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Frontiers of Earth Science

ISSN 2095-0195

ISSN 2095-0209(Online)

CN 11-5982/P

Postal Subscription Code 80-963

2018 Impact Factor: 1.205

Front. Earth Sci.    2021, Vol. 15 Issue (2) : 272-282    https://doi.org/10.1007/s11707-021-0925-6
RESEARCH ARTICLE
Biogenic gas generation effects on anthracite molecular structure and pore structure
Aikuan WANG1,2(), Pei SHAO3, Qinghui WANG1,2
1. Key Laboratory of Coalbed Methane Resources & Reservoir Formation Process (Ministry of Education), China University of Mining & Technology, Xuzhou 221008, China
2. School of Resources and Geosciences, China University of Mining & Technology, Xuzhou 221116, China
3. Department of Surveying and Planning, Shangqiu Normal University, Shangqiu 476000, China
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Abstract

This study carries out a simulated experiment of biogenic gas generation and studies the effects of gas generation on the pore structure and molecular structure of anthracite by mercury intrusion porosimetry, X-ray diffraction (XRD) and Fourier transform infrared spectroscopy (FT-IR). The results show that methanogenic bacteria can produce biogenic gas from anthracite. CO2 and CH4 are the main components of the generated biogas. After generation, some micropores (<10 nm) and transitional pores (10–100 nm) in the coal samples transform into large pores. In the high-pressure stage (pressure>100 MPa) of the mercury intrusion test, the specific surface area decreases by 19.79% compared with that of raw coal, and the pore volume increases by 7.25% in total. Microbial action on the molecular structure causes changes in the pore reconstruction. The FT-IR data show that the side chains and hydroxyl groups of the coal molecular structure in coal are easily metabolized by methanogenic bacteria and partially oxidized to form carboxylic acids. In addition, based on the XRD data, the aromatic lamellar structure in the coal is changed by microorganisms; it decreases in lateral size (La) and stacking thickness (Lc). This study enriches the theory of biogenic coalbed gas generation and provides a pathway for enhancing the permeability of high-rank coal reservoirs.

