Zhao Li , Fei Wang , Fudong Liu , Shaohua Xie , Changbin Zhang , Ping Ning , Kai Li , Hong He , Xiao Cheng Zeng
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引用次数: 0
摘要
Ag/Al2O3 催化剂中的 Ag 纳米粒子(AgNPs)在选择性催化氧化 NH3(NH3-SCO)中发挥着至关重要的作用。为了提高 NH3-SCO 的活性,在 Al2O3 上引入了锚定能力比 Ag 更强的 Cu,从而减少了 Ag 的可用锚定位点。由于 Ag 无法取代锚定的 Cu 物种,因此即使 Ag 负载较低,Ag 物种也会聚集成较大的 AgNPs。因此,这些增大的 AgNPs 成为 NH3-SCO 更为活跃的中心。最佳的银铜摩尔比为 2:3。这种 "预占锚定位 "策略可将银负载量减少到原来的 1/5,从而在保持活性的同时降低催化剂成本。原位漫反射红外傅立叶变换光谱(DRIFTS)研究表明,2Ag1.8Cu/Al(重量比)催化剂上的 NH3-SCO 在 200 °C 以下遵循肼机理,200-250 °C 期间与酰亚胺机理共存,250 °C 以上则完全遵循酰亚胺机理。这种策略适用于各种过渡金属,包括锰、钴、镍和铁,从而促进了具有成本效益的 AgNPs 的形成。
Catalytic oxidation of ammonia: A pre-occupied-anchoring-site strategy for enlarging Ag nanoparticles at low Ag loading and achieving enhanced activity and selectivity on Ag-CuOx/Al2O3 catalyst
The Ag nanoparticles (AgNPs) in Ag/Al2O3 catalysts play a crucial role in the selective catalytic oxidation of NH3 (NH3-SCO). To enhance NH3-SCO activity, Cu, which has stronger anchoring ability than Ag, is introduced onto Al2O3, reducing available anchoring sites for Ag. As Ag cannot displace anchored Cu species, Ag species agglomerate into larger AgNPs even with low Ag loading. Consequently, these enlarged AgNPs become more active centers for NH3-SCO. The optimal Ag:Cu molar ratio is confirmed as 2:3. This 'pre-occupied-anchoring-site’ strategy decreases Ag loading to 1/5 of the original, reducing catalyst costs while maintaining activity. In situ diffuse reflectance infrared Fourier-transform spectroscopy (DRIFTS) studies reveal that NH3-SCO on 2Ag1.8Cu/Al (weight ratio) catalyst follows the hydrazine mechanism below 200 °C, coexisting with the imide mechanism from 200–250 °C, and solely the imide mechanism beyond 250 °C. This strategy is applicable to various transition metals, including Mn, Co, Ni, and Fe, promoting cost-effective AgNPs formation.
期刊介绍:
Applied Catalysis B: Environment and Energy (formerly Applied Catalysis B: Environmental) is a journal that focuses on the transition towards cleaner and more sustainable energy sources. The journal's publications cover a wide range of topics, including:
1.Catalytic elimination of environmental pollutants such as nitrogen oxides, carbon monoxide, sulfur compounds, chlorinated and other organic compounds, and soot emitted from stationary or mobile sources.
2.Basic understanding of catalysts used in environmental pollution abatement, particularly in industrial processes.
3.All aspects of preparation, characterization, activation, deactivation, and regeneration of novel and commercially applicable environmental catalysts.
4.New catalytic routes and processes for the production of clean energy, such as hydrogen generation via catalytic fuel processing, and new catalysts and electrocatalysts for fuel cells.
5.Catalytic reactions that convert wastes into useful products.
6.Clean manufacturing techniques that replace toxic chemicals with environmentally friendly catalysts.
7.Scientific aspects of photocatalytic processes and a basic understanding of photocatalysts as applied to environmental problems.
8.New catalytic combustion technologies and catalysts.
9.New catalytic non-enzymatic transformations of biomass components.
The journal is abstracted and indexed in API Abstracts, Research Alert, Chemical Abstracts, Web of Science, Theoretical Chemical Engineering Abstracts, Engineering, Technology & Applied Sciences, and others.