氮碳包封Fe3C纳米颗粒作为高效富氧还原电催化剂
Nitrogen-carbon-encapsulated Fe3C nanoparticles as highly efficient earth-abundant oxygen reduction electrocatalysts
汪翠萍 1李智 1雷杰 1李松 1Stijn F.L.Mertens 2胡劲松3
作者信息
- 1. School of Chemical Engineering,Anhui Province Key Laboratory of Specialty Polymers,Anhui University of Science and Technology,Huainan 232001,China
- 2. Department of Chemistry,Energy Lancaster and Materials Science Lancaster,Lancaster University,Lancaster LA1 4YB,United Kingdom
- 3. School of Chemical Engineering,Anhui Province Key Laboratory of Specialty Polymers,Anhui University of Science and Technology,Huainan 232001,China;Institute of Energy,Hefei Comprehensive National Science Center,Hefei 230031,China
- 折叠
摘要
高活性MOF基催化剂的设计和合成为促进动力学不利的氧还原反应(ORR)过程开辟了新的途径.本研究通过在ZIF-8前驱体表面涂覆二茂铁甲酸,然后进行两步炭化工艺,设计和制备了一种具有新型结构的高效电催化剂,以提高ORR性能.两步炭化过程对于将热解Fe3C纳米颗粒封装到碳纳米管(CNTs)中以及将Fe单原子隔离到N掺杂碳(NC)基体上至关重要.此外,Fe元素的相对含量对优化催化剂的ORR性能至关重要.所制得Fe3C@CNTs/NC-M催化剂结构先进,在碱性溶液中表现出良好的长期稳定性和电催化ORR性能,其半波电位和极限电流分别达到0.941 V和6.31 mA cm-2.此外,该电催化剂在甲醇溶液中具有较强的耐受性和良好的稳定性.Fe3C@CNTs/NC-M锌空气电池(ZAB)具有1.525 V的开路电位,420 mA cm-2时的峰值功率密度为348 mW cm-2,10 mA cm-2时的最大容量为843 mA h gzn-1.因此,这种合成策略为构建具有有效和稳定的ORR性能的MOF基电催化材料提供了一条有效途径.
Abstract
The design and synthesis of the highly active metal-organic framework(MOF)-based catalysts open new avenues to facilitate the kinetically unfavorable oxygen re-duction reaction(ORR).In this paper,we elucidate the design and fabrication of an efficient electrocatalyst with a novel structure for the enhancement of the ORR performance by decorating the surface of the ZIF-8 precursor with ferrocene formic acid,followed by a two-step carbonization process,which is critical for the encapsulation of pyrolytic Fe3C na-noparticles(NPs)into carbon nanotubes(CNTs)and the isolation of Fe single atoms onto an N-doped carbon(NC)matrix.Moreover,the relative Fe content is vital to optimize the ORR performance of the catalysts.The resulting Fe3C@CNT/NC-M catalyst has an optimized structure.It shows great long-term stability and excellent electrocatalytic ORR performance in alkaline solution,with the half-wave potential and limiting current reaching 0.941 V and 6.31 mA cm-2,respectively.Furthermore,the electrocatalyst has a strong tolerance to and good stability in a methanol solution.The Fe3C@CNT/NC-M zinc-air battery delivers a large open-circuit potential of 1.525 V,a peak power density of 348 mW cm-2 at 420 mA cm-2,and a maximum capacity of 843 mA h gzn-1 at 10 mA cm-2.Thus,this synthetic strategy provides a promising pathway toward constructing MOF-based electrocatalytic materials with effective and stable ORR performance.
关键词
metal-organic frameworks/carbon nanotubes/N-doped carbon matrix/oxygen reduction reaction/Zn-air batteryKey words
metal-organic frameworks/carbon nanotubes/N-doped carbon matrix/oxygen reduction reaction/Zn-air battery引用本文复制引用
基金项目
安徽省自然科学基金(1908085J10)
国家自然科学基金(21671004)
Institute of Energy,Hefei Comprehensive National Science Center(21KZS216)
Scientific Research Foundation for High-level Talents of Anhui University of Science and Technology(2022yjrc50)
出版年
2024
NETL
NSTL
万方数据