Inherent anti-Fenton property of single-atom rhenium for the ultra-durable oxygen reduction reaction,Energy & Environmental Science

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Inherent anti-Fenton property of single-atom rhenium for the ultra-durable oxygen reduction reaction
Energy & Environmental Science ( IF 32.4 ) Pub Date : 2024-07-11 , DOI: 10.1039/d4ee02375g
Xin-Zheng Yue ₁ , Yun-Ce Liu ₁ , Bang-An Lu ₂ , Xin Du ₁ , Wen Lei ₁ , Zhong-Yi Liu ₁ , Sha-Sha Yi ₂ , Chao Lu _{1,

3}

Affiliation

It is of utmost urgency to construct M–N–C catalysts with inherent stability and high performances towards the oxygen reduction reaction (ORR). In principle, using the 4d and 5d transition metals (TM_4d,5d), particularly rhenium (Re), the desired M–N–C catalysts could be fabricated. However, it is a long-standing challenge to configure Re_5d single atom sites with ultra-durable ORR due to the occurrence of intractable Fenton reactions. In this contribution, we report a Re single-atom catalyst (Re-SAC) featuring a ReN₄ configuration that exhibits remarkable ORR activity and stability under alkaline conditions. Specifically, the half-wave potential (E_1/2) can reach a maximum of 0.89 V, and no significant changes in E_1/2 are observed after 10 000 cycles. The zinc–air battery demonstrates a superior open-circuit voltage of 1.55 V and exceptional durability, lasting over 300 h at 5 mA cm⁻². It was disclosed that incorporating Re into N–C structures effectively modulates the adsorption energy of ORR intermediates, thereby reducing the activation energy of the reaction. This work paves the way for designing high-performance single-atom catalysts based on TM_4d,5d centers for practical applications.

中文翻译：

单原子铼固有的抗芬顿特性，用于超耐久的氧还原反应

当务之急是构建具有固有稳定性和高性能的氧还原反应（ORR）M-N-C催化剂。原则上，使用 4d 和 5d 过渡金属 (TM _4d,5d )，特别是铼 (Re)，可以制造所需的 M-N-C 催化剂。然而，由于棘手的芬顿反应的发生，配置具有超耐久ORR的Re _5d 单原子位点是一个长期存在的挑战。在这篇文章中，我们报道了一种具有 ReN ₄ 构型的 Re 单原子催化剂 (Re-SAC)，在碱性条件下表现出显着的 ORR 活性和稳定性。具体而言，半波电位（E _1/2 ）最高可达0.89 V，并且在10 000次循环后，E _1/2 没有观察到明显变化。锌空气电池具有 1.55 V 的优异开路电压和卓越的耐用性，在 5 mA cm 电流下可持续使用 300 小时以上 ⁻² 。据透露，将Re掺入N-C结构中可以有效调节ORR中间体的吸附能，从而降低反应的活化能。这项工作为设计基于TM _4d,5d 中心的高性能单原子催化剂的实际应用铺平了道路。

更新日期：2024-07-11

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