Liu Zhiyuan, Wang Dong, Yang Huazeng, Feng Liu, Xu Xin, Si Weimeng, Hou Yongzhao, Wen Guangwu, Zhang Rui, Qiu Jieshan
School of Materials Science and Engineering, Shandong University of Technology, Zibo, 255000, P. R. China.
Shandong Silicon Nano New Material Technology Co. LTD, Zibo, 255000, P. R. China.
Angew Chem Int Ed Engl. 2024 Oct 14;63(42):e202409204. doi: 10.1002/anie.202409204. Epub 2024 Sep 12.
Two-dimensional (2D) nonlayered metal compounds with porous structure show broad application prospects in electrochemistry-related fields due to their abundant active sites, open ions/electrons diffusion channels, and faradaic reactions. However, scalable and universal synthesis of 2D porous compounds still remains challenging. Here, inspired by blowing gum, a metal-organic gel (MOG) rapid redox transformation (MRRT) strategy is proposed for the mass production of a wide variety of 2D porous metal oxides. Adequate crosslinking degree of MOG precursor and its rapid redox with NO are critical for generating gas pressure from interior to exterior, thus blowing the MOG into 2D carbon nanosheets, which further act as self-sacrifice template for formation of oxides with porous and ultrathin structure. The versatility of this strategy is demonstrated by the fabrication of 39 metal oxides, including 10 transition metal oxides, one II-main group oxide, two III-main group oxides, 22 perovskite oxides, four high-entropy oxides. As an illustrative verification, the 2D transition metal oxides exhibit excellent capacitive deionization (CDI) performance. Moreover, the assembled CDI cell could act as desalting battery to supply electrical energy during electrode regeneration. This MRRT strategy offers opportunities for achieving universal synthesis of 2D porous oxides with nonlayered structures and studying their electrochemistry-related applications.
具有多孔结构的二维（2D）非层状金属化合物因其丰富的活性位点、开放的离子/电子扩散通道和法拉第反应，在电化学相关领域展现出广阔的应用前景。然而，二维多孔化合物的可扩展且通用的合成仍然具有挑战性。在此，受吹口香糖的启发，提出了一种金属有机凝胶（MOG）快速氧化还原转变（MRRT）策略，用于大规模生产各种二维多孔金属氧化物。MOG前驱体足够的交联度及其与NO的快速氧化还原反应对于从内部到外部产生气体压力至关重要，从而将MOG吹制成二维碳纳米片，这些碳纳米片进一步作为自牺牲模板形成具有多孔和超薄结构的氧化物。通过制备39种金属氧化物证明了该策略的通用性，其中包括10种过渡金属氧化物、1种II主族氧化物、2种III主族氧化物、22种钙钛矿氧化物、4种高熵氧化物。作为一个示例性验证，二维过渡金属氧化物表现出优异的电容去离子（CDI）性能。此外，组装的CDI电池可以作为脱盐电池在电极再生期间提供电能。这种MRRT策略为实现具有非层状结构的二维多孔氧化物的通用合成及其电化学相关应用的研究提供了机会。
