期刊
APPLIED CATALYSIS B-ENVIRONMENTAL
卷 243, 期 -, 页码 294-303出版社
ELSEVIER SCIENCE BV
DOI: 10.1016/j.apcatb.2018.10.046
关键词
Ni single-atom catalysts; Edge-anchored; Defects; Electrochemical CO2 reduction; Density functional simulation
资金
- Australian Research Council [DP150102044, DP180100731, DP180100568, LE120100026]
- U.S. Department of Energy, Office of Science, Basic Energy Sciences, Materials Science and Engineering
- ORNL's Center for Nanophase Materials Sciences - Scientific User Facilities Division of U.S. Department of Energy
- National Natural Science Foundation of China [51521091]
- Australian Research Council [LE120100026] Funding Source: Australian Research Council
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.
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