构筑高效耐腐蚀的碳铠甲层包覆Co9Se8电催化剂用于海水基锌空气电池

doi:10.3866/PKU.WHXB202305004

物理化学学报 >> 2024, Vol. 40 >> Issue (6): 2305004.doi: 10.3866/PKU.WHXB202305004

所属专题：能源电催化

构筑高效耐腐蚀的碳铠甲层包覆Co₉Se₈电催化剂用于海水基锌空气电池

汪已萱†, 张灿辉†, 汪兴坤*(), 段嘉瑞, 童科程, 代水星, 初蕾, 黄明华*

中国海洋大学材料科学与工程学院, 山东青岛 266000

收稿日期:2023-05-08 修回日期:2023-07-26 录用日期:2023-07-27 发布日期:2023-11-29
通讯作者: Email: xingkunwang@163.com (汪兴坤)huangminghua@ouc.edu.cn; Tel.: 15965562297 (黄明华)
作者简介:
^†These authors contributed equally to this work.
基金资助:
国家自然科学基金(52261145700); 国家自然科学基金(22279124); 山东省自然科学基金(ZR2022ZD30)

Engineering Carbon-Chainmail-Shell Coated Co₉Se₈ Nanoparticles as Efficient and Durable Catalysts in Seawater-Based Zn-Air Batteries

Yixuan Wang, Canhui Zhang, Xingkun Wang*(), Jiarui Duan, Kecheng Tong, Shuixing Dai, Lei Chu, Minghua Huang*

School of Material Science and Engineering, Ocean University of China, Qingdao 266000, Shandong Province, China

Received:2023-05-08 Revised:2023-07-26 Accepted:2023-07-27 Published:2023-11-29
Contact: Email: xingkunwang@163.com (Xingkun Wang)huangminghua@ouc.edu.cn; Tel.: 15965562297 (Minghua Huang)
Supported by:
the National Natural Science Foundation of China(52261145700); the National Natural Science Foundation of China(22279124); the Natural Science Foundation of Shandong Province(ZR2022ZD30)

1. 附件.pdf(2359KB)

摘要/Abstract

摘要：

得益于较高的理论能量密度、环境友好性和丰富的海水储量，海水基锌-空气电池(S-ZABs)被认为是一种极具应用前景的储能和能源转换装置，是解决能源短缺和环境污染问题的能源装置之一。然而对于S-ZABs而言，构筑在海水中具有高耐氯离子腐蚀性与高性能的阴极氧还原反应电催化剂仍然具有挑战性。因此，我们通过高温硒化策略，在氮掺杂介孔碳材料上设计了超薄碳铠甲层封装的Co₉Se₈纳米颗粒高效ORR电催化剂(命名为NMC-Co₉Se₈)。外部的超薄碳铠甲层不仅可以改善催化过程中的电子转移过程，抑制纳米颗粒的团聚，而且可以作为盔甲保护内部活性位点免受Cl⁻吸附和腐蚀。得益于这种独特的结构，NMC-Co₉Se₈在0.1 mol∙L⁻¹ KOH海水电解质中表现出优异的ORR性能，其起始电位为0.904 V，半波电位为0.860 V。更重要的是，基于NMC-Co₉Se₈催化剂的S-ZABs可提供172.4 mW∙cm⁻²的功率密度和超过150 h的优异长期放电稳定性，均高于基于Pt/C的S-ZABs性能。这项工作为开发用于海水基锌-空气电池和其他能源转换技术具有耐氯离子腐蚀且高效的ORR催化剂提供了新思路。

关键词: Co₉Se₈纳米颗粒, 氧还原反应, 超薄碳铠甲层, 海水锌空气电池, 耐氯离子腐蚀

Abstract:

