催化学报
催化學報
최화학보
CHINESE JOURNAL OF CATALYSIS
2001年
2期
129-132
,共4页
铋钼复合氧化物%激光促进表面反应%异丁烷%选择氧化%甲基丙烯酸
鉍鉬複閤氧化物%激光促進錶麵反應%異丁烷%選擇氧化%甲基丙烯痠
필목복합양화물%격광촉진표면반응%이정완%선택양화%갑기병희산
用共沉淀法制备了Bi和Mo的复合氧化物固体材料.运用XRD,IR,TPD和激光促进表面反应(LSSR)技术研究了其晶体结构、表面构造、化学吸附特性和激光促进异丁烷选择氧化反应性能.结果表明:Bi-Mo-O复合氧化物含有α-Bi2Mo3O12和少量γ-Bi2MoO6晶相;其表面上存在着Lewis碱位(MoO和Mo—O—Bi键中的O)及Lewis酸位(Bi3+);异丁烷的两个甲基H分别吸附在两个相邻的Lewis碱位Mo=O上,形成双位分子吸附态;在常压和200℃条件下,用一定频率的激光激发Mo=O键1000次,异丁烷的转化率可达11.2%,其反应产物是异丁烯、甲基丙烯醛和甲基丙烯酸,其中甲基丙烯酸的选择性为90%.根据实验结果,探讨了激光促进异丁烷选择氧化为甲基丙烯酸的表面反应机理.
用共沉澱法製備瞭Bi和Mo的複閤氧化物固體材料.運用XRD,IR,TPD和激光促進錶麵反應(LSSR)技術研究瞭其晶體結構、錶麵構造、化學吸附特性和激光促進異丁烷選擇氧化反應性能.結果錶明:Bi-Mo-O複閤氧化物含有α-Bi2Mo3O12和少量γ-Bi2MoO6晶相;其錶麵上存在著Lewis堿位(MoO和Mo—O—Bi鍵中的O)及Lewis痠位(Bi3+);異丁烷的兩箇甲基H分彆吸附在兩箇相鄰的Lewis堿位Mo=O上,形成雙位分子吸附態;在常壓和200℃條件下,用一定頻率的激光激髮Mo=O鍵1000次,異丁烷的轉化率可達11.2%,其反應產物是異丁烯、甲基丙烯醛和甲基丙烯痠,其中甲基丙烯痠的選擇性為90%.根據實驗結果,探討瞭激光促進異丁烷選擇氧化為甲基丙烯痠的錶麵反應機理.
용공침정법제비료Bi화Mo적복합양화물고체재료.운용XRD,IR,TPD화격광촉진표면반응(LSSR)기술연구료기정체결구、표면구조、화학흡부특성화격광촉진이정완선택양화반응성능.결과표명:Bi-Mo-O복합양화물함유α-Bi2Mo3O12화소량γ-Bi2MoO6정상;기표면상존재착Lewis감위(MoO화Mo—O—Bi건중적O)급Lewis산위(Bi3+);이정완적량개갑기H분별흡부재량개상린적Lewis감위Mo=O상,형성쌍위분자흡부태;재상압화200℃조건하,용일정빈솔적격광격발Mo=O건1000차,이정완적전화솔가체11.2%,기반응산물시이정희、갑기병희철화갑기병희산,기중갑기병희산적선택성위90%.근거실험결과,탐토료격광촉진이정완선택양화위갑기병희산적표면반응궤리.
A composite oxide catalyst containing Bi and Mo is prepared bycoprecipitation m ethod. Its surface composition and structure, chemisorption properties and behav iors in laser-stimulated isobutane selective oxidation are investigated by tech niques of XRD, IR, TPD and laser-stimulated surface reaction (LSSR). The main p hase component of Bi-Mo-O is α-Bi2Mo3O12. Lewis basic sites O2-, located at the surfaceMo=O orMoOBibonds, and Lewis acid sites Bi3+ appear on the surface of the composite oxide. Two methyl hydrogen atoms in is obutane molecule can be chemisorbed on the terminal oxygen of neighboring Lewis basic sitesMo=O bonds on the surface of the oxide. Using the laser photons of 984 cm-1 frequancy to excite the Mo=O bond 1000 times under the conditions of 0.1 M Pa and 200 ℃, the conversion of isobutane obtained is about 11.2%, the reactio n products are isobutene, methylacrolein (MAL) and methacrylic acid (MAA), and t he selectivity for MAA is over 90%. Based on the experimental results above, apossible mechanism is proposed for the laser-stimulated isobatane selective oxid ation to MAA.