Nickel Speciation and Methane Dry Reforming Performance of Ni/CexZr1-xO2 Prepared by Different Synthesis Methods

Lyu, Yimeng; Jocz, Jennifer; Xu, Rui; Stavitski, Eli; Sievers, Carsten

doi:10.1021/acscatal.0c02426

Title: Nickel Speciation and Methane Dry Reforming Performance of Ni/Ce_xZr_1-xO₂ Prepared by Different Synthesis Methods

Journal Article · Thu Sep 03 00:00:00 EDT 2020 · ACS Catalysis

DOI:https://doi.org/10.1021/acscatal.0c02426· OSTI ID:1706600

Lyu, Yimeng ^[1];

^[1]; Xu, Rui ^[1]; Stavitski, Eli ^[2];

^[1]

Georgia Inst. of Technology, Atlanta, GA (United States)
Brookhaven National Lab. (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)

Herein, ceria–zirconia-supported Ni catalysts (Ni/Ce_0.83Zr_0.17O₂ or Ni/CZ) are prepared by dry impregnation, strong electrostatic adsorption, coprecipitation (CP), and combustion synthesis (CS). The nature and abundance of Ni species in these samples are characterized by X-ray adsorption spectroscopy, temperature-programmed reduction, and CO chemisorption. The bulk synthesis methods (i.e., CP and CS) produce Ni cations that are incorporated into the CZ lattice forming mixed-metal oxides with Ni³⁺ species at low Ni content. The formation of mixed-metal oxides increases the reducibility of CZ and increases the abundance of active surface oxygen. All NiO/CZ catalysts are active for methane dry reforming and retain some of their activity at a steady state. The initial methane conversion correlates linearly with the fraction of accessible Ni after reduction. The predominant path of catalyst deactivation strongly depends on the structure of the catalyst and, thus, on the synthesis method used. All catalysts experience agglomeration of Ni particles under reaction conditions. Improving the Ni dispersion to isolated species embedded in a support does not improve resistance to Ni particle growth. Coke formation is inversely related to the concentration of active surface oxygen. The dominant deactivation mechanism for catalysts made by CS is the encapsulation of Ni particles by the support.

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Research Organization:: Georgia Institute of Technology, Atlanta, GA (United States); Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II) and Center for Functional Nanomaterials (CFN)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division; National Science Foundation (NSF)

Grant/Contract Number:: SC0016486; SC0012704; ECCS-1542174

OSTI ID:: 1706600

Alternate ID(s):: OSTI ID: 1659329

Report Number(s):: BNL-220571-2020-JAAM

Journal Information:: ACS Catalysis, Vol. 10, Issue 19; ISSN 2155-5435

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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