【摘 要】
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The search for non-precious and efficient electrocatalysts towards the oxygen evolution reaction (OER) is of vital importance for the future advancement of multifarious renewable energy conversion/storage technologies.Electronic modulation via heteroatom
【机 构】
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School of Chemistry and Chemical Engineering,Southeast University,Jiangsu Optoelectronic Functional
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The search for non-precious and efficient electrocatalysts towards the oxygen evolution reaction (OER) is of vital importance for the future advancement of multifarious renewable energy conversion/storage technologies.Electronic modulation via heteroatom doping is recognized as one of the most forceful leverages to enhance the electrocatalytic activity.Herein,we demonstrate a delicate strategy for the in-situ confinement of S-doped NiO nanoparticles into N-doped carbon nanotube/nanofiber-coupled hier-archical branched superstructures (labeled as S-NiO@N-C NT/NFs).The developed strategy simultane-ously combines enhanced thermodynamics via electronic regulation with accelerated kinetics via nanoarchitectonics.The S-doping into NiO lattice and the 1 D/1 D-integrated hierarchical branched carbon substrate confer the resultant S-NiO@N-C NT/NFs with regulated electronic configuration,enriched oxy-gen vacancies,convenient mass diffusion pathways and superior architectural robustness.Thereby,the S-NiO@N-C NT/NFs display outstanding OER properties with an overpotential of 277 mV at 10 mA cm-2 and impressive long-term durability in KOH medium.Density functional theory (DFT) calculations further corroborate that introducing S-dopant significantly enhances the interaction with key oxygenate inter-mediates and narrow the band gap.More encouragingly,a rechargeable Zn-air battery using an air-cath-ode of Pt/C + S-NiO@N-C NT/NFs exhibits a lower charge voltage and preferable cycling stability in comparison with the commercial Pt/C + RuO2 counterpart.This study highlighting the concurrent consid-eration of electronic regulation,architectural design and nanocarbon hybridization may shed light on the future exploration of economical and efficient electrocatalysts.
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