Study on the Effect and Mechanism of Ru Precursors and Alkali Metal Modification on Ru/Pr6O11 Catalysts for Ammonia Decomposition

IF 2.3 4区化学 Q3 CHEMISTRY, PHYSICAL

Catalysis Letters Pub Date : 2025-04-04 DOI:10.1007/s10562-025-04992-z

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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引用次数: 0

Abstract

Facing with the problem of low activity at low temperatures of Ru-based ammonia decomposition catalyst, herein, the influence of Ru precursor and alkali metal modification on the hydrogen production activity of Ru/Pr₆O₁₁ catalyst were studied. The Cs/Ru₃(CO)₁₂/Pr₆O₁₁ catalyst exhibited the optimal activity (NH₃ conversion of 46.1% and H₂ production rate of 1.024 mmol·min⁻¹·gcat⁻¹ at 350 °C). Characterizations showed that Ru₃(CO)₁₂/Pr₆O₁₁ has the smallest Ru particle size and the most uniform size distribution, and the existence of PrO₂ phase in Ru(NO)(NO₃)₃/Pr₆O₁₁ and Cl⁻ groups in RuCl₃/Pr₆O₁₁ reduce the activity. Additionally, due to hydrogen spillover, SMSI and Ru re-distribution, the more alkaline alkali metal has a stronger promoting effect, which follows the law of volcanic curve. In-situ DRIFTS and DFT calculations showed that the rate determining step on Ru(0001) surface is the first dehydrogenation step of NH₃ with the activation barrier of 2.19 eV.

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来源期刊

Catalysis Letters 化学-物理化学

CiteScore

5.70

自引率

3.60%

发文量

327

审稿时长

1 months

期刊介绍： Catalysis Letters aim is the rapid publication of outstanding and high-impact original research articles in catalysis. The scope of the journal covers a broad range of topics in all fields of both applied and theoretical catalysis, including heterogeneous, homogeneous and biocatalysis. The high-quality original research articles published in Catalysis Letters are subject to rigorous peer review. Accepted papers are published online first and subsequently in print issues. All contributions must include a graphical abstract. Manuscripts should be written in English and the responsibility lies with the authors to ensure that they are grammatically and linguistically correct. Authors for whom English is not the working language are encouraged to consider using a professional language-editing service before submitting their manuscripts.