Highly Efficient SiC-Supported Ni-Based Catalystswith Enhanced Recycle Stability for One-Pot Cellobiose HydrolyticHydrogenation to Hexitols
2020
In
this contribution, SiC material was applied as the catalyst
support in the aqueous-phase reaction of one-pot cellobiose hydrolytic
hydrogenation to hexitols, with the less costly transition metal Ni.
Even with its neutral nature, more than 50% hexitol yield was achieved
with Ni contents as low as 3 wt % supporting on SiC, and further improved
to near 70% hexitol yield with Ni loadings increased to 5 wt %. The
catalytic performances were superior to the others supported with
different carriers (Al2O3, carbon nanotube (CNT),
and AC). DFT simulation results indicate that the H2 dissociation
energy on the Ni4/SiC(111) slab is at −26.9 kcal/mol,
which is substantially lower than those on the Ni4/Al2O3(100) slab (−34.1 kcal/mol) and Ni4/graphene slab (−32.5 kcal/mol, taken graphene as a
local structure of CNT). The hexitol yield on SiC-supported Ni catalyst
was further improved to 75.7% with Ir promoter, more importantly,
with a much enhanced recycle stability. Hexitol yield could be maintained
around 60% even after five cycles on Ir-promoted catalyst, compared
to 12% after only three cycles on Ni monometallic catalyst. ICP-OES
results revealed that the leaching of Ni was greatly inhibited with
the assistance of Ir. The results of the H2-TPR analysis
suggest an easier H2 activation ability observed on the
surface of Ir-promoted catalyst due to the synergetic effects between
Ni and Ir. The findings would shed light on SiC for further applications
in biomass conversion.
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