微调的氟化 MOF 可满足使用物理吸附去除痕量 CO2 和空气捕获的需求,Journal of the American Chemical Society

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微调的氟化 MOF 可满足使用物理吸附去除痕量 CO2 和空气捕获的需求
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2016-07-19 , DOI: 10.1021/jacs.6b05345
Prashant M. Bhatt ₁ , Youssef Belmabkhout ₁ , Amandine Cadiau ₁ , Karim Adil ₁ , Osama Shekhah ₁ , Aleksander Shkurenko ₁ , Leonard J. Barbour ₂ , Mohamed Eddaoudi ₁

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开发用于在低二氧化碳 (CO2) 浓度下，即从密闭空间 (<0.5%)，特别是从空气 (400 ppm) 捕获碳的功能性固态材料，对于能源和环境而言至关重要可持续性。在此，我们报告了一种水解稳定的氟化金属有机骨架 (MOF) NbOFFIVE-1-Ni 的精心构建，具有适当的孔隙系统（尺寸、形状和功能），非常适合有效和节能地去除微量二氧化碳。值得注意的是，对于 400 ppm CO2 的物理吸附剂，CO2 选择性 NbOFFIVE-1-Ni 表现出最高的 CO2 重量和体积吸收（约 1.3 mmol/g 和 51.4 cm(3) (STP) cm(-3)）和 298 K。实际上，NbOFFIVE-1-Ni 在真空下 328 K 下提供完整的 CO2 解吸，相关的中等能量输入为 54 kJ/mol，这是传统物理吸附剂完全解吸 CO2 的典型值，但远低于化学吸附剂。值得注意的是，收缩的方形通道使氟中心非常接近，允许增强 CO2 框架相互作用，随后在非常低的 CO2 浓度下实现前所未有的 CO2 选择性。对 NbOFFIVE-1-Ni 承载 CO2 分子的单晶 X 射线衍射研究证明，吸附的 CO2 精确定位在周期性排列的氟中心附近，促进了 CO2 的选择性吸附。在干燥和潮湿条件下的循环 CO2/N2 混合气体柱突破实验证实了在实际碳捕获条件下出色的 CO2 选择性。相关地，显着的水解稳定性使 NbOFFIVE-1-Ni 成为用于直接从密闭空间捕获空气和去除二氧化碳的新基准吸附剂。

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A Fine-Tuned Fluorinated MOF Addresses the Needs for Trace CO2Removal and Air Capture Using Physisorption

The development of functional solid-state materials for carbon capture at low carbon dioxide (CO2) concentrations, namely, from confined spaces (<0.5%) and in particular from air (400 ppm), is of prime importance with respect to energy and environment sustainability. Herein, we report the deliberate construction of a hydrolytically stable fluorinated metal-organic framework (MOF), NbOFFIVE-1-Ni, with the appropriate pore system (size, shape, and functionality), ideal for the effective and energy-efficient removal of trace carbon dioxide. Markedly, the CO2-selective NbOFFIVE-1-Ni exhibits the highest CO2 gravimetric and volumetric uptake (ca. 1.3 mmol/g and 51.4 cm(3) (STP) cm(-3)) for a physical adsorbent at 400 ppm of CO2 and 298 K. Practically, NbOFFIVE-1-Ni offers the complete CO2 desorption at 328 K under vacuum with an associated moderate energy input of 54 kJ/mol, typical for the full CO2 desorption in conventional physical adsorbents but considerably lower than chemical sorbents. Noticeably, the contracted square-like channels, affording the close proximity of the fluorine centers, permitted the enhancement of the CO2-framework interactions and subsequently the attainment of an unprecedented CO2 selectivity at very low CO2 concentrations. The precise localization of the adsorbed CO2 at the vicinity of the periodically aligned fluorine centers, promoting the selective adsorption of CO2, is evidenced by the single-crystal X-ray diffraction study on NbOFFIVE-1-Ni hosting CO2 molecules. Cyclic CO2/N2 mixed-gas column breakthrough experiments under dry and humid conditions corroborate the excellent CO2 selectivity under practical carbon capture conditions. Pertinently, the notable hydrolytic stability positions NbOFFIVE-1-Ni as the new benchmark adsorbent for direct air capture and CO2 removal from confined spaces.

更新日期：2016-07-19

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