Centralized and distributed hydrogen production using steam reforming: challenges and perspectives

Han, Ja-Ryoung; Park, So-Jin; Kim, Hyoung-Tae; Lee, Shinje; Lee, Jong Min

doi:10.1039/d1se01870a

Cited by 11 publications

(2 citation statements)

References 128 publications

(130 reference statements)

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“…In such processes, hydrogen is generated via catalyzed endothermic equilibrium reactions between a hydrocarbon ( e.g. , methanol, acetone, methane, formic acid, or ethylene glycol) and steam …”

Section: Introductionmentioning

confidence: 99%

“…photocatalytic, electrical, and biological processes utilized, including fermentation, biophotolysis, alkaline electrolysis, and water-splitting-based solar energy, steam reforming processes are considered the most feasible route for hydrogen production 6. In such processes, hydrogen is generated via catalyzed endothermic equilibrium reactions between a hydrocarbon (e.g., methanol, acetone, methane, formic acid, or ethylene glycol) and steam 7. …”

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confidence: 99%

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Selective Photocatalytic Dehydrogenation of Formic Acid by an In Situ-Restructured Copper-Postmetalated Metal–Organic Framework under Visible Light

et al. 2022

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Formic acid is considered as one of the most promising liquid organic hydrogen carriers. Its catalytic dehydrogenation process generally suffers from low activity, low reaction selectivity, low stability of the catalysts, and/or the use of noblemetal-based catalysts. Herein we report a highly selective, efficient, and noble-metal-free photocatalyst for the dehydrogenation of formic acid. This catalyst, UiO-66(COOH) 2 -Cu, is built by postmetalation of a carboxylic-functionalized Zr-MOF with copper. The visible-lightdriven photocatalytic dehydrogenation process through the release of hydrogen and carbon dioxide has been monitored in real-time via operando Fourier transform infrared spectroscopy, which revealed almost 100% selectivity with high stability (over 3 days) and a conversion yield exceeding 60% (around 5 mmol•g cat −1•h −1 ) under ambient conditions. These performance indicators make UiO-66(COOH) 2 -Cu among the top photocatalysts for formic acid dehydrogenation. Interestingly, the as-prepared UiO-66(COOH) 2 -Cu hetero-nanostructure was found to be moderately active under solar irradiation during an induction phase, whereupon it undergoes an in-situ restructuring process through intraframework cross-linking with the formation of the anhydride analogue structure UiO-66(COO) 2 -Cu and nanoclustering of highly active and stable copper sites, as evidenced by the operando studies coupled with steady-state isotopic transient kinetic experiments, transmission electron microscopy and X-ray photoelectron spectroscopy analyses, and Density Functional Theory calculations. Beyond revealing outstanding catalytic performance for UiO-66(COO) 2 -Cu, this work delivers an in-depth understanding of the photocatalytic reaction mechanism, which involves evolutive behavior of the postmetalated copper as well as the MOF framework over the reaction. These key findings pave the way toward the engineering of new and efficient catalysts for photocatalytic dehydrogenation of formic acid.

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Section: Introductionmentioning

confidence: 99%

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confidence: 99%