用于检测，捕获和“按需”释放一氧化碳的新型混合材料,ACS Applied Materials & Interfaces

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用于检测，捕获和“按需”释放一氧化碳的新型混合材料
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2018-04-13 00:00:00 , DOI: 10.1021/acsami.8b01776
Anaïs Pitto-Barry ₁ , Alexandru Lupan ₂ , Christopher Ellingford ₃ , Amr A. A. Attia ₂ , Nicolas P. E. Barry ₁

Affiliation

一氧化碳（CO）既是危害健康的物质，又是许多工业过程（如甲醇蒸汽重整和大规模氧化反应）的副产品。从氮中分离出CO（N ₂由于其电子结构，尺寸和理化性质（例如沸点）的相似性，在工业过程中被认为是困难的。一氧化碳也是燃料电池中的主要毒物，因为它吸附在催化剂的活性部位上。因此，发现能够在温和条件下有效捕获和释放CO的新材料具有最大的经济意义。但是，尚无在环境温度下在存在污染物（例如水，氮气，二氧化碳和氧气）的情况下专门吸收并轻松释放CO的方法。在这里，我们报告了一种新型的杂化材料的简单通用的制造方法，该杂化材料可以在温和的条件下捕获和释放一氧化碳。我们发现，封装在聚二甲基硅氧烷制成的网络中的含碳硼烷金属络合物即使在浸入水中时也会与CO发生反应，从而导致显着的颜色和红外特征变化。此外，我们发现，在环境温度和压力下，只需将网络浸入有机溶剂中不到1分钟即可轻松地从材料中释放出CO，这不仅提供了一种直接的回收方法，而且提供了一种新的回收方法。一氧化碳的“按需”释放。我们通过对缺电子的金属络合物进行羰基化反应来说明从网络中按需释放CO的利用，该反应导致形成CO加合物，并伴随着凝胶的再循环。

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New Class of Hybrid Materials for Detection, Capture, and “On-Demand” Release of Carbon Monoxide

Carbon monoxide (CO) is both a substance hazardous to health and a side product of a number of industrial processes, such as methanol steam reforming and large-scale oxidation reactions. The separation of CO from nitrogen (N₂) in industrial processes is considered to be difficult because of the similarities of their electronic structures, sizes, and physicochemical properties (e.g., boiling points). Carbon monoxide is also a major poison in fuel cells because of its adsorption onto the active sites of the catalysts. It is therefore of the utmost economic importance to discover new materials that enable effective CO capture and release under mild conditions. However, methods to specifically absorb and easily release CO in the presence of contaminants, such as water, nitrogen, carbon dioxide, and oxygen, at ambient temperature are not available. Here, we report the simple and versatile fabrication of a new class of hybrid materials that allows capture and release of carbon monoxide under mild conditions. We found that carborane-containing metal complexes encapsulated in networks made of poly(dimethylsiloxane) react with CO, even when immersed in water, leading to dramatic color and infrared signature changes. Furthermore, we found that the CO can be easily released from the materials by simply dipping the networks into an organic solvent for less than 1 min, at ambient temperature and pressure, which not only offers a straightforward recycling method, but also a new method for the “on-demand” release of carbon monoxide. We illustrated the utilization of the on-demand release of CO from the networks by carrying out a carbonylation reaction on an electron-deficient metal complex that led to the formation of the CO-adduct, with concomitant recycling of the gel. We anticipate that our sponge-like materials and scalable methodology will open up new avenues for the storage, transport, and controlled release of CO, the silent killer and a major industrial poison.

更新日期：2018-04-13

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