Kinetics of methane storage in the natural tobacco leaching filtrate in the hydrate form

doi:10.11949/0438-1157.20221242

Abstract

Abstract:

Hydrate storage of natural gas is recognized as a highly efficient gas storage technology with great potential. How to accelerate the formation of hydrates and ensure the environmental protection of hydration-promoting materials are the key to the practical application of hydration storage gas technology. In order to investigate the kinetics of methane hydrate formation in the natural tobacco leaching filtrate, the solutions by filtering tobacco shred/granule-water mixtures were used to store methane in hydrate under 8.0 MPa and 274.2 K. The experimental results showed that the solution with a water-tobacco mass ratio (liquid-solid ratio) of 5—100 had similar properties of surfactant, and its surface tension decreased by 36.7%—47.5% compared with pure water. Methane hydrate could be formed rapidly in active solutions. The content of active substance in tobacco shred leaching filtrate was significantly lower than that in tobacco granule leaching filtrate. When the liquid-solid ratio was low, tobacco shred leaching filtrate could store more gas in hydrate and had higher storage rate. When the liquid-solid ratio was high, tobacco granule leaching filtrate had better gas storage performance. Especially, the methane uptakes in tobacco granule leaching filtrate with liquid-solid ratio of 50 reached 118.5 mmol·mol^-1, and the gas storage rate was up to 2.98 mmol·mol^-1·min^-1.

Key words: tobacco leaching filtrate, methane storage, hydrate formation, kinetics, promotion

摘要：

水合物法储存天然气被公认为是一种极具潜力的高效储气技术。如何加速水合物生成，又能保证水合促进材料绿色环保，是水合固气技术实用化的关键。本文利用天然烟丝和烟末浸泡滤液在8.0 MPa和274.2 K的实验条件下进行静态水合储甲烷实验，研究甲烷水合物在烟滤液中的生成动力学特性。实验结果表明，水-烟质量比（液固比）为5~100的滤液与表面活性剂溶液性质相似，其表面张力比纯水下降36.7%~47.5%，甲烷水合物在该天然活性溶液中能快速生成。烟丝滤液中活性物含量明显低于烟末滤液，低液固比时，烟丝溶液有更高的水合储气量和储气速率；高液固比时，烟末滤液则表现出更优的水合储气性能，尤其在液固比为50时，烟末滤液中水合物储气量高达118.5 mmol·mol^-1，储气速率达2.98 mmol·mol^-1·min^-1。

关键词: 烟浸滤液, 甲烷储存, 水合物生成, 动力学, 促进

CLC Number:

TE 89

Han HU, Liang YANG, Chunxiao LI, Daoping LIU. Kinetics of methane storage in the natural tobacco leaching filtrate in the hydrate form[J]. CIESC Journal, 2023, 74(3): 1313-1321.

胡晗, 杨亮, 李春晓, 刘道平. 天然烟浸滤液水合物法储甲烷动力学研究[J]. 化工学报, 2023, 74(3): 1313-1321.

Figures/Tables 11

Fig.1 Experimental device

Fig.2 Temperature and pressure changes during the growth of methane hydrate

Fig.3 Gas storage capacity and gas storage rate of hydrate in tobacco solution when RL/S=5

Fig.4 Gas storage capacity and gas storage rate in tobacco solutions with different RL/S

Table 1 Experimental results of hydration gas storage

Hydrate system	R_L/S	C_{up, max}/ (mmol·mol^-1)	R_{up, max}/ (mmol·mol^-1·min^-1)	t_in/min
TS solution	5	71.7 (±2.3)	1.16	570
	10	83.4 (±3.0)	1.56	5
	20	—	—	—
	34	—	—	—
	50	—	—	—
	100	—	—	—
TG solution	5	21.1 (±6.1)	—	—
	10	71.9 (±1.9)	1.35	20
	20	85.3 (±2.5)	2.13	50
	34	80.4 (±4.2)	1.57	70
	50	118.5 (±1.9)	2.98	120
	100	—	—	—
deionized water	—	—	—	—

Fig.5 Concentration of active substances in different RL/S tabacco solutions

Fig.6 Interfacial tension in tobacco solutions with different RL/S

Table 2 Dissolved substance concentration and interfacial tension in tobacco solution under different liquid-solid ratios

Hydrate system	R_L/S	C_AS/%(mass)	IFT/(mN·m^-1)
TS solution	5	3.79 (±0.26)	42.08 (±0.056)
	10	1.34 (±0.09)	43.23 (±0.042)
	20	0.50 (±0.06)	44.73 (±0.053)
TG solution	5	7.47 (±0.38)	38.19 (±0.077)
	10	4.09 (±0.26)	42.17 (±0.074)
	20	2.23 (±0.10)	42.59 (±0.045)
	34	1.22 (±0.09)	43.58 (±0.075)
	50	0.80 (±0.08)	44.20 (±0.090)
	100	0.27 (±0.04)	46.08 (±0.063)
	200	0.12 (±0.01)	43.21 (±0.075)
deionized water	—	0	72.75

Fig.7 Gas storage of tabacco solutions with different RL/S

Fig.8 Maximum gas storage capacity and maximum gas storage rate of tabacco solutions with different RL/S

Fig.9 Methane hydrate formed in tabacco solution

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