Controlled One-pot Synthesis of Nickel Single Atoms Embedded in Carbon Nanotube and Graphene Supports with High Loading
Single-atom catalysts (SACs) have attracted much attentions due to the advantages of high catalysis efficiency and selectivity. However, the controllable and efficient synthesis of SACs remains a significant challenge. Herein, we report a controlled one-pot synthesis of nickel single atoms embedded...
| Main Authors: | , , , , , , , , , , , , , |
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| Format: | Journal Article |
| Language: | English |
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WILEY-V C H VERLAG GMBH
2020
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| Online Access: | https://onlinelibrary.wiley.com/doi/am-pdf/10.1002/cnma.202000223 http://hdl.handle.net/20.500.11937/90803 |
| _version_ | 1848765432681463808 |
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| author | Zhao, Shiyong Wang, T. Zhou, G. Zhang, L. Lin, C. Veder, Jean-Pierre Johannessen, B. Saunders, M. Yin, L. Liu, C. De Marco, Roland Yang, S.Z. Zhang, Q. Jiang, San Ping |
| author_facet | Zhao, Shiyong Wang, T. Zhou, G. Zhang, L. Lin, C. Veder, Jean-Pierre Johannessen, B. Saunders, M. Yin, L. Liu, C. De Marco, Roland Yang, S.Z. Zhang, Q. Jiang, San Ping |
| author_sort | Zhao, Shiyong |
| building | Curtin Institutional Repository |
| collection | Online Access |
| description | Single-atom catalysts (SACs) have attracted much attentions due to the advantages of high catalysis efficiency and selectivity. However, the controllable and efficient synthesis of SACs remains a significant challenge. Herein, we report a controlled one-pot synthesis of nickel single atoms embedded on nitrogen-doped carbon nanotubes (NiSA−N−CNT) and nitrogen-doped graphene (NiSA−N−G). The formation of NiSA−N−CNT is due to the solid-to-solid rolling up mechanism during the high temperature pyrolysis at 800 °C from the stacked and layered Ni-doped g-C3N4, g-C3N4−Ni structure to a tubular CNT structure. Addition of citric acid introduces an amorphous carbon source on the layered g-C3N4−Ni and after annealing at the same temperature of 800 °C, instead of formation of NiSA−N−CNT, Ni single atoms embedded in planar graphene type supports, NiSA−N−G were obtained. The density functional theory (DFT) calculation indicates the introduction of amorphous carbon source substantially reduces the structure fluctuation or curvature of layered g-C3N4-Ni intermediate products, thus interrupting the solid-to-solid rolling process and leading to the formation of planar graphene type supports for Ni single atoms. The as-synthesized NiSA−N−G with Ni atomic loading of ∼6 wt% catalysts shows a better activity and stability for the CO2 reduction reaction (CO2RR) than NiSA−N−CNT with Ni atomic loading of ∼15 wt% due to the open and exposed Ni single atom active sites in NiSA−N−G. This study demonstrates for the first time the feasibility in the control of the microstructure of carbon supports in the synthesis of SACs. |
| first_indexed | 2025-11-14T11:35:10Z |
| format | Journal Article |
| id | curtin-20.500.11937-90803 |
| institution | Curtin University Malaysia |
| institution_category | Local University |
| language | English |
| last_indexed | 2025-11-14T11:35:10Z |
| publishDate | 2020 |
| publisher | WILEY-V C H VERLAG GMBH |
| recordtype | eprints |
| repository_type | Digital Repository |
| spelling | curtin-20.500.11937-908032023-05-04T08:12:42Z Controlled One-pot Synthesis of Nickel Single Atoms Embedded in Carbon Nanotube and Graphene Supports with High Loading Zhao, Shiyong Wang, T. Zhou, G. Zhang, L. Lin, C. Veder, Jean-Pierre Johannessen, B. Saunders, M. Yin, L. Liu, C. De Marco, Roland Yang, S.Z. Zhang, Q. Jiang, San Ping Science & Technology Physical Sciences Technology Chemistry, Multidisciplinary Nanoscience & Nanotechnology Materials Science, Multidisciplinary Chemistry Science & Technology - Other Topics Materials Science Ni single-atom catalysts controlled synthesis carbon nanotube graphene carbon dioxide reduction (CO2RR) METAL-ORGANIC FRAMEWORKS OXYGEN REDUCTION ACTIVE-SITES CATALYSTS EFFICIENT ELECTROCATALYSTS PERFORMANCE NANOSHEETS EVOLUTION