Molecular simulation for adsorption and separation of CH<sub>4</sub>/H<sub>2</sub> in zeolites

姓名
邮箱
手机号码
标题
留言内容
验证码

Abstract

Based on the high-throughput calculation method of molecular simulation, except the structures with zero surface area and less than zero adsorption capacity, four geometric descriptors (largest cavity diameter, specific surface area, pore volume and porosity), an energy descriptor (heat of adsorption), adsorption capacity, and adsorption selectivity coefficient of 199 zeolites are obtained. By studying the correlation between structural characteristics and adsorption separation performance, the result shows that when the largest cavity diameter is 6 Å, the surface area is 1400–2100 m ²·g ^–1, and the pore volume is in a range of 0.2–0.3 cm ³·g ^–1, the zeolite has the greatest influence on the adsorption capacity and adsorption selectivity for methane molecules. At the same time, it is found that the largest cavity diameter and porosity of zeolite molecular sieves have a positive correlation, and there is also an obvious linear relationship between the CH ₄adsorption selectivity coefficient of the equimolar CH ₄/H ₂mixed component and the single-component CH ₄adsorption capacity. By using the grand canonical Monte Carlo simulation method, physical quantities such as adsorption isotherms and isosteric heats of adsorption for CH ₄and H ₂of three channel-shaped zeolites are obtained. The result shows that the pore structure (surface area and pore volume) of the channel-shaped zeolite has a greater influence on the CH ₄adsorption capacity than the energy effect (heat of adsorption), under the same external environment. Combining with the industrial background of steam methane reforming hydrogen production, the separation and selectivity performance of the CH ₄/H ₂mixed system under different components are further studied. The result reveals that there is no correlation between adsorption selectivity of ultra-microporous zeolite material for CH ₄and bulk pressure or feed ratio. According to the centroid distribution density of gas molecules, it is found that CH ₄preferentially occupies the space of smaller pore windows in the channel-shaped zeolite, while the distribution range of H ₂is larger but there is no unambiguous preferential adsorption site.

Keywords:

Authors and contacts

Corresponding author:Liu Xiu-Ying,liuxiuyingzx@126.com

Funds:Project supported by the National Natural Science Foundation of China (Grant Nos. 11304079, 11404094, 11504088), the Key Science and Technology Research Project of Henan Provincial Science and Technology Department, China (Grant No. 182102410076), and the Foundation for Young Core Teachers of Higher Education Institutions of Henan Province of China (Grant No. hnqg20140102)

FullText HTML: translate this paragraph

References

[1]
[2]
[3]
[4]
[5]
[6]
[7]
[8]
[9]
[10]
[11]
[12]
[13]
[14]
[15]
[16]
[17]
[18]
[19]
[20]
[21]
[22]
[23]
[24]
[25]
[26]
[27]
[28]
[29]
[30]
[31]
[32]
[33]
[34]
[35]
[36]

Cited By

DownLoad: Full-Size Img PowerPoint

Zeolite	Unit cell/Å	Cell angle/(°)	PLD/Å	ASA/(m²·g^–1)	POAV/(cm³·g^–1)
ASV	a=b= 8.674,c= 13.919	α=β=γ= 90	4.0279	1323.9	0.1923
BOF	a= 7.503,b= 12.773,c= 13.706	α=β=γ= 90	4.1832	1408.0	0.2207
FER	a= 19.018,b= 14.303,c= 7.541	α=β=γ= 90	4.2893	1545.5	0.2375

DownLoad: CSV

	原子	(ε/k_B)/K	σ/Å	q/e
CH₄		148.0	3.73	0
H₂	H	36.7	2.958	0.468
	com	0	0	–0.936
Zeolite	Si	22	2.3	1.5
	O	53	3.3	–0.75

DownLoad: CSV

[1]
[2]
[3]
[4]
[5]
[6]
[7]
[8]
[9]
[10]
[11]
[12]
[13]
[14]
[15]
[16]
[17]
[18]
[19]
[20]
[21]
[22]
[23]
[24]
[25]
[26]
[27]
[28]
[29]
[30]
[31]
[32]
[33]
[34]
[35]
[36]

