At present, there is no low pressure methanol synthesis from CO2/H2 with high yield despite the presence of an upstream process of aqueous phase reforming (APR) of biomass derivatives on an industrial scale for CO2/H2 production at ca. 2 MPa. This is due to the intrinsic thermodynamics of the system which leads to particularly high CO levels at low pressure through reversed water gas shift reaction (RWGS) for most studied catalysts. Here we report a new Pd@Zn core-shell catalyst that offers a significantly higher kinetic barrier to CO/H2O formation in CO2 hydrogenation to reduce the CO levels but facilitates CH3OH formation at or below 2 MPa with CH3OH selectivity maintained at ca. 70% compared to ca. 10% over industrial Cu catalysts. The corresponding methanol yield at 2 MPa reaches 6.1 gmethanol gactive metal-1 h-1, which is comparable to the best reported value among a wide variety of catalysts under 5 MPa. It is thus believed that this active Pd based catalyst opens up a promising possibility for low pressure and temperature methanol production using a renewable biomass resource for fossil-fuel-starved countries.
|Original language||English (US)|
|Number of pages||11|
|State||Published - 2017|
Bibliographical noteFunding Information:
The authors wish to thank EPSRC, UK (Oxford) and NSFC-21421004, 21373153, 21322307, China for the financial support for this collaborative work and are grateful to the Chinese Scholarship Council (CSC) of China for granting a PhD scholarship to FL to work at Oxford. The ECUST group acknowledges the computing time at the National Super Computing Center in Jinan, China. The authors thank Diamond Light Source to allow a rapid access to the EXAFS facilities on B18.
© The Royal Society of Chemistry 2017.