石墨烯优化固体聚合物电解质电解法分离氢同位素的模拟分析  

Simulation analysis of hydrogen isotope separation in graphene solid polymer electrolyte electrolysis

作　　者：卫飞 唐方东[3] 刘佳煜 忻智炜 曾友石[1] 楚鑫新[1] 刘卫[1] WEI Fei;TANG Fangdong;LIU Jiayu;XIN Zhiwei;ZENG Youshi;CHU Xinxin;LIU Wei(Shanghai Institute of Applied Physics,Chinese Academy of Sciences,Shanghai 201800,China;University of Chinese Academy of Sciences,Beijing 100049,China;Shanghai Institute of Measurement and Testing Technology,Shanghai 201203,China)

机构地区：[1]中国科学院上海应用物理研究所,上海201800 [2]中国科学院大学,北京100049 [3]上海市计量测试技术研究院,上海201203

出　　处：《核技术》2020年第10期50-56,共7页Nuclear Techniques

基　　金：上海市质量技术监督局科技计划项目(No.2017-01、No.2018-07)资助。

摘　　要：石墨烯作为一种新型的高选择渗透膜材料,有望提升固体聚合物电解质(Solid Polymer Electrolyte,SPE)电解法对氢同位素的分离效果。本研究将石墨烯与SPE电解法中的质子交换膜结合,探究了石墨烯对氢同位素分离性能的影响。基于B3LYP/6-31G(d)理论,采用Gaussian 09软件计算了石墨烯模型对质子的穿透势垒,同时考虑零点振动能的影响,得到了石墨烯对氢同位素离子的分离系数。计算结果表明:石墨烯模型对H+/D+和H+/T+的分离系数分别为12.4和37.5(293 K);几何结构的优化、缺陷的存在会降低质子的穿透势垒,并且Stone-Wales缺陷的存在会提升分离效果。因此,石墨烯能够有效提高SPE电解法对氢同位素的分离系数,有望推动建立真正高效的氢同位素分离技术。[Background]As a new type of high-selective permeable membrane material,graphene is expected to improve the separation effect of solid polymer electrolyte electrolysis(SPE)on hydrogen isotopes.[Purpose]In this study,graphene was combined with the proton exchange membrane in SPE electrolysis to explore the effect of its separation performance for hydrogen isotopes.[Methods]Based on the B3LYP/6-31G(d)theory,quantum chemistry calculation software Gaussian 09 was used to calculate the penetration barrier of the graphene model to protons.At the same time,the effect of zero-point vibrational energy was taken into account to obtain the separation coefficient of graphene for hydrogen isotope ions.[Results]The computation results of the separation coefficients of H+/D+and H+/T+are 12.4 and 37.5,respectively,at room temperature(293 K).The research resultants indicate that the optimized model structure and the presence of different types of defects reduce the penetration barrier of protons,the existence of Stone-Wales defect does improve the separation performance.[Conclusions]Graphene can be used to effectively improve the separation coefficient of hydrogen isotopes in SPE electrolysis,which is expected to promote the establishment of truly efficient hydrogen isotope separation technology.

关 键 词：石墨烯 氢同位素分离 密度泛函理论(Density Functional Theory DFT) SPE电解法 分离系数 

分 类 号：TL99[核科学技术—核技术及应用]