Study on the Effect and Mechanism of Support and Deposition-Precipitation Method on Ru-Based Catalysts for Ammonia Decomposition

IF 3.8 3区工程技术 Q2 ENGINEERING, CHEMICAL

Industrial & Engineering Chemistry Research Pub Date : 2024-12-10 DOI:10.1021/acs.iecr.4c03838

Bin Guan, Junyan Chen, Zhongqi Zhuang, Lei Zhu, Zeren Ma, Xuehan Hu, Chenyu Zhu, Sikai Zhao, Kaiyou Shu, Hongtao Dang, Junjie Gao, Luyang Zhang, Tiankui Zhu, Zhen Huang

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Abstract

Herein, the effects of support and the deposition-precipitation method on the Ru-based catalysts for NH₃ decomposition were studied. The results of the performance test, characterization, and DFT simulation show that the activity order of the catalysts with different supports is 5% Ru/MgO > 5% Ru/Al₂O₃ > 5% Ru/Pr₂O₃ > 5% Ru/La₂O₃. Ru/MgO exhibits the best ammonia decomposition performance (T₈₀ ≈ 480 °C), because its suitable pore structure is conducive to ammonia adsorption, and abundant strong alkaline sites produce a strong metal–support interaction. The ammonia decomposition performance of 5% Ru/MgO (DP) prepared by the deposition-precipitation method is much higher than that of 5% Ru/MgO (IM) prepared by the impregnation method (T₈₀ decreases from 480 to 440 °C). On Ru/MgO (DP), the distribution of Ru particles is more uniform and the particle size is relatively consistent, and the Ru/MgO (DP) has more basic sites and a more reasonable ratio of lattice oxygen to defect oxygen. Calculated by DFT, the energy barrier of the first dehydrogenation of NH₃ and the combined desorption of N is 1.31 and 1.51 eV, respectively, and the latter is the rate-determining step of the ammonia decomposition reaction in Ru/MgO.

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来源期刊

Industrial & Engineering Chemistry Research 工程技术-工程：化工

CiteScore

7.40

自引率

7.10%

发文量

1467

审稿时长

2.8 months

期刊介绍： ndustrial & Engineering Chemistry, with variations in title and format, has been published since 1909 by the American Chemical Society. Industrial & Engineering Chemistry Research is a weekly publication that reports industrial and academic research in the broad fields of applied chemistry and chemical engineering with special focus on fundamentals, processes, and products.