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Laser Stimulated Methane Direct Partial Oxidation to Methanol on the Surface of Non-crystal Fe0.5Al0.5PO4
Gao Feng,Zhong Shunhe
Author NameAffiliationE-mail
Gao Feng College ofChemical Engineering and Technology, Tianjin University, Tianjin 300072  
Zhong Shunhe College ofChemical Engineering and Technology, Tianjin University, Tianjin 300072 shzhong@public.tpt.tj.cn 
Abstract:
Crystal and non-crystal Fe0.5Al0.5PO4were prepared using dipping method and sol-gel method, respectively. Thesurfacestructure, latticeoxygen activity, chemisorption to methane and LSSR of the surface materials were investigated by XRD, IR, TPR and laser stimulated surface reaction tech-niques. The non-crystal Fe0.5Al0.5PO4has the structure of mixed small particles of FePO4and AlPO4, which isdifferent fromthe continued crystal Fe0.5Al0.5PO4structure. The activityof the latticeoxygen in non-crystal Fe0.5Al0.5PO4is more than that in the crystal Fe0.5Al0.5PO4. Methane can be adsorbed on the surface P=Obond with the molecular adsorption state, and the adsorption amount of methane on the non-crystal Fe0.5Al0.5PO4is greater than that on the crystal Fe0.5Al0.5PO4. While the 1083cm-1laser exciting the surface P=O bond, the reaction of methane partial oxid ation to methanol is occurred obvi-ously at the temperature higher than 100℃with the methanol selectivity higher than 80%. The efficient utilization of laser energy characterized by the methane conversion on non-crystal Fe0.5Al0.5PO4is more than thaton the crystalFe0.5Al0.5PO4, indicated that the amountof the laserenergy transferring from the excited surface bond into the solid body can be decreased by the microminiaturization of the solid micro-crystalline particles of the solid material.
Key words:  Methane, Methanol, Partial oxidation, Laser stimulated surface reaction, Non-crystal Phosphate
FundProject:国家自然科学基金资助项目(29674035)
非晶态Fe0.5Al0.5PO4表面上激光促进甲烷直接氧化合成甲醇的研究
高峰,钟顺和*
摘要:
用溶胶—凝胶法合成了非晶态Fe0.5Al0.5PO4。用XRD和TPR表征了其结构和晶格氧的活性;用IR和TPD表征了CH4在其表面上的吸附行为;用LSSR方法考察了CH4直接氧化合成CH3OH的反应规律。结果表明,Fe0.5Al0.5PO4具有非晶态的结构,FePO4和AlPO4的微区被均匀地相互隔离,导致固体本身不具有长程有序性。非晶态的Fe0.5Al0.5PO4与晶态的Fe0.5Al0.5PO4相比,其晶格氧的活性大且活性氧的含量高。CH4以分子态吸附于固体表面P=O键上,非晶态Fe0.5Al0.5PO4表面上CH4的吸附强度和吸附量都较晶态Fe0.5Al0.5PO4上大。用1073cm-1的激光激发固体表面P=O键,在100℃以上CH4的直接氧化反应顺利进行,CH3OH保持高选择性。在相同的反应条件下,非晶态Fe0.5Al0.5PO4能更有效地促进反应的进行,表明在激发相同表面化学键的情况下,固体表面材料的其它性质如粒度、比表面积和晶格氧的活性对反应也有一定程度的影响。
关键词:  甲烷  甲醇  部分氧化  激光促进表面反应  非晶态磷酸盐
DOI:10.1088/1674-0068/13/5/611-617
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