辐射研究与辐射工艺学报, 2024, 42 (1): 010201, 网络出版: 2024-03-27  

γ射线辐照合成氮掺杂石墨单炔/铁催化剂及其性能

Synthesis of nitrogen-doped graphyne/iron catalysts via γ-ray irradiation and their properties
作者单位
1 天津工业大学纺织科学与工程学院 天津 300387
2 江苏大学材料科学与工程学院高分子材料研究学院 镇江 212013
摘要
本研究通过γ辐照与氮掺杂协同调控改性制备石墨炔,将二维石墨炔转变为一维管状结构并作为基底负载铁纳米粒子用于燃料电池阴极氧化还原反应(ORR)。运用扫描电镜、X射线衍射、拉曼光谱、等温氮气吸附和其他表征手段,对制备出的复合材料的表面形貌、元素组成、结晶结构、缺陷程度等进行了表征分析。在碱性溶液中,采用循环伏安测试、线性扫描伏安测试、电化学交流阻抗谱测试等电化学测试方法分析制备催化剂的ORR性能、动力学以及稳定性。结果表明:经γ射线辐照后,氮掺杂石墨单炔负载铁纳米粒子(NGY-Fe)催化剂具有更大的比表面积(411.3 m2/g)和多级孔结构,利于暴露出活性中心,O2渗透屏障也有所下降,NGY-Fe的ORR活性显著提高,尤其是在稳定性与耐甲醇性上远优于市售的商业Pt/C催化剂。
Abstract
In this study, graphdiyne was prepared using a γ-irradiated N-doping photogram to transform two-dimensional graphdiyne into a one-dimensional tubular structure for use as substrate-supported iron nanoparticles for cathodic redox reaction (ORR) in fuel cells. Methods such as scanning electron microscopy, X-ray diffraction, Raman spectroscopy, and isothermal nitrogen adsorption and other characterization methods were used to characterize and analyze the surface morphology, element composition, crystalline structure, and defect degree of the prepared composites. In the alkaline solution, the prepared catalyst was characterized by ORR performance, four-electron selectivity, kinetics and stability via cyclic voltammetry test, linear sweep voltammetry test and electrochemical AC impedance spectroscopy test. The results showed that after γ-ray irradiation, the nitrogen-doped graphite monoalkyne-loaded iron nanoparticle (NGY-Fe) catalyst had a larger specific surface area (411.3 m2/g) and a multilevel pore structure, which was conducive to the exposure of the active center. Moreover, the O2 permeation barrier was decreased, and the ORR activity of the NGY-Fe was significantly improved, especially in terms of the stability and methanol resistance, which were far superior to those of the commercially available commercial Pt/C catalysts.

董英杰, 石海婷, 王硕, 闵春英, 王道喜, 邵瑞琪, 徐志伟. γ射线辐照合成氮掺杂石墨单炔/铁催化剂及其性能[J]. 辐射研究与辐射工艺学报, 2024, 42(1): 010201. Yingjie DONG, Haiting SHI, Shuo WANG, Chunying MIN, Daoxi WANG, Ruiqi SHAO, Zhiwei XU. Synthesis of nitrogen-doped graphyne/iron catalysts via γ-ray irradiation and their properties[J]. Journal of Radiation Research and Radiation Processing, 2024, 42(1): 010201.

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