Journal article
One-Pot Pyrolysis Method to Fabricate Carbon Nanotube Supported Ni Single-Atom Catalysts with Ultrahigh Loading
ACS Applied Energy Materials, Vol.1(10), pp.5286-5297
2018
Abstract
The practical application of single atom catalysts (SACs) is constrained by the low achievable loading of single metal atoms. Here, nickel SACs stabilized on a nitrogen-doped carbon nanotube structure (NiSA-N-CNT) with ultrahigh Ni atomic loading up to 20.3 wt % have been successfully synthesized using a new one-pot pyrolysis method employing Ni acetylacetonate (Ni(acac)2) and dicyandiamide (DCD) as precursors. The yield and formation of NiSA-N-CNT depends strongly on the Ni(acac)2/DCD ratio and annealing temperature. Pyrolysis at 350 and 650 °C led to the formation of Ni single atom dispersed melem and graphitic carbon nitride (Ni-melem and Ni-g-C3N4). Transition from a stacked and layered Ni-g-C3N4 structure to a bamboo-shaped tubular NiSA-N-CNT structure most likely occurs via a solid-to-solid curling or rolling-up mechanism, thermally activated at temperatures of 700-900 °C. Extended X-ray absorption fine structure (EXAFS) experiments and simulations show that Ni single atoms are stabilized in the N-CNT structure through nitrogen coordination, forming a structure with four nearest N coordination shell surrounded by two carbon shells, Ni-N4. The NiSA-N-CNT catalysts show an excellent activity and selectivity for the electrochemical reduction of CO2, achieving a turnover frequency (TOF) of 11.7 s-1 at -0.55 V (vs RHE), but a low activity for the O2 reduction and O2 evolution reactions, as compared to Ni nanoparticles supported on N-CNTs.
Details
- Title
- One-Pot Pyrolysis Method to Fabricate Carbon Nanotube Supported Ni Single-Atom Catalysts with Ultrahigh Loading
- Authors
- Shiyong Zhao (Author) - Curtin UniversityYi Cheng (Author) - Curtin UniversityJean-Pierre Veder (Author) - Curtin UniversityBernt Johannessen (Author) - Australian SynchrotronMartin Saunders (Author) - University of Western AustraliaLianji Zhang (Author) - Chinese Academy of Sciences, ChinaChang Liu (Author) - University of Surrey, United KingdomMatthew F Chisholm (Author) - Oak Ridge National Laboratory, United StatesRoland De Marco (Author) - University of the Sunshine CoastJian Liu (Author) - University of Surrey, United KingdomShi-Ze Yang (Author) - Oak Ridge National Laboratory, United StatesSan Ping Jiang (Author) - Oak Ridge National Laboratory, United States
- Publication details
- ACS Applied Energy Materials, Vol.1(10), pp.5286-5297
- Publisher
- American Chemical Society
- DOI
- 10.1021/acsaem.8b00903
- ISSN
- 2574-0962
- Organisation Unit
- Office of the Deputy Vice-Chancellor (Research and Innovation); University of the Sunshine Coast, Queensland
- Language
- English
- Record Identifier
- 99451249102621
- Output Type
- Journal article
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- Chemistry, Physical
- Energy & Fuels
- Materials Science, Multidisciplinary
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