Journal
JOURNAL OF CO2 UTILIZATION
Volume 17, Issue -, Pages 273-283Publisher
ELSEVIER SCI LTD
DOI: 10.1016/j.jcou.2016.11.016
Keywords
CO2 hydrogenation; Oxalate ligand functionalization; Methanol; Methyl formate; ZSM-5
Funding
- Mitsybishi Corporation Education Trust Fund, University Teknologi PETRONAS, Malaysia
- Ministry of Higher Education Malaysia [FRGS/2/2014/SG01/UTP/02/2]
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Co-synthesis of methanol and methyl formate (MF) was achieved in this study using expediently synthesized ZSM-5 supported oxalate ligand functionalized Cu/ZnO catalyst (CZOx/Z) in a continuous flow reactor. The catalyst characterization results showed that the synthesis protocol via oxalate ligand functionalization (OLF) achieved considerable reduction of CuO -> Cu2O -> Cu leading to highly reducible active metals with largely weak metal-support-interactions according to the X-ray photoelectron spectroscopy, Raman spectroscopy and temperature programmed reduction. The ZnO reduction peak was also observed to shift to lower reduction temperature. Furthermore, the NH3- and CO2- temperature programmed desorption studies showed that CZOx/Z has both acid and basic sites, but the acid sites were about four times higher. These qualities were ascribed to the OLF at the synthesis stage which also guarantees ultrafine active metal particle sizes with high degree of dispersion. The CZOx/Z showed exceptional CO2 hydrogenation activity at 250 degrees C and 2.25 MPa, the initial CO2 conversion increased marginally from 15.5 to 15.9% in the first 180 min and increased to 20.5% at 600 min time-on-stream. The increment was ascribed to reduction of remnant unreduced active metal species with methanol which simultaneously proceeds with dehydrogenation of produced methanol to form MF promoted by the acid sites. The methanol selectivity was 97.16% at 60 min TOS and later decreased to 64.64% at 180 min as the formation of MF increased owing to the progressive reduction of active metals with formed methanol. CZOx/Z is a promising catalyst for co-synthesis of methanol and MF. (C) 2016 Elsevier Ltd. All rights reserved.
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