Data-driven screening of pivotal subunits in edge-anchored single atom catalysts for oxygen reactions
Oxygen reduction reaction (ORR) and the oxygen evolution reaction (OER) are key reactions in diverse energy conversion devices, highlighting the importance of efficient catalysts. Edge-anchored single atom catalysts (E-SACs) emerge as a special class of atomic structure, but the detailed configurati...
| Main Authors: | , , , , , , |
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| Format: | Journal Article |
| Language: | English |
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2024
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| Online Access: | https://hdl.handle.net/10356/174656 |
| _version_ | 1826123982329348096 |
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| author | Ye, Qitong Yi, Xingxing Wang, Cai-Zhuang Zhang, Tao Liu, Yipu Lin, Shiwei Fan, Hong Jin |
| author2 | School of Physical and Mathematical Sciences |
| author_facet | School of Physical and Mathematical Sciences Ye, Qitong Yi, Xingxing Wang, Cai-Zhuang Zhang, Tao Liu, Yipu Lin, Shiwei Fan, Hong Jin |
| author_sort | Ye, Qitong |
| collection | NTU |
| description | Oxygen reduction reaction (ORR) and the oxygen evolution reaction (OER) are key reactions in diverse energy conversion devices, highlighting the importance of efficient catalysts. Edge-anchored single atom catalysts (E-SACs) emerge as a special class of atomic structure, but the detailed configuration and its correlation with catalytic activity remain little explored. Herein, a total of 78 E-SACs (E-TM-Nx-C) have been constructed based on 26 transition metal (TM) species with three coordination patterns. Using structural stability and ORR/OER catalytic activity as the evaluation criteria, a few catalytic structures comparable to Pt (111) for ORR and IrO2 (110) for OER are screened based on high-throughput calculations. The screening results unveil that the E-Rh-N4-C configuration exhibits most efficient bifunctional activity for both ORR and OER with an overpotential of 0.38 and 0.61 V, respectively. Electronic structure analysis confirms the distinctive edge effects on the electronic properties of TM and N species, and the feature importance derived from machine learning illustrates the efficacy of E-TM-Nx subunit configuration in determining the catalytic activity of E-SACs. Finally, the trained Gradient Boosting Regression (GBR) model exhibits acceptable accuracy in predicting the OH intermediates adsorption strength for E-SACs, thereby paving the way for expanding catalytic structures based on E-SACs. |
| first_indexed | 2024-10-01T06:13:13Z |
| format | Journal Article |
| id | ntu-10356/174656 |
| institution | Nanyang Technological University |
| language | English |
| last_indexed | 2024-10-01T06:13:13Z |
| publishDate | 2024 |
| record_format | dspace |
| spelling | ntu-10356/1746562024-04-08T15:35:21Z Data-driven screening of pivotal subunits in edge-anchored single atom catalysts for oxygen reactions Ye, Qitong Yi, Xingxing Wang, Cai-Zhuang Zhang, Tao Liu, Yipu Lin, Shiwei Fan, Hong Jin School of Physical and Mathematical Sciences Physics Data-driven screening Edge-anchored single-atom catalysts Oxygen reduction reaction (ORR) and the oxygen evolution reaction (OER) are key reactions in diverse energy conversion devices, highlighting the importance of efficient catalysts. Edge-anchored single atom catalysts (E-SACs) emerge as a special class of atomic structure, but the detailed configuration and its correlation with catalytic activity remain little explored. Herein, a total of 78 E-SACs (E-TM-Nx-C) have been constructed based on 26 transition metal (TM) species with three coordination patterns. Using structural stability and ORR/OER catalytic activity as the evaluation criteria, a few catalytic structures comparable to Pt (111) for ORR and IrO2 (110) for OER are screened based on high-throughput calculations. The screening results unveil that the E-Rh-N4-C configuration exhibits most efficient bifunctional activity for both ORR and OER with an overpotential of 0.38 and 0.61 V, respectively. Electronic structure analysis confirms the distinctive edge effects on the electronic properties of TM and N species, and the feature importance derived from machine learning illustrates the efficacy of E-TM-Nx subunit configuration in determining the catalytic activity of E-SACs. Finally, the trained Gradient Boosting Regression (GBR) model exhibits acceptable accuracy in predicting the OH intermediates adsorption strength for E-SACs, thereby paving the way for expanding catalytic structures based on E-SACs. Submitted/Accepted version This work was supported by the National Natural Science Foundation of China (Grant No. 22369003,Grant No. 52001306 and Grant No. 22005116) and the specific research fund of the Innovation Platform for Academicians of Hainan Province (YSPTZX202123), Hainan Provincial Natural Science Foundation of China (Grant No. 223QN185), Scientific Research Starting Foundation of Hainan University (Grant No. KYQD(ZR)−22022), and the Collaborative Innovation Center project of Hainan University (XTCX2022XXB01). 2024-04-07T02:59:15Z 2024-04-07T02:59:15Z 2024 Journal Article Ye, Q., Yi, X., Wang, C., Zhang, T., Liu, Y., Lin, S. & Fan, H. J. (2024). Data-driven screening of pivotal subunits in edge-anchored single atom catalysts for oxygen reactions. Advanced Functional Materials. https://dx.doi.org/10.1002/adfm.202400107 1616-301X https://hdl.handle.net/10356/174656 10.1002/adfm.202400107 2-s2.0-85185260522 en Advanced Functional Materials © 2024 Wiley-VCH GmbH. All rights reserved. This article may be downloaded for personal use only. Any other use requires prior permission of the copyright holder. The Version of Record is available online at http://doi.org/10.1002/adfm.202400107. application/pdf |
| spellingShingle | Physics Data-driven screening Edge-anchored single-atom catalysts Ye, Qitong Yi, Xingxing Wang, Cai-Zhuang Zhang, Tao Liu, Yipu Lin, Shiwei Fan, Hong Jin Data-driven screening of pivotal subunits in edge-anchored single atom catalysts for oxygen reactions |
| title | Data-driven screening of pivotal subunits in edge-anchored single atom catalysts for oxygen reactions |
| title_full | Data-driven screening of pivotal subunits in edge-anchored single atom catalysts for oxygen reactions |
| title_fullStr | Data-driven screening of pivotal subunits in edge-anchored single atom catalysts for oxygen reactions |
| title_full_unstemmed | Data-driven screening of pivotal subunits in edge-anchored single atom catalysts for oxygen reactions |
| title_short | Data-driven screening of pivotal subunits in edge-anchored single atom catalysts for oxygen reactions |
| title_sort | data driven screening of pivotal subunits in edge anchored single atom catalysts for oxygen reactions |
| topic | Physics Data-driven screening Edge-anchored single-atom catalysts |
| url | https://hdl.handle.net/10356/174656 |
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