Spinel oxide nanoparticles embedded in nitrogen-doped carbon nanofibers as a robust and self-standing bifunctional oxygen cathode for Zn–air batteries

Author(s): Xiang Chen ¹ ^, ² ^, ³ ^, ⁴ ^, ⁵ , Zhenhua Yan ¹ ^, ² ^, ³ ^, ⁴ ^, ⁵ , Meng Yu ¹ ^, ² ^, ³ ^, ⁴ ^, ⁵ , Hongming Sun ¹ ^, ² ^, ³ ^, ⁴ ^, ⁵ , Fangming Liu ¹ ^, ² ^, ³ ^, ⁴ ^, ⁵ , Qiyuan Zhang ¹ ^, ² ^, ³ ^, ⁴ ^, ⁵ , Fangyi Cheng ¹ ^, ² ^, ³ ^, ⁴ ^, ⁵ , Jun Chen ¹ ^, ² ^, ³ ^, ⁴ ^, ⁵

Publication date (Electronic): 2019

Journal: Journal of Materials Chemistry A

Publisher: Royal Society of Chemistry (RSC)

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Abstract

Self-standing nitrogen-doped carbon nanofibers with homogeneously embedded CoMn ₂O ₄ nanoparticles exhibit superior oxygen reduction/evolution catalytic activity and stability for metal–air batteries.

Abstract

Rechargeable metal–air batteries require nonprecious, efficient, and durable bifunctional electrodes for catalyzing the oxygen reduction/evolution reaction (ORR/OER). Here, we report a facile, scalable synthesis of a self-standing bifunctional electrode with CoMn ₂O ₄ (CMO) in situ embedded in nitrogen-doped carbon nanofibers (NCNFs) by electrospinning. Strong coupling between CMO and NCNFs facilitates the multiphase charge transport process. Meanwhile, the conductive carbonaceous network contributes to the overall stability by protecting CMO from corrosion and aggregation. As a result, the nanocomposite exhibits remarkable Pt-like ORR activity (onset/half-wave potential of 1.05/0.83 V) and high OER activity (overpotential of 340 mV at 10 mA cm ⁻²). The rechargeable Zn–air battery assembled with CMO/NCNF delivers a peak power density of 224 mW cm ⁻² and a low charge–discharge voltage gap of 0.85 V even after 350 cycles at 10 mA cm ⁻². Furthermore, the assembled bendable solid-state Zn–air battery shows rechargeability, suggesting the promising potential of spinel/carbon hybrids in flexible devices.

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Minhua Shao, Qiaowan Chang, Jean-Pol Dodelet … (2016)

The recent advances in electrocatalysis for oxygen reduction reaction (ORR) for proton exchange membrane fuel cells (PEMFCs) are thoroughly reviewed. This comprehensive Review focuses on the low- and non-platinum electrocatalysts including advanced platinum alloys, core-shell structures, palladium-based catalysts, metal oxides and chalcogenides, carbon-based non-noble metal catalysts, and metal-free catalysts. The recent development of ORR electrocatalysts with novel structures and compositions is highlighted. The understandings of the correlation between the activity and the shape, size, composition, and synthesis method are summarized. For the carbon-based materials, their performance and stability in fuel cells and comparisons with those of platinum are documented. The research directions as well as perspectives on the further development of more active and less expensive electrocatalysts are provided.

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A metal-free bifunctional electrocatalyst for oxygen reduction and oxygen evolution reactions.

Jintao Zhang, Zhenghang Zhao, Zhenhai Xia … (2015)

The oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) are traditionally carried out with noble metals (such as Pt) and metal oxides (such as RuO₂ and MnO₂) as catalysts, respectively. However, these metal-based catalysts often suffer from multiple disadvantages, including high cost, low selectivity, poor stability and detrimental environmental effects. Here, we describe a mesoporous carbon foam co-doped with nitrogen and phosphorus that has a large surface area of ∼1,663 m(2) g(-1) and good electrocatalytic properties for both ORR and OER. This material was fabricated using a scalable, one-step process involving the pyrolysis of a polyaniline aerogel synthesized in the presence of phytic acid. We then tested the suitability of this N,P-doped carbon foam as an air electrode for primary and rechargeable Zn-air batteries. Primary batteries demonstrated an open-circuit potential of 1.48 V, a specific capacity of 735 mAh gZn(-1) (corresponding to an energy density of 835 Wh kgZn(-1)), a peak power density of 55 mW cm(-2), and stable operation for 240 h after mechanical recharging. Two-electrode rechargeable batteries could be cycled stably for 180 cycles at 2 mA cm(-2). We also examine the activity of our carbon foam for both OER and ORR independently, in a three-electrode configuration, and discuss ways in which the Zn-air battery can be further improved. Finally, our density functional theory calculations reveal that the N,P co-doping and graphene edge effects are essential for the bifunctional electrocatalytic activity of our material.