Air-Stable Cu(I) Metal-Organic Framework for Hydrogen Storage

被引:35
|
作者
Sengupta, Debabrata [1 ]
Melix, Patrick [2 ,3 ]
Bose, Saptasree [1 ]
Duncan, Joshua [1 ]
Wang, Xingjie [1 ]
Mian, Mohammad Rasel [1 ]
Kirlikovali, Kent O. [1 ]
Joodaki, Faramarz [2 ]
Islamoglu, Timur [1 ]
Yildirim, Taner [4 ]
Snurr, Randall Q. [2 ]
Farha, Omar K. [1 ,2 ,5 ]
机构
[1] Northwestern Univ, Dept Chem, Evanston, IL 60208 USA
[2] Northwestern Univ, Dept Chem & Biol Engn, Evanston, IL 60208 USA
[3] Univ Leipzig, Wilhelm Ostwald Inst Phys & Theoret Chem, D-04103 Leipzig, Germany
[4] NIST, Ctr Neutron Res, Gaithersburg, MD 20899 USA
[5] Northwestern Univ, Int Inst Nanotechnol, Evanston, IL 60208 USA
关键词
TEMPERATURE; ACTIVATION; ADSORPTION; CAPACITY; BINDING;
D O I
10.1021/jacs.3c06393
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Metal-organic frameworks (MOFs) that contain open metal sites have the potential for storing hydrogen (H2) at ambient temperatures. In particular, Cu(I)-based MOFs demonstrate very high isosteric heats of adsorption for hydrogen relative to other reported MOFs with open metal sites. However, most of these Cu(I)-based MOFs are not stable in ambient conditions since the Cu(I) species display sensitivity toward moisture and can rapidly oxidize in air. As a result, researchers have focused on the synthesis of new air-stable Cu(I)-based materials for H-2 storage. Here, we have developed a de novo synthetic strategy to generate a robust Cu(I)-based MOF, denoted as NU-2100, using a mixture of Cu/Zn precursors in which zinc acts as a catalyst to transform an intermediate MOF into NU-2100 without getting incorporated into the final MOF structure. NU-2100 is air-stable and displays one of the initial highest isosteric heats of adsorption (32 kJ/mol) with good hydrogen storage capability under ambient conditions (10.4 g/L, 233 K/100 bar to 296 K/5 bar). We further elucidated the H2 storage performance of NU-2100 using a combination of spectroscopic analysis and computational modeling studies. Overall, this new synthetic route may enable the design of additional stable Cu(I)-MOFs for next-generation hydrogen storage adsorbents at ambient temperatures.
引用
收藏
页码:20492 / 20502
页数:11
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