Robust Barium Phosphonate Metal–Organic Frameworks Synthesized under Aqueous Conditions,ACS Materials Letters

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Robust Barium Phosphonate Metal–Organic Frameworks Synthesized under Aqueous Conditions
ACS Materials Letters ( IF 9.6 ) Pub Date : 2021-06-15 , DOI: 10.1021/acsmaterialslett.1c00275
Khalifah A. Salmeia _{1,

2} , Simone Dolabella _{3,

4} , Dambarudhar Parida ₂ , Terry J. Frankcombe ₅ , Akef T. Afaneh ₁ , Kyle E. Cordova ₆ , Bassem Al-Maythalony ₆ , Shanyu Zhao ₇ , Romain Civioc ₇ , Ali Marashdeh ₁ , Bernhard Spingler ₈ , Ruggero Frison ₃ , Antonia Neels _{3,

4}

Affiliation

The design and discovery of three-dimensional crystalline metal–organic frameworks (MOFs) from linkers with phosphonate coordinating groups and even alkaline earth metals is largely undeveloped. Herein, we report a strategy for realizing new, stable, and robust barium phosphonate MOFs, termed Empa-1 and Empa-2. The two-dimensional (2D) Empa-1 or three-dimensional (3D) Empa-2 could be realized by way of systematically modulating the ratio of Ba²⁺ with a tetratopic phosphonate-based linker that was crafted to incorporate nitrogen-rich triazine units bridged by a fixed piperazine core. In addition to this synthetic approach, temperature-dependent synchrotron-radiation powder X-ray diffraction analysis demonstrated that the 2D Empa-1 undergoes an irreversible phase transition upon heating and subsequent dehydration to form the 3D Empa-2. Given the presence of uncoordinated phosphonic acid moieties within the structure of 3D Empa-2, the CO₂ sorption capabilities are reported. We believe our ability to link the alkaline earth metal barium with a novel tetratopic phosphonate linker, as evidenced by the robust structures of Empa-1 and -2, paves the way for further exploration and discovery of new crystalline, porous frameworks with greater structural diversity, stability, and wide-scale practical applicability.

中文翻译：

在水性条件下合成的坚固的磷酸钡金属-有机骨架

从具有膦酸酯配位基团甚至碱土金属的连接体设计和发现的三维结晶金属有机骨架（MOF）在很大程度上尚未开发。在此，我们报告了一种实现新的、稳定且坚固的膦酸钡 MOF 的策略，称为 Empa-1 和 Empa-2。二维（2D）Empa-1或三维（3D）Empa-2可以通过系统调节Ba ²⁺的比例来实现带有基于四位膦酸酯的接头，该接头经过精心设计以包含由固定哌嗪核心桥接的富氮三嗪单元。除了这种合成方法之外，温度相关的同步辐射粉末 X 射线衍射分析表明，2D Empa-1 在加热和随后脱水后会发生不可逆的相变，形成 3D Empa-2。鉴于 3D Empa-2 结构中存在未配位的膦酸部分，CO ₂报告了吸附能力。我们相信我们能够将碱土金属钡与新型四位膦酸酯连接体连接起来，如 Empa-1 和 -2 的稳健结构所证明的那样，为进一步探索和发现具有更大结构多样性的新结晶多孔骨架铺平了道路，稳定性和广泛的实际适用性。

更新日期：2021-07-05

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