以 CeO2 或 ZrO2 改性 beta 沸石为载体的 Pd 催化剂在甲烷氧化中的催化性能

IF 5.9 2区 环境科学与生态学 Q1 ENVIRONMENTAL SCIENCES
Yingao Zhang , Zidi Yan , Min Xiao , Chunlei Zhang , Luna Ruan , Yanshuang Zhang , Yun Zhong , Yong Yan , Yunbo Yu , Hong He
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引用次数: 0

摘要

通过简单的湿法浸渍制备了两种氧化物-沸石复合载体(Ce-beta 和 Zr-beta),并将其用于制备甲烷催化氧化的钯基催化剂。Pd/6.8Zr-beta 催化剂表现出优异的甲烷氧化性能,T50 和 T90 分别达到 417 ℃ 和 451 ℃,并具有很强的水热稳定性。动力学分析表明,在催化剂中加入 Zr 能显著提高催化剂的效率,与 Pd/beta 催化剂相比,甲烷燃烧的翻转频率 (TOF) 几乎提高了两倍。这种性能的提高归功于 Zr 在沸石表面的分散,它不仅促进了活性 PdO 位点的形成,还通过促进反应过程中的氧迁移帮助维持了高 Pd2+ 含量,从而提高了催化剂的活性和稳定性。在 Pd/8.6Ce-beta 催化剂中,掺杂的 CeO2 容易在沸石孔隙中聚集,从而对催化剂的效率产生不利影响。这种聚集促进了非活性 Pd4+ 物种的形成,这是金属与支撑相互作用增强的结果。这一发现对于理解设计高活性甲烷氧化催化剂时选择掺杂剂的意义至关重要。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
Catalytic performance of Pd catalyst supported on CeO2 or ZrO2 modified beta zeolite for methane oxidation

Two kinds of oxide-zeolite composite support, Ce-beta and Zr-beta were prepared by a simple wet impregnation method and adopted for the preparation of palladium-based catalysts for catalytic oxidation of methane. The Pd/6.8Zr-beta catalyst showed superior methane oxidation performance, achieving T50 and T90 of 417 °C and 451 °C, respectively, together with robust hydrothermal stability. Kinetic analysis has shown that incorporating Zr into the catalyst significantly enhanced its efficiency, nearly tripling the turnover frequency (TOF) for methane combustion compared to the Pd/beta catalyst. This enhanced performance was attributed to the dispersion of Zr on the zeolite surface, which not only promoted the formation of active PdO sites but also helped maintain the high Pd2+ content via facilitating the oxygen migration during the reaction, thus improving both the catalyst's activity and stability. In the Pd/8.6Ce-beta catalyst, doped CeO2 tended to aggregate in the zeolite's pores, adversely affecting the catalyst's efficiency. This aggregation promoted the formation of inactive Pd4+ species, a result of the enhanced metal-support interaction. This finding is critical for understanding the implications of dopant selection in the design of high-activity methane oxidation catalysts.

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来源期刊
Journal of Environmental Sciences-china
Journal of Environmental Sciences-china 环境科学-环境科学
CiteScore
13.70
自引率
0.00%
发文量
6354
审稿时长
2.6 months
期刊介绍: The Journal of Environmental Sciences is an international journal started in 1989. The journal is devoted to publish original, peer-reviewed research papers on main aspects of environmental sciences, such as environmental chemistry, environmental biology, ecology, geosciences and environmental physics. Appropriate subjects include basic and applied research on atmospheric, terrestrial and aquatic environments, pollution control and abatement technology, conservation of natural resources, environmental health and toxicology. Announcements of international environmental science meetings and other recent information are also included.
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