多孔3D聚合物，用于高压甲烷存储和二氧化碳捕获,Journal of Materials Chemistry A

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多孔3D聚合物，用于高压甲烷存储和二氧化碳捕获
Journal of Materials Chemistry A ( IF 10.7 ) Pub Date : 2017-04-25 00:00:00 , DOI: 10.1039/c7ta00934h
Silvia Bracco _{1,

2,

3,

4} , Daniele Piga _{1,

2,

3,

4} , Irene Bassanetti _{1,

2,

3,

4} , Jacopo Perego _{1,

2,

3,

4} , Angiolina Comotti _{1,

2,

3,

4} , Piero Sozzani _{1,

2,

3,

4}

Affiliation

高表面积3D聚合物由于其高气体吸收以及对热和化学降解的稳定性而成为多孔材料中最有前景的一类。合成并比较了一系列具有芳香族结构单元的多孔有机聚合物，以探讨它们作为气体的吸附剂的高压性能，这些气体对能源和环境具有重要意义。特别注意在环境温度下高达180 bar的压力下甲烷的储存。从多种空间膨胀的芳族单体开始制备多孔聚合物：正在考虑环数，可变尺寸和形状的系统变化。大量的环（最多6个），它们充当多个反应性位点，并在多齿节点之间形成许多连接，形成了广泛的交叉链接框架。冷凝是通过两种替代的合成途径获得的，即，Yamamoto交叉偶联和Friedel-Crafts烷基化反应。多孔聚合物的结构特性和高稳定性，即使是机械压缩，也可以通过几种方法仔细确定，包括1D和2D固态NMR，FT IR和热分析。CH ₄多孔聚合物的吸收允许了解对压力的增量响应（最高值），并利用广泛的压力范围来定制用于存储和运输的气体吸附/解吸循环。由于显着地存在大的中孔和网络柔性，再加上高的表面积，因此在高压下获得了显着的收益，从而确保了极具竞争力的吸收/输送效率。在180 bar下，对于多孔有机聚合物（例如，咔唑基和三茂基材料）测量的吸附值高达445 cm ³ STP g ^-1。这些材料PAF1的基准达到吸附的CH ₄的916 cm ³ STP g ^-1值，超过了大多数最佳性能的MOF，COF和活性炭的性能。在室温下收集的CO ₂和N ₂吸附等温线使得能够评估此类聚合物网络对CO ₂选择性分离和捕获的适用性。总而言之，在此类材料中，直到高压，都进行了深入而广泛的比较筛选，为进一步的合成和应用工作提供了必要的参数。

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Porous 3D polymers for high pressure methane storage and carbon dioxide capture

High surface area 3D polymers represent one of the most promising classes of porous materials because of their high gas uptake and stability to thermal and chemical degradation. A series of porous organic polymers with aromatic building units have been synthesized and compared to explore their high-pressure performance as adsorbents of gases of relevant importance for energy and the environment. Particular attention was paid to methane storage up to pressures as high as 180 bar at ambient temperature. Porous polymers were prepared starting from a wide choice of spatially expanded aromatic monomers: a systematic change in the number of rings, variable size and shape was taken under consideration. The high number of rings (up to 6), which act as multiple reactive sites and form a number of connections between the multi-dentate nodes, result in an extensive cross-linked framework. Condensation was obtained by two alternative synthetic routes, viz., Yamamoto cross-coupling and Friedel–Crafts alkylation reactions. The structural characteristics and high stability of the porous polymers, even to mechanical compression, were carefully determined by several methods, including 1D and 2D solid state NMR, FT IR and thermal analyses. The CH₄ uptake in the porous polymers allowed an understanding of the incremental response to pressure, up to extremely high values, and the exploitation of the extensive pressure range to customize the gas adsorption/desorption cycles for storage and transportation. Owing to the notable presence of large mesopores and network flexibility, combined with high surface area, a remarkable gain at high pressure was achieved, ensuring a highly competitive uptake/delivery efficiency. At 180 bar, adsorption values up to 445 cm³ STP g⁻¹ were measured for porous organic polymers such as carbazolyl- and triptycene-based materials. The benchmark of these materials PAF1 reaches the value of 916 cm³ STP g⁻¹ of adsorbed CH₄, exceeding the performance of most of the best performing MOFs, COFs and activated carbons. CO₂ and N₂ adsorption isotherms collected at room temperature enabled the assessment of the suitability of such polymer networks for CO₂ selective separation and capture. In summary, the in-depth and extensive comparative screening within this class of materials up to high pressures provides the necessary parameters for further synthetic and applicative work.

更新日期：2017-05-31

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