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Fe-N-共掺杂介孔碳负载在还原氧化石墨烯上的双活性位点作为高效氧还原催化剂。

Fe-N-Doped Mesoporous Carbon with Dual Active Sites Loaded on Reduced Graphene Oxides for Efficient Oxygen Reduction Catalysts.

机构信息

Key Laboratory of Materials Physics and Anhui Key Laboratory of Nanomaterials and Nanotechnology, Institute of Solid State Physics, Hefei Institutes of Physical Science, Chinese Academy of Sciences , Hefei 230031, China.

University of Science and Technology of China , Hefei 230026, China.

出版信息

ACS Appl Mater Interfaces. 2018 Jan 24;10(3):2423-2429. doi: 10.1021/acsami.7b14443. Epub 2018 Jan 12.

Abstract

Transition metal/nitrogen/carbon (M-N/C) catalysts are considered as one of the most promising candidates to replace Pt/C catalysts for oxygen reduction reactions (ORRs). Here, we have designed novel reduced graphene oxide (rGO)-supported Fe-N-doped carbon (Fe-N-C/rGO) catalysts via simple pyrolysis of polypyrrole (Ppy)-FeO-GO composites. The as-prepared catalysts induced an onset potential of 0.94 V and a half-wave potential of 0.81 V in alkaline solutions, which is much better than those of the counterpart N-C and N-C/rGO catalysts and comparable to that of Pt/C catalysts. Moreover, the Fe-N-C/rGO catalysts showed improved durability and higher tolerance against methanol crossover than Pt/C in alkaline solutions. This superior ORR performance can be ascribed to the combined catalytic effect of both Fe-based nanoparticles (FeO, FeC) and Fe-N sites, as well as fast mass transfer and accessible active sites benefiting from the mesoporous structure and high specific surface area. This work provides new insight for synthesis of a more promising nonplatinum electrocatalyst for metal-air batteries and fuel-cell applications.

摘要

过渡金属/氮/碳(M-N/C)催化剂被认为是替代 Pt/C 催化剂用于氧还原反应(ORR)的最有前途的候选材料之一。在这里,我们通过简单地热解聚吡咯(Ppy)-FeO-GO 复合材料设计了新型还原氧化石墨烯(rGO)负载的 Fe-N 掺杂碳(Fe-N-C/rGO)催化剂。所制备的催化剂在碱性溶液中诱导出 0.94 V 的起始电位和 0.81 V 的半波电位,优于相应的 N-C 和 N-C/rGO 催化剂,与 Pt/C 催化剂相当。此外,与 Pt/C 催化剂相比,Fe-N-C/rGO 催化剂在碱性溶液中表现出更好的耐久性和对甲醇交叉的更高耐受性。这种优异的 ORR 性能可归因于 Fe 基纳米颗粒(FeO、FeC)和 Fe-N 位的协同催化作用,以及得益于介孔结构和高比表面积的快速质量传递和可及的活性位。这项工作为金属-空气电池和燃料电池应用中更有前途的非铂电催化剂的合成提供了新的见解。

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