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单源前驱体衍生的过渡金属合金嵌入氮掺杂多孔碳中作为高效氧析出电催化剂。

Single-Source-Precursor Derived Transition Metal Alloys Embedded in Nitrogen-Doped Porous Carbons as Efficient Oxygen Evolution Electrocatalysts.

机构信息

Department of Materials and Earth Sciences, Technical University of Darmstadt, 64287, Darmstadt, Germany.

College of Materials, Key Laboratory of High Performance Ceramic Fibers (Xiamen University), Ministry of Education, Xiamen, 361005, P.R. China.

出版信息

Chempluschem. 2022 Dec;87(12):e202200338. doi: 10.1002/cplu.202200338.

Abstract

Carbon supported metallic nanomaterials are of great interest due to their low-cost, high durability and promising functional performance. Herein, a highly active oxygen evolution reaction (OER) electrocatalyst comprised of defective carbon shell encapsulated metal (Fe, Co, Ni) nanoparticles and their alloys supported on in-situ formed N-doped graphene/carbon nanotube hybrid is synthesized from novel single-source-precursors (SSP). The precursors are synthesized by a facile one-pot reaction of tannic acid with polyethylenimine and different metal ions and subsequent pyrolysis of the SSP. Benefiting from the heteroatom doping of carbon and formation of well-encapsulated metal/alloy nanoparticles, the obtained FeNi@NC-900 catalyst possesses lowest overpotentials of 310 mV to achieve a current density of 10 mA cm for OER with a small Tafel slope value of 45 mV dec , indicating excellent catalytic performance due to the following features: (1) A synergistic electronic effect among metal alloy nanoparticles, nitrogen-doped carbon, and entangled carbon nanotubes; (2) penetration of electrolyte is promoted towards the active sites through the porous structure of the formed mesoporous carbon clusters; (3) the unique core-shell nanostructure of the hybrid material effectively curbs the degradation of electrocatalyst by protecting the alloy nanoparticles from harsh electrolyte. This work advances an inexpensive and facile method towards the development of transition metal-based hybrid material for potential energy storage and conversion.

摘要

由于成本低、耐久性高和有前途的功能性能,碳负载金属纳米材料受到了极大的关注。在此,通过新型单源前体(SSP)合成了由缺陷碳壳包裹的金属(Fe、Co、Ni)纳米颗粒及其合金和原位形成的 N 掺杂石墨烯/碳纳米管杂化的高活性氧析出反应(OER)电催化剂。前体通过单宁酸与聚乙烯亚胺和不同金属离子的简单一锅反应合成,然后对 SSP 进行热解。受益于碳的杂原子掺杂和封装良好的金属/合金纳米颗粒的形成,所得的 FeNi@NC-900 催化剂具有最低的过电位 310 mV,达到 10 mA cm 的电流密度 OER,具有小的塔菲尔斜率值 45 mV dec ,表明具有优异的催化性能,原因如下:(1)金属合金纳米颗粒、氮掺杂碳和缠结碳纳米管之间的协同电子效应;(2)通过形成的中孔碳簇的多孔结构促进电解质渗透到活性位点;(3)杂化材料的独特核壳纳米结构通过保护合金纳米颗粒免受苛刻电解质的影响有效抑制了电催化剂的降解。这项工作推进了一种廉价且简便的方法,用于开发用于潜在储能和转化的过渡金属基杂化材料。

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