• 文献标题:   Unsaturated edge-anchored Ni single atoms on porous microwave exfoliated graphene oxide for electrochemical CO2
  • 文献类型:   Article
  • 作  者:   CHENG Y, ZHAO SY, LI HB, HE S, VEDER JP, JOHANNESSEN B, XIAO JP, LU SF, PAN J, CHISHOLM MF, YANG SZ, LIU C, CHEN JG, JIANG SP
  • 作者关键词:   ni singleatom catalyst, edgeanchored, defect, electrochemical co2 reduction, density functional simulation
  • 出版物名称:   APPLIED CATALYSIS BENVIRONMENTAL
  • ISSN:   0926-3373 EI 1873-3883
  • 通讯作者地址:   Curtin Univ
  • 被引频次:   71
  • DOI:   10.1016/j.apcatb.2018.10.046
  • 出版年:   2019

▎ 摘  要

Supported single atom catalysts (SACs), emerging as a new class of catalytic materials, have been attracting increasing interests. Here we developed a Ni SAC on microwave exfoliated graphene oxide (Ni-N-MEGO) to achieve single atom loading of similar to 6.9 wt%, significantly higher than previously reported SACs. The atomically dispersed Ni atoms, stabilized by coordination with nitrogen, were found to be predominantly anchored along the edges of nanopores (< 6 nm) using a combination of X-ray absorption spectroscopy (XAS) and aberration corrected scanning transmission electron microscopy (AC-STEM). The Ni-N-MEGO exhibits an onset over potential of 0.18 V, and a current density of 53.6 mA mg(-1) at overpotential of 0.59 V for CO2 reduction reaction (CO2RR), representing one of the best non-precious metal SACs reported so far in the literature. Density functional theory (DFT) calculations suggest that the electrochemical CO2-to-CO conversion occurs more readily on the edge-anchored unsaturated nitrogen coordinated Ni single atoms that lead to enhanced activity toward CO2RR.