气候变化领域集成服务门户(CCPortal): Exploring the Chemical Space of Metal-Organic Frameworks with rht Topology for High Capacity Hydrogen Storage

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DOI	10.1021/acs.jpcc.4c00638
	Exploring the Chemical Space of Metal-Organic Frameworks with rht Topology for High Capacity Hydrogen Storage
	Liu, Kunhuan; Chen, Zhijie; Islamoglu, Timur; Lee, Seung-Joon; Chen, Haoyuan; Yildirim, Taner; Farha, Omar K.; Snurr, Randall Q.
发表日期	2024
ISSN	1932-7447
EISSN	1932-7455
起始页码	128
结束页码	18
卷号	128 期号:18
英文摘要	Hydrogen is considered a crucial clean energy vector to mitigate climate change, but due to the low volumetric energy density of gaseous hydrogen, it is difficult to store hydrogen for many practical applications. Cryogenic sorption-based methods, particularly using metal-organic frameworks (MOFs), have been considered as viable solutions to enhance the deliverable capacity of stored hydrogen, and among the many available MOFs, those with rht topology have demonstrated exceptional capacity. MOFs with rht topology are formed by the assembly of supermolecular building blocks (SBBs), but the diversity of SBBs in the literature on rht-MOFs is limited, resulting in an underexplored structural design space. In this study, we designed 380 MOFs made of 20 novel SBBs to investigate the effect of cavity size on hydrogen storage capacity and the underlying structure-property relationships. We performed grand canonical Monte Carlo simulations on 472 rht-MOFs, encompassing both existing and novel structures, to predict hydrogen loadings under cryogenic conditions (77 K/100 bar -> 160 K/5 bar) and to study the influence of SBB size and composition on the hydrogen uptake. Our simulations revealed the potential to achieve high volumetric capacities using a variety of SBBs as well as variations in excess uptake per surface area among different SBBs. Regression models were utilized to examine the correlations between the hydrogen capacities and textual properties such as crystal density, pore diameters, pore volume per unit mass, and surface area. We built a quantitative model to further understand the relation between pore volume and deliverable capacities. Notably, PCN-61 demonstrated the highest simulated volumetric deliverable capacity among the MOFs studied and corresponded to an ideal pore volume suggested by our model. The computational investigation was further validated by high-pressure gas adsorption measurements for PCN-61.
语种	英语
WOS研究方向	Chemistry ; Science & Technology - Other Topics ; Materials Science
WOS类目	Chemistry, Physical ; Nanoscience & Nanotechnology ; Materials Science, Multidisciplinary
WOS记录号	WOS:001227971300001
来源期刊	JOURNAL OF PHYSICAL CHEMISTRY C
文献类型	期刊论文
条目标识符	http://gcip.llas.ac.cn/handle/2XKMVOVA/303376
作者单位	Northwestern University; Northwestern University; National Institute of Standards & Technology (NIST) - USA
推荐引用方式 GB/T 7714	Liu, Kunhuan,Chen, Zhijie,Islamoglu, Timur,et al. Exploring the Chemical Space of Metal-Organic Frameworks with rht Topology for High Capacity Hydrogen Storage[J],2024,128(18).
APA	Liu, Kunhuan.,Chen, Zhijie.,Islamoglu, Timur.,Lee, Seung-Joon.,Chen, Haoyuan.,...&Snurr, Randall Q..(2024).Exploring the Chemical Space of Metal-Organic Frameworks with rht Topology for High Capacity Hydrogen Storage.JOURNAL OF PHYSICAL CHEMISTRY C,128(18).
MLA	Liu, Kunhuan,et al."Exploring the Chemical Space of Metal-Organic Frameworks with rht Topology for High Capacity Hydrogen Storage".JOURNAL OF PHYSICAL CHEMISTRY C 128.18(2024).