Citation: Chaozheng He, Menghui Xi, Chenxu Zhao, Ran Wang, Ling Fu, Jinrong Huo. Highly N₂ dissociation catalyst: Ir(100) and Ir(110) surfaces[J]. Chinese Chemical Letters, ;2025, 36(3): 109671. doi: 10.1016/j.cclet.2024.109671 shu

Highly N₂ dissociation catalyst: Ir(100) and Ir(110) surfaces

Chaozheng He ^a ,
Menghui Xi ^a ,
Chenxu Zhao ^{a, *,} ,
Ran Wang ^a ,
Ling Fu ^{b, *,} ,
Jinrong Huo ^c

a.
Institute of Environmental and Energy Catalysis, Shaanxi Key Laboratory of Optoelectronic Functional Materials and Devices, School of Materials Science and Chemical Engineering, Xi’an Technological University, Xi’an 710021, China
b.
College of Resources and Environmental Engineering, Tianshui Normal University, Tianshui 741001, China
c.
School of Sciences, Xi’an Technological University, Xi’an 710021, China

zhaochenxu@xatu.edu.cn

ful263@nenu.edu.cn

Received Date: 18 December 2023
Revised Date: 21 January 2024
Accepted Date: 22 February 2024
Available Online: 28 February 2024

Figures(5)

Density functional theory (DFT) was performed to systematically study the adsorption and dissociation of N₂ on Ir(100) and Ir(110) surfaces. By analyzing the properties, including adsorption energies, reaction barriers, and optimal adsorption sites, the hollow (H) sites were finally identified as favorable dissociation sites for N₂. The dissociation barriers of N₂ are 0.87 eV on Ir(100) and 1.12 eV on Ir(110), which can be overcome at around 348 and 448 K, respectively. Therefore, Ir(100) is screened as a promising catalyst for N₂ dissociation compared to Ir(110). This can be attributed to the significantly higher adsorption energy of N₂ on the H site of Ir(100) (−0.48 eV) compared to that on Ir(110) (−0.22 eV), leading to different dissociation mechanisms on Ir(100) and Ir(110). Ir(100) can dissociate N₂ directly on H site and Ir(110) should firstly capture N₂ via bridge site and further transfer the adsorbed N₂ to the H site, which will dramatically deteriorate the reactivity of N₂ dissociation. In addition, the following protonation processes of dissociated *N atoms are all exothermal at 348 K on Ir(100), indicating that the ammonia synthesis can occur spontaneously as the temperature higher than 348 K. These results have provided a reasonable materials design scheme for subsequent ammonia synthesis.
- Density functional theory,
- N₂ dissociation,
- Ir surface,
- Ammonia synthesis,
- Anti-bonding orbitals,
- Reaction barrier
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沈阳化工大学材料科学与工程学院沈阳 110142

Highly N2 dissociation catalyst: Ir(100) and Ir(110) surfaces

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通讯作者: 陈斌, bchen63@163.com

Highly N₂ dissociation catalyst: Ir(100) and Ir(110) surfaces