The charge redistribution strategy driven by heteroatom doping or defect engineering has been developed as an efficient method to endowinert carbon with significant oxygen reduction reaction (ORR) activity.T he synergetic effect between the two approaches is thus expected to be more effective for manipulating the charge distribution of carbon materials for exceptional ORR performance.Herein we report an ovel molecular design strategy to achieve a2 Dp orous turbostratic carbon nanomesh with abundant N-doped carbon defects (NDC). The molecular level integration of aromatic rings as the carbon source and urea units as the Ns ource and sacrificial template into the novel precursor of polyurea (PU) promises the formation of abundant carbon edge defects and N doping sites.Aspecial active site-a carbon edge defect doped with agraphitic valley Natom-was revealed to be responsible for the exceptional ORR performance of NDC material.
With the advantages of low cost, non-pollution, and strong controllability over composition, morphology, nanostructures, as well as surface characters, carbon-based nanomaterials are regarded as ideal substitutes of traditional platinum-based catalysts for oxygen reduction reaction (ORR) electrocatalysis in ORR-involved devices. Herein, an in situ ZnO activation-coupled electrospinning strategy was employed to facilely construct nitrogen-doped porous carbon nanofibers (NPCNF) for flexible Zn−air batteries. In situ formation and thermal removal of ZnO make a critical difference in construction of micro/meso-hierarchically porous structures as well as highly active N-doped sites, therefore generating self-standing carbon nanofibers with high nitrogen doping content as well as specific Brunauer− Emmett−Teller of 501 m 2 /g and 5.6 at. %. As a result, the prepared NPCNF as a self-standing electrode delivers an excellent performance both in alkaline liquid-state and quasi-solid-state Zn−air batteries, giving the possibility of applications in flexible devices.
Lithium‐sulfur batteries have been considered as potential electrochemical energy‐storage devices owing to their satisfactory theoretical energy density. Nonetheless, the inferior conversion efficiency of polysulfides in essence leads to fast capacity decay during the discharge/charge cycle. In this work, it is successfully demonstrated that the conversion efficiency of lithium polysulfides is remarkably enhanced by employing a well‐distributed atomic‐scale Fe‐based catalyst immobilized on nitrogen‐doped graphene (Fe@NG) as a coating of separator in lithium‐sulfur batteries. The quantitative electrocatalytic efficiency of the conversion of lithium polysulfides is determined through cyclic voltammetry. It is also proven that the Fe‐NX configuration with highly catalytic activity is quite beneficial for the conversion of lithium polysulfides. In addition, the adsorption and permeation experiments distinctly indicate that the strong anchoring effect, originated from the charge redistribution of N doping into the graphene matrix, inhibits the movement of lithium polysulfides. Thanks to these advantages, if the as‐prepared Fe@NG catalyst is combined with polypropylene and applied as a separator (Fe@NG/PP) in Li‐S batteries, a high initial capacity (1616 mA h g−1 at 0.1 C), excellent capacity retention (93 % at 0.2 C, 70 % at 2 C), and superb rate performance (820 mA h g−1 at 2 C) are achieved.
A novel transformation strategy assisted with ammonia treatment was successfully developed to fabricate ZIF-8-derived nitrogen-doped hierarchically porous carbon (NHPC/NH3).
The charge redistribution strategy driven by heteroatom doping or defect engineering has been developed as an efficient method to endow inert carbon with significant oxygen reduction reaction (ORR) activity. The synergetic effect between the two approaches is thus expected to be more effective for manipulating the charge distribution of carbon materials for exceptional ORR performance. Herein we report a novel molecular design strategy to achieve a 2D porous turbostratic carbon nanomesh with abundant N‐doped carbon defects (NDC). The molecular level integration of aromatic rings as the carbon source and urea units as the N source and sacrificial template into the novel precursor of polyurea (PU) promises the formation of abundant carbon edge defects and N doping sites. A special active site—a carbon edge defect doped with a graphitic valley N atom—was revealed to be responsible for the exceptional ORR performance of NDC material.
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