铁掺杂和氧化物杂化的协同作用增强了锰氧化物催化剂的低温NH3-SCR性能

IF 2.3 4区 化学 Q3 CHEMISTRY, PHYSICAL
Xuewen Li, Yaru Li, Menglin Wang, Can Wang, Wenxian Jing, Lisheng Fang, Yonghua Hu, Yundong Liang, Xianbiao Wang
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引用次数: 0

摘要

锰氧化物(MnOx)催化剂在低温氨选择性催化还原(NH₃-SCR)中具有良好的应用前景,但其对N₂选择性的限制和工作温度范围的狭窄仍然是挑战。为了解决这些问题,我们开发了一种浸渍掺杂和高温煅烧的方法,将Mn₂O₃与铁晶格和氧化物杂化。该杂化催化剂在175-300℃的宽温度范围内保持了90%以上的NOx转化率,同时实现了99%以上的N₂选择性。制备的Fe-Mn(0.15)呈球形,Fe和Mn均匀分布。通过XPS、XAFS、H₂-TPR、NH₃-TPD和催化活性测试,证实了晶格铁的掺杂略微降低了催化剂的还原性,并通过增加Lewis酸位提高了催化剂的低温活性(100-200℃)。同时,Fe₂O₃结构域通过丰富表面氧和Bronsted酸位点提高了高温性能(200-300℃)。这些协同作用调节了催化剂的酸性和氧化还原性能,促进了NH3的活化,同时抑制了过度氧化,从而获得了优异的NH3- scr性能。此外,现场DRIFTS测量证实,反应主要通过Langmuir-Hinshelwood (L-H)机制进行。这项工作揭示了Fe晶格掺杂和Fe₂O₃复合材料对MnOx的协同作用,为开发先进的低温催化剂提供了新的见解。图形抽象
本文章由计算机程序翻译,如有差异,请以英文原文为准。
Synergistic Effect of Iron Doping and Oxide Hybridization Enables Enhanced Low-Temperature NH3-SCR Performance of Manganese Oxide Catalyst

Manganese oxides (MnOx) catalysts are promising for low-temperature ammonia-selective catalytic reduction (NH₃-SCR), however, the limited N₂ selectivity and the narrow operational temperature range remain challenges. To address these issues, we developed a method involving impregnation doping and high-temperature calcination to hybridize Mn₂O₃ with iron lattice and oxide. This hybrid catalyst maintains a NOx conversion rate above 90% within the broad temperature window of 175–300 °C, while achieving N₂ selectivity above 99%. The as prepared Fe-Mn (0.15) exhibits spherical morphology with Fe and Mn uniformly distributed. Through XPS, XAFS, H₂-TPR, NH₃-TPD and catalytic activity tests, we verified that lattice iron doping slightly reduces the reducibility of the catalyst and enhances low-temperature activity (100–200 °C) by increasing Lewis acid sites. Meanwhile, the Fe₂O₃ domains promote high-temperature performance (200–300 °C) by enriching surface oxygen species and Bronsted acid sites. These synergistic effect regulates both the acidic and redox properties of the catalyst, facilitating NH3 activation while suppressing over-oxidation, leading to superior NH3-SCR performance. Furthermore, in situ DRIFTS measurements confirmed that the reaction proceeds predominantly via a Langmuir-Hinshelwood (L-H) mechanism. This work reveals the synergistic effects of Fe lattice doping and Fe₂O₃ composite on MnOx, offering new insights for developing advanced low-temperature catalysts.

Graphical Abstract

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来源期刊
Catalysis Letters
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.
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