With the depletion of fossil fuel resources and the increasing severity of environmental pollution, it has become imperative to seek energy conversion devices with low cost, high efficiency and excellent environmental compatibility. Considering their high theoretical energy density, affordability and environmentally friendly nature, Zn-air batteries (ZABs) are regarded as promising energy storage and conversion devices. The utilization of seawater in ZABs (S-ZABs) holds great potential, given the abundance of seawater reserves, offering economic and social benefits such as reducing electrolyte costs and alleviating competition for freshwater consumption in human activities. However, the application of S-ZABs remains challenging, particularly in constructing high-performance cathode oxygen reduction reaction (ORR) catalysts that are highly resistant to Cl⁻ corrosion in seawater-based electrolytes. In this study, we have engineered an ultrathin carbon-chainmail-shell encapsulated Co₉Se₈ nanoparticles on N-doped mesoporous carbon (named as NMC-Co₉Se₈) electrocatalysts using the high-temperature selenization strategy. The ultrathin carbon-chainmail-shell on the outside improves electron transfer during the electrocatalysis and suppresses nanoparticles agglomeration. Additionally, it could act as armor for protecting the inner active site from the adsorption of corrosive Cl⁻. Benefit from this unique structure, the NMC-Co₉Se₈ catalyst exhibits excellent ORR performance, with an onset potential of 0.904 V and a half-wave potential of 0.860 V in seawater-based electrolytes. The catalyst also affords the lowest Tafel slope (35.5 mV∙dec⁻¹) and the highest kinetics current density of 9.816 mA∙cm⁻² at 0.85 V among all investigated samples. Owing to the protective effect of the ultrathin carbon-chainmail-shell on the inner active sites, the NMC-Co₉Se₈ catalyst retains 91.6% of its initial activity after continuous operation for 50000 s, surpassing the commercial Pt/C catalyst (with a current retention rate of 62.8%). More importantly, the S-ZABs based on the NMC-Co₉Se₈ catalyst deliver a high maximum power density of 172.4 mW∙cm⁻² and a high specific capacity of 643.9 mAh∙g⁻¹, exceeding those of S-ZABs powered by the commercial Pt/C catalyst (151.2 mW∙cm⁻² and 548.3 mAh∙g⁻¹). Furthermore, the S-ZABs driven by the NMC-Co₉Se₈ catalyst demonstrate a discharge stability for up to 150 h and maintain a stable charge-discharge cycle stability over 200 h, demonstrating the practical application performance of the NMC-Co₉Se₈ catalyst. In practical applications, the S-ZABs driven by the NMC-Co₉Se₈ catalyst can illuminate a light-emitting diode (LED) with a driving voltage of 2 V for several hours. This work provides new ideas for developing efficient and durable catalysts with high Cl⁻ corrosion resistance for applications in seawater-based Zn-air batteries and other energy conversion technologies.

Key words: Co₉Se₈ nanoparticle, Oxygen reduction reaction, Ultrathin carbon-chainmail-shell, Seawater-based Zn-air battery, Cl^- corrosion-resistant

汪已萱, 张灿辉, 汪兴坤, 段嘉瑞, 童科程, 代水星, 初蕾, 黄明华. 构筑高效耐腐蚀的碳铠甲层包覆Co₉Se₈电催化剂用于海水基锌空气电池[J]. 物理化学学报, 2024, 40(6), 2305004. doi: 10.3866/PKU.WHXB202305004

Yixuan Wang, Canhui Zhang, Xingkun Wang, Jiarui Duan, Kecheng Tong, Shuixing Dai, Lei Chu, Minghua Huang. Engineering Carbon-Chainmail-Shell Coated Co₉Se₈ Nanoparticles as Efficient and Durable Catalysts in Seawater-Based Zn-Air Batteries[J]. Acta Phys. -Chim. Sin. 2024, 40(6), 2305004. doi: 10.3866/PKU.WHXB202305004

链接本文: https://www.whxb.pku.edu.cn/CN/10.3866/PKU.WHXB202305004

https://www.whxb.pku.edu.cn/CN/Y2024/V40/I6/2305004

图/表 5

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构筑高效耐腐蚀的碳铠甲层包覆Co₉Se₈电催化剂用于海水基锌空气电池

Engineering Carbon-Chainmail-Shell Coated Co₉Se₈ Nanoparticles as Efficient and Durable Catalysts in Seawater-Based Zn-Air Batteries

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