4.8 Article

Stabilizing Supported Ni Catalysts for Dry Reforming of Methane by Combined La Doping and Al Overcoating Using Atomic Layer Deposition

Journal

ACS CATALYSIS
Volume 12, Issue 17, Pages 10522-10530

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acscatal.2c02599

Keywords

catalyst design; atomic layer deposition; methane reforming; CO2 conversion; supported catalyst; catalyst stability; sintering; bimetallic catalysis

Funding

  1. Qatar National Research Fund (Qatar Foundation) [NPRP-EP X-100-2-024]
  2. U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DOE DE-FG0203ER15457]
  3. Soft and Hybrid Nanotechnology Experimental (SHyNE) Resource
  4. NSF-MRSEC program [DMR-1720139]
  5. IIN
  6. SHyNE Resource [NSF ECCS2025633]
  7. Northwestern University

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Deposition of La2O3 and Al2O3 on alumina-supported nickel catalyst can stabilize the catalytic activity and eliminate the induction period in the dry reforming of methane reaction.
Deposition of La2O3 and Al2O3 on Al2O3-supported Ni catalysts was performed to study their effects on heterogeneous catalysts for the dry reforming of methane (DRM) reaction. An alumina-supported Ni catalyst (Ni/Al2O3, 2 wt % of Ni), synthesized via incipient wetness impregnation, loses similar to 87% of its initial activity within 45 h under DRM conditions. While overcoating of Al2O3 on this catalyst via atomic layer deposition (ALD) helps stabilize the catalytic activity in long time-on-stream (TOS) tests, this overcoated catalyst is ca. 40 times less active than the uncoated catalyst at peak activity. This Al2O3-overcoated Ni/Al2O3 catalyst also exhibits a long induction period (similar to 20 h) due to the slow reduction of Ni2+ within the catalytically inactive nickel aluminate (NiAl2O4) phase, formed by the interaction of metallic Ni with the Al2O3 overcoat during pre-DRM treatment at the 700 degrees C reaction temperature. Here, we report that, while doping small amounts of La (similar to 0.03 wt %) into the Ni/Al2O3 catalyst does not significantly affect the catalytic activity or stability by itself, the addition of ALD-Al2O3 on top of the La2O3-promoted Ni catalysts significantly suppresses the long TOS deactivation, helps recover the peak activity of uncoated Ni/Al2O3, and eliminates the DRM induction period. This strategy obtains the stabilization benefits of Al2O3 overcoating on Ni/Al2O3 while, at the same time, avoiding the formation of undesirable NiAl2O4 species.

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