Cu/Sn-β Catalyst Enabling the One-Step Synthesis of Methyl Acetate from Methanol Alone via Dehydrogenation Coupling,ACS Sustainable Chemistry & Engineering

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Cu/Sn-β Catalyst Enabling the One-Step Synthesis of Methyl Acetate from Methanol Alone via Dehydrogenation Coupling
ACS Sustainable Chemistry & Engineering ( IF 7.1 ) Pub Date : 2022-07-14 , DOI: 10.1021/acssuschemeng.1c08749
Qiang Nie ₁ , Jiaqi Si ₁ , Chao Meng ₁ , Tian Lan ₁ , Weidong Sun ₁ , Guofeng Zhao ₁ , Ye Liu ₁ , Yong Lu _{1,

2}

Affiliation

Methyl acetate (MA) can be directly synthesized via a methanol dehydrocoupling reaction, which is attractive but urgently calls for a groundbreaking catalyst. Herein, we report a Cu/Sn-β system with Sn–Cu synergistic catalysis, enabling the one-step MA synthesis from methanol alone. Over the 3Cu/Sn-β-30 (Si/Sn molar ratio of 33, Cu loading of 3 wt %), a maximum MA space–time yield of 1.4 mol_MA kg_cat^–1 h^–1 is obtained with 4.1% methanol conversion and 56.4% MA selectivity at 220 °C. Electron transfer from Cu species to framework-confined Sn occurs and thus increases and stabilizes Cu⁺ sites. Lewis-acidic Sn(framework)/Cu⁺ pairs, with the assistance of Cu⁰ dehydrogenation, can transform a methanol molecule into bridged-adsorbed CH₂O*. The C–C coupling of CH₂O* with CH₃O* on another Sn site proceeds to form CH₃CHO* by leaving H on Cu⁺ and O (C–O bond cleavage of CH₃O*) on that Sn site. The CH₃CHO* subsequently condenses with CH₃O* adsorbed on the Cu⁰ site to form MA.

中文翻译：

Cu/Sn-β催化剂使甲醇脱氢偶联一步合成乙酸甲酯

乙酸甲酯 (MA) 可以通过甲醇脱氢偶联反应直接合成，这很有吸引力，但迫切需要一种突破性的催化剂。在此，我们报告了一种具有 Sn-Cu 协同催化作用的 Cu/Sn-β 体系，能够仅从甲醇中一步合成 MA。在 3Cu/Sn-β-30（Si/Sn 摩尔比为 33，Cu 负载量为 3 wt %）上，使用 4.1% 甲醇获得的最大 MA 时空产率为 1.4 mol _MA kg _cat^–1 h ^–1在 220 °C 下的转化率和 56.4% MA 选择性。电子从 Cu 物种转移到骨架限制的 Sn 发生，因此增加并稳定了 Cu ⁺位点。路易斯酸性Sn(骨架)/Cu ⁺对，在Cu ^{0的帮助下}脱氢，可以将甲醇分子转化为桥接吸附的 CH ₂ O*。_{CH 2} O* 与另一个 Sn 位点上的 CH ₃ O*的 C-C 偶联通过在该 Sn 位点上留下 Cu ⁺和 O（CH ₃ O* 的 C-O 键断裂）上的 H 来形成 CH ₃ CHO* . CH ₃ CHO* 随后与吸附在Cu ^{0位点上的CH}₃ O* 缩合形成MA。

更新日期：2022-07-14

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