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Deoxygenation of Biomass-Derlwed Feedstocks: Oxorhenium-Catalyzed Deoxydehydration of Sugars and Sugar Alcohols...

机译:生物质原料的脱氧:糖和糖醇经氧and催化的脱氧...

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摘要

The challenge associated with achieving successful conversion of cellulosic biomass to platform fuels and chemicals lies in the oxygen-rich nature of saccharides compared to the desired end products. To offset this difficulty, deoxygenation pathways had been previously explored with special attention given to the deoxydehydration (DODH) strategy, noted in Scheme 1. These efforts made use of [Re2(CO)10] and [6rRe(CO)5] as the catalyst, in conjunction with a secondary alcohol as solvent/reductant. Unfortunately, this approach has had limited success and then only with one C4 sugar (erythritol). However, the authors took note that the use of these catalysts appeared to require air and high temperature for activation, leading them to postulate that the actual active catalyst may be an oxidizedrhenium species, and that, consequently, oxorhenium compounds might represent superior catalysts for this reaction. In order to test this premise, they first studied the use of a series of oxorhenium compounds with 1,4-anhydroerythritol (1) as shown in Table 1. Based on this study, [CH3ReO3] (methyltrioxorhenium or MTO), was selected as the catalyst of choice for the deoxydehydration of a wide variety of polyols.
机译:与纤维素生物质成功转化为平台燃料和化学品相关的挑战在于,与所需最终产品相比,糖类的富氧特性。为了弥补这一困难,先前已经探索了脱氧途径,并特别注意了方案1中提到的脱氧脱水(DODH)策略。这些努力都以[Re2(CO)10]和[6rRe(CO)5]为基础。催化剂,与仲醇一起用作溶剂/还原剂。不幸的是,这种方法取得的成功有限,因此只能使用一种C4糖(赤藓糖醇)。但是,作者注意到,使用这些催化剂似乎需要空气和高温才能进行活化,导致它们推测实际的活性催化剂可能是氧化r物种,因此,氧化化合物可能是实现此目的的优良催化剂。反应。为了测试这一前提,他们首先研究了一系列含1,4-脱水赤藓糖醇(1)的氧化or化合物的使用,如表1所示。基于此研究,选择了[CH3ReO3](甲基三氧化or或MTO)作为是多种多元醇脱氧脱水的首选催化剂。

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