含铁矿物对高成熟有机质有水体系热解生气的影响

doi:10.11764/j.issn.1672-1926.2020.03.004

Abstract

Abstract:

In order to ascertain the effect of iron-bearing minerals on gas generation from water-organics reactions, three groups of isothermal pyrolysis involving a high-mature kerogen (kerogen + water, kerogen + pyrite + water, kerogen + magnetite + water) were conducted in hydrothermal conditions by a gold-tube system. Through determination of the yields of gas products, it is indicated that the presence of pyrite and magnetite both led to a certain decrease in the yields of hydrocarbon gases. For instance, the methane yields at Easy%R_O of 3.08% in hydrothermal experiments with pyrite and magnetite are about 8.5 and 13.3 mL/g_TOC lower than that in pyrolysis with only water. The yield and carbon isotopic ratios of CO₂ in pyrolysis involving water and pyrite are evidently higher than those in pyrolysis involving only water and involving water and magnetite. The H₂S yields in hydrothermal experiments with Fe-bearing minerals (especially magnetite) are much lower compared with those without minerals. The analysis of gas compositions shows that the presence of pyrite apparently resulted in the increase of gas dryness and the decrease of relative content of isomeric hydrocarbons. The hydrogen isotope of the gas product of the water-magnetite system is relatively lower than that of the water-only system, indicating that the addition of magnetite promoted the formation of early H₂ and hydrogenation occurred with the organic matter. These results indicate that the addition of iron-bearing minerals may inhibit the carbocation reaction, and the hydrogenation of water-organic matter may be mainly a radical reaction.

Key words: Kerogen, Pyrite, Magnetite, Catalytic inhibition, Organic-inorganic interaction

CLC Number:

TE122.1⁺1

Wen-jun ZHANG, Kun HE, Xian-qing LI, Jing-kui MI, Guo-yi HU. Effect of iron-bearing minerals on gas generation from pyrolysis of high-mature organic matter in hydrothermal conditions[J].Natural Gas Geoscience, 2020, 31(9): 1316-1325.

Figures/Tables 4

Table 1

Table 2

The yields, chemical and isotopic compositions of gas products in pyrolysis experiments"

