• 文献标题:   Universal Approach to Fabricating Graphene-Supported Single-Atom Catalysts from Doped ZnO Solid Solutions
  • 文献类型:   Article
  • 作  者:   MENG JS, LI JT, LIU JS, ZHANG XC, JIANG GP, MA L, HU ZY, XI SB, ZHAO YL, YAN MY, WANG PY, LIU X, LI QD, LIU JZ, WU TP, MAI LQ
  • 作者关键词:  
  • 出版物名称:   ACS CENTRAL SCIENCE
  • ISSN:   2374-7943 EI 2374-7951
  • 通讯作者地址:   Wuhan Univ Technol
  • 被引频次:   4
  • DOI:   10.1021/acscentsci.0c00458
  • 出版年:   2020

▎ 摘  要

Single-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.