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Unveiling the electronic properties of native solid electrolyte interphase layers on Mg metal electrodes using local electrochemistry
Chemical Science ( IF 7.6 ) Pub Date : 2023-08-30 , DOI: 10.1039/d3sc02840b
Carla Santana Santos 1 , Martina Romio 2 , Yuri Surace 2 , Nicolas Eshraghi 3 , Marco Amores 2 , Andreas Mautner 4, 5 , Christiane Groher 2 , Marcus Jahn 2 , Edgar Ventosa 6 , Wolfgang Schuhmann 1
Chemical Science ( IF 7.6 ) Pub Date : 2023-08-30 , DOI: 10.1039/d3sc02840b
Carla Santana Santos 1 , Martina Romio 2 , Yuri Surace 2 , Nicolas Eshraghi 3 , Marco Amores 2 , Andreas Mautner 4, 5 , Christiane Groher 2 , Marcus Jahn 2 , Edgar Ventosa 6 , Wolfgang Schuhmann 1
Affiliation
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Magnesium-ion batteries (MIBs) are of considerable interest as environmentally more sustainable, cheaper, and safer alternatives to Li-ion systems. However, spontaneous electrolyte decomposition occurs due to the low standard reduction potential of Mg, leading to the deposition of layers known as native solid electrolyte interphases (n-SEIs). These layers may inhibit the charge transfer (electrons and ions) and, therefore, reduce the specific power and cycle life of MIBs. We propose scanning electrochemical microscopy (SECM) as a microelectrochemical tool to locally quantify the electronic properties of n-SEIs for MIBs. These interphases are spontaneously formed upon contact of Mg metal disks with organoaluminate, organoborate, or bis(trifluoromethanesulfonyl)imide (TFSI)-based electrolyte solutions. Our results unveil increased local electronic and global ionic insulating properties of the n-SEI formed when using TFSI-based electrolytes, whereas a low electronically protecting character is observed with the organoaluminate solution, and the organoborate solution being in between them. Moreover, ex situ morphological and chemical characterization was performed on the Mg samples to support the results obtained by the SECM measurements. Differences in the electronic and ionic conductivities of n-SEIs perfectly correlate with their chemical compositions.
中文翻译：
利用局部电化学揭示镁金属电极上天然固体电解质中间相层的电子特性
镁离子电池 (MIB) 作为对环境更可持续、更便宜且更安全的锂离子系统替代品而备受关注。然而，由于镁的标准还原电位较低，会发生自发电解质分解，导致称为天然固体电解质中间相（n-SEI）的层沉积。这些层可能会抑制电荷转移（电子和离子），因此会降低 MIB 的比功率和循环寿命。我们建议扫描电化学显微镜（SECM）作为一种微电化学工具来局部量化 MIB 的 n-SEI 的电子特性。这些中间相是在镁金属盘与有机铝酸盐、有机硼酸盐或双(三氟甲磺酰基)亚胺(TFSI)基电解质溶液接触时自发形成的。我们的结果揭示了使用基于 TFSI 的电解质时形成的 n-SEI 的局部电子和整体离子绝缘性能增加，而有机铝酸盐溶液和介于两者之间的有机硼酸盐溶液则观察到较低的电子保护特性。此外，对镁样品进行了异位形态和化学表征，以支持 SECM 测量获得的结果。n-SEI 的电子和离子电导率的差异与其化学成分完全相关。
更新日期：2023-08-30
中文翻译：
利用局部电化学揭示镁金属电极上天然固体电解质中间相层的电子特性
镁离子电池 (MIB) 作为对环境更可持续、更便宜且更安全的锂离子系统替代品而备受关注。然而，由于镁的标准还原电位较低，会发生自发电解质分解，导致称为天然固体电解质中间相（n-SEI）的层沉积。这些层可能会抑制电荷转移（电子和离子），因此会降低 MIB 的比功率和循环寿命。我们建议扫描电化学显微镜（SECM）作为一种微电化学工具来局部量化 MIB 的 n-SEI 的电子特性。这些中间相是在镁金属盘与有机铝酸盐、有机硼酸盐或双(三氟甲磺酰基)亚胺(TFSI)基电解质溶液接触时自发形成的。我们的结果揭示了使用基于 TFSI 的电解质时形成的 n-SEI 的局部电子和整体离子绝缘性能增加，而有机铝酸盐溶液和介于两者之间的有机硼酸盐溶液则观察到较低的电子保护特性。此外，对镁样品进行了异位形态和化学表征，以支持 SECM 测量获得的结果。n-SEI 的电子和离子电导率的差异与其化学成分完全相关。
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