温度 /℃	时间 /d	Easy% R₀ /%	气体产率/（mL/g_TOC）										碳同位素 /‰（VPDB）		氢同位素 /‰（VSMOW）		含水体质种类
温度 /℃	时间 /d	Easy% R₀ /%	C₁	C₂	C₃	iC₄	nC₄	iC₅	nC₅	H₂	CO₂	H₂S	δ¹³C₁	δ¹³C₂	δ¹³C $C O 2$	δD₁	含水体质种类
330	1	0.79	0.086	0.005	—	—	—	—	—	—	14.05	—	—	—	-29.2	—	干酪根 + 水
330	7	1.05	0.067	0.004	—	—	—	-—	—	—	10.08	—	—	—	-29.1	—
330	10	1.11	0.223	0.048	0.014	0.001 0	0.001 1	0.000 2	0.000 2	—	22.54	—	—	-24.5	-29.1	-274.7
360	1	1.02	0.189	0.015	0.002	0.000 3	0.000 4	0.000 3	0.000 4	—	19.17	—	—	-24.4	-29.8	-269.1
360	5	1.29	0.572	0.028	0.002	0.000 3	0.000 4	0.000 4	0.000 6	—	26.41	—	-45.4	-25.3	-29.3	-272.2
360	7	1.42	0.957	0.045	0.002	0.000 4	0.000 4	0.000 2	0.000 3	—	27.77	—	-44.0	-26.2	-29.1	-275.3
360	10	1.5	0.715	0.029	0.001	0.000 3	0.000 3	0.000 3	0.000 1	—	20.96	—	-45.6	-26.4	-29.3	-266.6
380	1	1.24	0.437	0.027	0.001	0.000 4	0.000 4	0.000 2	0.000 2	—	20.79	—	-47.8	-25.9	-29.5	-266.9
380	5	1.56	0.721	0.029	0.000	0.000 3	0.000 3	0.000 4	0.000 4	—	11.09	0.01	-46.4	-25.6	-29.4	-273.5
380	7	1.72	2.419	0.100	0.002	0.000 5	0.000 5	0.000 7	0.000 3	0.008	27.86	0.30	-43.5	-25.1	-29.6	-282.1
380	10	1.82	3.471	0.130	0.002	0.000 4	0.000 3	0.000 2	0.000 2	0.006	30.21	0.81	42.3	-24.8	-29.0	-280.8
400	1	1.49	1.019	0.051	0.003	0.000 3	0.000 2	0.000 3	0.000 3	0.006	24.17	0.08	-41.3	-24.6	-29.1	-276.6
400	5	1.88	5.446	0.174	0.005	0.000 2	0.000 2	0.001 5	0.003 3	0.005	31.33	0.40	-38.5	-25.1	-28.7	-279.6
400	7	2.07	6.682	0.215	0.003	0.004 4	0.003 7	0.015 4	0.008 1	0.017	31.50	2.63	-38.1	-24.5	-28.7	-275.0
400	10	2.19	10.995	0.312	0.006	0.005 3	0.008 0	0.008 9	0.006 7	0.005	38.64	5.76	-37.9	-24.7	-29.0	-255.8
450	1	2.31	10.334	0.380	0.009	0.001 2	0.002 0	0.001 5	0.001 1	0.062	40.74	9.35	-37.7	-24.6	-28.6	-251.4
450	5	2.84	22.527	0.489	0.012	0.000 5	0.000 7	0.005 0	0.003 9	1.113	54.23	13.91	-34.8	-23.6	-27.7	-184.5
450	7	3.08	27.419	0.547	0.014	0.000 5	0.000 4	0.016 1	0.005 1	1.474	60.43	14.79	-33.6	-23.2	-28.0	-165.3
330	1	0.79	0.056	0.005	—	—	—	—	—	—	10.10	—	—	—	-29.1	—	干酪根 + 黄铁矿 + 水
330	5	0.95	0.083	0.005	—	—	—	—	—	—	13.26	—	—	—	-28.5	—
330	7	1.05	0.113	0.004	—	—	—	—	—	—	20.08	—	—	—	-28.8	—
330	10	1.11	0.112	0.003	—	—	—	—	—	—	21.28	—	—	—	-28.5	-252.4
360	1	1.02	0.200	0.011	—	—	—	—	—	—	17.25	—	-46.2	-26.4	—	-256.7
360	5	1.29	0.345	0.007	0.001	—	—	—	—	—	23.05	—	-45.2	-26.2	-28.4	-263.2
360	7	1.42	0.343	0.005	0.001	—	—	—	—	—	22.03	—	-43.1	-25.8	-27.9	-260.3
360	10	1.5	0.619	0.007	0.003	0.000 3	0.000 5	0.000 2	0.000 1	—	38.68	—	-41.5	-25.7	-27.5	-269.1
380	1	1.24	0.400	0.018	0.006	0.000 3	0.000 6	0.000 6	0.000 4	—	23.01	—	-43.9	-25.4	-28.8	-266.8
380	5	1.56	0.912	0.023	0.016	0.003 1	0.004 8	0.005 5	0.005 7	—	33.42	—	-42.6	-25.1	-28.7	-265.4
380	7	1.72	0.961	0.010	0.003	0.001 3	0.002 0	0.002 1	0.002 4	—	35.99	—	-42.5	-25.2	-28.6	-260.8
