Qiu Tianjie, Gao Song, Fu Yanchun, Xu Dong, Kong Dekai
Beijing Key Laboratory for Theory and Technology of Advanced Battery Materials, School of Materials Science and Engineering, Peking University, Beijing 100871, China.
CHN Energy New Energy Technology Research Institute Co., Ltd., Beijing 102211, China.
Materials (Basel). 2022 Jul 31;15(15):5292. doi: 10.3390/ma15155292.
Carbon dioxide (CO) is generally unavoidable during the production of fuel gases such as hydrogen (H) from steam reformation and syngas composed of carbon monoxide (CO) and hydrogen (H). Efficient separation of CO from these gases is highly important to improve the energetic utilization efficiency and prevent poisoning during specific applications. Metal-organic frameworks (MOFs), featuring ordered porous frameworks, high surface areas and tunable pore structures, are emerging porous materials utilized as solid adsorbents for efficient CO capture and separation. Furthermore, the construction of hierarchical MOFs with micropores and mesopores could further promote the dynamic separation processes, accelerating the diffusion of gas flow and exposing more adsorptive pore surface. Herein, we report a simple, efficient, one-pot template-mediated strategy to fabricate a hierarchically porous CuBTC (CuBTC-Water, BTC = 1,3,5-benzenetricarboxylate) for CO separation, which demonstrates abundant mesopores and the superb dynamic separation ability of CO/N. Therefore, CuBTC-Water demonstrated a CO uptake of 180.529 cm g at 273 K and 1 bar, and 94.147 cm g at 298 K and 1 bar, with selectivity for CO/N mixtures as high as 56.547 at 273 K, much higher than microporous CuBTC. This work opens up a novel avenue to facilely fabricate hierarchically porous MOFs through one-pot synthesis for efficient dynamic CO separation.
在通过蒸汽重整生产氢气(H)以及由一氧化碳(CO)和氢气(H)组成的合成气等燃料气体的过程中,二氧化碳(CO)通常是不可避免的。从这些气体中高效分离出CO对于提高能量利用效率以及防止在特定应用过程中发生中毒现象极为重要。金属有机框架材料(MOFs)具有有序的多孔框架、高比表面积和可调节的孔结构,是作为高效CO捕获和分离的固体吸附剂而出现的多孔材料。此外,构建具有微孔和介孔的分级MOFs可以进一步促进动态分离过程,加速气流扩散并暴露出更多的吸附孔表面。在此,我们报道了一种简单、高效的一锅法模板介导策略,用于制备用于CO分离的分级多孔CuBTC(CuBTC - 水,BTC = 1,3,5 - 苯三甲酸酯),该材料展示出丰富的介孔以及出色的CO/N动态分离能力。因此,CuBTC - 水在273 K和1 bar下的CO吸附量为180.529 cm³/g,在298 K和1 bar下为94.147 cm³/g,在273 K下对CO/N混合物的选择性高达56.547,远高于微孔CuBTC。这项工作为通过一锅法合成简便地制备分级多孔MOFs以实现高效动态CO分离开辟了一条新途径。