OXIDATION Single-atom catalysts (SACs) have attracted much attentions due to the advantages of high catalysis efficiency and selectivity. However, the controllable and efficient synthesis of SACs remains a significant challenge. Herein, we report a controlled one-pot synthesis of nickel single atoms embedded on nitrogen-doped carbon nanotubes (NiSA−N−CNT) and nitrogen-doped graphene (NiSA−N−G). The formation of NiSA−N−CNT is due to the solid-to-solid rolling up mechanism during the high temperature pyrolysis at 800 °C from the stacked and layered Ni-doped g-C3N4, g-C3N4−Ni structure to a tubular CNT structure. Addition of citric acid introduces an amorphous carbon source on the layered g-C3N4−Ni and after annealing at the same temperature of 800 °C, instead of formation of NiSA−N−CNT, Ni single atoms embedded in planar graphene type supports, NiSA−N−G were obtained. The density functional theory (DFT) calculation indicates the introduction of amorphous carbon source substantially reduces the structure fluctuation or curvature of layered g-C3N4-Ni intermediate products, thus interrupting the solid-to-solid rolling process and leading to the formation of planar graphene type supports for Ni single atoms. The as-synthesized NiSA−N−G with Ni atomic loading of ∼6 wt% catalysts shows a better activity and stability for the CO2 reduction reaction (CO2RR) than NiSA−N−CNT with Ni atomic loading of ∼15 wt% due to the open and exposed Ni single atom active sites in NiSA−N−G. This study demonstrates for the first time the feasibility in the control of the microstructure of carbon supports in the synthesis of SACs. 2020 Journal Article http://hdl.handle.net/20.500.11937/90803 10.1002/cnma.202000223 English https://onlinelibrary.wiley.com/doi/am-pdf/10.1002/cnma.202000223 http://purl.org/au-research/grants/arc/DP180100568 http://purl.org/au-research/grants/arc/DP180100731 WILEY-V C H VERLAG GMBH unknown |
| spellingShingle | Science & Technology Physical Sciences Technology Chemistry, Multidisciplinary Nanoscience & Nanotechnology Materials Science, Multidisciplinary Chemistry Science & Technology - Other Topics Materials Science Ni single-atom catalysts controlled synthesis carbon nanotube graphene carbon dioxide reduction (CO2RR) METAL-ORGANIC FRAMEWORKS OXYGEN REDUCTION ACTIVE-SITES CATALYSTS EFFICIENT ELECTROCATALYSTS PERFORMANCE NANOSHEETS EVOLUTION OXIDATION Zhao, Shiyong Wang, T. Zhou, G. Zhang, L. Lin, C. Veder, Jean-Pierre Johannessen, B. Saunders, M. Yin, L. Liu, C. De Marco, Roland Yang, S.Z. Zhang, Q. Jiang, San Ping Controlled One-pot Synthesis of Nickel Single Atoms Embedded in Carbon Nanotube and Graphene Supports with High Loading |
| title | Controlled One-pot Synthesis of Nickel Single Atoms Embedded in Carbon Nanotube and Graphene Supports with High Loading |
| title_full | Controlled One-pot Synthesis of Nickel Single Atoms Embedded in Carbon Nanotube and Graphene Supports with High Loading |
| title_fullStr | Controlled One-pot Synthesis of Nickel Single Atoms Embedded in Carbon Nanotube and Graphene Supports with High Loading |
| title_full_unstemmed | Controlled One-pot Synthesis of Nickel Single Atoms Embedded in Carbon Nanotube and Graphene Supports with High Loading |
| title_short | Controlled One-pot Synthesis of Nickel Single Atoms Embedded in Carbon Nanotube and Graphene Supports with High Loading |
| title_sort | controlled one-pot synthesis of nickel single atoms embedded in carbon nanotube and graphene supports with high loading |
| topic | Science & Technology Physical Sciences Technology Chemistry, Multidisciplinary Nanoscience & Nanotechnology Materials Science, Multidisciplinary Chemistry Science & Technology - Other Topics Materials Science Ni single-atom catalysts controlled synthesis carbon nanotube graphene carbon dioxide reduction (CO2RR) METAL-ORGANIC FRAMEWORKS OXYGEN REDUCTION ACTIVE-SITES CATALYSTS EFFICIENT ELECTROCATALYSTS PERFORMANCE NANOSHEETS EVOLUTION OXIDATION |
| url | https://onlinelibrary.wiley.com/doi/am-pdf/10.1002/cnma.202000223 https://onlinelibrary.wiley.com/doi/am-pdf/10.1002/cnma.202000223 https://onlinelibrary.wiley.com/doi/am-pdf/10.1002/cnma.202000223 http://hdl.handle.net/20.500.11937/90803 |