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Straightforward Synthesis of Hierarchically Porous Nitrogen-Doped Carbon via Pyrolysis of Chitosan/Urea/KOH Mixtures and Its Application as a Support for Formic Acid Dehydrogenation Catalysts

The development of cheap, simple, and green synthetic methods for hierarchically porous nitrogen-doped carbon, especially derived from renewable biomass, such as chitosan, remains a challenging topic. Here, we first synthesized hierarchically porous nitrogen-doped carbon (KIE-8) having graphene-like...

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Bibliographic Details
Published in:ACS sustainable chemistry & engineering 2017-11, Vol.5 (11), p.9935-9944
Main Authors: Lee, Dong-Wook, Jin, Min-Ho, Oh, Duckkyu, Lee, Sung-Wook, Park, Jong-Soo
Format: Article
Language:English
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Summary:The development of cheap, simple, and green synthetic methods for hierarchically porous nitrogen-doped carbon, especially derived from renewable biomass, such as chitosan, remains a challenging topic. Here, we first synthesized hierarchically porous nitrogen-doped carbon (KIE-8) having graphene-like structure via simple pyrolysis of a chitosan/urea/KOH mixture without any conventional sophisticated treatments, such as freeze-drying, hydrothermal carbonization, and soft or hard templating. On the basis of various analyses of KIE-8, we demonstrated that effect of urea on mesopore formation was insignificant; however, when KOH is used as an activating agent in the presence of urea, a large amount of mesopores can be created along with conventional KOH-derived micropores. In addition, it was revealed that chitosan-derived carbon nanosheets directed by urea are torn into chitosan-derived carbon nanoflakes via KOH activation, and mesopores originate from interstitial voids in aggregates of the carbon nanoflakes, and micropores are derived from in-plane pores in each nanoflake. KIE-8 was used as a catalyst support for formic acid dehydrogenation at room-temperature. Pd­(6 wt %)/KIE-8 catalysts provided excellent catalytic activity (TOF = 280.7 mol H2 mol metal–1 h–1), and we demonstrated that the pore structure and nitrogen structure of KIE-8 are crucial factors to determine the catalytic activity.
ISSN:2168-0485
2168-0485
DOI:10.1021/acssuschemeng.7b01888