沸石约束下双金属钯铈催化剂解禁甲烷高效氧化

IF 6.7 Q1 ENGINEERING, ENVIRONMENTAL
Xiaomai Chen, Xuefeng Shi, Peirong Chen, Bowen Liu, Meiyin Liu, Longwen Chen, Daiqi Ye, Xin Tu*, Wei Fan* and Junliang Wu*, 
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引用次数: 0

摘要

催化完全氧化是减少甲烷排放的有效方法,甲烷排放是全球变暖的重要因素。这种方法需要对烧结和水蒸气具有高度耐受性的活性催化剂。在这项工作中,我们证明了Pd纳米颗粒被限制在silicalite-1沸石中(Pd@S-1),使用简单的原位封装策略制备,在催化甲烷氧化方面具有高度活性和稳定性,并且由于限制效应而优于负载在S-1表面上的那些。通过在S-1沸石中共同限制适量的Ce,进一步提高了限制的Pd催化剂的活性(PdCe0.4@S-1),这归因于约束增强的Pd–Ce相互作用,促进氧空位和高活性氧物种的形成。此外,Ce的引入提高了S-1沸石的疏水性,并通过形成Pd–Ce混合氧化物,抑制了活性PdO相向非活性Pd(OH)2物种的转化。总体而言,双金属PdCe0.4@S-1催化剂在甲烷完全氧化过程中,即使在水蒸气存在的情况下,也能提供卓越的活性和耐用性。本研究为合理设计高性能、耐用的甲烷完全氧化钯催化剂提供了新的前景。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

Unlocking High-Efficiency Methane Oxidation with Bimetallic Pd–Ce Catalysts under Zeolite Confinement

Unlocking High-Efficiency Methane Oxidation with Bimetallic Pd–Ce Catalysts under Zeolite Confinement

Catalytic complete oxidation is an efficient approach to reducing methane emissions, a significant contributor to global warming. This approach requires active catalysts that are highly resistant to sintering and water vapor. In this work, we demonstrate that Pd nanoparticles confined within silicalite-1 zeolites (Pd@S-1), fabricated using a facile in situ encapsulation strategy, are highly active and stable in catalyzing methane oxidation and are superior to those supported on the S-1 surface due to a confinement effect. The activity of the confined Pd catalysts was further improved by co-confining a suitable amount of Ce within the S-1 zeolite (PdCe0.4@S-1), which is attributed to confinement-reinforced Pd–Ce interactions that promote the formation of oxygen vacancies and highly reactive oxygen species. Furthermore, the introduction of Ce improves the hydrophobicity of the S-1 zeolite and, by forming Pd–Ce mixed oxides, inhibits the transformation of the active PdO phase to inactive Pd(OH)2 species. Overall, the bimetallic PdCe0.4@S-1 catalyst delivers exceptional outstanding activity and durability in complete methane oxidation, even in the presence of water vapor. This study may provide new prospects for the rational design of high-performance and durable Pd catalysts for complete methane oxidation.

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来源期刊
ACS Environmental Au
ACS Environmental Au 环境科学-
CiteScore
7.10
自引率
0.00%
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0
期刊介绍: ACS Environmental Au is an open access journal which publishes experimental research and theoretical results in all aspects of environmental science and technology both pure and applied. Short letters comprehensive articles reviews and perspectives are welcome in the following areas:Alternative EnergyAnthropogenic Impacts on Atmosphere Soil or WaterBiogeochemical CyclingBiomass or Wastes as ResourcesContaminants in Aquatic and Terrestrial EnvironmentsEnvironmental Data ScienceEcotoxicology and Public HealthEnergy and ClimateEnvironmental Modeling Processes and Measurement Methods and TechnologiesEnvironmental Nanotechnology and BiotechnologyGreen ChemistryGreen Manufacturing and EngineeringRisk assessment Regulatory Frameworks and Life-Cycle AssessmentsTreatment and Resource Recovery and Waste Management
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