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Universal Approach to Fabricating Graphene-Supported Single-Atom Catalysts from Doped ZnO Solid Solutions
journal contribution
posted on 2020-07-07, 17:09 authored by Jiashen Meng, Jiantao Li, Jinshuai Liu, Xingcai Zhang, Gengping Jiang, Lu Ma, Zhi-Yi Hu, Shibo Xi, Yunlong Zhao, Mengyu Yan, Peiyao Wang, Xiong Liu, Qidong Li, Jefferson Zhe Liu, Tianpin Wu, Liqiang MaiSingle-atom catalysts
(SACs) have attracted widespread interest
for many catalytic applications because of their distinguishing properties.
However, general and scalable synthesis of efficient SACs remains
significantly challenging, which limits their applications. Here we
report an efficient and universal approach to fabricating a series
of high-content metal atoms anchored into hollow nitrogen-doped graphene
frameworks (M-N-Grs; M represents Fe, Co, Ni, Cu, etc.) at gram-scale.
The highly compatible doped ZnO templates, acting as the dispersants
of targeted metal heteroatoms, can react with the incoming gaseous
organic ligands to form doped metal–organic framework thin
shells, whose composition determines the heteroatom species and contents
in M-N-Grs. We achieved over 1.2 atom % (5.85 wt %) metal loading
content, superior oxygen reduction activity over commercial Pt/C catalyst,
and a very high diffusion-limiting current (6.82 mA cm–2). Both experimental analyses and theoretical calculations reveal
the oxygen reduction activity sequence of M-N-Grs. Additionally, the
superior performance in Fe-N-Gr is mainly attributed to its unique
electron structure, rich exposed active sites, and robust hollow framework.
This synthesis strategy will stimulate the rapid development of SACs
for diverse energy-related fields.
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Solutions Single-atom catalystsSAChigh-content metal atomsheteroatom speciesDoped ZnOUniversal ApproachM-N-Groxygen reduction activity sequencenitrogen-doped graphene frameworksmetal heteroatomsFabricating Graphene-Supported Sing...oxygen reduction activityscalable synthesisZnO templateselectron structureapplicationsynthesis strategyenergy-related fields
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