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首页> 外文期刊>Catalysis science & technology >Deoxydehydration of glycerol in presence of rhenium compounds: reactivity and mechanistic aspects
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Deoxydehydration of glycerol in presence of rhenium compounds: reactivity and mechanistic aspects

机译：Deoxydehydration甘油的存在铼化合物:反应性和机械方面

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摘要

Allyl alcohol (AA) was obtained by the deoxydehydration (DODH) of glycerol performed in the presence of a number of Re compounds (oxides, phosphine and halide derivatives) in alcoholic solvent or in neat conditions. Independently of starting Re species, the resulting catalytic process featured a delay time, necessary to start the formation of both AA and an Re-alkoxide precipitate. However, no delay time was detected by operating DODH using a preformed precipitate obtained by either Re source. As a consequence, and based on IR spectral analysis, it was hypothesized that the Re precipitate is the actual catalyst of DODH. The mechanism of DODH catalysis operated by methyltrioxorhenium (MTO) was studied by experimental and theoretical approaches. The results suggest that MTO releases methane with the formation of an Re-VII alkoxide that subsequently aggregates by yielding the precipitate. The Re-VII centre precipitate surface then undergoes reduction by forming Re-V catalytic spots. The calculated kinetics also indicate that the detected latency can be ascribed to the presence of two high barriers, i.e. methane release and Re-VII. ReV reduction, whereas the downstream processes, i.e. glycation and AA release, are not rate determining.
机译：烯丙醇(AA)获得的deoxydehydration (DODH)中执行的甘油存在大量的稀土化合物(氧化物,磷化氢和卤化物衍生品)的酒精溶剂或在整洁的环境。开始重新物种,由此产生的催化过程中延迟时间,必要的开始AA和Re-alkoxide的形成沉淀。通过操作DODH使用预成型的沉淀通过再保险来源获得。基于红外光谱分析,假设的沉淀是DODH的实际催化剂。催化由methyltrioxorhenium (MTO)研究了实验和理论方法。甲烷的形成一个Re-VII醇盐随后聚集的产生沉淀。表面然后由形成Re-V经历减少催化斑点。表明,延迟可以被检测到归结为两个高壁垒的存在,如甲烷释放和Re-VII。而下游流程,即糖化和AA释放,不是利率决定。

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