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用于可充电锌空气电池中高性能双功能氧电催化的协同Ru/Co-S键合单原子和纳米颗粒催化剂。

Synergistic Ru/Co-S bonded single-atom and nanoparticle catalysts for high-performance bifunctional oxygen electrocatalysis in rechargeable zinc-air batteries.

作者信息

Hu Xiaolin, Wu Zhenkun, Wang Changhao, Li Yunsong, Jing Chuan

机构信息

School of Physics and New Energy, Chongqing Key Laboratory of New Energy Storage Materials and Devices, Chongqing University of Technology, Chongqing 400054, China.

School of Physics and New Energy, Chongqing Key Laboratory of New Energy Storage Materials and Devices, Chongqing University of Technology, Chongqing 400054, China.

出版信息

J Colloid Interface Sci. 2025 Dec;699(Pt 1):138174. doi: 10.1016/j.jcis.2025.138174. Epub 2025 Jun 14.

DOI:10.1016/j.jcis.2025.138174
PMID:40517491
Abstract

The development of efficient and sustainable energy conversion and storage technologies is the focus of modern scientific and technological research. This study doped Ru single atoms into a zinc zeolite imidazole framework (Ru-ZIF-8), followed by the adsorption of Co nanoparticles at the interface for the first pyrolysis and the introduction of S for the second pyrolysis to obtain a composite bifunctional electrocatalyst composed of Ru single atoms and Co nanoparticles (Co@Ru-SAs-HSNC), with Ru/Co-S coordination and stable anchoring on a hollow N-doped carbon substrate. The theoretical calculation results revealed that the introduction of S atoms to replace N atoms and form Ru sites provided a greater driving force for the reaction, regulated the electronic structure, and slowed the deactivation of the sintering of the metal particles. The secondary pyrolysis could produce more active sites for the catalyst and form a more uniform and stable pore structure, improving the activity and stability of the catalyst. In an alkaline environment, Co@Ru-SAs-HSNC exhibited a high half-wave potential of 0.90 V in the oxygen reduction reaction (ORR) and a low overpotential of 278 mV at 50 mA cm in the oxygen evolution reaction (OER). Additionally, Co@Ru-SAs-HSNC was used as the positive electrode of a rechargeable zinc-air battery, achieving a 205 mW cm peak power density. As shown in the long-term constant-current charge-discharge tests, Co@Ru-SAs-HSNC had a cycle time of up to 1134 h with high round-trip efficiency.

摘要

高效且可持续的能量转换与存储技术的发展是现代科技研究的重点。本研究将钌单原子掺杂到锌沸石咪唑框架(Ru-ZIF-8)中,随后在界面处吸附钴纳米颗粒进行首次热解,并引入硫进行第二次热解,以获得由钌单原子和钴纳米颗粒组成的复合双功能电催化剂(Co@Ru-SAs-HSNC),其具有Ru/Co-S配位并稳定锚定在中空氮掺杂碳基底上。理论计算结果表明,引入硫原子取代氮原子并形成Ru位点为反应提供了更大的驱动力,调节了电子结构,并减缓了金属颗粒烧结失活的速度。二次热解可为催化剂产生更多活性位点并形成更均匀稳定的孔结构,提高催化剂的活性和稳定性。在碱性环境中,Co@Ru-SAs-HSNC在氧还原反应(ORR)中表现出0.90 V的高半波电位,在析氧反应(OER)中在50 mA cm时过电位低至278 mV。此外,Co@Ru-SAs-HSNC用作可充电锌空气电池的正极,实现了205 mW cm的峰值功率密度。如长期恒流充放电测试所示,Co@Ru-SAs-HSNC具有高达1134 h的循环时间和高往返效率。

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