Keywords biogenic gas      anthracite      pore structure      molecular structure     
Corresponding Author(s): Aikuan WANG   
Online First Date: 15 October 2021    Issue Date: 26 October 2021
 Cite this article:   
Aikuan WANG,Pei SHAO,Qinghui WANG. Biogenic gas generation effects on anthracite molecular structure and pore structure[J]. Front. Earth Sci., 2021, 15(2): 272-282.
 URL:  
https://academic.hep.com.cn/fesci/EN/10.1007/s11707-021-0925-6
https://academic.hep.com.cn/fesci/EN/Y2021/V15/I2/272
Coal samples Ro,max/
%
Proximate analyses/% Elemental analyses/% Maceral composition/%
Mad Ad Vdaf FCd Odaf Cdaf Hdaf Ndaf St,d Vitrinite Inertinite
SH1 2.44 1.16 12.95 9.84 78.48 3.58 91.27 3.44 1.35 0.31 74.2 20.2
SH2 2.87 2.10 8.66 7.16 84.80 2.01 93.33 2.95 1.10 0.55 79.2 18.3
Tab.1  Test data of basic properties of coal samples
Fig.1  Schematic diagram of the simulation experiment device.
Fig.2  The overall experimental procedure of the study.
Samples 20 d 40 d 60 d 80 d
Gas production/mL CO2
content/%
CH4 content/% Gas production/mL CO2
content/%
CH4 content/% Gas production/mL Gas production/mL CO2
content/%
CH4 content/%
SH1-BK 22.8 62.61 37.29 11.2 14.98 85.02 0 0 0.00 0.00
SH1-1 63.4 55.20 44.80 27.5 32.19 67.81 13.2 7.3 3.56 96.44
SH1-2 66 84.28 15.72 23.5 27.46 72.54 18.6 12.5 4.22 95.78
SH2-BK 20.6 51.83 48.07 13.5 15.87 84.13 0 0 0.00 0.00
SH2-1 79.8 68.39 31.61 29.1 22.82 77.18 15.4 13.7 4.02 95.98
SH2-2 71 47.91 52.09 24.6 21.80 78.20 16.7 10.4 3.98 96.02
Tab.2  Production and contents of biogas during different stages
Fig.3  The changes in the simulated gas production and gas composition during the experiment. (a) Change in the production of biogas of the anthracite samples; (b) change in gas compositions of all groups.
Fig.4  Mercury intrusion and extrusion curves of the samples.
Fig.5  XRD patterns of coal samples. (a) Raw coal samples; (b) after biogenic gas generation.
Fig.6  Infrared spectrogram of coal samples
Samples Total pore volume /(cm3·g1) Pore volume distribution/% Total specific surface area/ (m2·g1) Specific surface area distribution/%
Macropores Mesopores Transitional pores Micropores Macropores Mesopores Transitional pores Micropores
SH1-BK 0.031 6.45 3.23 25.81 64.52 20.071 0.00 0.10 8.48 91.41
SH1-1 0.032 15.63 3.13 21.88 59.38 17.562 0.03 0.10 7.25 92.63
SH1-2 0.031 19.35 6.45 22.58 51.61 15.178 0.03 0.19 9.61 90.16
SH2-BK 0.031 3.23 3.23 25.81 67.74 22.063 0.00 0.12 9.57 90.30
SH2-1 0.034 14.71 5.88 23.53 55.88 17.552 0.01 0.19 9.72 90.09
SH2-2 0.036 25.00 2.78 19.44 50.00 17.244 0.01 0.17 9.21 90.62
Tab.3  The pore volume and specific surface area distributions of each pore segment of the samples
Fig.7  Relation diagrams of stage mercury intrusion (a) and stage pore area (b) with pore diameters of raw and experimental coal samples after biodegradation.
Coal
samples
(002) Plane diffraction peak (100) Plane diffraction peak Coal structure parameters
2θ/(° ) θ/rad β002/rad 2θ/(° ) θ/rad β100/rad d002 Lc/Å La/Å Lc/d002
SH1-BK 25.46 0.22 0.08 42.22 0.37 0.14 3.5 19.52 22.27 5.58
SH1-1 25.44 0.22 0.08 44.15 0.39 0.14 3.5 19.25 21.82 5.5
SH1-2 25.67 0.22 0.08 44.04 0.38 0.14 3.47 19.11 21.63 5.51
SH2-BK 25.19 0.22 0.08 43.82 0.38 0.13 3.53 19.61 23.01 5.55
SH2-1 25.74 0.22 0.08 43.84 0.38 0.14 3.46 18.92 21.82 5.47
SH2-2 25.81 0.23 0.08 43.84 0.38 0.14 3.45 18.54 22.15 5.38
Tab.4  Peak fitting results of XRD peak parameters of coal samples
Parameters Meaning Numerical Representation Samples
SH1-BK SH1-1 SH1-2
I1 Branched chain of fat A(2940–2900 cm−1)/A(3000–2940 cm−1) 3.70 1.97 1.97
I2 Hydrogen-enriched degree A(3000–2800 cm−1)/A(1800–1500 cm−1) 0.91 0.16 0.05
