<br>锆 MOF 的相工程实现高效渗透能转换：直接成像揭示结构演化,Journal of the American Chemical Society

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锆 MOF 的相工程实现高效渗透能转换：直接成像揭示结构演化
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2024-04-18 , DOI: 10.1021/jacs.4c00716
Cailing Chen ₁ , Lingkun Meng ₂ , Li Cao ₁ , Daliang Zhang ₃ , Shuhao An ₁ , Lingmei Liu ₃ , Jianjian Wang ₃ , Guanxing Li ₁ , Tingting Pan ₁ , Jie Shen ₁ , Zhijie Chen ₄ , Zhan Shi ₅ , Zhiping Lai ₁ , Yu Han _{1,

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Affiliation

在金属有机框架（MOF）内以受控方式产生结构缺陷对合成提出了重大挑战，同时，识别这些缺陷的类型和分布也是一项艰巨的表征任务。在这项研究中，我们证明，通过采用 2-磺酰对苯二甲酸作为配体来合成 Zr（或 Hf）基 MOF，可以使用简单的混合结构轻松促进从常见fcu拓扑到罕见jmt拓扑的晶相转变。溶剂策略。 jmt阶段的特点是广泛开放的框架，可以被认为是fcu阶段的衍生阶段，是通过引入缺失簇缺陷而产生的。我们使用超低剂量高分辨率透射电子显微镜明确鉴定了 MOF 相、它们的中间态以及它们形成的新型核壳结构。除了促进相工程之外，MOF 中磺基的掺入还赋予了离子选择性，使其适用于通过混合基质膜制造来收集渗透能。含有jmt相MOF的膜在50倍盐度梯度（NaCl：0.5 M|0.01 M）下表现出10.08 W m ^–2的极高峰值功率密度，超过了商业化5 W m ^–2的阈值应用，可归因于这种新型 MOF 材料中大孔径、大孔隙率和丰富磺酸基的结合。

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Phase Engineering of Zirconium MOFs Enables Efficient Osmotic Energy Conversion: Structural Evolution Unveiled by Direct Imaging

Creating structural defects in a controlled manner within metal–organic frameworks (MOFs) poses a significant challenge for synthesis, and concurrently, identifying the types and distributions of these defects is also a formidable task for characterization. In this study, we demonstrate that by employing 2-sulfonylterephthalic acid as the ligand for synthesizing Zr (or Hf)-based MOFs, a crystal phase transformation from the common fcu topology to the rare jmt topology can be easily facilitated using a straightforward mixed-solvent strategy. The jmt phase, characterized by an extensively open framework, can be considered a derivative of the fcu phase, generated through the introduction of missing-cluster defects. We have explicitly identified both MOF phases, their intermediate states, and the novel core–shell structures they form using ultralow-dose high-resolution transmission electron microscopy. In addition to facilitating phase engineering, the incorporation of sulfonic groups in MOFs imparts ionic selectivity, making them applicable for osmotic energy harvesting through mixed matrix membrane fabrication. The membrane containing the jmt-phase MOF exhibits an exceptionally high peak power density of 10.08 W m^–2 under a 50-fold salinity gradient (NaCl: 0.5 M|0.01 M), which surpasses the threshold of 5 W m^–2 for commercial applications and can be attributed to the combination of large pore size, extensive porosity, and abundant sulfonic groups in this novel MOF material.

更新日期：2024-04-18

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