Boosting ORR performance by single atomic divacancy Zn–N₃C–C₈ sites on ultrathin N-doped carbon nanosheets
Single-atom catalysts (SACs) show great promise to improve the performance of catalysis because of their spatially isolated single-atom sites with unique electronic properties. Herein, we construct single Zn atoms anchored on ultrathin two-dimensional (2D) N-doped carbon nanosheets (Zn–SAs/UNCNS) as...
| Main Authors: | , , , , , , , , , |
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| Other Authors: | |
| Format: | Journal Article |
| Language: | English |
| Published: |
2022
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| Online Access: | https://hdl.handle.net/10356/163192 |
| _version_ | 1826111810189656064 |
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| author | Zhang, Tianyu Wang, Fanping Yang, Can Han, Xu Liang, Chen Zhang, Zedong Li, Yaping Han, Aijuan Liu, Junfeng Liu, Bin |
| author2 | School of Chemical and Biomedical Engineering |
| author_facet | School of Chemical and Biomedical Engineering Zhang, Tianyu Wang, Fanping Yang, Can Han, Xu Liang, Chen Zhang, Zedong Li, Yaping Han, Aijuan Liu, Junfeng Liu, Bin |
| author_sort | Zhang, Tianyu |
| collection | NTU |
| description | Single-atom catalysts (SACs) show great promise to improve the performance of catalysis because of their spatially isolated single-atom sites with unique electronic properties. Herein, we construct single Zn atoms anchored on ultrathin two-dimensional (2D) N-doped carbon nanosheets (Zn–SAs/UNCNS) as an efficient electrocatalyst for oxygen reduction reaction (ORR). The microenvironment of Zn–SAs/UNCNS with super ORR intrinsic activity was identified as the divacancy Zn–N3C–C8 by both experiments and theoretical simulations. Density functional theory (DFT) calculations reveal that the divacancy Zn–N3C–C8 sites exhibit near-Fermi electronic states distinct from those of graphene-enclosed Zn–N4–C10 and divacancy trans-Zn–N2C2–C8 sites, which greatly facilitate the ORR process. Furthermore, compared with 3D architecture, the single atomic divacancy Zn–N3C–C8 sites anchored on ultrathin 2D carbon nanosheets show more active site exposure and fast electron transport, which collectively boost the ORR performance, showing a high half-wave potential of 0.91 V versus reversible hydrogen electrode [RHE] and a super turnover frequency (4.99 e− site−1 s−1). |
| first_indexed | 2024-10-01T02:56:54Z |
| format | Journal Article |
| id | ntu-10356/163192 |
| institution | Nanyang Technological University |
| language | English |
| last_indexed | 2024-10-01T02:56:54Z |
| publishDate | 2022 |
| record_format | dspace |
| spelling | ntu-10356/1631922023-12-18T15:34:43Z Boosting ORR performance by single atomic divacancy Zn–N₃C–C₈ sites on ultrathin N-doped carbon nanosheets Zhang, Tianyu Wang, Fanping Yang, Can Han, Xu Liang, Chen Zhang, Zedong Li, Yaping Han, Aijuan Liu, Junfeng Liu, Bin School of Chemical and Biomedical Engineering School of Physical and Mathematical Sciences Engineering::Chemical engineering Single-Atom Catalyst Microenvironment Regulation Single-atom catalysts (SACs) show great promise to improve the performance of catalysis because of their spatially isolated single-atom sites with unique electronic properties. Herein, we construct single Zn atoms anchored on ultrathin two-dimensional (2D) N-doped carbon nanosheets (Zn–SAs/UNCNS) as an efficient electrocatalyst for oxygen reduction reaction (ORR). The microenvironment of Zn–SAs/UNCNS with super ORR intrinsic activity was identified as the divacancy Zn–N3C–C8 by both experiments and theoretical simulations. Density functional theory (DFT) calculations reveal that the divacancy Zn–N3C–C8 sites exhibit near-Fermi electronic states distinct from those of graphene-enclosed Zn–N4–C10 and divacancy trans-Zn–N2C2–C8 sites, which greatly facilitate the ORR process. Furthermore, compared with 3D architecture, the single atomic divacancy Zn–N3C–C8 sites anchored on ultrathin 2D carbon nanosheets show more active site exposure and fast electron transport, which collectively boost the ORR performance, showing a high half-wave potential of 0.91 V versus reversible hydrogen electrode [RHE] and a super turnover frequency (4.99 e− site−1 s−1). Published version 2022-11-28T07:19:35Z 2022-11-28T07:19:35Z 2022 Journal Article Zhang, T., Wang, F., Yang, C., Han, X., Liang, C., Zhang, Z., Li, Y., Han, A., Liu, J. & Liu, B. (2022). Boosting ORR performance by single atomic divacancy Zn–N₃C–C₈ sites on ultrathin N-doped carbon nanosheets. Chem Catalysis, 2(4), 836-852. https://dx.doi.org/10.1016/j.checat.2022.02.006 2667-1093 https://hdl.handle.net/10356/163192 10.1016/j.checat.2022.02.006 2-s2.0-85128385286 4 2 836 852 en Chem Catalysis © 2022 Elsevier Inc. This is an open-access article distributed under the terms of the Creative Commons CC-BY-NC-ND license. application/pdf |
| spellingShingle | Engineering::Chemical engineering Single-Atom Catalyst Microenvironment Regulation Zhang, Tianyu Wang, Fanping Yang, Can Han, Xu Liang, Chen Zhang, Zedong Li, Yaping Han, Aijuan Liu, Junfeng Liu, Bin Boosting ORR performance by single atomic divacancy Zn–N₃C–C₈ sites on ultrathin N-doped carbon nanosheets |
| title | Boosting ORR performance by single atomic divacancy Zn–N₃C–C₈ sites on ultrathin N-doped carbon nanosheets |
| title_full | Boosting ORR performance by single atomic divacancy Zn–N₃C–C₈ sites on ultrathin N-doped carbon nanosheets |
| title_fullStr | Boosting ORR performance by single atomic divacancy Zn–N₃C–C₈ sites on ultrathin N-doped carbon nanosheets |
| title_full_unstemmed | Boosting ORR performance by single atomic divacancy Zn–N₃C–C₈ sites on ultrathin N-doped carbon nanosheets |
| title_short | Boosting ORR performance by single atomic divacancy Zn–N₃C–C₈ sites on ultrathin N-doped carbon nanosheets |
| title_sort | boosting orr performance by single atomic divacancy zn n₃c c₈ sites on ultrathin n doped carbon nanosheets |
| topic | Engineering::Chemical engineering Single-Atom Catalyst Microenvironment Regulation |
| url | https://hdl.handle.net/10356/163192 |
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