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...

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Main Authors: 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
Other Authors: School of Materials Science and Engineering
Format: Journal Article
Language:English
Published: 2024
Subjects:
Online Access:https://hdl.handle.net/10356/180193
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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
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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
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