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Robust Electronic Correlation of Co-CoN_4 Hybrid Active Sites for Durable Rechargeable Zn-Air Batteries

机译:Robust Electronic Correlation of Co-CoN_4 Hybrid Active Sites for Durable Rechargeable Zn-Air Batteries

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摘要

The rational design of bifunctional catalysts with excellent activity and stabilitytoward the oxygen evolution reaction (OER) and oxygen reduction reaction(ORR) is essential for rechargeable Zn-air batteries (ZABs). In this study, a facilecoordination bridging strategy is proposed to construct bifunctional Co-CoN_4hybrid active sites embedded in porous N-rich carbon nanolamellas (denotedas Co-CoN_4@NCNs) for both the ORR and OER. Synchrotron X-ray absorptionspectroscopy and density functional theory calculations reveal that the increasedintrinsic ORR/OER activities can be attributed to the efficient interfacial chargetransfer between the atomic CoN sites and metallic Co sites due to theirrobust electronic correlation. In situ Raman spectroscopy confirms that theOER activity depends on the CoOOH intermediates formed during the reaction.Co-CoN4@NCNs exhibits superior bifunctional catalytic performance for theORR (E_(1/2) = 0.83 V) and OER (η = 310 mV at 10 mA cm~(?2)) conducted in alkalinemedia. The assembled rechargeable Co-CoN4@NCNs-based ZAB displays anopen-circuit voltage of 1.47 V, peak power density of 118.8 mW cm~(?2), specificcapacity of 776.7 mAh g~(?1), and outstanding cycling stability over 1500 cycles. Theregulation of the interfacial electronic properties can contribute to the rationaldesign of bifunctional electrocatalysts used in rechargeable metal-air batteries.

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