One-Pot Pyrolysis Method to Fabricate Carbon Nanotube Supported Ni Single-Atom Catalysts with Ultrahigh Loading
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 us...
| Main Authors: | , , , , , , , , , , , |
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| Format: | Journal Article |
| Language: | English |
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AMER CHEMICAL SOC
2018
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| Subjects: | |
| Online Access: | http://purl.org/au-research/grants/arc/DP180100568 http://hdl.handle.net/20.500.11937/90958 |
| _version_ | 1848765472004112384 |
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| author | Zhao, S. Cheng, Yi Veder, Jean-Pierre Johannessen, B. Saunders, M. Zhang, L. Liu, C. Chisholm, M.F. De Marco, Roland Liu, Jian Yang, S.Z. Jiang, San Ping |
| author_facet | Zhao, S. Cheng, Yi Veder, Jean-Pierre Johannessen, B. Saunders, M. Zhang, L. Liu, C. Chisholm, M.F. De Marco, Roland Liu, Jian Yang, S.Z. Jiang, San Ping |
| author_sort | Zhao, S. |
| building | Curtin Institutional Repository |
| collection | Online Access |
| description | 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. |
| first_indexed | 2025-11-14T11:35:47Z |
| format | Journal Article |
| id | curtin-20.500.11937-90958 |
| institution | Curtin University Malaysia |
| institution_category | Local University |
| language | English |
| last_indexed | 2025-11-14T11:35:47Z |
| publishDate | 2018 |
| publisher | AMER CHEMICAL SOC |
| recordtype | eprints |
| repository_type | Digital Repository |
| spelling | curtin-20.500.11937-909582023-05-03T07:27:02Z One-Pot Pyrolysis Method to Fabricate Carbon Nanotube Supported Ni Single-Atom Catalysts with Ultrahigh Loading Zhao, S. Cheng, Yi Veder, Jean-Pierre Johannessen, B. Saunders, M. Zhang, L. Liu, C. Chisholm, M.F. De Marco, Roland Liu, Jian Yang, S.Z. Jiang, San Ping Science & Technology Physical Sciences Technology Chemistry, Physical Energy & Fuels Materials Science, Multidisciplinary Chemistry Materials Science Ni single-atom catalysts bamboo-like carbon nanotubes one-pot pyrolysis synthesis rolling-up mechanism carbon dioxide reduction TOTAL-ENERGY CALCULATIONS EFFICIENT REDUCTION GRAPHENE NICKEL CO DIOXIDE ELECTROCATALYST NANOPARTICLES PERFORMANCE 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. 2018 Journal Article http://hdl.handle.net/20.500.11937/90958 10.1021/acsaem.8b00903 English http://purl.org/au-research/grants/arc/DP180100568 http://purl.org/au-research/grants/arc/DP180100731 AMER CHEMICAL SOC fulltext |
| spellingShingle | Science & Technology Physical Sciences Technology Chemistry, Physical Energy & Fuels Materials Science, Multidisciplinary Chemistry Materials Science Ni single-atom catalysts bamboo-like carbon nanotubes one-pot pyrolysis synthesis rolling-up mechanism carbon dioxide reduction TOTAL-ENERGY CALCULATIONS EFFICIENT REDUCTION GRAPHENE NICKEL CO DIOXIDE ELECTROCATALYST NANOPARTICLES PERFORMANCE Zhao, S. Cheng, Yi Veder, Jean-Pierre Johannessen, B. Saunders, M. Zhang, L. Liu, C. Chisholm, M.F. De Marco, Roland Liu, Jian Yang, S.Z. Jiang, San Ping One-Pot Pyrolysis Method to Fabricate Carbon Nanotube Supported Ni Single-Atom Catalysts with Ultrahigh Loading |
| title | One-Pot Pyrolysis Method to Fabricate Carbon Nanotube Supported Ni Single-Atom Catalysts with Ultrahigh Loading |
| title_full | One-Pot Pyrolysis Method to Fabricate Carbon Nanotube Supported Ni Single-Atom Catalysts with Ultrahigh Loading |
| title_fullStr | One-Pot Pyrolysis Method to Fabricate Carbon Nanotube Supported Ni Single-Atom Catalysts with Ultrahigh Loading |
| title_full_unstemmed | One-Pot Pyrolysis Method to Fabricate Carbon Nanotube Supported Ni Single-Atom Catalysts with Ultrahigh Loading |
| title_short | One-Pot Pyrolysis Method to Fabricate Carbon Nanotube Supported Ni Single-Atom Catalysts with Ultrahigh Loading |
| title_sort | one-pot pyrolysis method to fabricate carbon nanotube supported ni single-atom catalysts with ultrahigh loading |
| topic | Science & Technology Physical Sciences Technology Chemistry, Physical Energy & Fuels Materials Science, Multidisciplinary Chemistry Materials Science Ni single-atom catalysts bamboo-like carbon nanotubes one-pot pyrolysis synthesis rolling-up mechanism carbon dioxide reduction TOTAL-ENERGY CALCULATIONS EFFICIENT REDUCTION GRAPHENE NICKEL CO DIOXIDE ELECTROCATALYST NANOPARTICLES PERFORMANCE |
| url | http://purl.org/au-research/grants/arc/DP180100568 http://purl.org/au-research/grants/arc/DP180100568 http://hdl.handle.net/20.500.11937/90958 |