Synthesis of cobalt sulfide–NC composite catalyst assisted by polyaniline as nonprecious electrocatalyst for oxygen reduction reaction

IF 4.9 2区 化学 Q2 CHEMISTRY, PHYSICAL Molecular Catalysis Pub Date : 2025-04-10 DOI:10.1016/j.mcat.2025.115107
Jae Sang Lee , Won Suk Jung
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Abstract

The scarce, expensive Pt is the preferred catalyst for the oxygen reduction reaction (ORR) in metal–air batteries or fuel cells. In this study, a composite catalyst consisting of cobalt sulfide and polyaniline (PANI) was utilized for optimal ORR kinetics. Cobalt sulfide catalysts were prepared at different temperatures, the optimal cobalt sulfide catalyst was coated with PANI, and the coated catalyst was annealed to form a core–shell cobalt sulfide@NC composite catalyst. Structural characterization was performed via X-ray diffraction (XRD) and Raman spectroscopy, scanning electron microscopy, and high-resolution transmission electron microscopy (HR-TEM) were conducted to characterize the catalyst morphology. CoS-160 exhibited a flower-like structure; CoS-180, containing Co9S8, exhibited both flower-like and sheet structures; and CoS-200 exhibited a sheet structure. With an increase in temperature, XRD and Raman spectroscopy verified the formation of Co9S8, serving as ORR active sites, in CoS-180 and CoS-200. HR-TEM indicated that the Co9S8-x@NC catalysts had a core–shell structure. Among them, Co9S8–180@NC had the highest graphitization degree, and total nitrogen, pyridinic N, graphitic N contents, resulting in the highest onset potential, limiting current density and the lowest Tafel slope for ORR in alkaline media among the catalysts. In an accelerated stress test, a performance degradation of less than 1 % was observed, and a chronoamperometry test demonstrated a current retention rate of 95.49 %.

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聚苯胺辅助硫化钴- nc复合催化剂在氧还原反应中的合成
稀缺而昂贵的铂是金属空气电池或燃料电池中氧还原反应(ORR)的首选催化剂。本研究利用硫化钴和聚苯胺(PANI)组成的复合催化剂来优化 ORR 动力学。硫化钴催化剂在不同温度下制备,最佳硫化钴催化剂涂覆 PANI,涂覆催化剂退火形成核壳硫化钴@NC 复合催化剂。通过 X 射线衍射(XRD)和拉曼光谱进行了结构表征,扫描电子显微镜和高分辨率透射电子显微镜(HR-TEM)对催化剂形态进行了表征。CoS-160 呈现花状结构;含有 Co9S8 的 CoS-180 同时呈现花状和片状结构;CoS-200 则呈现片状结构。随着温度的升高,XRD 和拉曼光谱验证了 CoS-180 和 CoS-200 中作为 ORR 活性位点的 Co9S8 的形成。HR-TEM 表明 Co9S8-x@NC 催化剂具有核壳结构。其中,Co9S8-180@NC 的石墨化程度、总氮、吡啶 N、石墨 N 含量最高,因此在碱性介质中的 ORR 起始电位、极限电流密度最高,Tafel 斜率最低。在加速应力测试中,观察到的性能衰减小于 1%,而计时器测试显示的电流保持率为 95.49%。
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来源期刊
Molecular Catalysis
Molecular Catalysis Chemical Engineering-Process Chemistry and Technology
CiteScore
6.90
自引率
10.90%
发文量
700
审稿时长
40 days
期刊介绍: Molecular Catalysis publishes full papers that are original, rigorous, and scholarly contributions examining the molecular and atomic aspects of catalytic activation and reaction mechanisms. The fields covered are: Heterogeneous catalysis including immobilized molecular catalysts Homogeneous catalysis including organocatalysis, organometallic catalysis and biocatalysis Photo- and electrochemistry Theoretical aspects of catalysis analyzed by computational methods
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