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钴和氮共掺杂的多孔碳/碳纳米管杂化物,锚定镍纳米颗粒作为氧还原反应的高性能电催化剂。

Cobalt and nitrogen co-doped porous carbon/carbon nanotube hybrids anchored with nickel nanoparticles as high-performance electrocatalysts for oxygen reduction reactions.

作者信息

Wu Yan, Ge Liya, Veksha Andrei, Lisak Grzegorz

机构信息

Residues and Resource Reclamation Centre, Nanyang Environment and Water Research Institute, Nanyang Technological University, 1 Cleantech Loop, Clean Tech One, Singapore 637141, Singapore.

出版信息

Nanoscale. 2020 Jun 28;12(24):13028-13033. doi: 10.1039/d0nr02773a. Epub 2020 Jun 15.

Abstract

Non-precious metal-nitrogen-carbon (MNC) materials have been recognized as alternatives to noble-metal catalysts, such as Au/C, Pt/C and Ru/C. As the precursors of MNC catalysts, carbonized zeolite imidazole frameworks (ZIFs) have been widely studied due to their porosity and the composition of ligands, including carbon and nitrogen. Herein, we successfully synthesize a non-precious metal-based ORR catalyst with nickel nanoparticles anchored on cobalt and nitrogen co-doped porous carbon/carbon nanotubes (Ni/Co-NC), employing ZIF-67 metal-organic frameworks as precursors. The Ni/Co-NC catalyst shows an excellent onset potential of 0.984 V and a half-wave potential of 0.869 V in 0.1 M KOH, comparable to those of commercial Pt/C. The excellent ORR performance of Ni/Co-NC was attributed to the synergistic coexistence of the atomically dispersed metal species coordinated with nitrogen (metal-N sites) and carbon-encapsulated nickel nanoparticles as well as the hierarchical porous structure in the catalyst. In addition, the Ni/Co-NC catalyst possesses outstanding anti-poisoning capacity and long-term duration against methanol crossover in an alkaline environment. The obtained results enable the Ni/Co-NC catalyst to explore potential applications in energy conversion and storage systems.

摘要

非贵金属-氮-碳(MNC)材料已被公认为是贵金属催化剂(如Au/C、Pt/C和Ru/C)的替代品。作为MNC催化剂的前驱体,碳化沸石咪唑框架(ZIFs)因其孔隙率以及包括碳和氮在内的配体组成而受到广泛研究。在此,我们以ZIF-67金属有机框架为前驱体,成功合成了一种非贵金属基氧还原反应(ORR)催化剂,即镍纳米颗粒锚定在钴和氮共掺杂的多孔碳/碳纳米管(Ni/Co-NC)上。在0.1 M KOH中,Ni/Co-NC催化剂表现出优异的起始电位0.984 V和半波电位0.869 V,与商业Pt/C相当。Ni/Co-NC优异的ORR性能归因于与氮配位的原子分散金属物种(金属-N位点)和碳包覆的镍纳米颗粒的协同共存以及催化剂中的分级多孔结构。此外,Ni/Co-NC催化剂在碱性环境中具有出色的抗中毒能力和对甲醇渗透的长期耐久性。所获得的结果使Ni/Co-NC催化剂能够探索在能量转换和存储系统中的潜在应用。

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