A Noble-Metal-Free Metal-Organic Framework (MOF) Catalyst for the Highly Efficient Conversion of CO2 with Propargylic Alcohols

被引:165
作者
Hou, Sheng-Li [1 ,2 ]
Dong, Jie [1 ,2 ]
Jiang, Xiao-Lei [1 ,2 ]
Jiao, Zhuo-Hao [1 ,2 ]
Zhao, Bin [1 ,2 ]
机构
[1] Nankai Univ, MOE, Coll Chem, Key Lab Adv Energy Mat Chem, Tianjin 300071, Peoples R China
[2] Nankai Univ, Collaborat Innovat Ctr Chem Sci & Engn, Tianjin 300071, Peoples R China
关键词
carbon dioxide fixation; cyclizations; heterogeneous catalysis; metal-organic frameworks (MOFs); noble-metal-free; ALKYLIDENE CYCLIC CARBONATES; CHEMICAL FIXATION; LUMINESCENT PROBE; DIOXIDE; NANOPARTICLES; CAPTURE; HYDROGENATION; CYCLOADDITION; CYCLIZATION; ACTIVATION;
D O I
10.1002/anie.201811506
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Cyclization of propargylic alcohols with CO2 is an important reaction in industry, and noble-metal catalysts are often employed to ensure the high product yields under environmentally friendly conditions. Herein a porous noble-metal-free framework 1 with large 1D channels of 1.66 nm diameter was synthesized for this reaction. Compound 1 exhibits excellent acid/base stability, and is even stable in corrosive triethylamine for one month. Catalytic studies indicate that 1 is an effective catalyst for the cyclization of propargylic alcohols and CO2 without any solvents under mild conditions, and the turnover number (TON) can reach to a record value of 14 400. Furthermore, this MOF catalyst also has rarely seen catalytic activity when the biological macromolecule ethisterone was used as a substrate. Mechanistic studies reveal that the synergistic catalytic effect between Cu-I and In-III plays a key role in the conversion of CO2.
引用
收藏
页码:577 / 581
页数:5
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