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

Journal Article · · ACS Catalysis
 [1];  [2];  [3]; ORCiD logo [2]; ORCiD logo [2]; ORCiD logo [2];  [2]; ORCiD logo [2]; ORCiD logo [4]; ORCiD logo [1]
  1. Mississippi State Univ., Mississippi State, MS (United States)
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  3. Northern Illinois Univ., DeKalb, IL (United States)
  4. Northern Illinois Univ., DeKalb, IL (United States); Argonne National Lab. (ANL), Argonne, IL (United States)
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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. In addition, 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.

Research Organization:
Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS); Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Science (CNMS)
Sponsoring Organization:
Mississippi State University; USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division; USDOE Office of Science - Office of Basic Energy Sciences
Grant/Contract Number:
AC02-06CH11357; AC05-00OR22725
OSTI ID:
1883779
Journal Information:
ACS Catalysis, Journal Name: ACS Catalysis Journal Issue: 5 Vol. 12; ISSN 2155-5435
Publisher:
American Chemical Society (ACS)Copyright Statement
Country of Publication:
United States
Language:
English

References (21)

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Cooperative catalysis of metal and acid functions in Re-HZSM-5 catalysts for ethane dehydroaromatization journal April 2019
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Quantification of rhenium oxide dispersion on zeolite: Effect of zeolite acidity and mesoporosity journal April 2019
Plasma-Catalytic Ammonia Reforming of Methane over Cu-Based Catalysts for the Production of HCN and H 2 at Reduced Temperature journal January 2021
Tuning the Number of Active Sites and Turnover Frequencies by Surface Modification of Supported ReO 4 /(SiO 2 –Al 2 O 3 ) Catalysts for Olefin Metathesis journal February 2021
Catalytic Light Alkanes Conversion through Anaerobic Ammodehydrogenation journal June 2021
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Ammonia synthesis by N2 and steam electrolysis in molten hydroxide suspensions of nanoscale Fe2O3 journal August 2014
Beyond fossil fuel–driven nitrogen transformations journal May 2018

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
COx free H2
COx-free H2
ammonia reforming
anti-coke
isolated ReOx
light alkanes