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An efficient base-metal NiMn/TiO2 catalyst for CO2 methanation

DOI: 10.1021/acscatal.9b01968 DOI Help

Authors: Wilbert L. Vrijburg (Eindhoven University of Technology) , Emanuele Moioli (École Polytechnique Fédérale de Lausanne (EPFL) Valais/Wallis, Energypolis; Empa Materials Science & Technology) , Wei Chen (Eindhoven University of Technology) , Min Zhang (Eindhoven University of Technology) , Bas Terlingen (Eindhoven University of Technology) , Bart Zijlstra (Eindhoven University of Technology) , Ivo A. W. Filot (Eindhoven University of Technology) , Andreas Zuttel (École Polytechnique Fédérale de Lausanne (EPFL) Valais/Wallis, Energypolis; Empa Materials Science & Technology) , Evgeny A. Pidko (Eindhoven University of Technology) , Emiel J.m. Hensen (Eindhoven University of Technology)
Co-authored by industrial partner: No

Type: Journal Paper
Journal: Acs Catalysis

State: Published (Approved)
Published: July 2019
Diamond Proposal Number(s): 16250

Open Access Open Access

Abstract: Energy storage solutions are a vital component of the global transition towards renewable energy sources. The Power-to-Gas (PtG) concept, which stores surplus renewable energy in the form of methane, has therefore become increasingly relevant in recent years. At present, supported Ni nanoparticles are preferred as industrial catalysts for CO2 methanation due to their low cost and high methane selectivity. However, commercial Ni catalysts are not active enough in CO2 methanation to reach the high CO2 conversion (>99 %) required by the specifications for injection in the natural gas grid. Herein we demonstrate the promise of promotion of Ni by Mn, another low-cost base metal, for obtaining very active CO2 methanation catalysts, with results comparable to more expensive precious metal-based catalysts. The origin of this improved performance is revealed by a combined approach of nanoscale characterization, mechanistic study, and density functional theory calculations. Nanoscale characterization with STEM-EDX and X-ray absorption spectroscopy shows that NiMn catalysts consist of metallic Ni particles decorated by oxidic Mn2+ species. A mechanistic study combining IR spectroscopy of surface adsorbates, transient kinetic analysis with isotopically labelled CO2, density functional theory calculations and microkinetics simulations ascertain that the MnO clusters enhance CO2 adsorption and facilitate CO2 activation. A macroscale perspective was achieved by simulating the Ni and NiMn catalytic activity in a Sabatier reactor, which revealed that NiMn catalysts have the potential to meet the demanding PtG catalyst performance requirements, and can largely replace the need for expensive and scarce noble metal catalysts.

Journal Keywords: CO2 hydrogenation; Nickel; Manganese; Synergy; Mechanism

Subject Areas: Chemistry, Energy

Instruments: B18-Core EXAFS

Added On: 22/07/2019 12:03


Discipline Tags:

Catalysis Physical Chemistry Earth Sciences & Environment Climate Change Energy Energy Storage Sustainable Energy Systems Chemistry

Technical Tags:

Spectroscopy X-ray Absorption Spectroscopy (XAS) Extended X-ray Absorption Fine Structure (EXAFS)