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层状金属有机骨架衍生的具有双模态孔的 Fe-N-C 非贵金属电催化剂用于高效氧还原。

Lamellar Metal Organic Framework-Derived Fe-N-C Non-Noble Electrocatalysts with Bimodal Porosity for Efficient Oxygen Reduction.

机构信息

State Key Laboratory of Heavy Oil Processing, School of Chemical Engineering, China University of Petroleum , Qingdao 266580, China.

Beijing National Laboratory for Molecular Sciences and CAS Key Laboratory of Molecular Nanostructure and Nanotechnology, Institute of Chemistry, Chinese Academy of Sciences , 2 North First Street, Zhongguancun, Beijing 100190, China.

出版信息

ACS Appl Mater Interfaces. 2017 Feb 15;9(6):5272-5278. doi: 10.1021/acsami.6b15154. Epub 2017 Feb 1.

Abstract

Developing highly efficient and stable non-Pt electrocatalysts for the oxygen reduction reaction (ORR) to replace the state-of-the-art noble metal is essential for commercialization of fuel cells. Fe-N-C-based electrocatalysts are considered as a promising alternative to commercial Pt/C. An efficient electrocatalyst commonly requires large density of active site, high surface area, and desirable porosity, especially multimodal porosity with both large pores for efficient mass transfer and small pores for exposing as many active sites as possible. Herein, a lamellar metal organic framework (MOF) was developed as a precursor to directly achieve such a highly active Fe-N-C electrocatalyst with high surface area and desirable bimodal porosity. The mesopores arising from the special lamellar morphology of MOF benefits efficient mass transfer, and the nanopores resulting from pyrolysis of the MOF makes the majority of active sites accessible to electrolyte and thus effective for ORR. Uniform distribution of active elements N, C, and Fe at the molecular level in MOF precursor ensures abundant well-dispersed highly active sites in the catalyst. As a result, the catalyst exhibited superior ORR electrocatalytic activity and stability to commercial Pt/C. This strategy, using rarely reported lamellar MOF to prepare ORR catalysts with the merits mentioned, could inspire the exploration of a wide range of electrocatalysts from lamellar MOF precursors for various applications.

摘要

开发高效稳定的非铂电催化剂用于氧还原反应(ORR)以替代最先进的贵金属对于燃料电池的商业化至关重要。基于 Fe-N-C 的电催化剂被认为是商业 Pt/C 的一种很有前途的替代品。高效电催化剂通常需要大量的活性位点、高的表面积和理想的孔隙率,特别是具有大孔以实现高效传质和小孔以尽可能暴露更多活性位点的多模态孔隙率。在此,开发了层状金属有机骨架(MOF)作为前体,直接实现具有高表面积和理想双模态孔隙率的高活性 Fe-N-C 电催化剂。MOF 的特殊层状形态产生的中孔有利于高效传质,而 MOF 的热解产生的纳米孔使大多数活性位点能够与电解质接触,从而有效进行 ORR。MOF 前体中活性元素 N、C 和 Fe 在分子水平上的均匀分布确保了催化剂中存在丰富的分散良好的高活性位点。因此,该催化剂表现出优于商业 Pt/C 的 ORR 电催化活性和稳定性。这种使用很少报道的层状 MOF 来制备具有上述优点的 ORR 催化剂的策略,可以激发从层状 MOF 前体制备各种应用的电催化剂的广泛探索。

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