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Alkali-Promoted Trimetallic Co−Rh−Mo Sulfide Catalysts for Higher Alcohols Synthesis from Synthesis Gas: Comparison of MWCNT and Activated Carbon Supports

2010; American Chemical Society; Volume: 49; Issue: 15 Linguagem: Inglês

10.1021/ie100427j

1520-5045

Venkateswara Rao Surisetty, Ajay K. Dalai, Janusz A. Koziński,

Electrocatalysts for Energy Conversion

Multiwalled carbon nanotubes (MWCNTs) and activated carbon were used as supports for the Co (4.5 and 6 wt %) promoted K (9 wt %) modified Rh−Mo catalysts (1.5 wt % Rh and 15 wt % Mo). The catalysts were extensively characterized in both oxide and sulfide phases. A drastic fall in surface area over the activated carbon-supported catalysts was observed after impregnating with metal species. Diffraction peaks were observed in the X-ray diffraction (XRD) patterns of the sulfided alkali-modified trimetallic catalysts, due to the characteristic reflections of the K−Mo−S mixed phase. H2-temperature programmed reduction (TPR) profiles showed that the reduction behavior of metal species was improved with the addition of Co. The activated carbon-supported trimetallic catalysts showed less activity and selectivity compared to the MWCNT-supported catalyst, and metal dispersions were higher on the MWCNT-supported catalysts. The MWCNT-supported, alkali-promoted trimetallic catalyst with 4.5 wt % Co showed the highest total alcohols yield of 0.244 g/(g cat h), ethanol selectivity of 20.1%, and higher alcohols selectivity of 31.4% at 320 °C and 8.28 MPa using a gas hourly space velocity (GHSV) of 3.6 m3 (STP)/(kg catalyst h). A maximum total alcohol yield of 0.261 g/(g cat h) and a selectivity of 42.9% were obtained on the 4.5 wt % Co−Rh−Mo−K/MWCNT catalyst, at a temperature of 330 °C. The total alcohol yield increased from 0.163 to 0.256 g/(g cat h) with increased pressure from 5.52 MPa (800 psig) to 9.65 MPa (1400 psig) over the 4.5 wt % Co−Rh−Mo−K/MWCNT catalyst.