Capture of Carbon Dioxide from Air and Flue Gas in the Alkylamine-Appended Metal–Organic Framework mmen-Mg2(dobpdc),Journal of the American Chemical Society

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Capture of Carbon Dioxide from Air and Flue Gas in the Alkylamine-Appended Metal–Organic Framework mmen-Mg2(dobpdc)
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2012-04-12 , DOI: 10.1021/ja300034j
Thomas M. McDonald ₁ , Woo Ram Lee ₂ , Jarad A. Mason ₁ , Brian M. Wiers ₁ , Chang Seop Hong ₂ , Jeffrey R. Long ₁

Affiliation

Two new metal-organic frameworks, M(2)(dobpdc) (M = Zn (1), Mg (2); dobpdc(4-) = 4,4'-dioxido-3,3'-biphenyldicarboxylate), adopting an expanded MOF-74 structure type, were synthesized via solvothermal and microwave methods. Coordinatively unsaturated Mg(2+) cations lining the 18.4-Å-diameter channels of 2 were functionalized with N,N'-dimethylethylenediamine (mmen) to afford Mg(2)(dobpdc)(mmen)(1.6)(H(2)O)(0.4) (mmen-Mg(2)(dobpdc)). This compound displays an exceptional capacity for CO(2) adsorption at low pressures, taking up 2.0 mmol/g (8.1 wt %) at 0.39 mbar and 25 °C, conditions relevant to removal of CO(2) from air, and 3.14 mmol/g (12.1 wt %) at 0.15 bar and 40 °C, conditions relevant to CO(2) capture from flue gas. Dynamic gas adsorption/desorption cycling experiments demonstrate that mmen-Mg(2)(dobpdc) can be regenerated upon repeated exposures to simulated air and flue gas mixtures, with cycling capacities of 1.05 mmol/g (4.4 wt %) after 1 h of exposure to flowing 390 ppm CO(2) in simulated air at 25 °C and 2.52 mmol/g (9.9 wt %) after 15 min of exposure to flowing 15% CO(2) in N(2) at 40 °C. The purity of the CO(2) removed from dry air and flue gas in these processes was estimated to be 96% and 98%, respectively. As a flue gas adsorbent, the regeneration energy was estimated through differential scanning calorimetry experiments to be 2.34 MJ/kg CO(2) adsorbed. Overall, the performance characteristics of mmen-Mg(2)(dobpdc) indicate it to be an exceptional new adsorbent for CO(2) capture, comparing favorably with both amine-grafted silicas and aqueous amine solutions.

中文翻译：

在烷基胺附加金属-有机骨架 mmen-Mg2(dobpdc) 中从空气和烟道气中捕获二氧化碳

两种新的金属有机骨架 M(2)(dobpdc)（M = Zn (1), Mg (2)；dobpdc(4-) = 4,4'-dioxido-3,3'-biphenyldicarboxylate），采用通过溶剂热和微波方法合成了扩展的 MOF-74 结构类型。内衬 2 的 18.4 Å 直径通道的配位不饱和 Mg(2+) 阳离子用 N,N'-二甲基乙二胺 (mmen) 进行功能化，以提供 Mg(2)(dobpdc)(mmen)(1.6)(H(2) O)(0.4) (mmen-Mg(2)(dobpdc))。该化合物在低压下表现出卓越的 CO(2) 吸附能力，在 0.39 mbar 和 25 °C、与从空气中去除 CO(2) 和 3.14 mmol 相关的条件下吸收 2.0 mmol/g (8.1 wt %) /g (12.1 wt %) 在 0.15 bar 和 40 °C，与从烟道气中捕获 CO(2) 相关的条件。动态气体吸附/解吸循环实验表明，mmen-Mg(2)(dobpdc) 可以在重复暴露于模拟空气和烟气混合物中再生，暴露 1 小时后循环容量为 1.05 mmol/g (4.4 wt%)在 25 °C 和 2.52 mmol/g (9.9 wt %) 的模拟空气中流动 390 ppm CO(2) 在 15 分钟后暴露于在 N(2) 中流动 15% CO(2) 在 40 °C。在这些过程中从干燥空气和烟道气中去除的 CO(2) 的纯度估计分别为 96% 和 98%。作为一种烟道气吸附剂，通过差示扫描量热实验估计再生能量为 2.34 MJ/kg CO(2) 吸附。总体而言，mmen-Mg(2)(dobpdc) 的性能特征表明它是一种用于 CO(2) 捕获的特殊新型吸附剂，

更新日期：2012-04-12

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