Consolidating the Oxygen Reduction with Sub-Polarized Graphitic Fe–N4 Atomic Sites for an Efficient Flexible Zinc–Air Battery

IF 9.6 1区材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Nano Letters Pub Date : 2024-11-07 DOI:10.1021/acs.nanolett.4c03665

Wenfang Zhai, Jialei Li, Yahui Tian, Hang Liu, Yaoda Liu, Zhixin Guo, Thangavel Sakthivel, Licheng Bai, Xue-Feng Yu, Zhengfei Dai

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Abstract

The effectuation of the Zn–air battery (ZAB) is appealing for active and durable catalysts to kinetically drive the sluggish cathodic oxygen reduction reaction (ORR). Atomic metal-N_x-C sites are widely witnessed with Pt-like activity, but their demetalations still severely restrict the durability in ORR. Here we have profiled an ordered hierarchical porous carbon supported Fe–N₄ single-atom (FeNC) catalyst by a template derivation method for efficient ORR and flexible ZAB studies. The FeNC structure is observed with a sub-polarized graphitic Fe–N₄ coordination with a shortened Fe–N bond for potentially consolidating the ORR, together with the hierarchical porous matrix for kinetical mass transfer. Resultantly, the optimized FeNC catalyst showcases Pt-beyond alkaline ORR activity (E_1/2 = 0.95 V) with long-term durability for 100 h, delivering the flexible ZAB device with high power density (251 mW cm^–2) and durable cycle life (80 h). This research underscores the criterion in rationalizing active and robust ORR catalysts through metal–nitrogen bond modulation.

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将氧还原与次极化石墨化 Fe-N4 原子位点相结合，制造高效柔性锌-空气电池

锌-空气电池（ZAB）的实现需要活性持久的催化剂来驱动缓慢的阴极氧还原反应（ORR）。原子金属-Nx-C 位点具有类似铂的活性，但它们的脱金属性仍然严重限制了 ORR 的耐久性。在此，我们采用模板推导法研究了一种有序分层多孔碳支撑的 Fe-N4 单原子（FeNC）催化剂，用于高效 ORR 和灵活的 ZAB 研究。通过观察发现，FeNC 结构具有亚极化石墨化的 Fe-N4 配位，Fe-N 键缩短，有可能巩固 ORR，而分层多孔基质则可实现动力学传质。因此，优化后的 FeNC 催化剂具有超越铂的碱性 ORR 活性（E1/2 = 0.95 V）和 100 小时的长期耐久性，可提供具有高功率密度（251 mW cm-2）和持久循环寿命（80 小时）的灵活 ZAB 器件。这项研究强调了通过金属-氮键调制实现活性和稳健 ORR 催化剂的合理化标准。

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来源期刊

Nano Letters 工程技术-材料科学：综合

CiteScore

16.80

自引率

2.80%

发文量

1182

审稿时长

1.4 months

期刊介绍： Nano Letters serves as a dynamic platform for promptly disseminating original results in fundamental, applied, and emerging research across all facets of nanoscience and nanotechnology. A pivotal criterion for inclusion within Nano Letters is the convergence of at least two different areas or disciplines, ensuring a rich interdisciplinary scope. The journal is dedicated to fostering exploration in diverse areas, including: - Experimental and theoretical findings on physical, chemical, and biological phenomena at the nanoscale - Synthesis, characterization, and processing of organic, inorganic, polymer, and hybrid nanomaterials through physical, chemical, and biological methodologies - Modeling and simulation of synthetic, assembly, and interaction processes - Realization of integrated nanostructures and nano-engineered devices exhibiting advanced performance - Applications of nanoscale materials in living and environmental systems Nano Letters is committed to advancing and showcasing groundbreaking research that intersects various domains, fostering innovation and collaboration in the ever-evolving field of nanoscience and nanotechnology.