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Gold nanoparticles in environmental catalysis: Influence of the Fe-modified alumina supports on the catalytic behavior of supported gold nanoparticles in CO oxidation in the presence of ammonia

机译:环境催化中的金纳米颗粒:在氨气存在下,Fe修饰的氧化铝载体对负载的金纳米颗粒在CO氧化中的催化行为的影响

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The preferable utilization of ammonia and carbon monoxide from industrial kiln gases is their processing into the initial components of solid state synthesis. The kiln gas of industrial synthesis of the nanostructured lithium iron phosphate LFP material contains both ammonia and carbon monoxide, and NH3 can be processed into (NH4)(2)HPO4, whereas CO should be transformed into CO2 in order to be used for Li2CO3 synthesis. This work focuses on the preparation of catalysts that can preferentially oxidize CO with a minimal NH3 conversion in their rich mixtures. The Au nanoparticles (particle size below 3 nm) were supported on the theta-Al2O3 modified with 1-5 wt.% Fe that resulted in the Au catalysts highly effective in CO oxidation at 200-250 degrees C in the presence of NH3. The TPR-H-2 and DRIFT spectroscopy revealed almost complete reduction of the gold precursor surface after calcination in air at 300 degrees C, as well as the presence of residual organic moieties in the samples. Variation in the procedure of modifying treatment and Fe precursor realized a different Fe3+ environment and affected the catalytic behavior. The FeO species of the exchange bonded Fe3+ ions favored NH3 oxidation, whereas distribution of Fe3+ as isolated ions decreased the activity in NH3 oxidation. Compared to the Au/FeOx/theta-Al2O3 and Au/theta-Al2O3 samples, the Au/theta-Al2-xFexO3 catalysts were more active in CO oxidation. These catalysts exhibited the widest temperature window between the complete CO conversion and the detectable NH3 conversion. The catalysts were thermally stable and maintained the activity both in CO and NH3 oxidation after treatment at 500 degrees C. (C) 2016 Elsevier B.V. All rights reserved.
机译:来自工业窑炉气体的氨和一氧化碳的优选利用是将其加工成固态合成的初始组分。纳米结构的磷酸锂铁LFP材料的工业合成窑炉气体同时含有氨和一氧化碳,并且NH3可以加工成(NH4)(2)HPO4,而CO应该转化为CO2才能用于Li2CO3合成。这项工作集中在催化剂的制备上,这些催化剂可以在其丰富的混合物中以最小的NH3转化率优先氧化CO。 Au纳米颗粒(粒径小于3 nm)负载在用1-5 wt。%Fe改性的theta-Al2O3上,这导致Au催化剂在NH3存在下在200-250摄氏度的CO氧化中非常有效。 TPR-H-2和DRIFT光谱表明,在300摄氏度的空气中煅烧后,金前驱体表面几乎完全还原,并且样品中存在残留有机部分。改性处理程序和Fe前驱体的变化实现了不同的Fe3 +环境并影响了催化性能。交换键合的Fe3 +离子的FeO种类有利于NH3氧化,而Fe3 +作为分离离子的分布降低了NH3氧化的活性。与Au / FeOx / theta-Al2O3和Au / theta-Al2O3样品相比,Au / theta-Al2-xFexO3催化剂在CO氧化中更具活性。这些催化剂在完全CO转化和可检测的NH3转化之间显示出最宽的温度范围。催化剂在500℃下处理后具有热稳定性,并且在CO和NH3氧化中均保持活性。(C)2016 Elsevier B.V.保留所有权利。

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