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  1. Carbon nanocomposites based on transition-metal oxides have been attracting extensive attention as cost-effective catalysts towards the oxygen reduction reaction (ORR). However, the activity remains subpar as compared to state-of-the-art platinum catalysts. One way to enhance the ORR performance is to dope a second metal into the nanocomposite to manipulate the electronic structure and hence the interactions with key reaction intermediates. Herein, dual metal (Ru and Fe) and nitrogen codoped carbon (RuFe-NC) nanocomposites were synthesized by controlled pyrolysis of a Fe–Ru–Fe trinuclear complex along with zeolitic imidazolate framework-8. The obtained porous nanocomposites consisted of Ru-doped Fe 2 O 3 nanoparticles embedded within a carbon scaffold, and exhibited an ORR activity in alkaline media rivaling that of commercial Pt/C, which was also markedly better than those of the monometallic counterparts and nanocomposites prepared with a simple mixture of the individual monometallic compound precursors. Structural characterization suggests that the use of the trinuclear complex facilitated the atomic dispersion of ruthenium within the iron oxide nanoparticles and charge transfer between the metal centers led to a high ORR activity. Results from this study suggest that rational design of heteronuclear complexes may be a unique strategy in the structural engineering of carbon-metal nanocomposites for high-performancemore »electrocatalysis.« less
    Free, publicly-accessible full text available June 6, 2023
  2. Carbon-based nanocomposites have been attracting extensive attention as high-performance catalysts in alkaline media towards the electrochemical reduction of oxygen. Herein, polyacrylonitrile nanoflowers are synthesized via a free-radical polymerization route and used as a structural scaffold and precursor, whereby controlled pyrolysis leads to the ready preparation of carbon nanocomposites (FeNi-NCF) doped with both metal (Fe and Ni) and nonmetal (N) elements. Transmission electron microscopy studies show that the FeNi-NCF composites retain the flower-like morphology, with the metal species atomically dispersed into the flaky carbon petals. Remarkably, despite a similar structure, elemental composition, and total metal content, the FeNi-NCF sample with a high Fe:Ni ratio exhibits an electrocatalytic performance towards oxygen reduction reaction (ORR) in alkaline media that is similar to that by commercial Pt/C, likely due to the Ni to Fe electron transfer that promotes the adsorption and eventual reduction of oxygen, as evidenced in X-ray photoelectron spectroscopic measurements. Results from this study underline the importance of the electronic properties of metal dopants in the manipulation of the ORR activity of carbon nanocomposites.
  3. It is a challenge to selectively hydrogenate 4-nitrostyrene to 4-nitroethylbenzene, due to the similar energy barrier of hydrogenation of the nitro and vinyl groups. Herein, we demonstrate that such selective hydrogenation can be achieved by Pd@Ru core–shell nanocubes that are prepared by epitaxial growth of a face-centered cubic Ru shell on Pd cubes. The core–shell structure of Pd@Ru nanocubes is confirmed by transmission electron microscopy, X-ray diffraction spectroscopy, and elemental mapping measurements. It is found that the electronic structure and hence the catalytic activity of the Pd@Ru nanocubes can be readily modulated by the Ru shell thickness. This is manifested in electrochemical CO stripping measurements where a decrease of CO adsorption energy is observed on Pd@Ru nanocubes with the increase of the Ru shell thickness. Results from this study suggest that deliberate structural engineering can be exploited to prepare bimetallic core–shell nanostructures for highly active and selective hydrogenation of organic molecules with multifunctional moieties.
  4. Zinc-ion battery (ZIB) has been attracting extensive attention due to its high theoretical capacity, high safety, and low cost. However, the exploration of suitable cathode materials to host Zn ions remains a challenge, owing to the strong electrostatic interactions and large steric hindrance effects between Zn ion and host materials. Great efforts have been devoted to the optimization of the structure and electrochemical property of the cathode materials. In this review article, we summarize recent cathode-based strategies to address the issues of performance degradation and structural collapse of electrode materials within the context of microstructure design and ion/charge transport mechanism, and include a perspective to highlight the challenges and promises in the exploitation of cathode materials for further enhancement of the performance of ZIBs.