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面向高性能电催化剂的研究:原子分散的 Fe/N 掺杂分级多孔碳中 Fe-N 位点的原子级重构诱导。

Towards High-Performance Electrocatalysts for Oxygen Reduction: Inducing Atomic-Level Reconstruction of Fe-N Site for Atomically Dispersed Fe/N-Doped Hierarchically Porous Carbon.

机构信息

State Key Laboratory of Chemical Resource Engineering, Laboratory of Electrochemical Process and Technology for Materials, Beijing University of Chemical Technology, Beijing, 100029, China.

Beijing Advanced Innovation Center for Soft Matter Science and Engineering, Beijing University of Chemical Technology, Beijing, 100029, China.

出版信息

Chemistry. 2018 Jun 21;24(35):8848-8856. doi: 10.1002/chem.201800937. Epub 2018 Jun 1.

DOI:10.1002/chem.201800937
PMID:29682804
Abstract

A rational and effective strategy for the synthesis of a high-performance non-precious metal electrocatalyst for oxygen reduction reaction (ORR) was developed by inducing reconstruction of Fe-N site on pig-bone-derived nitrogen-doped hierarchically porous carbon. The resultant Fe/N-doped carbon electrocatalyst possessed abundant atomically dispersed non-planar Fe-N ORR active sites, with absolute presence of active D1 (Fe -N ) and D3 (N-Fe -N ) sites, as well as large specific surface area and three-dimensional porous structure with hierarchical micro-/meso-/macro-pore distribution, which increased the utilization of active sites and promoted mass transport of ORR reactants. This resulted in a remarkably superior ORR activity with half-wave potential of 0.87 V (20 mV higher than Pt/C) and kinetic current density of 10.9 mA cm at 0.85 V (2.3-fold of Pt/C) in alkaline electrolyte. This methodology provides a route for atomic-level design of high-performance ORR electrocatalyst.

摘要

通过在猪骨衍生的氮掺杂分级多孔碳上诱导 Fe-N 位的重构,开发了一种用于氧还原反应(ORR)的高性能非贵金属电催化剂的合理有效策略。所得的 Fe/N 掺杂碳电催化剂具有丰富的原子分散的非平面 Fe-N ORR 活性位,绝对存在活性 D1(Fe-N)和 D3(N-Fe-N)位,以及大的比表面积和具有分级微/介/大孔分布的三维多孔结构,这增加了活性位的利用率并促进了 ORR 反应物的质量传递。这导致在碱性电解质中具有显着优越的 ORR 活性,半波电位为 0.87 V(比 Pt/C 高 20 mV),在 0.85 V 时的动力学电流密度为 10.9 mA cm(是 Pt/C 的 2.3 倍)。该方法为高性能 ORR 电催化剂的原子级设计提供了一条途径。

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