Rh-Mn/tungsten carbides for direct synthesis of mixed alcohols from syngas: Effects of tungsten carbide phases

Authors
Da Won, BaJeong, Min HyeKim, Myeong HunChung, Chan-HwaMoon, Dong JuSuh, Young-WoongBaik, Joon HyunBae, Jong Wook
Issue Date
2018-01-01
Publisher
ELSEVIER SCIENCE BV
Citation
MICROPOROUS AND MESOPOROUS MATERIALS, v.255, pp.44 - 52
Abstract
Effects of the crystalline tungsten carbide (WxC) phases on an ordered mesoporous bimetallic Rh-Mn/WxC, which were prepared by changing carbon source to tungsten (C/W) ratios of the WxC support using a hard-template of an ordered mesoporous SBA-15, were investigated for a direct synthesis of mixed alcohols by CO hydrogenation from syngas. The C/W ratios on the mesoporous Rh-Mn/WxC showed a significantly different catalytic activity, especially on the C-1 - C-3 alcohol productivity. The Rh-Mn/WxC prepared at C/W molar ratio of 10 having a metastable W2C main phase (Rh-Mn/WxC(10)) revealed a higher CO conversion of 8.1% and selectivity to higher alcohols of 54.4% compared to other catalysts having a main crystalline phases of WO3 or WC. The enhanced catalytic activity and selectivity to mixed alcohols on the Rh-Mn/WxC(10) were attributed to the largely exposed smaller active Rh nanoparticles with its stronger interactions with the metastable W2C phases. The superior activity was originated from the intimate interactions of Rh nanoparticles with Mn promoter by maintaining proper oxidation states confirmed by surface ratios of the metallic Rh to oxidized Rhn+ species. The stable preservation of the ordered mesoporous structures of the W2C phase in the amorphous carbon matrixes significantly altered the chemical states of the small Rh nanoparticles below 2 nm in size by preferentially existing on the outer surfaces of the W2C support, which resulted in showing an enhanced productivity of higher C-1 - C-3 alcohols with 171.8 g/(kg(cat).h). (C) 2017 Elsevier Inc. All rights reserved.
Keywords
BIOMASS-DERIVED SYNGAS; CO HYDROGENATION; C-2-OXYGENATES SYNTHESIS; CATALYTIC CONVERSION; ETHANOL SYNTHESIS; SYNTHESIS GAS; CARBON; RHODIUM; PERFORMANCE; MECHANISM; BIOMASS-DERIVED SYNGAS; CO HYDROGENATION; C-2-OXYGENATES SYNTHESIS; CATALYTIC CONVERSION; ETHANOL SYNTHESIS; SYNTHESIS GAS; CARBON; RHODIUM; PERFORMANCE; MECHANISM; Mixed alcohol synthesis; CO hydrogenation; Mesoporous tungsten carbide (WxC); Bimetallic Rh-Mn; Metastable W2C
ISSN
1387-1811
URI
https://pubs.kist.re.kr/handle/201004/121819
DOI
10.1016/j.micromeso.2017.07.026
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KIST Article > 2018
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