Tunable Synthesis of Ethanol or Methyl Acetate via Dimethyl Oxalate Hydrogenation on Confined Iron Catalysts,ACS Catalysis

当前位置： X-MOL 学术 › ACS Catal. › 论文详情

Our official English website, www.x-mol.net, welcomes your feedback! (Note: you will need to create a separate account there.)

Tunable Synthesis of Ethanol or Methyl Acetate via Dimethyl Oxalate Hydrogenation on Confined Iron Catalysts
ACS Catalysis ( IF 11.3 ) Pub Date : 2021-04-07 , DOI: 10.1021/acscatal.1c00339
Yannan Sun _{1,

2} , Qingxiang Ma ₃ , Qingjie Ge ₁ , Jian Sun ₁

Affiliation

Oxygenated chemicals are essential to modern industries. However, selective syntheses with controllable products are still challenging over a single heterogeneous catalyst. Herein, a confined iron catalyst is designed for balanced syntheses of ethanol and methyl acetate via dimethyl oxalate (DMO) hydrogenation. With the characteristic structure of a microsphere, the Fe@C catalyst promotes the enrichment of hydrogen to reach a tunable selectivity of ethanol (84.3%) and methyl acetate (77.9%). The highest selectivity of methyl acetate is reached at a H₂/DMO molar ratio as low as 20, which is the lowest among catalysts reported for DMO hydrogenation by now. The molecule-level mechanism of DMO hydrogenation is further investigated. It proves that Fe₅C₂ in Fe@C is the main active center of DMO hydrogenation and Fe₃O₄ promotes the conversion of the intermediate especially in a low H₂/DMO molar ratio. This work provides a strategy for tuning targeted oxygenated chemicals.

中文翻译：

约束铁催化剂上草酸二甲酯加氢可调谐合成乙醇或乙酸甲酯

含氧化合物对现代工业至关重要。但是，具有可控产物的选择性合成对于单一非均相催化剂仍然具有挑战性。本文中，设计了一种铁约束催化剂，用于通过草酸二甲酯（DMO）加氢平衡合成乙醇和乙酸甲酯。Fe @ C催化剂具有微球的特征结构，可促进氢的富集，从而达到乙醇（84.3％）和乙酸甲酯（77.9％）的可调选择性。H ₂ / DMO摩尔比低至20时，乙酸甲酯的选择性最高，这是迄今为止报道的DMO加氢催化剂中最低的。进一步研究了DMO加氢的分子级机理。证明了Fe ₅ C ₂在Fe @ C中，Fe ₃ O ₄是DMO氢化的主要活性中心，Fe ₃ O ₄促进中间体的转化，特别是在低H ₂ / DMO摩尔比的情况下。这项工作为调整目标含氧化合物提供了一种策略。

更新日期：2021-04-16

点击分享查看原文

点击收藏

阅读更多本刊新发论文本刊介绍/投稿指南