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      • Fe, N, S-codoped carbon frameworks derived from nanocrystal superlattices towards enhanced oxygen reduction activity

        Angang Dong,Wenqian Han,Yuchi Yang,Baixu Zhu,Biwei Wang,Jinxiang Zou 나노기술연구협의회 2019 Nano Convergence Vol.6 No.4

        Recently, iron, nitrogen and sulfur codoped carbon-based materials have gained increasing attention for their synergistic effect towards superior electrocatalytic oxygen reduction performance. To gain insight into the contributions of the heteroatoms, we developed a facile and reproducible method for constructing Fe, N, S-codoped carbon frameworks derived from self-assembled Fe3O4 nanocrystal superlattices. The material constructed by the suggested method exhibited excellent ORR activity with more positive half-wave potential (∼ 0.869 V, vs RHE), higher diffusion-limiting current density (∼ 5.88 mA/cm2) and smaller Tafel slope (45 mV/dec) compared with Fe, N-codoped carbon frameworks and Pt/C. Notably, Fe3O4 nanocrystals served as both the building blocks for constructing carbon frameworks and the source of Fe residues leaving in the frameworks at the same time. By artificially tailoring the doping type and level as well as the homogeneousness of heteroatoms, the results discussed herein prove the importance of each kind of heteroatom in boosting ORR activity.

      • Stabilization of Battery Electrode/Electrolyte Interfaces Employing Nanocrystals with Passivating Epitaxial Shells

        Kim, Chunjoong,Phillips, Patrick J.,Xu, Linping,Dong, Angang,Buonsanti, Raffaella,Klie, Robert F.,Cabana, Jordi American Chemical Society 2015 Chemistry of materials Vol.27 No.1

        <P>Chemical degradation at electrode/electrolyte interfaces in high-energy storage devices, such as Li-ion batteries, imposes durability challenges that affect their life and cost. In oxide electrodes, degradation is linked to the presence of redox active transition metals at the surface. Here, we demonstrate a strategy toward the stabilization of interfaces using core–epitaxial shell nanocrystals. The core of the nanocrystal is composed of an electroactive oxide, which is passivated by an ultrathin epitaxial oxide shell enriched in a redox inactive ion. This approach imparts interfacial stability while preserving the high storage capability and fast carrier transport of the material, compared to unmodified versions. The validity of the concept is proved with Li<SUB>1+<I>x</I></SUB>Mn<SUB>2–<I>x</I></SUB>O<SUB>4</SUB> nanocrystals with a 1–2 nm Al-rich shell, which showed reduced sensitivity to harsh environments, compared to bare counterparts. The approach is generalizable to any transition-metal-based battery system where electrode–electrolyte interactions must be controlled.</P><P><B>Graphic Abstract</B> <IMG SRC='http://pubs.acs.org/appl/literatum/publisher/achs/journals/content/cmatex/2015/cmatex.2015.27.issue-1/cm503615w/production/images/medium/cm-2014-03615w_0006.gif'></P><P><A href='http://pubs.acs.org/doi/suppl/10.1021/cm503615w'>ACS Electronic Supporting Info</A></P>

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