Unsaturated edge-anchored Ni single atoms on porous microwave exfoliated graphene oxide for electrochemical CO2

© 2018 Elsevier B.V. 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 ~6.9 wt%, significantly higher than...

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Bibliographic Details
Main Authors: Cheng, Y., Zhao, S., Li, H., He, S., Veder, Jean-Pierre, Johannessen, B., Xiao, J., Lu, S., Pan, J., Chisholm, M., Yang, S., Liu, C., Chen, J., Jiang, San Ping
Format: Journal Article
Published: Elsevier BV 2019
Online Access:http://purl.org/au-research/grants/arc/DP150102044
http://hdl.handle.net/20.500.11937/73310
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Summary:© 2018 Elsevier B.V. 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 ~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 overpotential 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.