Inherent mass transfer engineering of a Co, N co-doped carbon material towards oxygen reduction reaction
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Abstract Dual‐metal center catalysts (DMCs) have shown the ability to enhance the oxygen reduction reaction (ORR) owing to their distinctive structural configurations. However, the precise modulation of electronic structure and the in‐depth understanding of synergistic mechanisms between dual metal sites of DMCs at the atomic level remain challenging. Herein, mimicking the ferredoxin, Fe‐based DMCs (Fe 2 N 6 ‐S) are strategically designed and fabricated, in which additional Fe and S sites are synchronously installed near the Fe sites and serve as “dual modulators” for coarse‐ and fine‐tuning of the electronic modulation, respectively. The as‐prepared Fe 2 N 6 ‐S catalyst exhibits enhanced ORR activity and outstanding Zinc‐air (Zn–air) battery performance compared to the conventional single Fe site catalysts. The theoretical and experimental results reveal that introducing the second metal Fe creates a dual adsorption site that alters the O 2 adsorption configuration and effectively activates the O─O bond, while the synergistic effect of dual Fe sites results in the downward shift of the d‐band center, facilitating the release of OH*. Additionally, local electronic engineering of heteroatom S for Fe sites further facilitates the formation of the rate‐determining step OOH*, thus accelerating the reaction kinetics.
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Oxygenophilic ionic liquids promote the oxygen reduction reaction in Pt-free carbon electrocatalysts
We propose a novel idea to improve the surface properties of carbon-based Pt-free electrocatalysts in Polymer Electrolyte Membrane Fuel Cells (PEMFCs) and Alkaline Fuel Cells (AFCs).
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A comprehensive review on the active sites of doped graphene and the mechanism of their oxygen reduction reaction (ORR) with a summary of the feasible approaches for further improvement of their ORR activities.
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The hollow PtxNi1−x/C nanocrystallites are capable of fulfilling cost, electrocatalytic performance, and durability requirements of proton-exchange membrane fuel cell applications.
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A synergetic catalytic system was built based on Pt NPs and atomic Ni–N–C joint active sites for better ORR electrocatalysis.
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Recent developments of hollow carbon sphere-based materials as efficient electrocatalysts for the oxygen reduction reaction (ORR) are summarized, particularly focusing on surface and interface engineering strategies that greatly enhance ORR performance.
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Polymer electrolyte membrane fuel cells represent a next-generation power supply technology that may be used in a diverse range of applications. Towards this end, the rational design and engineering of functional nanomaterials as low-cost, high-performance catalysts is of critical significance in the wide-spread commercialization of fuel cell technology. One major bottleneck is the oxygen reduction reaction (ORR) at the cathode. Whereas platinum-based nanoparticles have been used as the catalysts of choice, further engineering of the nanoparticles is urgently needed to enhance the catalytic performance and concurrently reduce the costs. Extensive research has also been extended to non-platinum metals or even metal-free nanocatalysts that may be viable alternatives to platinum. In this review article, we will summarize recent progress in these areas of research within the context of interfacial electron transfer: (a) interactions between metal elements in alloy nanoparticles, (b) metal-ligand interfacial bonding interactions, (c) metal-carbon substrate interactions, and (d) heteroatom doping of graphitic carbons. Results have shown that ready manipulation of the electronic interactions between the catalyst surface and oxygen species may serve as a fundamental mechanism for the optimization of the catalytic performance.
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Oxygen reduction reaction-favoring PtPdAg hollow nanoparticle, nanodimer and nanowire catalysts are synthesized, all of which have been demonstrated to be promoting factors for the ORR. PtPdAg/C nanodimers exhibit excellent performance for the ORR with the highest mass activity.
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