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Facile Fabrication of Functionalized Separators for Lithium-Ion Batteries with Ionic Conduction Path Modifications via the γ-Ray Co-irradiation Grafting Process
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2021-06-04 , DOI: 10.1021/acsami.1c06460 Haoshen Ma 1 , Jiaxiang Liu 1 , Haiming Hua 2 , Longqing Peng 2 , Xiu Shen 2 , Xin Wang 2 , Peng Zhang 1 , Jinbao Zhao 1, 2
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2021-06-04 , DOI: 10.1021/acsami.1c06460 Haoshen Ma 1 , Jiaxiang Liu 1 , Haiming Hua 2 , Longqing Peng 2 , Xiu Shen 2 , Xin Wang 2 , Peng Zhang 1 , Jinbao Zhao 1, 2
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Separators play a vital role in electronic insulation and ionic conduction in lithium-ion batteries. The common improvement strategy of polyolefin separators is mostly based on modifications with a coating layer, which is simple and effective to some extent. However, the improvement is often accompanied by negative effects such as the increase of the thickness and the blockage of the porous structure, resulting in the decrease of energy density and power density. The porous structure of the separators serves as a conduction path for ions to travel back and forth between the anode and cathode, which has an important impact on the performance of lithium-ion batteries. If the porous structure of the separators can be modified, it will essentially affect the ionic transport behavior through the whole conduction path. Herein, we provide a simple and effective method to functionalize the porous polyolefin separator via the γ-ray co-irradiation grafting process, where high-energy γ-ray is used to generate active sites on the polymer chain to initiate the grafting polymerization of chosen monomers with selected functional groups. In this work, 4,4,5,5-tetramethyl-2-vinyl-1,3,2-dioxaborolane, a kind of borane molecule with an electron-deficient group, was chosen as the grafting monomer. After the γ-ray co-irradiation grafting process, both the surface and pores of the polyolefin separators were functionalized by electron-deficient groups in the borane molecule and the whole electrolyte conduction path within the separator was activated. Due to the electron-deficient effect of the B atom, the lithium-ion conduction is promoted and the lithium-ion transference number can be increased to 0.5. As a result, the half-cell assembled with the functionalized separator shows better cycle stability and better capacity retention under high current rate.
中文翻译：
通过 γ 射线共辐照接枝工艺轻松制造具有离子传导路径修饰的锂离子电池功能化隔膜
隔膜在锂离子电池的电子绝缘和离子传导方面起着至关重要的作用。聚烯烃隔板常见的改进策略多以涂层改性为主，在一定程度上简单有效。然而，这种改进往往伴随着厚度增加和多孔结构堵塞等负面影响，导致能量密度和功率密度降低。隔膜的多孔结构作为离子在正负极之间来回穿行的传导路径，对锂离子电池的性能有重要影响。如果可以修改隔膜的多孔结构，它将在本质上影响通过整个传导路径的离子传输行为。在此处，我们提供了一种简单有效的方法，通过 γ 射线共辐照接枝工艺对多孔聚烯烃隔膜进行功能化，其中使用高能 γ 射线在聚合物链上产生活性位点，以引发所选单体的接枝聚合选定的官能团。在这项工作中，4,4,5,5-tetramethyl-2-vinyl-1,3,2-dioxaborolane 是一种具有缺电子基团的硼烷分子，被选为接枝单体。在γ射线共辐照接枝过程后，聚烯烃隔膜的表面和孔隙均被硼烷分子中的缺电子基团功能化，隔膜内的整个电解质传导路径被激活。由于B原子的缺电子效应，促进锂离子传导，锂离子迁移数可提高到0.5。因此，组装有功能化隔膜的半电池在高电流速率下表现出更好的循环稳定性和更好的容量保持率。
更新日期：2021-06-16
中文翻译：
通过 γ 射线共辐照接枝工艺轻松制造具有离子传导路径修饰的锂离子电池功能化隔膜
隔膜在锂离子电池的电子绝缘和离子传导方面起着至关重要的作用。聚烯烃隔板常见的改进策略多以涂层改性为主，在一定程度上简单有效。然而，这种改进往往伴随着厚度增加和多孔结构堵塞等负面影响，导致能量密度和功率密度降低。隔膜的多孔结构作为离子在正负极之间来回穿行的传导路径，对锂离子电池的性能有重要影响。如果可以修改隔膜的多孔结构，它将在本质上影响通过整个传导路径的离子传输行为。在此处，我们提供了一种简单有效的方法，通过 γ 射线共辐照接枝工艺对多孔聚烯烃隔膜进行功能化，其中使用高能 γ 射线在聚合物链上产生活性位点，以引发所选单体的接枝聚合选定的官能团。在这项工作中，4,4,5,5-tetramethyl-2-vinyl-1,3,2-dioxaborolane 是一种具有缺电子基团的硼烷分子，被选为接枝单体。在γ射线共辐照接枝过程后，聚烯烃隔膜的表面和孔隙均被硼烷分子中的缺电子基团功能化，隔膜内的整个电解质传导路径被激活。由于B原子的缺电子效应，促进锂离子传导，锂离子迁移数可提高到0.5。因此，组装有功能化隔膜的半电池在高电流速率下表现出更好的循环稳定性和更好的容量保持率。
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