Separation of acetylene, ethylene and ethane over single layered graphdiyne membranes: Performance and insights from quantum mechanical views
Separation of acetylene, ethylene and ethane over single layered graphdiyne membranes: Performance and insights from quantum mechanical views
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单层石墨二炔膜分离乙炔、乙烯和乙烷：量子力学观点的性能和见解
DOI：
10.1016/j.jece.2022.107733
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发表时间：
2022-04
影响因子：
7.7
通讯作者：
Yuliang Li
中科院分区：
文献类型：
--
作者：
Yong Wu;Pei Nian;Zhe Liu;Jinpeng Zhang;Hui Zhang;Nailiang Wang;Bai Hongcun;Yuliang Li
乙烯几乎是全世界聚合物工业最关键的基础化学品。传统的蒸汽裂解制乙烯过程中，会不可避免地释放出乙炔、乙烷等副产物。如何有效分离乙炔、乙烯、乙烷这三种烃类气体，长期以来一直困扰着乙烯生产的工业过程。本文从量子化学的角度研究了石墨烯单层膜对乙炔、乙烯和乙烷的分离性能。采用密度泛函理论计算了石墨炔膜分离三种气体的扩散能垒、选择性和渗透性。结果表明，在300 K时，乙炔/乙烯、乙炔/乙烷和乙烯/乙烷的选择性分别可达2 × 106、5 × 108和184。乙炔在300 K时的磁导率约为1.9 × 10− 4 mol·m−2·s−1·Pa−1，比工业标准高出约5个数量级。在400 K左右，乙烯渗透率可达到工业标准.结合能量分解分析（EDA）和约化密度梯度（RDG）分析，探讨了三种气体在石墨炔膜上扩散过程中的相互作用，给出了分离性能的量子力学解释。根据EDA结果，气体吸附行为是由分散效应。而在气体向膜扩散过程中，排斥效应和静电效应增强，分散效应减弱。此外，通过RDG分析，直观地描绘了气体分子与石墨二炔膜的相互作用强度、面积和类型。
Ethylene is nearly the most crucial basic chemicals all over the word for polymer industry. In the process of ethylene preparation by traditional steam cracking, by-products such as acetylene and ethane are released unavoidably. How to effectively separate these three hydrocarbon gases, acetylene, ethylene, and ethane, has plagued the industrial process of ethylene production for a long time. This work explores the separation performance of acetylene, ethylene and ethane over single layered graphdiyne membranes from viewpoint of quantum chemistry. The diffusion energy barrier, selectivity and permeability of the three gases separated by graphdiyne membranes are investigated in details by using the density functional theory calculations. The results show that the selectivity of acetylene/ethylene, acetylene/ethane, and ethylene/ethane can reach 2 × 106,5 × 108and 184 respectively at 300 K. The permeability of acetylene at 300 K is about 1.9 × 10−4mol·m−2·s−1·Pa−1, which is about 5 orders of magnitude higher than the industry standard. The permeability for ethylene can reach the industry standard at about 400 K. Combined with energy decomposition analysis (EDA) and reduced density gradient (RDG) analysis, the interaction of the three gas in diffusion processes over graphdiyne membranes is explored, and the quantum mechanical explanation of the separation performance is given. According to EDA results, gas adsorption behavior is dominated by the dispersion effect. However, the repulsive effect and electrostatic effect increase in the gas diffusion approaching to the membrane, and the dispersion effect decreases. In addition, the interaction strength, area and type of gas molecules and graphdiyne membrane are visually depicted via RDG analysis.
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影响因子：
7.7
作者：
Yi Wang;Qiang Li;G. Tang;Nanxin Zhang
通讯作者：
Yi Wang;Qiang Li;G. Tang;Nanxin Zhang
DOI：
10.1016/j.jmaa.2016.11.058
发表时间：
2016-05
期刊：
arXiv: Spectral Theory
影响因子：
--
作者：
B. Helffer;M. Sundqvist
通讯作者：
B. Helffer;M. Sundqvist
影响因子：
9.5
作者：
Zhaoqi Zhu
通讯作者：
Zhaoqi Zhu
影响因子：
2.1
作者：
Z. Domínguez;M. Galván;M. Cortez;M. Salas;Rocío Meza;M. A. Leyva-Ramírez;Barbara Gordillo
通讯作者：
Z. Domínguez;M. Galván;M. Cortez;M. Salas;Rocío Meza;M. A. Leyva-Ramírez;Barbara Gordillo
影响因子：
2.1
作者：
H. Ullah;M. Khan;T. Hayat
通讯作者：
H. Ullah;M. Khan;T. Hayat