I3 aromatization A(3100–3000 cm−1)/A(3000–2800 cm−1) 1.92 1.03 1.44
I4 Hydroxyl expansion vibration A(3600–3000 cm−1) 1.97 0.89 1.14
I5 Carboxyl expansion vibration A(1500–1350 cm−1) 0.32 1.01 0.55
Tab.5  FI-IR parameters and their meanings of coal structure
Fig.8  Schematic diagram of the effect of biogenic coalbed gas generation on anthracite pore structure and molecular structure.
1 S Beckmann, M Krüger, B Engelen, A A Gorbushina, H Cypionka (2011). Role of Bacteria, Archaea and Fungi involved in methane release in abandoned coalmines. Geomicrobiol J, 28(4): 347–358
https://doi.org/10.1080/01490451.2010.503258
2 A Chakhmakhchev (2007). Worldwide coalbed methane overview, In: SPE hydrocarbon Economics and Evaluation Symposium, SPE. Soc Petrol Eng, 17–23
3 S Chen, D Tang, S Tao, H Xu, S Li, J Zhao, Y Cui, Z Li (2018a). Characteristics of in-situ stress distribution and its significance on the coalbed methane (CBM) development in Fanzhuang-Zhengzhuang Block, Southern Qinshui Basin, China. J Petrol Sci Eng, 161: 108–120
https://doi.org/10.1016/j.petrol.2017.11.042
4 Y L Chen, Y Qin, C T Wei, L L Huang, Q M Shi, C F Wu, X Y Zhang (2018b). Porosity changes in progressively pulverized anthracite subsamples: implications for the study of closed pore distribution in coals. Fuel, 225: 612–622
https://doi.org/10.1016/j.fuel.2018.03.164
5 D Ritter, D Vinson E Barnhart, D Akob, M Fields, F Cunningham, W Orem, J McIntosh (2015). Enhanced microbial coalbed methane generation: a review of research, commercial activity, and remaining challenges. Int J Coal Geol, 146: 28–41
https://doi.org/10.1016/j.coal.2015.04.013
6 M Faiz, L Stalker, N Sherwood, A Saghafi, M Wold, S Barclay, J Choudhury, W Barker, I Wang (2003). Bio-enhancement of coal bed methane resources in the southern Sydney Basin. APPEA J, 43(1): 595–610
https://doi.org/10.1071/AJ02033
7 X H Fu, X D Zhang, C T Wei (2021). Review of research on testing, simulation and prediction of coal bed methane content. J China U Min Techn, 50(1): 13–31 (in Chinese)
8 H Fu, D Yan, S Yang, X Wang, Z Zhang, M Sun (2020). Characteristics of in situ stress and its influence on coalbed methane development: a case study in the eastern part of the southern Junggar Basin, NW China. Energy Sci Eng, 8(2): 515–529
https://doi.org/10.1002/ese3.533
9 L Gao, S C Brassell, M Mastalerz, A Schimmelmann (2013). Microbial degradation of sedimentary organic matter associated with shale gas and coalbed methane in eastern Illinois Basin (Indiana), USA. Int J Coal Geol, 107: 152–164
https://doi.org/10.1016/j.coal.2012.09.002
10 M S Green, K C Flanegan, P C Gilcrease (2008). Characterization of a methanogenic consortium enriched from a coalbed methane well in the Powder River Basin, USA. Int J Coal Geol, 76(1–2): 34–45
https://doi.org/10.1016/j.coal.2008.05.001
11 Y T Guo, M R Bustin (1998). Micro-FTIR spectroscopy of liptinite macerals in coal. Int J Coal Geol, 36(3–4): 259–275
https://doi.org/10.1016/S0166-5162(97)00044-X
12 R Haider, M A Ghauri, J R SanFilipo, E J Jones, W H Orem, C A Tatu, K Akhtar, N Akhtar (2013). Fungal degradation of coal as a pretreatment for methane production. Fuel, 104: 717–725
https://doi.org/10.1016/j.fuel.2012.05.015
13 J V Ibarra, R Moliner, A J Bonet (1994). FT-IR investigation on char formation during the early stages of coal pyrolysis. Fuel, 73(6): 918–924
https://doi.org/10.1016/0016-2361(94)90287-9
14 E J P Jones, M A Voytek, M D Corum, W H Orem (2010). Stimulation of methane generation from nonproductive coal by addition of nutrients or a microbial consortium. Appl Environ Microbiol, 76(21): 7013–7022
https://doi.org/10.1128/AEM.00728-10 pmid: 20817801
