摘要：Efficient CO2/C2H2 separation at ambient conditions is an essential but challenging process owing to their similar molecular sizes and physical properties. In this work, a novel approach of charge/strain-regulated gas capture and separation was proposed, which offered the advantages of reversibility and controllable kinetics. Highly selective CO2 separation from CO2/C2H2 with porous g-C9N7 nanosheets were demonstrated with varying charge densities and strains using molecular dynamics (MD) simulations and first-principle density function theory (DFT) calculations. The remarkable CO2 permeance up to 5.85 x 10(7) GPU can be achieved by charge engineering. Under the condition of tensile strain, a controllable CO2 separation performance was exhibited, whose CO2 permeance increased with increasing the applied strain. The maximum permeance was 3.44 x 10(7) GPU with 9% strained g-C9N7 membrane. More interestingly, a promising approach combining the charge regulation with strain engineering was explored to investigate the synergistic effect. Under conditions of 2 e(-) charge and 3% tensile strain on g-C9N7 membrane, the CO2 permeance reached 4.24 x 107 GPU, which was 1.6 times of CO2 permeability when only 2 e(-) was added and 10 times of CO2 permeance when only 3% strain was added. Additionally, the energy barrier of CO2 decreased with the increasing degree of regulation (charge and strain engineering) on the g-C9N7 membrane, indicating that the g-C9N7 membrane can be served as an excellent candidate for CO2/C2H2 separation. These results provide useful guidance for developing advanced materials and applying new regulation techniques to realize highly tunable and selective CO2/C2H2 separation.

关键字：CO2 capture and separation; Charge regulation; Strain engineering; Permeance; Membrane

ISSN号：1385-8947

卷、期、页：卷: 435子辑: 2

发表日期：2022-05-01

影响因子：13.272900

期刊分区（SCI为中科院分区）：一区

收录情况：SCIE（科学引文索引网络版）

发表期刊名称：CHEMICAL ENGINEERING JOURNAL

参与作者：李小芳,孙为超

通讯作者：李雪,赵莉,侯晓楠,朱建伟,谢恩泽

第一作者：赫文豪,刘子龙,张潇,刘月亮,张遂安,卢贵武

论文类型：期刊论文

论文概要：李雪,赫文豪,刘子龙,张潇,赵莉,侯晓楠,刘月亮,朱建伟,李小芳,张遂安,孙为超,谢恩泽,卢贵武，Highly selective CO2/C2H2 separation with porous g-C9N7 nanosheets by charge and strain engineering，CHEMICAL ENGINEERING JOURNAL，2022，卷: 435子辑: 2

论文题目：Highly selective CO2/C2H2 separation with porous g-C9N7 nanosheets by charge and strain engineering