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Zinc‐Mediated Template Synthesis of Fe‐N‐C Electrocatalysts with Densely Accessible Fe‐N<i><sub>x</sub></i> Active Sites for Efficient Oxygen Reduction

Guangbo Chen, Pan Liu, Zhongquan Liao, Fanfei Sun, Yanghua He, Haixia Zhong, Tao Zhang, Ehrenfried Zschech, Mingwei Chen, Gang Wu, Jian Zhang, Xinliang Feng

2020Advanced Materials428 citationsDOIOpen Access PDF

Abstract

Abstract Owing to their earth abundance, high atom utilization, and excellent activity, single iron atoms dispersed on nitrogen‐doped carbons (Fe‐N‐C) have emerged as appealing alternatives to noble‐metal platinum (Pt) for catalyzing the oxygen reduction reaction (ORR). However, the ORR activity of current Fe‐N‐C is seriously limited by the low density and inferior exposure of active Fe‐N x species. Here, a novel zinc‐mediated template synthesis strategy is demonstrated for constructing densely exposed Fe‐N x moieties on hierarchically porous carbon (SA‐Fe‐NHPC). During the thermal treatment of 2,6‐diaminopyridine/ZnFe/SiO 2 complex, the zinc prevents the formation of iron carbide nanoparticles and the SiO 2 template promotes the generation of hierarchically pores for substantially improving the accessibility of Fe‐N x moieties after subsequent leaching. As a result, the SA‐Fe‐NHPC electrocatalysts exhibit an unprecedentedly high ORR activity with a half‐wave potential ( E 1/2 ) of 0.93 V in a 0.1 m KOH aqueous solution, which outperforms those for Pt/C catalyst and state‐of‐the‐art noble metal‐free electrocatalysts. As the air electrode in zinc–air batteries, the SA‐Fe‐NHPC demonstrates a large peak power density of 266.4 mW cm −2 and superior long‐term stability. Therefore, the developed zinc‐mediated template synthesis strategy for boosting the density and accessibility of Fe‐N x species paves a new avenue toward high‐performance ORR electrocatalysts.

Topics & Concepts

Materials scienceOxygen reductionOxygen reduction reactionReduction (mathematics)ZincOxygenNanotechnologyInorganic chemistryChemical engineeringMetallurgyPhysical chemistryElectrochemistryElectrodeOrganic chemistryChemistryMathematicsEngineeringGeometryElectrocatalysts for Energy ConversionFuel Cells and Related MaterialsAdvanced battery technologies research
Zinc‐Mediated Template Synthesis of Fe‐N‐C Electrocatalysts with Densely Accessible Fe‐N<i><sub>x</sub></i> Active Sites for Efficient Oxygen Reduction | Litcius