当前位置: X-MOL 学术J. Am. Chem. Soc. › 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.)
Quest for an optimal methane hydrates formation in the pores of hydrolytically stable MOFs
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2020-07-11 , DOI: 10.1021/jacs.0c01459
Carlos Cuadrado-Collados 1 , Georges Mouchaham 2 , Luke Daemen 3 , Yongqiang Cheng 3 , Anibal Ramirez-Cuesta 3 , Himanshu Aggarwal 2 , Alexander Missyul 4 , Mohamed Eddaoudi 2 , Youssef Belmabkhout 2, 5 , Joaquin Silvestre-Albero 1
Affiliation  

Porous MOFs capable of storing relatively high amount of dry methane (CH4) in adsorbed phase are largely explored, how-ever solid CH4 storage in confined pores of MOFs in the form of hydrates is yet to be discovered. Here we report a rational approach to form CH4 hydrates by taking advantage of the optimal pore confinement in relatively narrow cavities of hydro-lytically stable MOFs. Unprecedentedly, we were able to isolate methane hydrate (MH) nanocrystals with a sI structure en-capsulated inside MOF pores with an optimal cavity dimension. It was found, that confined nanocrystals require cavities slightly larger than the unit cell crystal size of MHs (1.2 nm), as exemplified in the experimental case study performed on Cr-soc-MOF-1 vs smaller cavities of Y-shp-MOF-5. Under these conditions, the excess amount of methane stored in the pores of Cr-soc-MOF-1 in the form of MH was found to be 50% larger than the corresponding dry adsorbed amount at 10 MPa. More importantly, the pressure gradient driving the CH4 storage/delivery process could be drastically reduced com-pared to the conventional CH4 adsorbed phase storage on the dry Cr-soc-MOF-1 (≤3 MPa vs. 10 MPa).

中文翻译:

寻找在水解稳定的 MOF 孔中形成最佳甲烷水合物的方法

能够在吸附相中储存相对大量干甲烷 (CH4) 的多孔 MOF 得到了大量探索,但尚未发现以水合物形式在 MOF 的密闭孔中储存固体 CH4。在这里,我们报告了一种合理的方法,通过利用水解稳定 MOF 相对狭窄的空腔中的最佳孔隙限制来形成 CH4 水合物。前所未有地,我们能够分离出具有 sI 结构的甲烷水合物 (MH) 纳米晶体,该结构封装在具有最佳腔尺寸的 MOF 孔内。研究发现,受限纳米晶体需要比 MHs 的晶胞晶体尺寸(1.2 nm)稍大的腔,如在 Cr-soc-MOF-1 上进行的实验案例研究与 Y-shp-MOF-的较小腔相比, 5. 在这些条件下,发现以 MH 形式储存在 Cr-soc-MOF-1 孔隙中的过量甲烷比 10 MPa 下相应的干吸附量大 50%。更重要的是,与干燥 Cr-soc-MOF-1 上的传统 CH4 吸附相存储(≤3 MPa vs. 10 MPa)相比,驱动 CH4 存储/输送过程的压力梯度可以显着降低。
更新日期:2020-07-11
down
wechat
bug