Potassium promoter regulates electronic structure and hydrogen spillover of ultrasmall Ru nanoclusters catalyst for ammonia synthesis
The effects of promoters on Ru nanoparticles (≥2 nm) catalysts for NH3 synthesis have been extensively elaborated, but their roles on ultrasmall Ru nanoclusters (NCs, 1–2 nm) remain largely unknown and need to be further uncovered. Herein, a series of K-promoted MgO supported Ru NCs were synthesized...
Main Authors: | , , , , , , , , , , , , |
---|---|
Other Authors: | |
Format: | Journal Article |
Language: | English |
Published: |
2024
|
Subjects: | |
Online Access: | https://hdl.handle.net/10356/180193 |
_version_ | 1826112923440775168 |
---|---|
author | Peng, Xuanbei Luo, Yongjin Zhang, Tianhua Deng, Jinxiu Zhou, Yanliang Li, Jiaxin Ni, Jun Lin, Bingyu Lin, Jianxin Wu, Dongshuang Zheng, Lirong Wang, Xiuyun Jiang, Lilong |
author2 | School of Materials Science and Engineering |
author_facet | School of Materials Science and Engineering Peng, Xuanbei Luo, Yongjin Zhang, Tianhua Deng, Jinxiu Zhou, Yanliang Li, Jiaxin Ni, Jun Lin, Bingyu Lin, Jianxin Wu, Dongshuang Zheng, Lirong Wang, Xiuyun Jiang, Lilong |
author_sort | Peng, Xuanbei |
collection | NTU |
description | The effects of promoters on Ru nanoparticles (≥2 nm) catalysts for NH3 synthesis have been extensively elaborated, but their roles on ultrasmall Ru nanoclusters (NCs, 1–2 nm) remain largely unknown and need to be further uncovered. Herein, a series of K-promoted MgO supported Ru NCs were synthesized and investigated for NH3 synthesis. The addition of 5wt.%K onto Ru/MgO NCs leads to a significantly high NH3 synthesis rate of 21.7 mmolNH3 gcat−1h−1 at 400 °C and 0.2 MPa, close to the thermodynamic equilibrium. Out studies reveal that anchoring K onto Ru NCs can increase the electron density and cause an upshift of the d-band center of Ru entities. Moreover, the addition of K regulates the hydrogen affinity and accelerates the migration of hydrogen from the Ru NCs surface to MgO support, which is crucial in avoiding the hydrogen poisoning effect on Ru NCs. With the synergistic effect of the Ru NCs sites bridged by H-spillover, makes the K-mediated Ru/MgO NCs catalysts efficient for NH3 synthesis at mild conditions. |
first_indexed | 2024-10-01T03:15:03Z |
format | Journal Article |
id | ntu-10356/180193 |
institution | Nanyang Technological University |
language | English |
last_indexed | 2024-10-01T03:15:03Z |
publishDate | 2024 |
record_format | dspace |
spelling | ntu-10356/1801932024-09-23T07:42:40Z Potassium promoter regulates electronic structure and hydrogen spillover of ultrasmall Ru nanoclusters catalyst for ammonia synthesis Peng, Xuanbei Luo, Yongjin Zhang, Tianhua Deng, Jinxiu Zhou, Yanliang Li, Jiaxin Ni, Jun Lin, Bingyu Lin, Jianxin Wu, Dongshuang Zheng, Lirong Wang, Xiuyun Jiang, Lilong School of Materials Science and Engineering Engineering Ammonia synthesis Ultrasmall Ru nanoclusters The effects of promoters on Ru nanoparticles (≥2 nm) catalysts for NH3 synthesis have been extensively elaborated, but their roles on ultrasmall Ru nanoclusters (NCs, 1–2 nm) remain largely unknown and need to be further uncovered. Herein, a series of K-promoted MgO supported Ru NCs were synthesized and investigated for NH3 synthesis. The addition of 5wt.%K onto Ru/MgO NCs leads to a significantly high NH3 synthesis rate of 21.7 mmolNH3 gcat−1h−1 at 400 °C and 0.2 MPa, close to the thermodynamic equilibrium. Out studies reveal that anchoring K onto Ru NCs can increase the electron density and cause an upshift of the d-band center of Ru entities. Moreover, the addition of K regulates the hydrogen affinity and accelerates the migration of hydrogen from the Ru NCs surface to MgO support, which is crucial in avoiding the hydrogen poisoning effect on Ru NCs. With the synergistic effect of the Ru NCs sites bridged by H-spillover, makes the K-mediated Ru/MgO NCs catalysts efficient for NH3 synthesis at mild conditions. The work was supported by the National Key Research and Development Program (2022YFA1604101, 2021YFB4000400), National Natural Science Foundation of China (22222801, 2221005, 22038002, 92361303, 22108037), and the Key R&D plan of Shanghai Science and Technology Commission (21DZ1209002). 