Rational construction of flexible free-standing electrocata-lysts featuring long-lasting durability,high efficiency,and wide temperature tolerance under harsh practical operations are fundamentally significant for commercial zinc-air batteries.Here,3D flexible free-standing bifunctional membrane electrocatalysts composed of covalently cross-linked supramolecu-lar polymer networks with nitrogen-deficient carbon nitride nanotubes are fab-ricated(referred to as PEMAC@NDCN)by a facile self-templated approach.PEMAC@NDCN demonstrates the lowest reversible oxygen bifunctional activ-ity of 0.61 V with exceptional long-lasting durability,which outperforms those of commercial Pt/C and RuO2.Theoretical calculations and control experi-ments reveal the boosted electron transfer,electrolyte mass/ion transports,and abundant active surface site preferences.Moreover,the constructed alkaline Zn-air battery with PEMAC@NDCN air-cathode reveals superb power density,capacity,and discharge-charge cycling stability(over 2160 cycles)compared to the reference Pt/C+RuO2.Solid-state Zn-air batteries enable a high power density of 211 mW cm-2,energy density of 1056 Wh kg-1,stable charge-discharge cycling of 2580 cycles for 50 mA cm-2,and wide temperature tolerance from-40 to 70℃with retention of 86％capacity compared to room-temperature counterparts,illustrating prospects over harsh operations.

Nayantara K.Wagh;Sambhaji S.Shinde;Chi Ho Lee;Sung-Hae Kim;Dong-Hyung Kim;Han-Don Um;Sang Uck Lee;Jung-Ho Lee

Department of Materials Science and Chemical Engineering,Hanyang University,Ansan,Republic of Korea;Department of Applied Chemistry,Center for Bionano Intelligence Education and Research,Hanyang University,Ansan,Republic of Korea;Department of Chemical Engineering,Kangwon National University,Chuncheon,Gangwon 24341,Republic of Korea

纳微快报（英文）

[1]Nayantara K.Wagh;Sambhaji S.Shinde;Chi Ho Lee;Sung-Hae Kim;Dong-Hyung Kim;Han-Don Um;Sang Uck Lee;Jung-Ho Lee-.Supramolecular Polymer Intertwined Free-Standing Bifunctional Membrane Catalysts for All-Temperature Flexible Zn-Air Batteries)[J].纳微快报（英文）,2022(11):341-360

Intertwined,supramolecu,PEMAC,NDCN,C+RuO2

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