The development of economically viable techniques for producing hydrogen from liquid organic carriers is a grand challenge with important societal and environmental sustainability implications. One of main issues that remain to be solved in this area is the lack of an efficient catalyst to reversibly produce hydrogen under mild conditions and to achieve high selectivity for H2without producing greenhouse gases, such as carbon dioxide. Catalytic hydrogen generation from polyalcohols has the potential to have the carbon pre-sequestered in stable C-C bonds that remain unaltered during the process, thus preventing CO2release and ensuring a completely carbon-neutral energy cycle upon subsequent hydrogenation to regenerate the polyalcohols. A common feature for efficient dehydrogenation catalysts is the presence of highly active sites that are favorable for C-H and O-H bond activation. We are developing nanoporous Metal-Organic Frameworks (MOFs) to catalyze hydrogen production from polyalcohols, such as ethyleneglycol and glycerol. MOF possess unsurpassed tailorability in pore size and environment and high chemical robustness required for industrial-scale processes. Moreover, as solid materials, MOFs are easily separated from product mixtures. Here, we describe experiments using theversatile IRMOF-74(n) series as a catalytic platform for hydrogen production from ethyleneglycol and glycerol. Residual Gas Analysis experiments demonstrate that hydrogen is produced at a high rate in the presence of IRMOF-74 catalysts without detectable amounts of carbon dioxide. The MOF catalysts are recyclable and reusable and retain their crystallinity and framework structure after the catalytic process. These studies represent the first step towards gaining an understanding of the factors that affect the catalytic activity and selectivity of MOFs for sustainable hydrogen storage in liquid organic carriers.

Sustainable hydrogen storage in polyalcohols enabled by metal-organic framework catalysts

2019 Spring National Meeting

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