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Selective Transformation of Methanol to Ethanol in the Presence of Syngas over Composite Catalysts
ACS Catalysis ( IF 11.3 ) Pub Date : 2022-07-01 , DOI: 10.1021/acscatal.2c01725 Fuyong Zhang 1 , Kuo Chen 1 , Qingmei Jiang 1 , Shun He 1 , Qijia Chen 1 , Zhiming Liu 1 , Jincan Kang 1 , Qinghong Zhang 1 , Ye Wang 1
ACS Catalysis ( IF 11.3 ) Pub Date : 2022-07-01 , DOI: 10.1021/acscatal.2c01725 Fuyong Zhang 1 , Kuo Chen 1 , Qingmei Jiang 1 , Shun He 1 , Qijia Chen 1 , Zhiming Liu 1 , Jincan Kang 1 , Qinghong Zhang 1 , Ye Wang 1
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The direct synthesis of ethanol from methanol via precise C–C coupling is a highly attractive but challenging target. Herein, we report the selective production of ethanol from methanol in the presence of syngas (CO/H2) by tandem catalysis over composite catalysts composed of mordenite (H–MOR) zeolite coated by carbon layer (H–MOR–DA@C) and Pt–Sn/CNT. This tandem route starts from methanol carbonylation with CO to acetic acid over H–MOR–DA@C, followed by acetic acid hydrogenation to ethanol over Pt–Sn/CNT. The selectivity of ethanol reached up to 60% with a CH3OH conversion of 98%. As compared to the H–MOR–DA matrix, the side reaction of ethanol dehydration to ethylene is effectively hindered over composite catalysts with H–MOR–DA coated by carbon layer. The special “carbon nest” with oxygenated functional groups such as ester or carboxylic acid, existing on the surface of H–MOR–DA@C, is crucial to preventing ethanol from dehydration, and thus improves the ethanol selectivity and catalytic stability. This work offers an effective strategy for direct synthesis of ethanol from methanol and design of efficient composite catalysts for tandem catalysis by controlling the reaction pathway.
中文翻译：
合成气存在下复合催化剂上甲醇选择性转化为乙醇
通过精确的 C-C 偶联从甲醇直接合成乙醇是一个极具吸引力但具有挑战性的目标。在此，我们报道了在合成气 (CO/H 2 ) 存在下，在由碳层包覆的丝光沸石 (H-MOR) 沸石 (H-MOR-DA@C) 组成的复合催化剂上，通过串联催化从甲醇选择性生产乙醇。和 Pt-Sn/CNT。该串联路线从甲醇与 CO 的羰基化反应开始，通过 H-MOR-DA@C 生成乙酸，然后通过 Pt-Sn/CNT 将乙酸加氢生成乙醇。CH 3对乙醇的选择性高达60%OH转化率为98%。与 H-MOR-DA 基体相比，H-MOR-DA 被碳层包覆的复合催化剂有效地阻碍了乙醇脱水制乙烯的副反应。H-MOR-DA@C表面存在的具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。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。
更新日期：2022-07-01
中文翻译：
合成气存在下复合催化剂上甲醇选择性转化为乙醇
通过精确的 C-C 偶联从甲醇直接合成乙醇是一个极具吸引力但具有挑战性的目标。在此，我们报道了在合成气 (CO/H 2 ) 存在下，在由碳层包覆的丝光沸石 (H-MOR) 沸石 (H-MOR-DA@C) 组成的复合催化剂上，通过串联催化从甲醇选择性生产乙醇。和 Pt-Sn/CNT。该串联路线从甲醇与 CO 的羰基化反应开始，通过 H-MOR-DA@C 生成乙酸，然后通过 Pt-Sn/CNT 将乙酸加氢生成乙醇。CH 3对乙醇的选择性高达60%OH转化率为98%。与 H-MOR-DA 基体相比，H-MOR-DA 被碳层包覆的复合催化剂有效地阻碍了乙醇脱水制乙烯的副反应。H-MOR-DA@C表面存在的具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。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。
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