Ru alloying with La or Y for ammonia synthesis via integrated dissociative and associative mechanism with superior operational stability

Tianhua Zhang; Jie Zhu; Junjie Wang; Xuanbei Peng; Jinxiu Deng; Shiyao Wang; Yi Song; Yanliang Zhou; Jun Ni; Xiuyun Wang; Shijing Liang; Xingyi Lin; Ying Zheng; Lirong Zheng; Chak tong Au; Lilong Jiang

doi:10.1016/j.ces.2021.117255

Ru alloying with La or Y for ammonia synthesis via integrated dissociative and associative mechanism with superior operational stability

Tianhua Zhang
, Jie Zhu
, Junjie Wang
, Xuanbei Peng
, Jinxiu Deng
, Shiyao Wang
, Yi Song
, Yanliang Zhou
, Jun Ni
, Xiuyun Wang
, Shijing Liang
, Xingyi Lin
, Ying Zheng
, Lirong Zheng
, Chak tong Au
, Lilong Jiang

School of Materials Sience and Engineering

Fuzhou University
Northwestern Polytechnical University Xian
Western University
CAS - Institute of High Energy Physics

Research output: Contribution to journal › Article › peer-review

19 Scopus citations

Abstract

The alloying of Ru with rare-earth elements (REEs) is an effective approach for the modification of the electronic structure of Ru. Here, for the first time, we report the formation of Ru-M (M = La or Y) alloys that are endowed with a completely new type of active sites. Over the Ru-M (M = La or Y) catalysts, N₂ activation in ammonia synthesis follows neither the well-known dissociative nor the associative route but rather a co-operation of both, leading to outstanding performance. The developed RuLa/HZ catalyst exhibits a NH₃ synthesis rate of 14.73 mmol g_cat⁻¹ h⁻¹ at 400 °C and 1 MPa without obvious deactivation in a run of 1756 h (ca.73 days).

Original language	English
Article number	117255
Journal	Chemical Engineering Science
Volume	252
DOIs	https://doi.org/10.1016/j.ces.2021.117255
State	Published - 28 Apr 2022

Keywords

Ammonia synthesis
DFT calculation
Integration of the dissociative and associative mechanism
Maximization of electronic effect
Ru-M (M=La or Y) alloying

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10.1016/j.ces.2021.117255

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Zhang, T., Zhu, J., Wang, J., Peng, X., Deng, J., Wang, S., Song, Y., Zhou, Y., Ni, J., Wang, X., Liang, S., Lin, X., Zheng, Y., Zheng, L., Au, C. T., & Jiang, L. (2022). Ru alloying with La or Y for ammonia synthesis via integrated dissociative and associative mechanism with superior operational stability. Chemical Engineering Science, 252, Article 117255. https://doi.org/10.1016/j.ces.2021.117255

@article{8a58170c49cf4f5697ac6182463a8569,

title = "Ru alloying with La or Y for ammonia synthesis via integrated dissociative and associative mechanism with superior operational stability",

abstract = "The alloying of Ru with rare-earth elements (REEs) is an effective approach for the modification of the electronic structure of Ru. Here, for the first time, we report the formation of Ru-M (M = La or Y) alloys that are endowed with a completely new type of active sites. Over the Ru-M (M = La or Y) catalysts, N2 activation in ammonia synthesis follows neither the well-known dissociative nor the associative route but rather a co-operation of both, leading to outstanding performance. The developed RuLa/HZ catalyst exhibits a NH3 synthesis rate of 14.73 mmol gcat−1 h−1 at 400 °C and 1 MPa without obvious deactivation in a run of 1756 h (ca.73 days).",

keywords = "Ammonia synthesis, DFT calculation, Integration of the dissociative and associative mechanism, Maximization of electronic effect, Ru-M (M=La or Y) alloying",

author = "Tianhua Zhang and Jie Zhu and Junjie Wang and Xuanbei Peng and Jinxiu Deng and Shiyao Wang and Yi Song and Yanliang Zhou and Jun Ni and Xiuyun Wang and Shijing Liang and Xingyi Lin and Ying Zheng and Lirong Zheng and Au, \{Chak tong\} and Lilong Jiang",

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year = "2022",

month = apr,

day = "28",

doi = "10.1016/j.ces.2021.117255",

language = "英语",

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Zhang, T, Zhu, J, Wang, J, Peng, X, Deng, J, Wang, S, Song, Y, Zhou, Y, Ni, J, Wang, X, Liang, S, Lin, X, Zheng, Y, Zheng, L, Au, CT & Jiang, L 2022, 'Ru alloying with La or Y for ammonia synthesis via integrated dissociative and associative mechanism with superior operational stability', Chemical Engineering Science, vol. 252, 117255. https://doi.org/10.1016/j.ces.2021.117255

TY - JOUR

T1 - Ru alloying with La or Y for ammonia synthesis via integrated dissociative and associative mechanism with superior operational stability

AU - Zhang, Tianhua

AU - Zhu, Jie

AU - Wang, Junjie

AU - Peng, Xuanbei

AU - Deng, Jinxiu

AU - Wang, Shiyao

AU - Song, Yi

AU - Zhou, Yanliang

AU - Ni, Jun

AU - Wang, Xiuyun

AU - Liang, Shijing

AU - Lin, Xingyi

AU - Zheng, Ying

AU - Zheng, Lirong

AU - Au, Chak tong

AU - Jiang, Lilong

PY - 2022/4/28

Y1 - 2022/4/28

N2 - The alloying of Ru with rare-earth elements (REEs) is an effective approach for the modification of the electronic structure of Ru. Here, for the first time, we report the formation of Ru-M (M = La or Y) alloys that are endowed with a completely new type of active sites. Over the Ru-M (M = La or Y) catalysts, N2 activation in ammonia synthesis follows neither the well-known dissociative nor the associative route but rather a co-operation of both, leading to outstanding performance. The developed RuLa/HZ catalyst exhibits a NH3 synthesis rate of 14.73 mmol gcat−1 h−1 at 400 °C and 1 MPa without obvious deactivation in a run of 1756 h (ca.73 days).

AB - The alloying of Ru with rare-earth elements (REEs) is an effective approach for the modification of the electronic structure of Ru. Here, for the first time, we report the formation of Ru-M (M = La or Y) alloys that are endowed with a completely new type of active sites. Over the Ru-M (M = La or Y) catalysts, N2 activation in ammonia synthesis follows neither the well-known dissociative nor the associative route but rather a co-operation of both, leading to outstanding performance. The developed RuLa/HZ catalyst exhibits a NH3 synthesis rate of 14.73 mmol gcat−1 h−1 at 400 °C and 1 MPa without obvious deactivation in a run of 1756 h (ca.73 days).

KW - Ammonia synthesis

KW - DFT calculation

KW - Integration of the dissociative and associative mechanism

KW - Maximization of electronic effect

KW - Ru-M (M=La or Y) alloying

UR - https://www.scopus.com/pages/publications/85119902430

U2 - 10.1016/j.ces.2021.117255

DO - 10.1016/j.ces.2021.117255

M3 - 文章

AN - SCOPUS:85119902430

SN - 0009-2509

VL - 252

JO - Chemical Engineering Science

JF - Chemical Engineering Science

M1 - 117255

ER -

Ru alloying with La or Y for ammonia synthesis via integrated dissociative and associative mechanism with superior operational stability

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