Scalable two-step annealing method for preparing ultra-high-density single-atom catalyst libraries
The stabilization of transition metals as isolated centres with high areal density on suitably tailored carriers is crucial for maximizing the industrial potential of single-atom heterogeneous catalysts. However, achieving single-atom dispersions at metal contents above 2 wt% remains challenging. He...
| Main Authors: | , , , , , , , , , , , , , , , , |
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| Format: | Journal Article |
| Language: | English |
| Published: |
2022
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| Online Access: | https://hdl.handle.net/10356/161098 |
| _version_ | 1811689110468820992 |
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| author | Hai, Xiao Xi, Shibo Mitchell, Sharon Harrath, Karim Xu, Haomin Akl, Dario Faust Kong, Debin Li, Jing Li, Zejun Sun, Tao Yang, Huimin Cui, Yige Su, Chenliang Zhao, Xiaoxu Li, Jun Pérez-Ramírez, Javier Lu, Jiong |
| author2 | School of Materials Science and Engineering |
| author_facet | School of Materials Science and Engineering Hai, Xiao Xi, Shibo Mitchell, Sharon Harrath, Karim Xu, Haomin Akl, Dario Faust Kong, Debin Li, Jing Li, Zejun Sun, Tao Yang, Huimin Cui, Yige Su, Chenliang Zhao, Xiaoxu Li, Jun Pérez-Ramírez, Javier Lu, Jiong |
| author_sort | Hai, Xiao |
| collection | NTU |
| description | The stabilization of transition metals as isolated centres with high areal density on suitably tailored carriers is crucial for maximizing the industrial potential of single-atom heterogeneous catalysts. However, achieving single-atom dispersions at metal contents above 2 wt% remains challenging. Here we introduce a versatile approach combining impregnation and two-step annealing to synthesize ultra-high-density single-atom catalysts with metal contents up to 23 wt% for 15 metals on chemically distinct carriers. Translation to a standardized, automated protocol demonstrates the robustness of our method and provides a path to explore virtually unlimited libraries of mono- or multimetallic catalysts. At the molecular level, characterization of the synthesis mechanism through experiments and simulations shows that controlling the bonding of metal precursors with the carrier via stepwise ligand removal prevents their thermally induced aggregation into nanoparticles. The drastically enhanced reactivity with increasing metal content exemplifies the need to optimize the surface metal density for a given application. Moreover, the loading-dependent site-specific activity observed in three distinct catalytic systems reflects the well-known complexity in heterogeneous catalyst design, which now can be tackled with a library of single-atom catalysts with widely tunable metal loadings. |
| first_indexed | 2024-10-01T05:42:53Z |
| format | Journal Article |
| id | ntu-10356/161098 |
| institution | Nanyang Technological University |
| language | English |
| last_indexed | 2024-10-01T05:42:53Z |
| publishDate | 2022 |
| record_format | dspace |
| spelling | ntu-10356/1610982022-08-15T07:58:04Z Scalable two-step annealing method for preparing ultra-high-density single-atom catalyst libraries Hai, Xiao Xi, Shibo Mitchell, Sharon Harrath, Karim Xu, Haomin Akl, Dario Faust Kong, Debin Li, Jing Li, Zejun Sun, Tao Yang, Huimin Cui, Yige Su, Chenliang Zhao, Xiaoxu Li, Jun Pérez-Ramírez, Javier Lu, Jiong School of Materials Science and Engineering Engineering::Materials Atoms Heterogeneous Catalyst The stabilization of transition metals as isolated centres with high areal density on suitably tailored carriers is crucial for maximizing the industrial potential of single-atom heterogeneous catalysts. However, achieving single-atom dispersions at metal contents above 2 wt% remains challenging. Here we introduce a versatile approach combining impregnation and two-step annealing to synthesize ultra-high-density single-atom catalysts with metal contents up to 23 wt% for 15 metals on chemically distinct carriers. Translation to a standardized, automated protocol demonstrates the robustness of our method and provides a path to explore virtually unlimited libraries of mono- or multimetallic catalysts. At the molecular level, characterization of the synthesis mechanism through experiments and simulations shows that controlling the bonding of metal precursors with the carrier via stepwise ligand removal prevents their thermally induced aggregation into nanoparticles. The drastically enhanced reactivity with increasing metal content exemplifies the need to optimize the surface metal density for a given application. Moreover, the loading-dependent site-specific activity observed in three distinct catalytic systems reflects the well-known complexity in heterogeneous catalyst design, which now can be tackled with a library of single-atom catalysts with widely tunable metal loadings. Ministry of Education (MOE) J. Lu acknowledges support from MOE grant (R-143-000-B47-114), the Ministry of Education (Singapore) through the Research Centre of Excellence program (Award EDUN C-33-18-279-V12, Institute for Functional Intelligent Materials) and the National University of Singapore Flagship Green Energy Program (R-143-000-A55-646). X.Z. acknowledges support from a Presidential Postdoctoral Fellowship, Nanyang Technological University, Singapore via grant 03INS000973C150. S.M., D.F.A., and J.P.-R. acknowledge funding from the NCCR Catalysis, a National Centre of Competence in Research funded by the Swiss National Science Foundation. Jun Li acknowledges financial support by the National Natural Science Foundation of China (grant number 22033005) and the Guangdong Provincial Key Laboratory of Catalysis (2020B121201002). 2022-08-15T07:58:03Z 2022-08-15T07:58:03Z 2022 Journal Article Hai, X., Xi, S., Mitchell, S., Harrath, K., Xu, H., Akl, D. F., Kong, D., Li, J., Li, Z., Sun, T., Yang, H., Cui, Y., Su, C., Zhao, X., Li, J., Pérez-Ramírez, J. & Lu, J. (2022). Scalable two-step annealing method for preparing ultra-high-density single-atom catalyst libraries. Nature Nanotechnology, 17(2), 174-181. https://dx.doi.org/10.1038/s41565-021-01022-y 1748-3387 https://hdl.handle.net/10356/161098 10.1038/s41565-021-01022-y 34824400 2-s2.0-85119827384 2 17 174 181 en R-143-000-B47-114 EDUN C-33-18-279-V12 R-143-000-A55-646 03INS000973C150 Nature Nanotechnology © 2021 The Author(s), under exclusive licence to Springer Nature Limited. All rights reserved. |
| spellingShingle | Engineering::Materials Atoms Heterogeneous Catalyst Hai, Xiao Xi, Shibo Mitchell, Sharon Harrath, Karim Xu, Haomin Akl, Dario Faust Kong, Debin Li, Jing Li, Zejun Sun, Tao Yang, Huimin Cui, Yige Su, Chenliang Zhao, Xiaoxu Li, Jun Pérez-Ramírez, Javier Lu, Jiong Scalable two-step annealing method for preparing ultra-high-density single-atom catalyst libraries |
| title | Scalable two-step annealing method for preparing ultra-high-density single-atom catalyst libraries |
| title_full | Scalable two-step annealing method for preparing ultra-high-density single-atom catalyst libraries |
| title_fullStr | Scalable two-step annealing method for preparing ultra-high-density single-atom catalyst libraries |
| title_full_unstemmed | Scalable two-step annealing method for preparing ultra-high-density single-atom catalyst libraries |
| title_short | Scalable two-step annealing method for preparing ultra-high-density single-atom catalyst libraries |
| title_sort | scalable two step annealing method for preparing ultra high density single atom catalyst libraries |
| topic | Engineering::Materials Atoms Heterogeneous Catalyst |
| url | https://hdl.handle.net/10356/161098 |
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