Abstract
SummaryAs a major greenhouse gas, the continuous increase of carbon dioxide (CO2) in the atmosphere has caused serious environmental problems, although CO2 is also an abundant, inexpensive, and nontoxic carbon source. Here, we use metal-organic framework (MOF) with highly ordered hierarchical structure as adsorbent and catalyst for chemical fixation of CO2 at atmospheric pressure, and the CO2 can be converted to the formate in excellent yields. Meanwhile, we have successfully integrated highly ordered macroporous and mesoporous structures into MOFs, and the macro-, meso-, and microporous structures have all been presented in one framework. Based on the unique hierarchical pores, high surface area (592 m2/g), and high CO2 adsorption capacity (49.51 cm3/g), the ordered macroporous-mesoporous MOFs possess high activity for chemical fixation of CO2 (yield of 77%). These results provide a promising route of chemical CO2 fixation through MOF materials.
Highlights
We introduce the bionics ideas into the traditional preparation methods, imitating the hierarchical structure of biological systems to build hierarchical metal-organic framework (MOF) structures and introducing the fine hierarchical structure of natural biomaterials into the MOFs to prepare a new type of hierarchical MOF materials
Both the macro- and mesoporous templates were assembled into the MOFs at the same time by ethanol evaporation process
The highly ordered macroporous and mesoporous structures could be successfully introduced into the MOF structure to construct a hierarchical structure by using the one-pot method
Summary
From natural zeolite to meso- and macroporous materials, porous materials have been extensively applied in ion exchange (Okada et al, 2015; Li et al, 2018; Qi et al, 2015), separation (Gupta et al, 2017; Chu and Pan, 2012; Dumee et al, 2013), catalysis (An et al, 2014; Sun et al, 2016; Qian et al, 2009), drug delivery (Wang et al, 2017; Shin et al, 2017), and other fields (Kitagawa et al, 2004). MOF is a coordination polymer composed of inorganic metal structural units and organic ligands through covalent or ionic covalent bonds Owing to their unique high specific surface area and adjustable pore structure (Furukawa et al, 2010; Ferey et al, 2005; Aijaz et al, 2014), as well as diverse structure and excellent catalysis performance, MOFs have been widely used as functional materials in the areas of selective catalysis (Liu et al, 2014; Kornienko et al, 2015; Huang et al, 2018; Czaja et al, 2009), gas storage (Ma and Zhou, 2010; Yoon et al, 2013), optoelectronic materials (Chen et al, 2007; Allendorf et al, 2009; Stavila et al, 2014; Choi et al, 2014; Kong et al, 2016; Avci et al, 2018; Guan et al, 2017; Zheng et al, 2017), drug controlled release (Horcajada et al, 2010; Taylor-Pashow et al, 2009; Zheng et al, 2016), and molecular separation (Kang et al, 2014; Zhang et al, 2016; Zheng et al, 2017; Liu et al, 2018).
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