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A spin transition mechanism for cooperative adsorption in metal-organic frameworks

机译：金属有机骨架中协同吸附的自旋跃迁机制

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摘要

Cooperative binding, whereby an initial binding event facilitates the uptake of additional substrate molecules, is common in biological systems such as haemoglobin(1,2).It was recently shown that porous solids that exhibit cooperative binding have substantial energetic benefits over traditional adsorbents(3), but few guidelines currently exist for the design of such materials. In principle, metal-organic frameworks that contain coordinatively unsaturated metal centres could act as both selective(4-7) and cooperative adsorbents if guest binding at one site were to trigger an electronic transformation that subsequently altered the binding properties at neighbouring metal sites(8-10). Here we illustrate this concept through the selective adsorption of carbon monoxide (CO) in a series of metal-organic frameworks featuring coordinatively unsaturated iron(ii) sites. Functioning via a mechanism by which neighbouring iron(ii) sites undergo a spin-state transition above a threshold CO pressure, these materials exhibit large CO separation capacities with only small changes in temperature. The very low regeneration energies that result may enable more efficient Fischer-Tropsch conversions and extraction of CO from industrial waste feeds, which currently underutilize this versatile carbon synthon(11). The electronic basis for the cooperative adsorption demonstrated here could provide a general strategy for designing efficient and selective adsorbents suitable for various separations.
机译：在诸如血红蛋白（1,2）等生物系统中，合作结合通常通过初始结合事件促进其他底物分子的吸收。最近发现，表现出合作结合的多孔固体比传统吸附剂具有更大的能量优势（3）。 ），但目前很少有此类材料设计指南。原则上，如果客体在一个位点结合会触发电子转变，从而随后改变相邻金属位点的结合特性，则包含有机不饱和金属中心的金属有机骨架既可以充当选择性吸附剂（4-7），也可以充当协同吸附剂（8）。 -10）。在这里，我们通过选择性吸附一氧化碳（CO）在具有协调性不饱和铁（ii）位点的一系列金属有机框架中阐明了这一概念。这些材料通过一种机制使相邻的铁（ii）位点经历高于阈值CO压力的自旋态转变，这些材料表现出大的CO分离能力，并且温度变化很小。产生的非常低的再生能量可以实现费-托更有效的转化，并从工业废料中提取CO，而目前，这种利用不足的是通用碳合成器（11）。本文展示的协同吸附的电子基础可以为设计适用于各种分离的高效选择性吸附剂提供一般策略。

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  • 来源
    《Nature》 |2017年第7674期|96-100|共5页
  • 作者

    Reed Douglas A.; Keitz Benjamin K.; Oktawiec Julia; Mason Jarad A.; Runcevski Tomce; Xiao Dianne J.; Darago Lucy E.; Rocell Valentina C.; Bordiga Silvia; Long Jeffrey R.;

  • 作者单位

    Univ Calif Berkeley, Dept Chem, Berkeley, CA 94720 USA;

    Univ Calif Berkeley, Dept Chem, Berkeley, CA 94720 USA|Univ Texas Austin, Dept Chem Engn, Austin, TX 78712 USA;

    Univ Calif Berkeley, Dept Chem, Berkeley, CA 94720 USA;

    Univ Calif Berkeley, Dept Chem, Berkeley, CA 94720 USA;

    Univ Calif Berkeley, Dept Chem, Berkeley, CA 94720 USA|Lawrence Berkeley Natl Lab, Div Mat Sci, Berkeley, CA 94720 USA;

    Univ Calif Berkeley, Dept Chem, Berkeley, CA 94720 USA;

    Univ Calif Berkeley, Dept Chem, Berkeley, CA 94720 USA;

    Univ Turin, Dept Chem, NIS & INSTM Ctr Reference, Via Quarello 15, I-10135 Turin, Italy;

    Univ Turin, Dept Chem, NIS & INSTM Ctr Reference, Via Quarello 15, I-10135 Turin, Italy;

    Univ Calif Berkeley, Dept Chem, Berkeley, CA 94720 USA|Lawrence Berkeley Natl Lab, Div Mat Sci, Berkeley, CA 94720 USA|Univ Calif Berkeley, Dept Chem & Biomol Engn, Berkeley, CA 94720 USA;

  • 收录信息 美国《科学引文索引》(SCI);美国《工程索引》(EI);美国《生物学医学文摘》(MEDLINE);美国《化学文摘》(CA);
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