Composite Porous Liquid for Recyclable Sequestration, Storage and In Situ Catalytic Conversion of Carbon Dioxide at Room Temperature
Composite Porous Liquid for Recyclable Sequestration, Storage and In Situ Catalytic Conversion of Carbon Dioxide at Room Temperature
复制标题
DOI：
10.1002/cssc.202100931
复制
发表时间：
2021-07-14
期刊：
影响因子：
8.4
通讯作者：
Sharma, Kamendra P.
中科院分区：
文献类型：
--
作者：
Bhattacharjee, Archita;Kumar, Raj;Sharma, Kamendra P.
永久性气孔与流动性相结合，使多孔液体具有流动可加工性，否则在多孔固体中看不到。尽管多孔液体已被用于不同气体的隔离和分离，但利用原位化学反应将吸附的气体转化为实用化学品的研究仍然很少。在这里，我们展示了一种新型的无溶剂和杂化(介观)多孔液体复合材料的设计和开发，首次证明了这种复合材料可以用于吸附的二氧化碳的原位碳矿化。由聚合物-表面活性剂修饰的空心二氧化硅纳米棒和碳酸酐酶组成的可回收多孔液体复合材料不仅在273K和1atm下隔离(5.5 cm(3)g(-1))并储存二氧化碳，而且还能够驱动CO2水合成HCO3-离子的原位酶反应，随后由于与预溶出的钙离子反应而转化为CaCO3。光学显微镜和电子显微镜结合X射线衍射揭示了方解石和文石晶体的形核和生长。此外，通过通过由界面通道分隔的不同隔室中互补的钙离子和HCO3-离子的扩散来执行相同的反应，可以利用多孔复合材料的类液体特性。这些研究提供了在多孔液体中进行化学反应以从吸附分子中开发实用化学品的概念的证据。
Permanent pores combined with fluidity renders flow processability to porous liquids otherwise not seen in porous solids. Although porous liquids have been utilized for sequestration of different gases and their separation, there is still a dearth of studies for deploying in situ chemical reactions to convert adsorbed gases into utility chemicals. Here, we show the design and development of a new type of solvent-less and hybrid (meso-)porous liquid composite, which, as demonstrated for the first time, can be used for in situ carbon mineralization of adsorbed CO2. The recyclable porous liquid composite comprising polymer-surfactant modified hollow silica nanorods and carbonic anhydrase enzyme not only sequesters (5.5 cm(3) g(-1) at 273 K and 1 atm) and stores CO2 but is also capable of driving an in situ enzymatic reaction for hydration of CO2 to HCO3- ion, subsequently converting it to CaCO3 due to reaction with pre-dissolved Ca2+. Light and electron microscopy combined with X-ray diffraction reveals the nucleation and growth of calcite and aragonite crystals. Moreover, the liquid-like property of the porous composite material can be harnessed by executing the same reaction via diffusion of complimentary Ca2+ and HCO3- ions through different compartments separated by an interfacial channel. These studies provide a proof of concept of deploying chemical reactions within porous liquids for developing utility chemical from adsorbed molecules.