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通过空间隔离策略合理合成铁/氮掺杂碳催化剂用于酸性和碱性介质中的高效氧还原反应

Rational Synthesis of Iron/Nitrogen-Doped Carbon Catalyst through a Spatial Isolation Strategy for Efficient Oxygen Reduction in Acidic and Alkaline Media.

作者信息

Feng Bomin, Wu Xiuju, Li Ling, Gao Wei, Hu Weihua, Li Chang Ming

机构信息

Key Laboratory of Luminescent and Real-Time Analytical Chemistry, (Southwest University), Ministry of Education, School of Materials & Energy, Southwest University, Chongqing, 400715, P.R. China.

Institution Chongqing Key Lab for Advanced Materials and Clean Energies of Technologies, School of Materials and Energy, Southwest University, Chongqing, 400715, P.R. China.

出版信息

Chemistry. 2019 Sep 2;25(49):11560-11565. doi: 10.1002/chem.201902521. Epub 2019 Aug 12.

Abstract

It remains challenging to rationally synthesize iron/nitrogen-doped carbon (Fe/N-C) catalysts with rich Fe-N atomic active sites for improved oxygen reduction reaction (ORR) electrocatalysis. A highly efficient Fe/N-C catalyst, which has been synthesized through a spatial isolation strategy, is reported. Derived from bioinspired polydopamine (PDA)-based hybrid microsphere precursors, it is a multifunctional carrier that loads atomically dispersed Fe /Zn ions through coordination interactions and N-rich melamine through electrostatic attraction and covalent bonding. The Zn ions and melamine in the precursor efficiently isolate Fe atoms upon pyrolysis to form rich Fe-N atomic active sites, and generate abundant micropores during high-temperature treatment; as a consequence, the resultant Fe-N/C catalyst contains rich catalytically active Fe-N sites and a hierarchical porous structure. The catalyst exhibits improved ORR activity that is superior to and close to that of Pt/C in alkaline and acidic solutions, respectively.

摘要

合理合成具有丰富Fe-N原子活性位点的铁/氮掺杂碳(Fe/N-C)催化剂以改善氧还原反应(ORR)电催化仍然具有挑战性。本文报道了一种通过空间隔离策略合成的高效Fe/N-C催化剂。它源自受生物启发的基于聚多巴胺(PDA)的混合微球前驱体,是一种多功能载体,通过配位相互作用负载原子分散的Fe/Zn离子,并通过静电吸引和共价键负载富含氮的三聚氰胺。前驱体中的Zn离子和三聚氰胺在热解时有效地隔离Fe原子,形成丰富的Fe-N原子活性位点,并在高温处理过程中产生大量微孔;因此,所得的Fe-N/C催化剂含有丰富的催化活性Fe-N位点和分级多孔结构。该催化剂在碱性和酸性溶液中分别表现出优于Pt/C且接近Pt/C的ORR活性。

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