Lithium-sulfur (Li-S) batteries have been identified as the greatest potential next- generation energy-storage systems because of the large theoretical energy density of 2600 Wh kg−1. However, its practical application on a massive scale is impeded by severe capacity loss resulted from the notorious polysulfides shuttle. Here, we first present a novel technique to synthesize sandwich-type nitrogen and sulfur codoped graphene-backboned porous carbon (NSGPC) to modify the commercial polypropylene separator in Li-S batteries. The as-synthesized NSGPC exhibits a unique micro/mesoporous carbon framework, large specific surface area (2439.0 m2 g−1), high pore volume (1.78 cm3 g−1), good conductivity, and in situ nitrogen (1.86 at %) and sulfur (5.26 at %) co-doping. Benefiting from the particular physical properties and chemical components of NSGPC, the resultant NSGPC-coated separator not only can facilitate rapid Li+ ions and electrons transfer, but also can restrict the dissolution of polysulfides to alleviate the shuttle effect by combining the physical absorption and strong chemical adsorption. As a result, Li-S batteries with NSGPC-coated separator exhibit high initial reversible capacity (1208.6 mAh g−1 at 0.2 C), excellent rate capability (596.6 mAh g−1 at 5 C), and superior cycling stability (over 500 cycles at 2 C with 0.074% capacity decay each cycle). Propelling our easy-designed pure sulfur cathode to a extremely increased mass loading of 3.4 mg cm−2 (70 wt. % sulfur), the Li-S batteries with this functional composite separator exhibit a superior high initial capacity of 1171.7 mAh g−1, which is quite beneficial to commercialized applications.
Recently, lithium-sulfur (Li-S) batteries have been greeted by a huge ovation owing to their very high theoretical specific capacity (1675 mAh·g−1) and theoretical energy density (2600 Wh·kg−1). However, the full commercialization of Li-S batteries is still hindered by dramatic capacity fading resulting from the notorious “shuttle effect” of polysulfides. Herein, we first describe the development of a facile, inexpensive, and high-producing strategy for the fabrication of N-, O-, and S-tri-doped porous carbon (NOSPC) via pyrolysis of natural wheat straw, followed by KOH activation. The as-obtained NOSPC shows characteristic features of a highly porous carbon frame, ultrahigh specific surface area (3101.8 m2·g−1), large pore volume (1.92 cm3·g−1), good electrical conductivity, and in situ nitrogen (1.36 at %), oxygen (7.43 at %), and sulfur (0.7 at %) tri-doping. The NOSPC is afterwards selected to fabricate the NOSPC-sulfur (NOSPC/S) composite for the Li-S batteries cathode material. The as-prepared NOSPC/S cathode delivers a large initial discharge capacity (1049.2 mAh·g−1 at 0.2 C), good cycling stability (retains a reversible capacity of 454.7 mAh·g−1 over 500 cycles at 1 C with a low capacity decay of 0.088% per cycle), and superior rate performance (619.2 mAh·g−1 at 2 C). The excellent electrochemical performance is mainly attributed to the synergistic effects of structural restriction and multidimensional chemical adsorptions for cooperatively repressing the polysulfides shuttle.
Pore is the main adsorption and desorption space of coalbed methane (CBM). Pore size configuration and connectivity affect the adsorption/desorption hysteresis effect. Using tectonically deformed coal (TDC) and original structure coal of medium- and high-rank coal as the research objects, through the N2/CO2 adsorption experiment to analyze the pore size distribution and connectivity of different scales. We investigate the control mechanism of heterogeneous evolution in the key pore scales against adsorption/desorption hysteresis characteristics during coal metamorphism and deformation by combining the CH4 isothermal adsorption/desorption experiment under 30°C equilibrium moisture. The findings indicate that the super micropores (<2 nm) are mainly combination ink bottle-shaped pores and have worse connectivity as the degree of metamorphism and deformation increases. The super micropores occupy the vast majority of pore volume and specific surface area; its pore size distribution curve change presents an “M” bimodal type and is mainly concentrated in two pore segments of 0.45–0.70 nm and 0.70–0.90 nm. The effect of ductile deformation exerts a significantly greater effect on super micropores than brittle deformation. The exhibited adsorption–desorption characteristics are the result of the combined effect of the unique pore structure of the TDCs and different moisture contents. The presence of a large number of super micropores is the most important factor influencing the degree of gas desorption hysteresis. The “ink-bottle effect” is the primary cause of gas desorption hysteresis. For CBM development, some novel methods to increase desorption and diffusion rate at the super micropores scale should be considered.
We selected, as the objects of our research, lignite from the Beizao Mine, gas coal from the Caiyuan Mine, coking coal from the Xiqu Mine, and anthracite from the Guhanshan Mine. We used the mercury intrusion method and the low-temperature liquid nitrogen adsorption method to analyze the structure and shape of the coal pores and calculated the fractal dimensions of different aperture segments in the coal. The experimental results show that the fractal dimension of the aperture segment of lignite, gas coal, and coking coal with an aperture of greater than or equal to 10 nm, as well as the fractal dimension of the aperture segment of anthracite with an aperture of greater than or equal to 100 nm, can be calculated using the mercury intrusion method; the fractal dimension of the coal pore, with an aperture range between 2.03 nm and 361.14 nm, can be calculated using the liquid nitrogen adsorption method, of which the fractal dimensions bounded by apertures of 10 nm and 100 nm are different. Based on these findings, we defined and calculated the comprehensive fractal dimensions of the coal pores and achieved the unity of fractal dimensions for full apertures of coal pores, thereby facilitating, overall characterization for the heterogeneity of the coal pore structure.
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