Zhang Xiangrui, Wang Hequn, Xiao Tiantian, Chen Xiaoyi, Li Wen, Xu Yihan, Lin Jianlong, Wang Zhe, Peng Hailin, Zhang Sheng
Key Laboratory for Green Chemical Technology of Ministry of Education, Haihe Laboratory of Sustainable Chemical Transformations, School of Chemical Engineering and Technology, Tianjin University, Tianjin 300072, China.
Beijing Graphene Institute, Beijing 100095, P. R. China.
Langmuir. 2023 Apr 11;39(14):4975-4983. doi: 10.1021/acs.langmuir.2c03453. Epub 2023 Mar 30.
Hydrogen isotope separation has been effectively achieved electrochemically by passage of gaseous H/D through graphene/Nafion composite membranes. Nevertheless, deuteron nearly does not exist in the form of gaseous D in nature but as liquid water. Thus, it is a more feasible way to separate and enrich deuterium from water. Herein, we have successfully transferred monolayer graphene to a rigid and porous polymer substrate, PITEM (polyimide track-etched membrane), which could avoid the swelling problem of the Nafion substrate as well as keep the integrity of graphene. Meanwhile, defects in the large area of CVD graphene could be successfully repaired by interfacial polymerization resulting in a high separation factor. Moreover, a new model was proposed for the proton transport mechanism through monolayer graphene based on the kinetic isotope effect (KIE). In this model, graphene plays a significant role in the H/D separation process by completely breaking the O-H/O-D bond, which can maximize the KIE, leading to increased H/D separation performance. This work suggests a promising application for using monolayer graphene in the industry and proposes a pronounced understanding of proton transport in graphene.
通过使气态H/D通过石墨烯/全氟磺酸复合膜,已经通过电化学方法有效地实现了氢同位素分离。然而,自然界中氘几乎不以气态D的形式存在,而是以液态水的形式存在。因此,从水中分离和富集氘是一种更可行的方法。在此,我们成功地将单层石墨烯转移到刚性多孔聚合物基底聚酰亚胺径迹蚀刻膜(PITEM)上,这可以避免全氟磺酸基底的溶胀问题,并保持石墨烯的完整性。同时,通过界面聚合可以成功修复大面积化学气相沉积(CVD)石墨烯中的缺陷,从而得到高分离因子。此外,基于动力学同位素效应(KIE),提出了一种新的质子通过单层石墨烯传输机制的模型。在该模型中,石墨烯在H/D分离过程中起着重要作用,它通过完全断裂O-H/O-D键,使KIE最大化,从而提高H/D分离性能。这项工作表明单层石墨烯在工业上有广阔的应用前景,并对石墨烯中的质子传输有了更深入的理解。