[1]	Wang Chang-Chao, Nie Qing-Miao, Shi Liang, Chen Nai-Bo, Hu Lai-Gui, Yan Bo.Kinetic Monte Carlo simulation of selective area growth of mix deposited organic molecules. Acta Physica Sinica, 2024, 73(12): 126801.doi:10.7498/aps.73.20231779
[2]	Cui Zi-Chun, Yang Mo-Han, Ruan Xiao-Peng, Fan Xiao-Li, Zhou Feng, Liu Wei-Min.High-throughput calculation of interfacial friction of two-dimensional material. Acta Physica Sinica, 2023, 72(2): 026801.doi:10.7498/aps.72.20221676
[3]	Xu Xiao-Yan.Quantum Monte Carlo study of strongly correlated electrons. Acta Physica Sinica, 2022, 71(12): 127101.doi:10.7498/aps.71.20220079
[4]	Shangguan Dan-Hua, Yan Wei-Hua, Wei Jun-Xia, Gao Zhi-Ming, Chen Yi-Bing, Ji Zhi-Cheng.Efficient Monte Carlo algorithm of time-dependent particle transport problem in multi-physics coupling calculation. Acta Physica Sinica, 2022, 71(9): 090501.doi:10.7498/aps.71.20211474
[5]	Su Wen-Xia, Lu Hai-Ming, Zeng Zi-Rui, Zhang Yi-Fei, Liu Jian, Xu Kun, Wang Dun-Hui, Du You-Wei.High-throughput computation on relationship between composition and magnetic phase transition temperature of LaFe_11.5Si_1.5-based magnetic refrigeration materials. Acta Physica Sinica, 2021, 70(20): 207501.doi:10.7498/aps.70.20211085
[6]	Wu Si-Yuan, Wang Yu-Qi, Xiao Rui-Juan, Chen Li-Quan.Development and application of battery materials database. Acta Physica Sinica, 2020, 69(22): 226104.doi:10.7498/aps.69.20201542
[7]	Lin Shu, Yan Yang-Jiao, Li Yong-Dong, Liu Chun-Liang.Monte-Carlo method of computing multipactor threshold in microwave devices. Acta Physica Sinica, 2014, 63(14): 147902.doi:10.7498/aps.63.147902
[8]	Guo Hai-Chao, Shi Fan, Ma Zheng-Fei, Zhou Zhi-Wen, Zhou Yi-Ran.Molecular simulations of adsorption and separation of natural gas on zeolitic imidazolate frameworks. Acta Physica Sinica, 2013, 62(17): 176802.doi:10.7498/aps.62.176802
[9]	Liu Xiu-Ying, Li Xiao-Feng, Zhang Li-Ying, Fan Zhi-Qin, Ma Xing-Ke.The theoretical study on CH4 adsorption in different zeolites. Acta Physica Sinica, 2012, 61(14): 146802.doi:10.7498/aps.61.146802
[10]	Fan Xiao-Hui, Zhao Xing-Yu, Wang Li-Na, Zhang Li-Li, Zhou Heng-Wei, Zhang Jin-Lu, Huang Yi-Neng.Monte Carlo simulations of the relaxation dynamics of the spatial relaxation modes in the molecule-string model. Acta Physica Sinica, 2011, 60(12): 126401.doi:10.7498/aps.60.126401
[11]	Fu Fang-Zheng, Li Ming.Calculating the threshold of random laser by using Monte Carlo method. Acta Physica Sinica, 2009, 58(9): 6258-6263.doi:10.7498/aps.58.6258
[12]	Zhang Wei-Hua, Li Jia-Ming.A method to determine the orientations of adsorbed molecules by near edge structures and selection rules. Acta Physica Sinica, 2009, 58(3): 1548-1555.doi:10.7498/aps.58.1548
[13]	Huang Xiao-Jing, You Rong-Yi.Distribution of partial electric field and CO molecules adsorbed on the surface of nanostructured nanoellipsoids. Acta Physica Sinica, 2009, 58(2): 1200-1204.doi:10.7498/aps.58.1200
[14]	Dai Wei, Luo Jiang-Shan, Tang Yong-Jian, Wang Chao-Yang, Chen Shan-Jun, Sun Wei-Guo.Simulation of hydrogen adsorption in molecular sieves. Acta Physica Sinica, 2009, 58(3): 1890-1895.doi:10.7498/aps.58.1890
[15]	Lin Liang-Shu, Xue Yan-Ling, Jiang Qi-Cheng, Zhang Xiao-Min, Wu Peng, Liu Yue-Ming.Highly efficient emission of Er3+ in a functionalized mesoporous silica. Acta Physica Sinica, 2008, 57(9): 5989-5995.doi:10.7498/aps.57.5989
[16]	Shen Xiao-Zhi, Yuan Ping, Wang Jie, Guo Yi-Xiao, Qiao Hong-Zhen, Zhao Xue-Yan.Fit parameter to calculate transition probability. Acta Physica Sinica, 2008, 57(7): 4066-4069.doi:10.7498/aps.57.4066
[17]	Hao Fan-Hua, Hu Guang-Chun, Liu Su-Ping, Gong Jian, Xiang Yong-Chun, Huang Rui-Liang, Shi Xue-Ming, Wu Jun.Monte-Carlo method in calculating the γ spectrum of plutonium volume source. Acta Physica Sinica, 2005, 54(8): 3523-3529.doi:10.7498/aps.54.3523
[18]	Zhang Xian-Ren, Shen Zhi-Gang, Chen Jian-Feng, Wang Wen-Chuan.Adsorption of linear ethane molecules in MCM-41 by molecular simulation. Acta Physica Sinica, 2003, 52(1): 163-168.doi:10.7498/aps.52.163
[19]	PAN ZHENG-YING, CHEN JIAN-XIN, WU SHI-MING, HUO YU-KUN.MONTE CARLO CALCULATION OF PREFERENTIAL SPUTTE-RING IN MULTI-COMPONENT TARGET. Acta Physica Sinica, 1990, 39(2): 319-324.doi:10.7498/aps.39.319
[20]	WANG GUANG-RUI, CHEN SHI-GANG, HAO BAI-LIN.ON THE NONCONVERGENCE PROBLEM IN COMPUTING THE CAPACITY OF STRANGE ATTRACTORS. Acta Physica Sinica, 1984, 33(3): 437-440.doi:10.7498/aps.33.437

Catalog

Vol. 70, Issue 15 - 2021-08-05

Metrics

Abstract views:5059
PDF Downloads:96
Cited By:0

Search

Article