2024-09-23T07:42:40Z 2024-09-23T07:42:40Z 2024 Journal Article Peng, X., Luo, Y., Zhang, T., Deng, J., Zhou, Y., Li, J., Ni, J., Lin, B., Lin, J., Wu, D., Zheng, L., Wang, X. & Jiang, L. (2024). Potassium promoter regulates electronic structure and hydrogen spillover of ultrasmall Ru nanoclusters catalyst for ammonia synthesis. Chemical Engineering Science, 292, 120021-. https://dx.doi.org/10.1016/j.ces.2024.120021 0009-2509 https://hdl.handle.net/10356/180193 10.1016/j.ces.2024.120021 2-s2.0-85188130987 292 120021 en Chemical Engineering Science © 2024 Elsevier Ltd. All rights reserved. |
spellingShingle | Engineering Ammonia synthesis Ultrasmall Ru nanoclusters Peng, Xuanbei Luo, Yongjin Zhang, Tianhua Deng, Jinxiu Zhou, Yanliang Li, Jiaxin Ni, Jun Lin, Bingyu Lin, Jianxin Wu, Dongshuang Zheng, Lirong Wang, Xiuyun Jiang, Lilong Potassium promoter regulates electronic structure and hydrogen spillover of ultrasmall Ru nanoclusters catalyst for ammonia synthesis |
title | Potassium promoter regulates electronic structure and hydrogen spillover of ultrasmall Ru nanoclusters catalyst for ammonia synthesis |
title_full | Potassium promoter regulates electronic structure and hydrogen spillover of ultrasmall Ru nanoclusters catalyst for ammonia synthesis |
title_fullStr | Potassium promoter regulates electronic structure and hydrogen spillover of ultrasmall Ru nanoclusters catalyst for ammonia synthesis |
title_full_unstemmed | Potassium promoter regulates electronic structure and hydrogen spillover of ultrasmall Ru nanoclusters catalyst for ammonia synthesis |
title_short | Potassium promoter regulates electronic structure and hydrogen spillover of ultrasmall Ru nanoclusters catalyst for ammonia synthesis |
title_sort | potassium promoter regulates electronic structure and hydrogen spillover of ultrasmall ru nanoclusters catalyst for ammonia synthesis |
topic | Engineering Ammonia synthesis Ultrasmall Ru nanoclusters |
url | https://hdl.handle.net/10356/180193 |
work_keys_str_mv | AT pengxuanbei potassiumpromoterregulateselectronicstructureandhydrogenspilloverofultrasmallrunanoclusterscatalystforammoniasynthesis AT luoyongjin potassiumpromoterregulateselectronicstructureandhydrogenspilloverofultrasmallrunanoclusterscatalystforammoniasynthesis AT zhangtianhua potassiumpromoterregulateselectronicstructureandhydrogenspilloverofultrasmallrunanoclusterscatalystforammoniasynthesis AT dengjinxiu potassiumpromoterregulateselectronicstructureandhydrogenspilloverofultrasmallrunanoclusterscatalystforammoniasynthesis AT zhouyanliang potassiumpromoterregulateselectronicstructureandhydrogenspilloverofultrasmallrunanoclusterscatalystforammoniasynthesis AT lijiaxin potassiumpromoterregulateselectronicstructureandhydrogenspilloverofultrasmallrunanoclusterscatalystforammoniasynthesis AT nijun potassiumpromoterregulateselectronicstructureandhydrogenspilloverofultrasmallrunanoclusterscatalystforammoniasynthesis AT linbingyu potassiumpromoterregulateselectronicstructureandhydrogenspilloverofultrasmallrunanoclusterscatalystforammoniasynthesis AT linjianxin potassiumpromoterregulateselectronicstructureandhydrogenspilloverofultrasmallrunanoclusterscatalystforammoniasynthesis AT wudongshuang potassiumpromoterregulateselectronicstructureandhydrogenspilloverofultrasmallrunanoclusterscatalystforammoniasynthesis AT zhenglirong potassiumpromoterregulateselectronicstructureandhydrogenspilloverofultrasmallrunanoclusterscatalystforammoniasynthesis AT wangxiuyun potassiumpromoterregulateselectronicstructureandhydrogenspilloverofultrasmallrunanoclusterscatalystforammoniasynthesis AT jianglilong potassiumpromoterregulateselectronicstructureandhydrogenspilloverofultrasmallrunanoclusterscatalystforammoniasynthesis |