Rock-Salt MnS0.5Se0.5 Nanocubes Assembled on N-Doped Graphene Forming van der Waals Heterostructured Hybrids as High-Performance Anode for Lithium- and Sodium-Ion Batteries
Rock-Salt MnS0.5Se0.5 Nanocubes Assembled on N-Doped Graphene Forming van der Waals Heterostructured Hybrids as High-Performance Anode for Lithium- and Sodium-Ion Batteries
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岩盐 MnS0.5Se0.5 纳米立方体组装在氮掺杂石墨烯上形成范德华异质结构杂化物作为锂和钠离子电池的高性能阳极
DOI：
10.1021/acsami.1c04776
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发表时间：
2021
影响因子：
9.5
通讯作者：
Qing Yang
中科院分区：
文献类型：
--
作者：
Shiqi Xing;Jing Yang;Mairman Muska;Huanran Li;Qing Yang
锰系硫系化合物具有理论容量大、价格低、毒性低等优点，在组装锂离子电池和钠离子电池(LiBS/SIB)方面具有潜在的应用潜力，但其低电导率和易团聚行为可能会阻碍其在技术上的应用。本文首次在较低的温度下，以乙酰丙酮、二苯基二卤化锰和十八烯为原料，在岩盐相中合成了MnS0.5Se0.5纳米立方体，并将其与N掺杂的石墨烯组装成了一种新型的异质结构纳米杂化材料(简称MnS0.5Se0.5/N-G杂化材料)，这对包括LiBS和/或SIBs在内的金属离子电池的制备具有很大的潜力。研究表明，在固溶体MnS0.5Se0.5纳米立方体中，通过MnS和MnSe的非平衡合金化，产生了致密的空位，增加了活性中心，在低温溶液合成路线中实现了偏析和缺陷。同时，引入N掺杂石墨烯在MnS0.5Se0.5和N掺杂石墨烯之间形成异质结界面，可以有效地提高其导电性，避免活性MnS0.5Se0.5纳米立方体的团聚，并显著改善其电化学性能。因此，MnS0.5Se0.5/N-G杂化材料具有优异的Li/Na存储容量、出色的倍率性能以及令人满意的持久稳定性(LiBS/SiB的存储容量为1039/457 mA/g-1，为0.1A/g-1)。此外，用阴极LiFePO4(LFP)构建的阳极MnS0.5Se0.5/N-G的全电池LiBS进一步证实了其实际应用的前景。
Manganese-based chalcogenides would be of latent capacity in serving as anodes for assembling lithium- and/or sodium-ion batteries (LIBs/SIBs) due to their large theoretical capacity, low price, and low-toxicity functionality, while the low electroconductivity and easy agglomeration behavior may impede their technical applications. Here, a solid-state solution of MnS0.5Se0.5nanocubes in rock-salt phase has been synthesized for the first time at a relatively low temperature from the precursors of Mn(II) acetylacetonate with dibenzyl dichalcogens in oleylamine with octadecene, and the MnS0.5Se0.5nanocubes have been assembled with N-doped graphene to form a new kind of heterostructured nanohybrids (shortened as MnS0.5Se0.5/N-G hybrids), which are very potential for the fabrication of metal-ion batteries including LIBs and/or SIBs. Investigations revealed that there have been dense vacancies generated and active sites increased via nonequilibrium alloying of MnS and MnSe into the solid-solution MnS0.5Se0.5nanocubes with segregation and defects achieved in the low-temperature solution synthetic route. Meanwhile, the introduction of N-doped graphene forming heterojunction interfaces between MnS0.5Se0.5and N-doped graphene would efficiently enhance their electroconductivity and avoid agglomeration of the active MnS0.5Se0.5nanocubes with considerably improved electrochemical properties. As a result, the MnS0.5Se0.5/N-G hybrids delivered superior Li/Na storage capacities with outstanding rate performance as well as satisfactorily lasting stability (1039/457 mA h g–1at 0.1 A g–1for LIBs/SIBs). Additionally, full-cell LIBs of the anodic MnS0.5Se0.5/N-G constructed with cathodic LiFePO4(LFP) further confirmed the promising future for their practical application.