Journal
CHEMSUSCHEM
Volume 11, Issue 19, Pages 3396-3401Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/cssc.201801521
Keywords
electronic interactions; hydrogen generation; melem; palladium; polyoxometalate
Funding
- National Natural Science Foundation of China [21206052]
- Fundamental Research Funds for the Central Universities [JUSRP51623A]
- Division of Chemical Sciences, Geosciences and Biosciences, Office of Basic Energy Sciences, U.S. Department of Energy
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Pd nanoparticles (NPs) anchored on a phosphotungstic acid attached melem porous hybrid (PW/melem) were prepared by hybridization of phosphotungstic acid Pd salt and melem, followed by chemical reduction. PW/melem was demonstrated to be an outstanding support that can stabilize and disperse small Pd NPs (2 nm), and significantly boost their efficiency for H-2 generation from the dehydrogenation of formic acid (FA). Experimental results and mechanistic investigations indicate that a strong electronic interaction exists between Pd NPs and the PW anions; the PW anions accept electrons from Pd first and, during FA dehydrogenation, the reduced blue PW donates electrons to Pd. Moreover, melem plays an important role in hydrogen transfer and can accelerate H-2 generation. The overall synergistic effect of PW and melem endows Pd NPs with extremely high activity and stability for complete FA conversion at 50 degrees C, achieving a high turnover frequency of 15393 h(-1).
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