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用于高效且高选择性锂/镁分离的同系物焊接结晶碳氮化物膜

Congener-welded crystalline carbon nitride membrane for robust and highly selective Li/Mg separation.

作者信息

Zhang Yuanyuan, Zhou Ke, Su Shigang, Gao Jun, Liu Jian, Jiang Lei

机构信息

Qingdao Institute of Bioenergy and Bioprocess Technology, Chinese Academy of Sciences, Shandong Energy Institute, Qingdao New Energy Shandong Laboratory, Qingdao 266101, China.

College of Materials Science and Engineering, Qingdao University of Science and Technology, Qingdao 266042, China.

出版信息

Sci Adv. 2024 Jun 14;10(24):eadm9620. doi: 10.1126/sciadv.adm9620.

Abstract

Extracting lithium from salt-lake brines critically relies on the separation of Li and Mg, which could combat the lithium shortage. However, designing robust sieving membrane with high Li/Mg selectivity in the long-time operation has remained highly challenging. Here, we demonstrate a bioinspired congener-welded crystalline carbon nitride membrane that can accomplish efficient and stable monovalent ion sieving over divalent Mg ion. The crystalline carbon nitrides have uniform and narrow pore size to reject the large hydrated Mg and rich ligating sites to facilitate an almost barrierless Li transport as suggested by ab initio simulations. These crystals were then welded by vapor-deposited congeners, i.e., amorphous polymer carbon nitride, which have similar composition and chemistry with the crystals, forming intimate and compatible crystal/polymer interface. As a result, our membrane can sieve out highly dilute Li (0.002 M) from concentrated Mg (1.0 M) with a high selectivity of 1708, and can be continuously operated for 10 days.

摘要

从盐湖卤水中提取锂关键依赖于锂和镁的分离,这有助于应对锂短缺问题。然而,设计在长时间运行中具有高锂/镁选择性的坚固筛分膜仍然极具挑战性。在此,我们展示了一种受生物启发的同系物焊接结晶氮化碳膜,它能够实现高效且稳定的一价离子筛分,而排斥二价镁离子。结晶氮化碳具有均匀且狭窄的孔径以排斥大尺寸的水合镁离子,并且具有丰富的配位位点,从头算模拟表明这有利于锂几乎无阻碍地传输。然后通过气相沉积的同系物,即非晶态聚合物氮化碳,将这些晶体焊接起来,该聚合物与晶体具有相似的组成和化学性质,形成紧密且相容的晶体/聚合物界面。结果,我们的膜能够从高浓度镁(1.0 M)中筛出高度稀释的锂(0.002 M),选择性高达1708,并且能够连续运行10天。

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