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MOF-Derived Isolated Fe Atoms Implanted in N-Doped 3D Hierarchical Carbon as an Efficient ORR Electrocatalyst in Both Alkaline and Acidic Media
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2019-06-27 00:00:00 , DOI: 10.1021/acsami.9b07436
Xiaodong Chen 1 , Ning Wang 2, 3 , Kui Shen 1 , Yangkai Xie 1 , Yongpeng Tan 1 , Yingwei Li 1
Affiliation  

In order to improve the catalytic performance of oxygen reduction reaction (ORR), it is pivotal to increase the density and accessibility of the active sites. Herein, we have developed a template-free melamine-assisted cocalcined strategy to afford Fe-embedded and N-doped carbons (Fe–N–C) with not only high density of atomically dispersed Fe–Nx active sites but also abundant three-dimensional interconnected mesopores by directly pyrolyzing Fe-ZIF-8 covered with a controllable melamine layer. It is demonstrated that the introduction of melamine in the precursor plays a key role in constructing various carbonized products with controllable morphology, porosity, and components. With an optimal mass ratio 1:1 of melamine to Fe-ZIF-8, the resultant [email protected] exhibits excellent ORR activity and stability, which exceeds 20 wt % commercial Pt/C catalyst (with a half-wave potential of 0.88 V vs 0.85 V) in an alkaline electrolyte and is even comparable to the commercial Pt/C catalyst (with a half-wave potential of 0.78 V vs 0.80 V) in an acidic electrolyte. To the best of our knowledge, [email protected] can be ranked among the best nonprecious metal electrocatalysts for ORR in both alkaline and acidic media. The present synthetic strategy may provide a new opportunity for the design and construction of metal–organic framework-derived nanomaterials with rational composition and a desired porous structure to boost their electrocatalytic performance.

中文翻译:

MOF衍生的孤立Fe原子植入N掺杂的3D分层碳中作为碱性和酸性介质中的高效ORR电催化剂

为了提高氧还原反应(ORR)的催化性能,提高活性位点的密度和可及性至关重要。在这里,我们开发了一种无模板的三聚氰胺辅助共煅烧策略,以提供不仅具有高原子分散的Fe-N x密度的Fe嵌入碳和N掺杂碳(Fe–N–C)。通过直接热解覆盖有可控三聚氰胺层的Fe-ZIF-8,可以使活性位点以及丰富的三维互连中孔发生。已证明在前体中引入三聚氰胺在构造具有可控形态,孔隙率和组分的各种碳化产物中起着关键作用。在三聚氰胺与Fe-ZIF-8的最佳质量比为1:1的情况下,所得的[受电子邮件保护]具有出色的ORR活性和稳定性,超过了20 wt%的商用Pt / C催化剂(半波电势为0.88 V碱性电解液中的Pt / C催化剂(半波电位为0.78 V对0.80 V),甚至可以与市售的Pt / C催化剂(半波电位为0.78 V对0.80 V)相比。据我们所知,在碱性和酸性介质中,[受电子邮件保护]均可被评为ORR最好的非贵金属电催化剂之一。当前的合成策略可能为金属和有机骨架衍生的纳米材料的设计和构建提供新的机会,这种纳米材料具有合理的组成和所需的多孔结构以增强其电催化性能。
更新日期:2019-06-27
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