Catalysts for the Selective Oxidation of Methanol

被引:40
作者
Brookes, Catherine [1 ,2 ]
Bowker, Michael [1 ,2 ]
Wells, Peter P. [2 ,3 ]
机构
[1] Cardiff Univ, Sch Chem, Cardiff Catalysis Inst, Main Bldg,Pk Pl, Cardiff CF10 3AT, S Glam, Wales
[2] Res Complex Harwell RCaH, Rutherford Appleton Lab, UK Catalysis Hub, Harwell OX11 0FA, Oxon, England
[3] UCL, Dept Chem, 20 Gordon St, London WC1H 0AJ, England
来源
CATALYSTS | 2016年 / 6卷 / 07期
基金
英国工程与自然科学研究理事会;
关键词
methanol oxidation; active site; redox; formaldehyde synthesis; model catalysts; surface specificity; XAFS; iron molybdate; spectroscopy; core-shell catalysts; IRON-MOLYBDATE CATALYSTS; MOLYBDENUM TRIOXIDE; FORMALDEHYDE OXIDATION; STRUCTURE SENSITIVITY; OXIDE CATALYSTS; REDOX PROCESSES; SURFACE; MOO3; TEMPERATURE; MECHANISM;
D O I
10.3390/catal6070092
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
In industry, one of the main catalysts typically employed for the selective oxidation of methanol to formaldehyde is a multi-component oxide containing both bulk Fe-2(MoO4)(3) and excess MoO3. It is thought that the excess MoO3 primarily acts to replace any molybdenum lost through sublimation at elevated temperatures, therefore preventing the formation of an unselective Fe2O3 phase. With both oxide phases present however, debate has arisen regarding the active component of the catalyst. Work here highlights how catalyst surfaces are significantly different from bulk structures, a difference crucial for catalyst performance. Specifically, Mo has been isolated at the surface as the active surface species. This leaves the role of the Fe in the catalyst enigmatic, with many theories postulated for its requirement. It has been suggested that the supporting Fe molybdate phase enables lattice oxygen transfer to the surface, to help prevent the selectivity loss which would occur in the resulting oxygen deficit environment. To assess this phenomenon in further detail, anaerobic reaction with methanol has been adopted to evaluate the performance of the catalyst under reducing conditions.
引用
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页数:27
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