Ce和Nb共掺杂提高MnOx催化剂的低温脱硝性能

IF 8.1 1区 工程技术 Q1 ENGINEERING, CHEMICAL Separation and Purification Technology Pub Date : 2025-01-22 DOI:10.1016/j.seppur.2025.131768
Yanping Yang, Shengchen Li, Shunli Shi, Jie Hu, Zexi Xuchen, Shunmin Ding, Dan zhao, Shengjun Deng, Weiming Xiao, Shuhua Wang, Chao Chen
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引用次数: 0

摘要

锰氧化物(MnOx)催化剂以其优异的催化性能在低温nh3选择性催化还原(NH3-SCR)中具有广阔的应用前景。然而,烟气中存在碱金属,特别是钾(K),导致催化剂失活,限制了它们的工业应用。本研究考察了Ce和Nb掺杂对MnOx耐K性和低温NH3-SCR活性的协同效应。Ce和Nb改性可以调节MnOx的表面酸度和氧化还原性能。此外,对K中毒前后催化剂的相结构、表面态和活性位点进行了表征。结果表明,Nb0.05Ce0.05MnOx表现出优异的低温性能,在125 ~ 250℃时NO转化率达到90% %以上,同时具有显著的抗K中毒·NH3-TPD能力,原位实验表明酸位的丢失是K中毒的主要原因。该机理遵循L-H机理,l -酸位点为催化剂表面的主要活性位点,桥接硝酸盐为关键中间态。该研究为提高mnox基催化剂的低温脱氮工业适用性提供了有价值的见解。
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Enhancing the K-resistance of MnOx catalysts via Ce and Nb co-doping for low-temperature NOx elimination
Manganese oxide (MnOx) catalysts are promising for low-temperature NH3-Selective Catalytic Reduction (NH3-SCR) with their superior catalytic performance. However, the presence of alkali metals in flue gases, particularly potassium (K), leads to catalyst deactivation and limits their industrial application. This study investigates the synergistic effects of Ce and Nb doping on the K resistance and low-temperature NH3-SCR activity of MnOx. The surface acidity and redox properties of MnOx were modulated by Ce and Nb modification. In addition, the phase structure, surface state and active sites of the catalysts were characterized before and after K poisoning. The results indicated that Nb0.05Ce0.05MnOx exhibited exceptional low-temperature performance, achieving over 90 % NO conversion at 125-250°C, along with significant resistance to K poisoning·NH3-TPD and in-situ experiments revealed that the loss of acid sites is the primary cause of K poisoning. The mechanism follows the L-H mechanism with L-acid sites as the main active sites on the catalyst surface and bridging nitrate as the key intermediate state. This research provides valuable insights into enhancing the industrial applicability of MnOx-based catalysts for low-temperature denitrification.
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来源期刊
Separation and Purification Technology
Separation and Purification Technology 工程技术-工程:化工
CiteScore
14.00
自引率
12.80%
发文量
2347
审稿时长
43 days
期刊介绍: Separation and Purification Technology is a premier journal committed to sharing innovative methods for separation and purification in chemical and environmental engineering, encompassing both homogeneous solutions and heterogeneous mixtures. Our scope includes the separation and/or purification of liquids, vapors, and gases, as well as carbon capture and separation techniques. However, it's important to note that methods solely intended for analytical purposes are not within the scope of the journal. Additionally, disciplines such as soil science, polymer science, and metallurgy fall outside the purview of Separation and Purification Technology. Join us in advancing the field of separation and purification methods for sustainable solutions in chemical and environmental engineering.
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