15 Y H Li, G Q Lu, V Rudolph (1999). Compressibility and fractal dimension of fine coal particles in relation to pore structure characterisation using mercury porosimetry. Part Part Syst Charact, 16(1): 25–31
https://doi.org/10.1002/(SICI)1521-4117(199905)16:1<25::AID-PPSC25>3.0.CO;2-T
16 A H Liu, X H Fu, B Luo, P Luo, C Jiao (2013). Comprehensive analysis of CBM recovery inLhigh rank coal reservoir of Jincheng area. Int J Min Sci Technol, 23(3): 447–452
https://doi.org/10.1016/j.ijmst.2013.05.009
17 Y Liu, Y Zhu, S Liu, S Chen, W Li, Y Wang (2018). Molecular structure controls on micropore evolution in coal vitrinite during coalification. Int J Coal Geol, 199: 19–30
https://doi.org/10.1016/j.coal.2018.09.012
18 S Miyazaki (2005). Coalbed methane growing rapidly as Australia gas supply diversifies. Oil Gas J, 103(28): 32–36
19 A Opara, D J Adams, M L Free, J McLennan, J Hamilton (2012). Microbial production of methane and carbon dioxide from lignite, bituminous coal, and coal waste materials. Int J Coal Geol, 96–97: 1–8
https://doi.org/10.1016/j.coal.2012.02.010
20 T J Penner, J M Foght, K Budwill (2010). Microbial diversity of western Canadian subsurface coal beds and methanogenic coal enrichment cultures. Int J Coal Geol, 82(1–2): 81–93
https://doi.org/10.1016/j.coal.2010.02.002
21 Y Qin, T A Moore, J Shen, Z B Yang, Y L Shen, G Wang (2018). Resources and geology of coalbed methane in China: a review. Int Geol Rev, 60(5–6): 777–812
https://doi.org/10.1080/00206814.2017.1408034
22 P Shao, A Wang, W F Wang (2018). Experimental simulation of biogenic coalbed gas generation from lignite and high-volatile bituminous coals. Fuel, 219: 111–119
https://doi.org/10.1016/j.fuel.2018.01.087
23 D Strąpoć, M Mastalerz, K Dawson, J Macalady, A V Callaghan, B Wawrik, C Turich, M Ashby (2011). Biogeochemistry of microbial coal-bed methane. Annu Rev Earth Planet Sci, 39(1): 617–656
https://doi.org/10.1146/annurev-earth-040610-133343
24 A K Wang, P Shao (2019). Generation processes and geochemical analysis of simulated biogenic coalbed methane from lignite. Geochem Int, 57(12): 1295–1305
https://doi.org/10.1134/S0016702919120115
25 B Wang, C Tai, L Wu, L Chen, J Liu, B Hu, D Song (2017). Methane production from lignite through the combined effects of exogenous aerobic and anaerobic microflora. Int J Coal Geol, 173: 84–93
https://doi.org/10.1016/j.coal.2017.02.012
26 P D Warwick, F C Breland Jr, P C Hackley (2008). Biogenic origin of coalbed gas in the northern Gulf of Mexico Coastal Plain, USA. Int J Coal Geol, 76(1–2): 119–137
https://doi.org/10.1016/j.coal.2008.05.009
27 D P Xia, H Y Guo, J Q Ma, Q Si, X B Su (2014). Impact of biogenic methane metabolism on pore structure of coals. Nat Gas Geosci, 25(07): 1097–1102 (in Chinese)
28 Y Yao, D Liu, Y Qiu (2013). Variable gas content, saturation, and accumulation characteristics of Weibei coalbed methane pilot-production field in the southeastern Ordos Basin, China. AAPG Bull, 97(8): 1371–1393
https://doi.org/10.1306/02131312123
29 S P Yoon, J Y Jeon, H S Lim (2016). Stimulation of biogenic methane generation from lignite through supplying an external substrate. Int J Coal Geol, 162: 39–44
https://doi.org/10.1016/j.coal.2016.05.009
30 J Yun, F Y Xu, L Liu, N N Zhong, X B Wu (2012). New progress and future prospects of CBM exploration and development in China. Int J Min Sci Technol, 22(3): 363–369
https://doi.org/10.1016/j.ijmst.2012.04.014
31 Q R Zheng, F G Zeng, S T Zhang (2011). FT-IR study on structure evolution of middle maturate coals. Journal of China Coal Society, 36(03): 481–486 (in Chinese)
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