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Shengzhi He, and Chunwen Sun, Fe-loaded S, N co-doped carbon catalyst for oxygen reduction reaction with enhanced electrocatalytic activity and durability, Int. J. Miner. Metall. Mater., (2025). https://doi.org/10.1007/s12613-025-3215-6
Shengzhi He, and Chunwen Sun, Fe-loaded S, N co-doped carbon catalyst for oxygen reduction reaction with enhanced electrocatalytic activity and durability, Int. J. Miner. Metall. Mater., (2025). https://doi.org/10.1007/s12613-025-3215-6
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铁基硫氮共掺杂碳催化剂可实现氧还原反应电催化活性和耐久性的协同增强

摘要: 氧还原反应(ORR)是锌-空气电池(ZAB)的关键反应,但其中间体生成较多、反应活化能较高,本征动力学速率缓慢,因而ORR效率是这类器件性能的关键影响因素。ORR催化剂能够有效地降低反应活化能,加快反应速率,从而提高电池效率,并且ORR催化剂的稳定性与电池的循环寿命密不可分。本文旨在开发一种高活性、高稳定性的铁基硫氮共掺杂碳(Fe/SNC)作为ZAB的阴极催化剂。本文制备了不同S含量的Fe/SNC催化剂,并采用电化学测量和恒电流充放电试验研究了不同Fe/SNC催化剂的电催化性能。研究结果表明,制备的Fe/SNC-10(Fe/S摩尔比为1:10)催化剂表现出0.902 V的半波电位(E1/2)和优异的稳定性,经过5000次CV循环后E1/2仅降低20 mV,其ORR活性和稳定性优于商业Pt/C催化剂和大多数已报道的铁基氮掺杂碳(Fe/NC)。研究表明,S掺杂有助于Fe/NC催化活性的提升,并且催化活性与硫掺量的曲线呈现火山型。硫的原子半径比氮和碳大,掺杂后导致碳载体上产生缺陷,增大了催化剂的比表面积。此外,硫的电负性比氮小,掺杂后改变了Fe–Nx活性中心的电子结构。由Fe/SNC-10催化剂组装的ZAB具有1.44 V的开路电位、129 mW·cm−2的峰值功率密度和848 mA·h·g−1的放电比容量。由Fe/SNC-10+RuO2组装的ZAB能够在5 mA·cm−2下稳定运行超过1000 h。Fe/SNC催化剂的合理设计为高效非贵金属催化剂的研究和储能器件的开发提供了新的途径。未来硫氮共掺杂碳催化剂在电催化、环境保护、有机合成和能源转换等领域的应用将得到进一步拓展。随着科学技术的不断进步,相信硫氮共掺杂碳催化剂将为人类社会的可持续发展做出更大的贡献。

 

Fe-loaded S, N co-doped carbon catalyst for oxygen reduction reaction with enhanced electrocatalytic activity and durability

Abstract: Heteroatom-doped carbon is considered a promising alternative to commercial Pt/C as an efficient catalyst for the oxygen reduction reaction (ORR). This study presents the synthesis of iron-loaded, sulfur and nitrogen co-doped carbon (Fe/SNC) via in situ incorporation of 2-aminothiazole molecules into zeolitic imidazolate framework-8 (ZIF-8) through coordination between metal ions and organic ligands. Sulfur and nitrogen doping in carbon supports effectively modulates the electronic structure of the catalyst, increases the Brunauer–Emmett–Teller surface area, and exposes more Fe–Nx active centers. Fe-loaded, S and N co-doped carbon with Fe/S molar ratio of 1:10 (Fe/SNC-10) exhibits a half-wave potential of 0.902 V vs. RHE. After 5000 cycles of cyclic voltammetry, its half-wave potential decreases by only 20 mV vs. RHE, indicating excellent stability. Due to sulfur’s lower electronegativity, the electronic structure of the Fe–Nx active center is modulated. Additionally, the larger atomic radius of sulfur introduces defects into the carbon support. As a result, Fe/SNC-10 demonstrates superior ORR activity and stability in alkaline solution compared with Fe-loaded N-doped carbon (Fe/NC). Furthermore, the zinc–air battery assembled with the Fe/SNC-10 catalyst shows enhanced performance relative to those assembled with Fe/NC and Pt/C catalysts. This work offers a novel design strategy for advanced energy storage and conversion applications.

 

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