Hydrogen sulfide (H2S) is an industrial exhausted gas that is highly toxic to humans and the environment. Combining desulfurization and fabrication of cathode materials for lithium–sulfur batteries (LSBs) can solve this issue with a double benefit. Herein, the amino-functionalized lotus root-like carbon nanofibers (NH2-PLCNFs) are prepared by the amination of electrospinning carbon nanofibers under dielectric barrier discharge plasma. Selective catalytic oxidation of H2S to elemental sulfur (S) is achieved over the metal-free NH2-PLCNFs catalyst, and the obtained composite S@NH2-PLCNFs is further used as cathode in LSBs. NH2-PLCNFs enable efficient desulfurization (removal capacity as high as 3.46 g H2S g−1 catalyst) and strongly covalent stabilization of S on modified carbon nanofibers. LSBs equipped with S@NH2-PLCNFs deliver a high specific capacity of 705.8 mA h g−1 at 1 C after 1000 cycles based on the spatial confinement and the covalent stabilization of electroactive materials on amino-functionalized porous carbon matrix. It is revealed that S@NH2-PLCNFs obtained by this kind of chemical vapor deposition leads to a more homogeneous S distribution and superior electrochemical performance to the sample S/NH2-PLCNF-M prepared by the traditional molten infusion. This work opens a new avenue for the combination of environment protection and energy storage.
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Amorphous carbon derived from biomass unusually combines the merits of large specific surface area and abundant micropores, offering massive anchoring points for ion adsorption in electrolyte. Nevertheless, the short-range ordered structure in amorphous carbon hinders the fast electron transfer. Conversely, graphitic carbon with long-range ordered structure is beneficial for electron transfer. Thus, a low-cost strategy is required to marry hierarchical porous structure with long-range ordered structure, resulting in a long/short-range interconnected porous carbon and then leading to fast ion and electron transfer. Herein, we modified the solid-phase conversion process of biomass by employing the features of liquid-phase carbonization for petroleum asphalt. With the assistance of asphalt, the large specific surface area (> 2,000 m2·g-1), high ratio of mesopores (ca. 60%) together with long-range ordered structure are in-situ created in as-made porous carbon. Thanks to the well configured structure in small scale, the as-made co-converted carbon can be operated in high-viscosity EMIMBF4 electrolyte with a superior capacitance (315 F·g-1@1 A·g-1). Besides, the as-assembled symmetric supercapacitor can deliver a super-high specific energy of 174 Wh·kg-1@2.0 kW·kg-1. This work provides a new version for designing highly porous biomass-derived carbon with long/short-range alternating structure at molecular level.
An anti-oxidized NiS2 electrocatalyst with improved catalytic activity was developed using a Fe-induced conversion strategy. X-ray photoelectron spectroscopy reveals that betatopic Ni species with high valence states are present within the Fe-NiS2 matrix and relatively less oxidized layers exist on the catalyst's surface, indicating its greatly enhanced anti-oxidized capability. Density functional theory calculations reveal that the Ni and Fe sites on the Fe-NiS2 catalyst surface possess strong adsorption capacity toward hydroxyl ions compared with the Ni sites on NiS2. Benefiting from its unique microstructure and modulated electronic structure due to the effects of iron species, the Fe-NiS2 catalyst prepared on carbon fiber delivers a remarkably enhanced catalytic activity and superior long-life durability for overall water splitting. The present results provide an efficient strategy for the design and configuration of anti-oxidation catalysts, especially for energy storage and catalysis.
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