Qingzhong Xue

Critical role of small micropores in high CO2 uptake

Microporous carbon materials with extremely small pore size are prepared by employing polyaniline as a carbon precursor and KOH as an activating agent. CO(2) sorption performance of the materials is systematically investigated at the temperatures of 0, 25 and 75 °C. The prepared carbons show very high CO(2) uptake of up to 1.86 and 1.39 mmol g(-1) under 1 bar, 75 °C and 0.15 bar, 25 °C, respectively. These values are amongst the highest CO(2) capture amounts of the known carbon materials. The relation between CO(2) uptake and pore size at different temperatures is studied. An interesting and innovative point that the micropores with pore size smaller than a critical value play a crucial role in CO(2) adsorption at different temperatures is demonstrated. It is found that the higher the sorption temperature is, the smaller this critical value of pore size is. Pores smaller than 0.54 nm are manifested to determine CO(2) capture capacity at high sorption temperature, e.g. 75 °C. This research proposes a basic principle for designing highly efficient CO(2) carbon adsorbents; that is, the adsorbents should be primarily rich in extremely small micropores.

On the origin of the high capacitance of carbon derived from seaweed with an apparently low surface area

Low surface area carbon materials, derived from pyrolyzing biomass or polymers, often possess high areal capacitances. However, the well-accepted pseudocapacitance introduced by heteroatoms could not explain this phenomenon without doubt. In order to explore the nature of the energy storage mechanism in these low surface area carbon materials, we prepared a series of laver-based carbon materials by regulating the heteroatom contents and investigated their electrochemical performance. Combining the results of advanced pore structure analyses and electrochemical measurements, we disclose that the presence of ultramicropores, which could not be probed by adsorbates such as nitrogen gas or argon, but are accessible to carbon dioxide or electrolyte ions, plays a most dominant role in the high capacitance of low surface area carbon materials. In this contribution, the previously accepted viewpoint that the capacitance is mainly derived from heteroatoms undergoing Faradaic reactions is challenged.

Oxygen-containing functional group-facilitated CO2 capture by carbide-derived carbons

A series of carbide-derived carbons (CDCs) with different surface oxygen contents were prepared from TiC powder by chlorination and followed by HNO3 oxidation. The CDCs were characterized systematically by a variety of means such as Fourier transform infrared spectroscopy, X-ray photoelectron spectroscopy, ultimate analysis, energy dispersive spectroscopy, N2 adsorption, and transmission electron microscopy. CO2 adsorption measurements showed that the oxidation process led to an increase in CO2 adsorption capacity of the porous carbons. Structural characterizations indicated that the adsorbability of the CDCs is not directly associated with its microporosity and specific surface area. As evidenced by elemental analysis, X-ray photoelectron spectroscopy, and energy dispersive spectroscopy, the adsorbability of the CDCs has a linear correlation with their surface oxygen content. The adsorption mechanism was studied using quantum chemical calculation. It is found that the introduction of O atoms into the carbon surface facilitates the hydrogen bonding interactions between the carbon surface and CO2 molecules. This new finding demonstrated that not only the basic N-containing groups but also the acidic O-containing groups can enhance the CO2 adsorbability of porous carbon, thus providing a new approach to design porous materials with superior CO2 adsorption capacity.