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研究论文

局域电场耦合Cl固定策略提升海水氧还原反应性能

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  • a海南大学,海洋科学与工程学院,海口,海南,570229,中国

    b南开大学,先进能源材料化学教育部重点实验室,天津,300071,中国

刘育荣,张淼,于彦会,刘亚琳,李静,史晓东,康振烨,吴道雄,饶鹏,梁颖,田新龙

网络出版日期: 2025-06-03

Local Electric Fields Coupled with Cl Fixation Strategy Improves Seawater Oxygen Reduction Reaction Performance

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  • a School of Marine Science and Engineering, Hainan University Haikou 570228, Hainan, China 

    b Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education) Nankai University, Tianjin 300071, China

Yurong Liu, Miao Zhang , Yanhui Yu , Yalin Liu , Jing Li , Xiaodong Shi , Zhenye Kang , Daoxiong Wu , Peng Rao , Ying Liang , and Xinlong Tian

Online published: 2025-06-03

摘要

开发适用于海水电解质的高性能氧还原反应(ORR)电催化剂是实现海水锌空气电池(SZABs)发展的关键。本文提出了一种在双金属单原子催化剂(DSACs)中构建局域电场耦合Cl固定策略,所制备催化剂在海水电解质中表现出优异的ORR性能,其半波电位(E1/2)高达0.868 V,组装的SZABs最大功率密度(Pmax)达182 mW cm−2,显著优于Pt/C催化剂(E1/2: 0.846 V; Pmax: 150 mW cm−2)。原位表征和理论计算表明,Fe位点比Co位点具有更强的Cl吸附亲和力,能够在ORR过程中优先吸附海水中的Cl,并通过同离子排斥效应构筑低Cl浓度的局域微环境,从而抑制Cl对Co活性中心的吸附和腐蚀,实现优异的催化稳定性。此外,Fe-Co原子对之间的定向电荷迁移形成局域电场,优化了Co位点对含氧中间体的吸附能,进一步提升ORR催化活性。

本文引用格式

刘育荣, 张淼, 于彦会, 刘亚琳, 李静, 史晓东, 康振烨, 吴道雄, 饶鹏, 梁颖, 田新龙 . 局域电场耦合Cl固定策略提升海水氧还原反应性能[J]. 电化学, 0 : 0 . DOI: 10.61558/2993-074X.3566

Abstract

The development of robust electrocatalyst for oxygen reduction reaction (ORR) in seawater electrolyte is the key to realize the seawater electrolyte-based zinc-air batteries (SZABs). Herein, constructing a local electric field coupled with Cl fixation strategy in dual single-atom catalysts (DSACs) is proposed, and the resultant catalyst delivers considerable ORR performance in seawater electrolyte, with a high half-wave potential (E1/2) of 0.868 V and a good maximum power density (Pmax) of 182 mW cm−2 in the assembled SZABs, much higher than those of the Pt/C catalyst (E1/2: 0.846 V; Pmax: 150 mW cm−2). The in-situ characterization and theoretical calculations reveal that the Fe sites have a higher Cladsorption affinity than the Co sites, preferentially adsorbs Clin seawater electrolyte during the ORR process, thus constructs a low-concentration Cl local microenvironment through the common-ion exclusion effect, which prevents Cl adsorption and corrosion the Co active centers, achieving impressive catalytic stability. In addition, the directional charge movement between Fe and Co atomic pairs constructs a local electric field, optimizing the adsorption energy of Co sites for oxygen-containing intermediates, and further improving the ORR activity.
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