Operando Hydroxylation of the Sn-Co Diatomic Catalyst Boosting Ultrastable Zn-Air Batteries.

IF 9.1 1区材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Nano Letters Pub Date : 2025-07-03 DOI:10.1021/acs.nanolett.5c02744

Lulu Lyu,Xu Hu,Wenqi Fan,Bing Shao,Qichen Wang,Gilseob Kim,Jong-Woan Chung,Zhen Zhou,Yong-Mook Kang

引用次数: 0

Abstract

Diatomic catalysts (DAs) exhibit superior catalytic activity for the oxygen reduction reaction (ORR) due to the synergistic interplay between dual metals. However, their dynamic evolution remains unexplored under the working conditions. Herein, Sn-Co diatomic pairs on N-doped carbon with an asymmetric N3Sn-CoN3 structure (SnCoN6 DA) are rationally designed for promoting ORR activity and durability. The operando hydroxylation of SnCoN6 DA regulates O2 adsorption on Co, allowing more d orbitals to hybridize with O2 s/p orbitals. Furthermore, the *OH-Sn moiety serves as an electron modulator that upshifts the d-band center of Co, enabling stronger binding with *OOH and expediting subsequent O-O cleavage. Accordingly, the operando hydroxylation of SnCoN6 DA positively shifts the half-wave potential by 54 mV and enhances the kinetic current density by 16.1 times compared to those of the Co single-atom catalyst. The constructed Zn-air battery shows an ultralong cycling life span (more than 3650 h at 5 and 10 mA cm-2).

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Sn-Co双原子催化剂的操作羟基化促进超稳定锌空气电池。

由于双金属间的协同作用，双原子催化剂在氧还原反应（ORR）中表现出优异的催化活性。然而，它们在工作条件下的动态演变仍未被探索。为了提高ORR活性和耐久性，合理设计了n掺杂碳上具有不对称N3Sn-CoN3结构（SnCoN6 DA）的Sn-Co双原子对。SnCoN6 DA的operando羟基化调节Co对O2的吸附，使更多的d轨道与O2 s/p轨道杂化。此外，*OH-Sn部分充当电子调制器，使Co的d带中心上移，使与*OOH的结合更强，并加速随后的O-O裂解。与Co单原子催化剂相比，SnCoN6 DA的operando羟基化使半波电位正向移动了54 mV，使动力学电流密度提高了16.1倍。所构建的锌空气电池具有超长的循环寿命（在5和10 mA cm-2下超过3650小时）。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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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

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