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Suppressing Unfavorable Interfacial Reactions Using Polyanionic Oxides as Efficient Buffer Layers: Low-Cost Li3PO4 Coatings for Sulfide-Electrolyte-Based All-Solid-State Batteries
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2023-03-07 , DOI: 10.1021/acsami.2c21511 Joo Young Lee 1 , Sungwoo Noh 2 , Ju Yeong Seong 2 , Sangheon Lee 2 , Yong Joon Park 1
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2023-03-07 , DOI: 10.1021/acsami.2c21511 Joo Young Lee 1 , Sungwoo Noh 2 , Ju Yeong Seong 2 , Sangheon Lee 2 , Yong Joon Park 1
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The poor electrochemical performance of all solid-state batteries (ASSBs) that use sulfide electrolytes can be attributed to undesirable side reactions at the cathode/sulfide-electrolyte interface; this issue can be addressed via surface coating. Ternary oxides such as LiNbO3 and Li2ZrO3 are generally used as coating materials because of their high chemical stabilities and ionic conductivities. However, their relative high cost discourages their use in mass production. In this study, Li3PO4 was introduced as a coating material for ASSBs, because phosphates possess good chemical stabilities and ionic conductivities. Phosphates also prevent the exchange of S2– and O2– in the electrolyte and cathode and, thus, inhibit interfacial side reactions caused by ionic exchange, because they contain the same anion (O2–) and cation (P5+) species as those present in the cathode and sulfide electrolyte, respectively. Furthermore, the Li3PO4 coatings can be prepared using low-cost source materials such as polyphosphoric acid and lithium acetate. We investigated the electrochemical performance of the Li3PO4-coated cathodes and found that the Li3PO4 coating significantly improved the discharge capacities, rate capabilities, and cyclic performances of the all-solid-state cell. While the discharge capacity of the pristine cathode was ∼181 mAh·g–1, that of 0.15 wt % Li3PO4-coated cathode was ∼194–195 mAh·g–1. And the capacity retention of the Li3PO4-coated cathode over 50 cycles was much superior (∼84–85%) to that of the pristine sample (∼72%). Simultaneously, the Li3PO4 coating reduced the side reactions and interdiffusion at the cathode/sulfide-electrolyte interfaces. The results of this study demonstrate the potential of low-cost polyanionic oxides, such as Li3PO4, as commercial coating materials for ASSBs.
中文翻译：
使用聚阴离子氧化物作为有效缓冲层抑制不利的界面反应：用于基于硫化物电解质的全固态电池的低成本 Li3PO4 涂层
所有使用硫化物电解质的固态电池 (ASSB) 的电化学性能不佳可归因于阴极/硫化物-电解质界面处的不良副反应；这个问题可以通过表面涂层来解决。三元氧化物如LiNbO 3和Li 2 ZrO 3由于其高化学稳定性和离子电导率通常用作涂层材料。然而，它们相对较高的成本阻碍了它们在大规模生产中的使用。在这项研究中，Li 3 PO 4被引入作为 ASSB 的涂层材料，因为磷酸盐具有良好的化学稳定性和离子电导率。磷酸盐还可以防止 S 2–和 O 2–的交换在电解质和阴极中，因此抑制由离子交换引起的界面副反应，因为它们分别含有与阴极和硫化物电解质中存在的相同的阴离子 (O 2– ) 和阳离子 (P 5+ ) 物质。此外，Li 3 PO 4涂层可以使用低成本原料如多磷酸和乙酸锂来制备。我们研究了 Li 3 PO 4涂层正极的电化学性能，发现 Li 3 PO 4涂层显着提高了全固态电池的放电容量、倍率性能和循环性能。原始阴极的放电容量为～181 mAh·g –1，而 0.15 wt% Li 3 PO 4涂层阴极的放电容量为～194–195 mAh·g –1。Li 3 PO 4涂层正极在 50 个循环后的容量保持率(~84–85%) 远优于原始样品 (~72%)。同时，Li 3 PO 4涂层减少了阴极/硫化物-电解质界面处的副反应和相互扩散。这项研究的结果证明了低成本聚阴离子氧化物的潜力，例如 Li 3PO 4，作为 ASSB 的商业涂层材料。
更新日期：2023-03-07
中文翻译：
使用聚阴离子氧化物作为有效缓冲层抑制不利的界面反应：用于基于硫化物电解质的全固态电池的低成本 Li3PO4 涂层
所有使用硫化物电解质的固态电池 (ASSB) 的电化学性能不佳可归因于阴极/硫化物-电解质界面处的不良副反应；这个问题可以通过表面涂层来解决。三元氧化物如LiNbO 3和Li 2 ZrO 3由于其高化学稳定性和离子电导率通常用作涂层材料。然而，它们相对较高的成本阻碍了它们在大规模生产中的使用。在这项研究中，Li 3 PO 4被引入作为 ASSB 的涂层材料，因为磷酸盐具有良好的化学稳定性和离子电导率。磷酸盐还可以防止 S 2–和 O 2–的交换在电解质和阴极中，因此抑制由离子交换引起的界面副反应，因为它们分别含有与阴极和硫化物电解质中存在的相同的阴离子 (O 2– ) 和阳离子 (P 5+ ) 物质。此外，Li 3 PO 4涂层可以使用低成本原料如多磷酸和乙酸锂来制备。我们研究了 Li 3 PO 4涂层正极的电化学性能，发现 Li 3 PO 4涂层显着提高了全固态电池的放电容量、倍率性能和循环性能。原始阴极的放电容量为～181 mAh·g –1，而 0.15 wt% Li 3 PO 4涂层阴极的放电容量为～194–195 mAh·g –1。Li 3 PO 4涂层正极在 50 个循环后的容量保持率(~84–85%) 远优于原始样品 (~72%)。同时，Li 3 PO 4涂层减少了阴极/硫化物-电解质界面处的副反应和相互扩散。这项研究的结果证明了低成本聚阴离子氧化物的潜力，例如 Li 3PO 4，作为 ASSB 的商业涂层材料。
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