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This content will become publicly available on October 16, 2018

Title: Tuning Ni-catalyzed CO 2 hydrogenation selectivity via Ni-ceria support interactions and Ni-Fe bimetallic formation

CO 2 hydrogenation over Fe-modified Ni/CeO 2 catalysts was investigated in a batch reactor using time-resolved in situ FTIR spectroscopy. Low loading of Ni/CeO 2 was associated with high selectivity to CO over CH 4, while higher Ni loading improved CO 2 hydrogenation activity with a reduced CO selectivity. X-ray absorption near-edge structure (XANES) analysis revealed Ni to be metallic for all catalysts including the CO-selective low loading 0.5% Ni catalyst, suggesting that the selectivity trend is due to structural rather than oxidation state effects. The loading amount of 1.5% Ni was selected for co-impregnation with Fe, based on the significant shift in product selectivity towards CH 4 for that loading amount, in order to shift the selectivity towards CO while maintaining high activity. Temperature programmed reduction (TPR) results indicated bimetallic interactions between Ni and Fe, and XANES analysis showed that about 70% of Fe in the bimetallic catalysts was oxidized. The Ni-Fe catalysts demonstrated improved selectivity towards CO without significantly compromising activity, coupling the high activity of Ni catalysts and the high CO selectivity of Fe. The general trends in Ni loading and bimetallic modification should guide efforts to develop non-precious metal catalysts for the selective production of COmore » by CO 2 hydrogenation.« less
Authors:
 [1] ;  [1] ;  [2] ;  [2] ;  [3]
  1. Columbia Univ., New York, NY (United States). Department of Chemical Engineering
  2. Brookhaven National Lab. (BNL), Upton, NY (United States). Chemistry Department
  3. Columbia Univ., New York, NY (United States). Department of Chemical Engineering; Brookhaven National Lab. (BNL), Upton, NY (United States). Chemistry Department
Publication Date:
Report Number(s):
BNL-203438-2018-JAAM
Journal ID: ISSN 0926-3373
Grant/Contract Number:
SC0012704
Type:
Accepted Manuscript
Journal Name:
Applied Catalysis. B, Environmental
Additional Journal Information:
Journal Volume: 224; Journal Issue: C; Journal ID: ISSN 0926-3373
Publisher:
Elsevier
Research Org:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; CO2 reduction; Ni loading; Ni-Fe bimetallic catalysts; Metal oxide; XANES
OSTI Identifier:
1430879