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An, Kwangjin
Advanced Nanocatalysis Lab (An Lab)
Research Interests
  • Nanoparticle catalytsts, catalytic activity, selectivity, and stability, strong metal-support interactions, biofuel conversion

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Integration of Interfacial and Alloy Effects to Modulate Catalytic Performance of Metal-Organic-Framework-Derived Cu-Pd Nanocrystals toward Hydrogenolysis of 5-Hydroxymethylfurfural

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Title
Integration of Interfacial and Alloy Effects to Modulate Catalytic Performance of Metal-Organic-Framework-Derived Cu-Pd Nanocrystals toward Hydrogenolysis of 5-Hydroxymethylfurfural
Author
Sarkar, ChitraKoley, ParamitaShown, IndrajitLee, JihyeonLiao, Yen-FaAn, KwangjinTardio, JamesNakka, LingaiahChen, Kuei-HsienMondal, John
Issue Date
2019-06
Publisher
AMER CHEMICAL SOC
Citation
ACS SUSTAINABLE CHEMISTRY & ENGINEERING, v.7, no.12, pp.10349 - 10362
Abstract
Selective formation of 2,5-dimethylfuran (DMF) by hydrogenolysis of lignocellulosic biomass-derived 5-hydroxymethylfurfural (HMF) is highly desirable for renewable liquid biofuel production. Here we have synthesized Cu-Pd bimetallic nanoparticles embedded in carbon matrix (Cu-Pd@C) by simple pyrolysis of Pd-impregnated Cu-based metal-organic frameworks (MOFs) followed by conventional hydrogenation route. It was found that Cu-Pd@C-B (solid-gas-phase hydrogenation route) with Cu-Pd bimetallic alloying exhibited brilliant catalytic performance at 120 degrees C under 15 bar H-2 pressure to produce liquid DMF biofuel with 96.5% yield from HMF as compared with the Cu-Pd@C-A catalyst (liquid phase hydrogenation route), which gave 46.4% yield under the same conditions. X-ray photoelectron spectroscopy (XPS) and X-ray absorption near-edge structure (XANES) studies reveal that Pd in Cu-Pd@C-B catalyst is electronically promoted by Cu with the unique intrinsic synergy of increased Pd-Pd bond distance and decreased Cu-Cu bond length, which eventually modulate the local atomic structural environment and result in enhanced catalytic activity. Moreover, the entrapped bimetallic nanoparticles with carbon shells in Cu-Pd@C-B catalyst further protect the active catalytic site from migration, aggregation, and leaching during hydrogenolysis reaction and improve the stability of the catalyst.
URI
https://scholarworks.unist.ac.kr/handle/201301/27025
URL
https://pubs.acs.org/doi/10.1021/acssuschemeng.9b00350
DOI
10.1021/acssuschemeng.9b00350
ISSN
2168-0485
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