Oxygen-Doped γ-Mo2N as High-Performance Catalyst for Ammonia Decomposition

IF 12.1 2区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Small Pub Date : 2025-02-16 DOI:10.1002/smll.202410803
Yi Shi, Xiao Wang, Lingling Zhang, Xiang Chu, Li Liu, Baokang Geng, Ruize Jiang, Shibo Zhang, Shuyan Song, Hongjie Zhang
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Abstract

γ-Mo2N catalysts exhibit excellent activity and stability in ammonia decomposition reactions. However, the influence of oxygen on its activity is still unknown. In this work, two γ-Mo2N catalysts with different oxygen content are synthesized using temperature-programmed nitridation of α-MoO3. The γ-Mo2N catalysts are highly oxidized and their ammonia decomposition performance is closely related to their oxygen content. The activity of γ-Mo2N with high oxygen content (HO-γ-Mo2N) is much higher, whose H2 formation rate at 550 °C is 3.3 times higher than the γ-Mo2N with low oxygen content (LO-γ-Mo2N). This is mainly attributed to two aspects: on the one hand, the higher valence state of Mo in the HO-γ-Mo2N leads to stronger Mo─NH3 bonds, which promotes the adsorption and activation of NH3. On the other hand, the H generated by N─H bond breaking is more easily migrated to O, which avoids excessive H occupying the γ-Mo2N active sites and alleviates the negative effect of hydrogen poisoning.

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掺氧γ-Mo2N作为氨分解的高性能催化剂
γ-Mo2N催化剂在氨分解反应中表现出良好的活性和稳定性。然而,氧对其活性的影响尚不清楚。本文采用α-MoO3的程序升温硝化法制备了两种不同氧含量的γ-Mo2N催化剂。γ-Mo2N催化剂具有高氧化性,其氨分解性能与其氧含量密切相关。高氧含量γ-Mo2N (HO-γ-Mo2N)的活性要高得多,在550℃时的H2生成速率是低氧含量γ-Mo2N (LO-γ-Mo2N)的3.3倍。这主要归因于两个方面:一方面,Mo在HO-γ-Mo2N中的价态越高,Mo─NH3键越强,促进了NH3的吸附和活化。另一方面,N─H键断裂产生的H更容易向O迁移,避免了过量的H占据γ-Mo2N活性位点,减轻了氢中毒的负面影响。
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来源期刊
Small
Small 工程技术-材料科学:综合
CiteScore
17.70
自引率
3.80%
发文量
1830
审稿时长
2.1 months
期刊介绍: Small serves as an exceptional platform for both experimental and theoretical studies in fundamental and applied interdisciplinary research at the nano- and microscale. The journal offers a compelling mix of peer-reviewed Research Articles, Reviews, Perspectives, and Comments. With a remarkable 2022 Journal Impact Factor of 13.3 (Journal Citation Reports from Clarivate Analytics, 2023), Small remains among the top multidisciplinary journals, covering a wide range of topics at the interface of materials science, chemistry, physics, engineering, medicine, and biology. Small's readership includes biochemists, biologists, biomedical scientists, chemists, engineers, information technologists, materials scientists, physicists, and theoreticians alike.
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