厦大张庆红/康金灿ACS Catal.: 转化率达98%！合成气存在下H-MOR-DA@C上甲醇选择性转化为乙醇

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碳氢化合物燃料和增值化学品(包括低级烯烃、芳烃和含氧化合物)，可以通过C-C偶联反应由甲醇生产。与甲醇到烃的转化相比，由于产物中存在氧，通过精确的C-C偶联从甲醇合成乙醇具有很高的原子经济性。甲醇直接转化为乙醇和H2O(2CH3{attr}3228{/attr}→C2H5OH + H2O)在热力学上是可行的，但C-H和C-O键的活化仍然极具挑战性。


基于此，厦门大学张庆红和康金灿等报道了在合成气存在下，在由碳层改性的丝光沸石和Pt-Sn/CNT组成的复合催化剂(H-MOR-DA@C)上，通过串联催化将甲醇直接转化为乙醇。
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这种串联路线从H-MOR-DA@C上甲醇和CO羰基化为乙酸开始，然后乙酸在Pt-Sn/CNT加氢转化为乙醇，CH3OH对乙醇的选择性高达60%且转化率为98%。与H-MOR-DA基体相比，H-MOR-DA被碳层包覆有效地阻碍了乙醇脱水制乙烯的副反应；H-MOR-DA@C表面存在的带有酯或羧酸等含氧官能团的特殊“碳巢”对于防止乙醇脱水至关重要，从而提高了乙醇的选择性和催化稳定性。
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此外，研究人员还利用其他碳源(葡萄糖、果糖和蔗糖)采用相同的水热法对H-MOR-DA进行改性，目标产物乙醇在由改性沸石样品和Pt-Sn/CNT组成的复合催化剂上形成的选择性为32-41%，CH3OH转化率约为86%。
因此，无论碳源如何，水热碳化都是修饰H-MOR-DA的通用方法。这项工作为从甲醇直接合成乙醇和通过控制反应途径设计用于串联催化的高效复合催化剂提供了有效的策略。
Selective Transformation of Methanol to Ethanol in the Presence of Syngas over Composite Catalysts. ACS Catalysis, 2022. DOI: 10.1021/acscatal.2c01725




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