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用于室温下二氧化碳的可回收封存、储存及原位催化转化的复合多孔液体

Composite Porous Liquid for Recyclable Sequestration, Storage and In Situ Catalytic Conversion of Carbon Dioxide at Room Temperature.

作者信息

Bhattacharjee Archita, Kumar Raj, Sharma Kamendra P

机构信息

Department of Chemistry, Indian Institute of Technology Bombay, Mumbai, 400076, India.

出版信息

ChemSusChem. 2021 Aug 23;14(16):3303-3314. doi: 10.1002/cssc.202100931. Epub 2021 Jul 14.

Abstract

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 CO . The recyclable porous liquid composite comprising polymer-surfactant modified hollow silica nanorods and carbonic anhydrase enzyme not only sequesters (5.5 cm  g at 273 K and 1 atm) and stores CO but is also capable of driving an in situ enzymatic reaction for hydration of CO to HCO ion, subsequently converting it to CaCO due to reaction with pre-dissolved Ca . 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 Ca and HCO 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.

摘要

永久性孔隙与流动性相结合,使多孔液体具有流动加工性,而这在多孔固体中是看不到的。尽管多孔液体已被用于捕获不同气体及其分离,但利用原位化学反应将吸附气体转化为实用化学品的研究仍然匮乏。在此,我们展示了一种新型无溶剂混合(介孔)多孔液体复合材料的设计与开发,首次证明其可用于吸附二氧化碳的原位碳矿化。这种由聚合物 - 表面活性剂改性的中空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,不仅能捕获(在273K和1个大气压下为5.5 cm³ g⁻¹)和储存二氧化碳,还能够驱动二氧化碳水合生成碳酸氢根离子的原位酶促反应,随后由于与预先溶解的钙离子反应将其转化为碳酸钙。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成核与生长。此外,通过互补的钙离子和碳酸氢根离子通过由界面通道分隔的不同隔室的扩散来进行相同反应,可以利用多孔复合材料的液体状性质。这些研究为在多孔液体中进行化学反应以从吸附分子开发实用化学品提供了概念验证。

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