistry and chemical engineering challenges in direct coal liquefaction technology[J]. Chem Ind Eng Prog, 2010,29(2):193-195.
2. [2]
  ZIELKE C W, STRUCK R T, EVANS J M, COSTANZA C P, GORIN E. Molten zinc halide catalysts for hydrocracking of coal extract and coal[J]. Ind Eng Chem Process Des Dev, 1966,5(2):158-164. doi: 10.1021/i260018a009
3. [3]
  CURRAN G P, STRUCK R T, GORIN E. Mechanism of hydrogen-transfer process to coal and coal extract[J]. Ind Eng Chem Process Des Dev, 1967,6(2):166-173. doi: 10.1021/i260022a003
4. [4]
  IKENAGA N, KAN-NAN S, SAKODA T, SUZUKI T. Coal hydroliquefaction using highly dispersed catalyst precursors[J]. Catal Today, 1997,39(1/2):99-109.
5. [5]
  GODO M, SAITO M, ISHIHAVE A. Elucidation of coal liquefaction mechanisms using a tritiated molecular hydrogen in the presence and absence of H₂S[J]. Fuel, 1998,77(9/10):947-952.
6. [6]
  MCMILLEN D F, MALHOTRA R, HUM G P, CHANG S J. Hydrogen-transfer-promoted bond scission initiated by coal fragments[J]. Energy Fuels, 1987,1(2):193-198.
7. [7]
  MCMILLEN D F, MALHOTRA R, CHANG S J, OGIER W C, NIGENDA S E. Mechanisms of hydrogen transfer and bond scission of strongly bonded coal structures in donor-solvent systems[J]. Fuel, 1987,66(12):1611-1620. doi: 10.1016/0016-2361(87)90351-6
8. [8]
  MALHOTRA R, MCMILLEN D F, TSE D S, LORENTS D C, RUOFF R S. Hydrogen-transfer reactions catalyzed by fullerenes[J]. Energy Fuels, 1993,7(5):685-686. doi: 10.1021/ef00041a020
9. [9]
  VERNON L W. Free radical chemistry of coal liquefaction:Role of molecular hydrogen[J]. Fuel, 1980,59(2):102-106. doi: 10.1016/0016-2361(80)90049-6
10. [10]
  ZONG Z M, WEI X Y. Effects of molecular hydrogen and hydrogen donor additives on 1, 2-di (1-naphthyl) ethane thermolysis[J]. Fuel Process Technol, 1994,41(1):79-85. doi: 10.1016/0378-3820(94)90061-2
11. [11]
  KUHLMANN E J, JUNG D Y, GUPTILL R P, DYKE C A, ZANG H K. Coal liquefaction using a hydrogenated creosote oil solvent:H-atom transfer from hydrogen donor components in the solvent[J]. Fuel, 1985,64(11):1552-1557. doi: 10.1016/0016-2361(85)90372-2
12. [12]
  DEPEYRE D, URHAN M, FLICOTEAUX C. Pyrolysis of hydrocarbon mixtures characteristic of coal:Application to dibenzyl mixture[J]. Fuel, 1985,64(12):1655-1661. doi: 10.1016/0016-2361(85)90389-8
13. [13]
  CRONAUER D C, SHAH Y T, RUBERTO R G. Mechanism and kinetics of selected hydrogen transfer reactions typical of coal Liquefaction[J]. Ind Eng Chem Process Des Dev, 1978,17281. doi: 10.1021/i260067a013
14. [14]
  LI X, HU S X, JIN L, HU H Q. Role of iron-based catalyst and hydrogen transfer in direct coal liquefaction[J]. Energy Fuels, 2008,22(2):1126-1129. doi: 10.1021/ef7006062
15. [15]
  WANG Jian-you. Characteristics of catalytic-hydrogenation in direct Shenhua coal liquefaction[D]. Dalian: Dalian University of Technology, 2013: 81-85.
16. [16]
  SHU Ge-ping. Direct Coal Liquefaction[M]. Beijing:Coal Industry Press, 2003:91-95.
17. [17]
  SHI Shi-dong. Engineering Fundamentals of Direct Coal Liquefaction[M]. Beijing:Chemical Industry Press, 2012:224-231.
18. [18]
  KOTANIGAWA T, YOKOYAMA S, YAMAMOTO M, MAEKAWA Y. Catalytic activities of sulphate and sulphide in sulphur-promoted iron oxide catalyst for coal liquefaction[J]. Fuel, 1989,68:618-621. doi: 10.1016/0016-2361(89)90161-0
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