380	10	1.82	1.422	0.011	0.003	0.001 0	0.001 3	0.002 1	0.003 2	0.006	47.51	—	-39.9	-26.4	-29.1	-265.4
400	1	1.49	0.798	0.061	0.049	0.017 7	0.021 7	0.001 4	0.006 0	0.005	27.20	—	-40.6	-26.1	-29.5	-266.8
400	5	1.88	2.233	0.020	0.011	0.006 0	0.007 7	0.010 2	0.003 9	0.007	39.81	—	-39.8	-24.6	-28.7	-265.1
400	7	2.07	3.088	0.019	0.004	0.002 5	0.003 3	0.002 9	0.002 3	0.007	44.61	—	-37.8	-25.1	-28.6	-261.5
400	10	2.19	2.848	0.015	0.005	0.001 9	0.002 3	0.003 3	0.002 8	0.006	45.04	—	-37.4	-25.9	-28.5	-256.4
450	1	2.31	5.857	0.052	0.009	0.000 4	0.000 4	0.000 9	0.000 7	0.000	50.13	0.06	-37.0	-25.8	-28.6	-241.7
450	5	2.84	8.387	0.044	0.007	0.000 3	0.000 3	0.001 4	0.001 0	0.357	76.85	11.10	-32.4	-24.2	-28.4	-168.4
450	7	3.08	18.935	0.188	0.006			0.000 4	0.000 4	0.713	64.84	31.55	-31.8	-24.1	-28.2	-155.6
330	1	0.79	0.083	0.005	0.001	0.000 2	0.000 4	0.000 2	0.000 1	—	5.60	—	—	-31.0	-30.7	—	干酪根 + 磁铁矿 + 水
330	5	0.95	0.132	0.006	0.000	0.000 6	0.000 9	0.002 8	0.000 8	—	7.46	—	—	-29.4	-30.4	—
330	7	1.05	0.138	0.007	0.001	0.000 9	0.001 1	0.002 8	0.001 2	—	8.17	—		-29.3	-30.1
330	10	1.11	0.186	0.009	0.000	0.000 7	0.000 8	0.001 6	0.001 9	—	8.24	—	—	-29.8	-30.0
360	1	1.02	0.231	0.012	0.001	0.000 6	0.000 6	0.002 0	0.000 8	—	6.26	—	-48.6	-31.2	-30.4	-262.7
360	5	1.29	0.538	0.018	0.001	0.000 4	0.000 4	0.001 1	0.001 2	—	8.91	—	-47.1	-28.6	-30.1	-281.1
360	7	1.42	0.774	0.021	0.001	0.000 3	0.000 3	0.005 4	0.002 5	—	13.76	—	-45.8	-25.4	-30.0	-276.8
360	10	1.5	0.814	0.022	0.002	0.002 1	0.001 9	0.000 5	0.002 5	—	11.01	—	-44.9	-25.8	-30.1	-275.1
380	1	1.24	0.525	0.021	0.001	0.000 6	0.000 5	0.000 2	0.000 4	—	7.09	—	-43.9	-26.0	-30.4	-276.3
380	5	1.56	1.475	0.029	0.005	0.001 8	0.001 7	0.000 3	0.000 4	—	18.00	—	-42.3	-24.3	-30.0	-276.6
380	7	1.72	1.940	0.046	0.001	—	—	—	—	0.004	11.03	—	-42.6	-23.8	-30.2	-289.1
380	10	1.82	1.834	0.023	0.001	—	—	—	—	0.004	17.37	—	-41.6	-23.3	-30.0	-281.1
400	1	1.49	1.077	0.041	0.001	—	—	—	—	0.004	10.40	—	-40.8	-23.8	-29.9	-270.8
400	5	1.88	3.720	0.051	0.001	—	—	—	—	0.005	21.62	—	-39.7	-23.1	-29.4	-266.4
400	7	2.07	4.773	0.036	0.001	—	—	—	—	0.005	22.72	—	-38.8	-22.6	-29.3	-259.5
400	10	2.19	4.230	0.016	0.001	—	—	—	—	0.006	26.91	—	-38.9	-22.6	-28.6	-256.3
450	1	2.31	9.312	0.114	0.003	—	—	—	—	0.006	23.08	—	-36.2	-18.2	-28.9	-249.6
450	5	2.84	13.041	0.017	0.004	—	—	—	—	0.005	42.76	—	-33.7	-19.6	-28.7	-189.7
450	7	3.08	14.128	0.034	0.009	—	—	—	—	0.009	53.22	—	-33.3	-19.4	-28.3	-171.4

Table 2

Fig.1

Fig.2

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Effect of iron-bearing minerals on gas generation from pyrolysis of high-mature organic matter in hydrothermal conditions

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