Biomimetic Frustrated Lewis Pair Catalysts for Hydrogenation of CO to Methanol at Low Temperatures

被引：3

作者：

Zhang, Jiejing ^{[1
]}

Li, Longfei ^{[1
]}

Xie, Xiaofeng ^{[1
]}

Song, Xue-Qing ^{[1
]}

Schaefer, Henry F. ^{[2
]}

机构：

[1] Hebei Univ, Key Lab Pharmaceut Qual Control Hebei Prov, Key Lab Med Chem & Mol Diag, Coll Pharm,Minist Educ, Baoding 071002, Hebei, Peoples R China

[2] Univ Georgia, Ctr Computat Quantum Chem, Athens, GA 30602 USA

来源：

ACS ORGANIC & INORGANIC AU | 2024年 / 4卷 / 02期

基金：

中国国家自然科学基金;

关键词：

CO hydrogenation; biomimetic FLP catalysts; density functional theory; 1,1-addition; base-free; CARBON-MONOXIDE HYDROGENATION; NUCLEIC-ACID BASES; HOMOGENEOUS HYDROGENATION; GAS; REDUCTION; POLYURETHANES; ACTIVATION; COMPLEXES; MECHANISM; ALCOHOLS;

D O I：

10.1021/acsorginorgau.3c00064

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

The industrial production of methanol through CO hydrogenation using the Cu/ZnO/Al2O3 catalyst requires harsh conditions, and the development of new catalysts with low operating temperatures is highly desirable. In this study, organic biomimetic FLP catalysts with good tolerance to CO poison are theoretically designed. The base-free catalytic reaction contains the 1,1-addition of CO into a formic acid intermediate and the hydrogenation of the formic acid intermediate into methanol. Low-energy spans (25.6, 22.1, and 20.6 kcal/mol) are achieved, indicating that CO can be hydrogenated into methanol at low temperatures. The new extended aromatization-dearomatization effect involving multiple rings is proposed to effectively facilitate the rate-determining CO 1,1-addition step, and a new CO activation model is proposed for organic catalysts.

引用

页码：258 / 267

页数：10

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