Synthesis and Electrochemical Performance of Microporous Carbon Using a Zinc(II)-Organic Coordination Polymer
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Microporous carbon was prepared using a novel procedure based on a zinc(Ⅱ)-organic coordination polymer. The polymer was prepared through the coordination interaction of zinc ions with tartaric acid, and then it was introduced into the open networks of resorcinol/formaldehyde (R/F) resol using hydrogen-bonding interactions. The R/F resol and zinc-organic coordination compound system copolymerized to produce an R/F and zinc-organic coordination copolymer. The copolymer was then heat-treated at 950℃ to decompose and evaporate zinc to fabricate microporous carbon materials. The carbon materials possessed relatively regular large micropores, with a specific surface area of up to 1260 m2·g-1 and a total pore volume of 0.63 cm3 ·g-1 . The resultant microporous carbon materials were used as supercapacitor electrodes, exhibiting an equivalent series resistance of 0.46 Ω, and ideal capacitive behavior with a rectangular shape in cyclic voltammograms. Galvanostatic charge/discharge measurements of the carbon materials gave a specific capacitance of 196 F ·g-1 at a current density of 1A·g-1 and 137F·g-1 at a large current density of 10A·g-1 . A high retention of 98% was measured for the long-term cycling stability (～1000 cycles) of the mesoporous carbon. Overall, the microporous carbon materials exhibited very good electrochemical performance. This study highlights the potential of well-designed microporous carbon materials as electrodes for diverse supercapacitor applications.Keywords:
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Abstract A highly effective and facile synthesis route is developed to create and tailor metal‐decorated and nitrogen‐functionalized active microporous carbon materials from ZIF‐8. Clear metal‐ and pyrrolic‐N‐induced enhancements of the cyclic CO 2 uptake capacities and binding energies are achieved, particularly at a much lower carbonization temperature of 700 °C than those often reported (1000 °C). The high‐temperature carbonization can enhance the porosity but only at the expense of considerable losses of sample yield and metal and N functional sites. The findings are comparatively discussed with carbons derived from metal–organic frameworks (MOFs) reported previously. Furthermore, the porosity of the MOF‐derived carbon is critically dependent on the structure of the precursor MOF and the crystal growth. The current strategy offers a new and effective route for the creation and tuning of highly active and functionalized carbon structures in high yields and with low energy consumption.
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Metal–organic frameworks (MOFs) have been used as templates to synthesize a variety of functional materials. Pyrolysis of Zn-MOFs typically yields materials that retain the high surface area of the parent MOF while imparting mesoporosity due to carbothermal reduction and Zn evaporation. When non-Zn containing MOFs are used, significant loss in surface area and porosity after pyrolysis is observed. To overcome these limitations, a hierarchical microporous/mesoporous analogue of microporous MIL-125 (Ti) was synthesized and subjected to pyrolysis at various temperatures. By varying the pyrolysis temperature, both Ti content and phase in the final materials could be altered. The resulting materials exhibited enhanced mesoporosity and activity as catalysts in the oxidation of dibenzothiophene when compared to pyrolyzed microporous MIL-125. This increased activity was attributed to the greater mesoporosity of the hierarchical materials. This work demonstrated that the properties of MOF-templated materials can be tuned by altering the morphology of the precursor MOF.
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Highly porous carbon nanosheets that are oriented and interlinked are prepared by a one-step KOH activation of polymerized glucose spheres (pGSs) that are hydrothermally derived from glucose at 180 °C yet without carbonization. This is totally unexpected because a spherical microporous carbon is produced by a normally employed two-step process that includes a precarbonization and a successive KOH activation. In our one-step activation, the melt of potassium species directed the formation of oriented carbon nanosheets; the oxygen constituents in the pGSs are critical for the morphological evolution from sphere to sheet. The carbon nanosheets have a large surface area (2633 m2 g–1) and a high pore volume (1.86 cm3 g–1). The oriented structure and hierarchical porosity impose advantages for mass transfer and ion accommodation and give rise to an ultrahigh rate performance (184 F g–1 at 100 A g–1) of the carbon nanosheets in supercapacitors in comparison with the case of microporous carbon spheres (56 F g–1 at 100 A g–1).
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A simple, rapid and versatile method was developed to increase the pore sizes and pore volumes of microporous MOFs (HKUST-1, ZIF-8, ZIF-67, and ZIF-90) by employing organic amine as the template. The resultant hierarchically porous HKUST-1 exhibited significantly enhanced adsorption capacities and faster diffusion rates for CH4 and CO2 gas storage.
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