Bridging the Gap between the Direct and Hydrocarbon Pool Mechanisms of the Methanol-to-Hydrocarbons Process.
Bridging the Gap between the Direct and Hydrocarbon Pool Mechanisms of the Methanol-to-Hydrocarbons Process.
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DOI：
10.1002/anie.201803279
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发表时间：
2018-07-02
期刊：
影响因子：
--
通讯作者：
Weckhuysen BM
中科院分区：
文献类型：
--
作者：
Chowdhury AD;Paioni AL;Houben K;Whiting GT;Baldus M;Weckhuysen BM
经过多年的长期努力，在甲醇制烃（MTH）过程中形成直接碳-碳（C - C）键的途径最近被揭开。然而，在MTH过程中“直接机制”衍生分子（即乙酸甲酯）的相关性以及随后向常规烃池（HCP）物种的转化途径尚未确定。这一MTH化学难题的重要组成部分不仅从基本角度来看是必不可少的，而且对于最大化催化性能也很重要。利用先进的固体核磁共振光谱和操作氧化物紫外/可见漫反射光谱与在线质谱仪相结合，在商业相关的H‐SAPO‐34催化剂上对MTH过程进行了探测。光谱证据提供了（烯烃和芳香）HCP物质的形成，这些物质确实完全来源于直接含C - C键的醋酸甲酯的乙酰基。从MTH过程中获得了新的机理见解，包括烃基共催化有机反应中心的鉴定。
After a prolonged effort over many years, the route for the formation of a direct carbon−carbon (C−C) bond during the methanol‐to‐hydrocarbon (MTH) process has very recently been unveiled. However, the relevance of the “direct mechanism”‐derived molecules (that is, methyl acetate) during MTH, and subsequent transformation routes to the conventional hydrocarbon pool (HCP) species, are yet to be established. This important piece of the MTH chemistry puzzle is not only essential from a fundamental perspective, but is also important to maximize catalytic performance. The MTH process was probed over a commercially relevant H‐SAPO‐34 catalyst, using a combination of advanced solid‐state NMR spectroscopy and operando UV/Vis diffuse reflectance spectroscopy coupled to an on‐line mass spectrometer. Spectroscopic evidence is provided for the formation of (olefinic and aromatic) HCP species, which are indeed derived exclusively from the direct C−C bond‐containing acetyl group of methyl acetate. New mechanistic insights have been obtained from the MTH process, including the identification of hydrocarbon‐based co‐catalytic organic reaction centers.
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