Tailoring the physical and catalytic properties of lanthanum oxycarbonate nanoparticles

被引:15
作者
Bosch, C. Estruch [1 ]
Copley, M. P. [1 ]
Eralp, T. [1 ]
Bilbe, E. [1 ]
Thybaut, J. W. [2 ]
Marin, G. B. [2 ]
Collier, P. [1 ]
机构
[1] Johnson Matthey Technol Ctr, Blounts Court Rd, Reading RG4 9NH, Berks, England
[2] Univ Ghent, Lab Chem Technol, Tech Lane Ghent Sci Pk,Campus A 914, B-9052 Ghent, Belgium
基金
欧盟第七框架计划;
关键词
Lanthanum oxide; Lanthanum carbonate; Flame spray pyrolysis; Basicity; Nanoparticles; Oxidative coupling of methane; OXIDE CATALYSTS; PHOSPHATE BINDER; METHANE; CARBONATE; HYDROXIDE; CRYSTAL; PERFORMANCE; MORPHOLOGY; OXIDATION; MGO;
D O I
10.1016/j.apcata.2017.01.019
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
The synthesis of lanthanum oxide and its carbonate analogues has been performed by flame spray pyrolysis (FSP). Two different feeds have been studied: an organic solution and an aqueous/organic microemulsion. A key experimental parameter of FSP, the O-2 dispersion, i.e., the flow rate of the dispersing gas in the FSP nozzle, exhibits an effect on the properties of the materials prepared. Increasing the level of O-2 dispersion led to an increase in surface area and a decrease in mean particle size and basicity when a lanthanum containing organic solution was used as FSP feed. Lanthanum can form different phases, such as oxides, hydroxides, oxycarbonates and carbonates. The increase of O-2 dispersion also produced a phase change, going from a mixture of type la and type II La2O2CO3 and La2O3 to pure La2O3. The use of an aqueous/organic microemulsion feed, which had a higher viscosity than the organic feed, resulted in materials with a lower surface area and a higher mean particle size than those prepared using the organic solution at the same O-2 dispersion. In this case a mixture of type II La2O2CO3 and La2O3 was obtained. The materials were tested for oxidative coupling of methane (OCM). We were able to demonstrate that the OCM performance of the materials could be modified by changing the synthesis parameters. For example, lower O-2 dispersion produced the highest CH4 and O-2 conversions. We also demonstrated that on ageing the mean particle size remain stable; however, the phases do not, showing a new phase, La(OH)(3), formation and resulting in an increase in OCM activity. While the OCM performances are modest they do demonstrate the power of this approach for controlled synthesis of lanthanum materials. (C) 2017 Elsevier B.V. All rights reserved.
引用
收藏
页码:104 / 112
页数:9
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