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Ammonia-Assisted Light Alkane Anti-coke Reforming on Isolated ReOx Sites in Zeolite...

Publication Type
Journal Name
ACS Catalysis
Publication Date
Page Numbers
3165 to 3172

The conventional reforming produces H2 with stoichiometric amounts of CO and CO2 from hydrocarbons. Here, we show that COx-free H2 can be produced from ammonia-assisted reforming (ammoreforming) of natural gas liquids (CnH2n+2 + nNH3 = nHCN + (2n + 1) H2, n = 2 or 3) at the same conditions as the steam reforming. Such a process co-produces HCN, which can be easily separated from H2 and used as value-added chemicals or for NH3 recycling through hydrolysis. The ammoreforming of ethane and propane was realized over the Re-modified HZSM-5 zeolite rather than the traditional Pt-based catalyst for the BMA process (methane ammoreforming). The specific activity of the Re/HZSM-5 catalysts at 650 °C is up to 1 molH2/gRe/min (or 180 min–1) during ethane ammoreforming. The catalyst is highly coke resistant and shows only slight deactivation with a time-on-stream up to 20 h. Characterization of the fresh and used catalysts by X-ray absorption and Raman spectroscopies suggested that the isolated ReOx site grafted by AlO4– tetrahedral in the zeolite framework is responsible for the outstanding catalytic activity and coke resistibility.