Utilizing MOF precursors toward one-step, calcination-free synthesis of MnO2 superstructures for superior lithium storage
Utilizing MOF precursors toward one-step, calcination-free synthesis of MnO2 superstructures for superior lithium storage
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利用 MOF 前体一步、免煅烧合成 MnO2 超结构，实现卓越的锂存储
DOI：
10.1039/d2se01224c
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发表时间：
2022
影响因子：
5.6
通讯作者：
Xiaoshi Hu
中科院分区：
文献类型：
--
作者：
Yang Fan;Deli Luo;Yan Wu;Tianlang Peng;Qi Qi;Xubing Han;Jinxin Zhou;Yanling Wang;Bao Lin;Qinqin Xiong;Yongjun Yuan;Haiying Qin;Xiaoshi Hu
在室温和环境气氛下，合理控制合成不同领域的结构相关过渡金属氧化物材料仍然是一个挑战。在本文中，我们提出了一种简单的一步无煅烧的方法，通过在室温下用适当浓度的开放碱性水溶液同时离子交换和氧化预先制备的mn基M2(dobdc) （dobdc = 2,5-二羟基-1,4-苯二甲酸酯）MOF （CPO-27-Mn）模板，合理和绿色地合成三维分层多面体状二氧化锰（MnO2）的超结构。以及它们在可充电锂电池中的应用。具体来说，我们提出在溶液相过程中，阴离子dobdc4 -配体与OH -交换后，生成的中间氢氧化锰与溶液中的溶解O2反应生成MnO2。电化学评价表明，合成的层次化二氧化锰超结构具有优异的电化学性能，具有较高的可逆比可逆性（866.4 mA h g−1），在1000 mA g−1下循环300次后具有优异的倍率性能和长期循环稳定性（797.9 mA h g−1）。这种独特的新型mof衍生方案为设计制造先进的过渡金属氧化物功能纳米材料提供了另一种视角。
Rationally controlled synthesis of transition metal oxide materials for structure-related applications in diverse areas at room temperature and ambient atmosphere remains a challenge. In this article, we propose a facile one-step calcination-free approach for the rational and green synthesis of 3D hierarchical polyhedron-shaped superstructures of manganese dioxide (MnO2) through the simultaneous ion exchange and oxidation of a preformed Mn-based M2(dobdc) (dobdc = 2,5-dihydroxy-1,4-benzenedicarboxylate) MOF (CPO-27-Mn) template with an adequate open aqueous alkaline solution of a moderate concentration at room temperature, as well as their application in rechargeable lithium cells. Concretely, we proposed that during the solution-phase process, upon exchange of the anionic dobdc4− ligand with OH−, the resultant intermediate manganese hydroxide reacts with dissolved O2 in solution to form MnO2. Electrochemical evaluation showed that the as-synthesized hierarchical MnO2 superstructures exhibited excellent electrochemical performance, including high reversible specific reversibility (866.4 mA h g−1), superior rate capability and long-term cycling stability (797.9 mA h g−1 after 300 cycles at 1000 mA g−1) when serving as anodes. This unique novel MOF-derived protocol provides an alternative perspective on the designed fabrication of advanced transition metal oxide functional nanomaterials.