物理化学学报 >> 2023, Vol. 39 >> Issue (8): 2210039.doi: 10.3866/PKU.WHXB202210039

所属专题： 能源电催化

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钴原子团簇用于高效氧还原反应

于彦会, 饶鹏, 封苏阳, 陈民, 邓培林(), 李静, 苗政培(), 康振烨, 沈义俊, 田新龙()   

  • 收稿日期:2022-10-27 录用日期:2022-11-14 发布日期:2022-11-21
  • 通讯作者: 邓培林,苗政培,田新龙 E-mail:dengpeilin@hainanu.edu.cn;zpmiao92@hainanu.edu.cn;tianxl@hainanu.edu.cn
  • 作者简介:第一联系人：

    †These authors contributed equally to this work.

  • 基金资助:
    海南省自然科学基金(222RC548);国家自然科学基金(22109034);国家自然科学基金(22109035);国家自然科学基金(52164028);国家自然科学基金(62105083);海南省博士后科学基金(RZ2100007123);南海海洋资源利用国家重点实验室基金(海南大学);南海海洋资源利用国家重点实验室基金(MRUKF2021029);海南大学科研启动基金(KYQD(ZR)-20008);海南大学科研启动基金(20082);海南大学科研启动基金(20083);海南大学科研启动基金(20084);海南大学科研启动基金(21065);海南大学科研启动基金(21124);海南大学科研启动基金(21125);海南省院士创新平台资金资助项目

Atomic Co Clusters for Efficient Oxygen Reduction Reaction

Yanhui Yu, Peng Rao, Suyang Feng, Min Chen, Peilin Deng(), Jing Li, Zhengpei Miao(), Zhenye Kang, Yijun Shen, Xinlong Tian()   

  • Received:2022-10-27 Accepted:2022-11-14 Published:2022-11-21
  • Contact: Peilin Deng, Zhengpei Miao, Xinlong Tian E-mail:dengpeilin@hainanu.edu.cn;zpmiao92@hainanu.edu.cn;tianxl@hainanu.edu.cn
  • Supported by:
    the Hainan Provincial Natural Science Foundation of China(222RC548);the National Natural Science Foundation of China(22109034);the National Natural Science Foundation of China(22109035);the National Natural Science Foundation of China(52164028);the National Natural Science Foundation of China(62105083);the Postdoctoral Science Foundation of Hainan Province(RZ2100007123);the Foundation of State Key Laboratory of Marine Resource Utilization in South China Sea(海南大学);the Foundation of State Key Laboratory of Marine Resource Utilization in South China Sea(MRUKF2021029);the Start-up Research Foundation of Hainan University(KYQD(ZR)-20008);the Start-up Research Foundation of Hainan University(20082);the Start-up Research Foundation of Hainan University(20083);the Start-up Research Foundation of Hainan University(20084);the Start-up Research Foundation of Hainan University(21065);the Start-up Research Foundation of Hainan University(21124);the Start-up Research Foundation of Hainan University(21125);the specific research fund of The Innovation Platform for Academicians of Hainan Province

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摘要：

探索非贵金属材料作为高效氧还原反应催化剂是迫切需要的，但具有一定的挑战性。本文采用等离子体轰击和酸洗相结合的策略合成了Co原子团簇修饰的多孔碳载体催化剂(CoAC/NC)。通过多种表征手段证实了的原子团簇特征。所得到的CoAC/NC催化剂在三电极体系和锌-空电池方面都表现出优异的氧还原反应活性。该催化剂的氧还原反应半波电位为0.887 V，显著优于商业Pt/C催化剂，且表现出优异的稳定性。此外，该催化剂组装的锌-空电池的峰值功率密度为181.5 mW∙cm−2，同样远高于Pt/C催化剂。这项工作不仅合成了一种高效的氧还原反应催化剂，而且为原子团簇催化剂的理性设计和实际应用提供了新的见解。

关键词: 原子团簇催化剂, 电催化剂, 等离子轰击, 钴团簇, 氧还原反应

Abstract:

Environment-friendly energy storage and conversion technologies, such as metal–air batteries and fuel cells, are considered promising approaches to address growing environmental concerns. The oxygen reduction reaction (ORR) is the core of renewable energy conversion technology and plays an irreplaceable role in this fundamental issue. However, the complex multi-reaction process of the ORR presents a bottleneck that limits efforts to accelerate its kinetics. Traditionally, Pt and Pt-based catalysts are regarded as a good choice to improve the sluggish kinetics of the ORR. However, because Pt-based catalysts are expensive and have low durability, their use to resolve the energy crisis and current environmental challenges is impractical. Hence, exploring low-cost, highly active, and durable ORR catalysts as potential alternatives to commercial Pt/C is an urgent undertaking. Atomic cluster catalysts (ACCs) may be suitable alternatives to commercial Pt/C catalysts owing to their ultra-high atomic utilization efficiency, unique electronic structure, and stable nanostructures. However, despite the significant progress achieved in recent years, ACCs remain unusable for practical applications. In this study, a facile plasma bombing method combined with an acid washing strategy is proposed to fabricate an atomic Co cluster-decorated porous carbon supports catalyst (CoAC/NC) showing improved ORR performance. The typical atomic cluster features of the resultant CoAC/NC catalyst are confirmed using comprehensive characterization techniques. The CoAC/NC catalyst exhibits considerable ORR activity with a half-wave potential of as high as 0.887 V (versus a reversible hydrogen electrode (RHE)), which is much higher than that of a commercial Pt/C catalyst. More importantly, the CoAC/NC catalyst displays excellent battery performance when applied to a Zn-air battery, showing a peak power density of 181.5 mW∙cm−2 and long discharge ability (over 67 h at a discharge current density of 5 mA∙cm−2). The desirable ORR performance of the fabricated CoAC/NC catalyst could be mainly attributed to the high atom utilization efficiency and stable active sites endowed by the unique Co atomic clusters, as well as synergistic effects between the neighboring Co atoms of these clusters. Moreover, the high specific surface area and wide pore distribution of the catalyst offer abundant accessible active sites for the ORR. This work not only provides an outstanding alternative to commercial Pt catalysts for the ORR but also offers new insights into the rational design and practical application of ACCs.

Key words: Atomic cluster catalyst, Electrocatalyst, Plasma bombing, Co cluster, Oxygen reduction reaction