Unlocking Optimal Performance of PGM-Free CeCuOx Mixed Oxide Catalysts for CO and C3H6 Emission Conversion

IF 2.3 4区 化学 Q3 CHEMISTRY, PHYSICAL
Sheikh Muhammad Farhan, Longwei Cheng, Pan Wang, JianJun Yin, Zhijian Chen
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Abstract

A sustainable and cost-effective alternative for environmental applications is the use of PGM-free catalysts, which are crucial for pollutant removal. This research employed the sol-gel method to synthesize stable and effective mesoporous CeCuOx mixed oxide catalysts to facilitate the oxidation of CO and C3H6 emissions at lower temperatures. Additionally, pure CeO2 and CuO were also synthesized for comparative analysis. Catalytic performance was considerably increased by doping CeO2 with Cu, whereas pure CuO and CeO2 showed modest activity. XRD, SEM, BET, XPS, Raman spectroscopy, H2-TPR, and CO-TPD showed that increasing Ce content produced a consistent pore structure without aggregation. In contrast, higher Cu concentration resulted in bulk CuO production, which led to decreased catalytic performance. In particular, the production of isolated CuOx species partly covered or clogged pores when the Cu level was above 20 wt%, which reduced the total number of effective sites for O2 activation. Compared to other mixed and pure oxides, the ideal catalyst, Ce7Cu3Ox (T90, CO = 178 °C), showed smaller particle size, higher specific surface area, and a larger lattice oxygen species and oxygen vacancies concentration. Additionally, it showed the best CO and C3H6 conversion due to its high Ce3+ concentration and interfacial active Cu species ratio. H2-TPR and CO-TPD analyses demonstrated that Ce-Cu mixed oxides with optimal Ce/Cu ratios, particularly Ce7Cu3Ox and Ce5Cu5Ox, achieve enhanced reducibility and balanced CO adsorption, which are critical for maximizing catalytic reactivity. The catalytic activity exhibited the following sequence: Ce7Cu3Ox > Ce5Cu5Ox > Ce9Cu1Ox > Ce3Cu7Ox > Ce1Cu9Ox > CuO > CeO2. This investigation offers a valuable perspective on the mechanisms of Ce-Cu interaction, which contributes to developing high-performance CeCuOx catalysts that are free of PGMs and operate under realistic reaction conditions.

Graphical abstract

Abstract Image

解锁无pgm CeCuOx混合氧化物催化剂CO和C3H6排放转化的最佳性能
一种可持续的、具有成本效益的环境应用替代方案是使用不含pgm的催化剂,这对去除污染物至关重要。本研究采用溶胶-凝胶法合成了稳定有效的中孔CeCuOx混合氧化物催化剂,以促进CO和C3H6在低温下的氧化排放。此外,还合成了纯CeO2和纯CuO进行对比分析。CeO2掺杂Cu后,催化性能明显提高,而纯CuO和CeO2的催化活性不高。XRD、SEM、BET、XPS、拉曼光谱、H2-TPR和CO-TPD均表明,随着Ce含量的增加,孔隙结构趋于一致,无聚集现象。相反,Cu浓度升高导致大量生成CuO,导致催化性能下降。当Cu含量高于20% wt%时,分离CuOx的生成部分覆盖或堵塞了孔隙,减少了O2活化的有效位点总数。与其他混合氧化物和纯氧化物相比,理想催化剂Ce7Cu3Ox (T90, CO = 178℃)具有更小的粒径、更高的比表面积、更大的晶格氧种类和氧空位浓度。此外,由于其较高的Ce3+浓度和界面活性Cu种比,其CO和C3H6的转化率最好。H2-TPR和CO- tpd分析表明,具有最佳Ce/Cu比的Ce-Cu混合氧化物,特别是Ce7Cu3Ox和Ce5Cu5Ox,具有更强的还原性和平衡的CO吸附,这是最大化催化活性的关键。催化活性表现为Ce7Cu3Ox >; Ce5Cu5Ox > Ce9Cu1Ox > Ce3Cu7Ox > Ce1Cu9Ox > CuO > CeO2。该研究为Ce-Cu相互作用机理的研究提供了有价值的视角,有助于开发不含pgm的高性能CeCuOx催化剂,并在实际反应条件下运行。图形抽象
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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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