4.8 Article

Harnessing Strong Metal-Support Interaction to Proliferate the Dry Reforming of Methane Performance by In Situ Reduction

Journal

ACS APPLIED MATERIALS & INTERFACES
Volume 14, Issue 10, Pages 12140-12148

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acsami.1c20889

Keywords

dry reforming of methane; nickel; cerium oxide; strong metal-support interaction; aggregation

Funding

  1. National Research Foundation of Korea (NRF) - Korea government (MSIT) [2021R1A2C2092130, 2020R1A2C2103137, 2020R1F1A1076359, CPS21131-100]
  2. Nano-Material Technology Development Program through the National Research Foundation of Korea (NRF) - Ministry of Science and ICT [2018M3A7B4070990]
  3. Materials, Components & Equipment Research Program - Gyeonggi Province
  4. National Research Council of Science & Technology (NST), Republic of Korea [CPS21131-100] Funding Source: Korea Institute of Science & Technology Information (KISTI), National Science & Technology Information Service (NTIS)
  5. National Research Foundation of Korea [2021R1A2C2092130, 2018M3A7B4070990, 2020R1A2C2103137, 2020R1F1A1076359] Funding Source: Korea Institute of Science & Technology Information (KISTI), National Science & Technology Information Service (NTIS)

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The strong bonding between the metal and support known as strong metal-support interaction (SMSI) can inhibit the aggregation of metal nanoparticles and carbon deposition during hydrocarbon reforming. This interaction is significantly affected by the heat treatment and reducing conditions during catalyst preparation. A mild reduction process using dry methane gas is proposed to increase the exposed interface between the metal and support and enhance the catalytic activity of the nanocatalyst. The effects of this process on the chemical state of Ni-cerium oxide nanocatalysts were investigated, leading to the formation of a significant amount of the Ni3+ phase and improved SMSI.
The strong bonding at the interface between the metal and the support, which can inhibit the undesirable aggregation of metal nanoparticles and carbon deposition from reforming of hydrocarbon, is well known as the classical strong metal-support interaction (SMSI). SMSI of nanocatalysts was significantly affected by heat treatment and reducing conditions during catalyst preparation.the heat treatment and reduction conditions during catalyst preparation. SMSI can be weakened by the decrement of metal-doped sites in the supporting oxide and can often deactivate catalysts by the encapsulation of active sites through these processes. To retain SMSI near the active sites and to enhance the catalytic activity of the nanocatalyst, it is essential to increase the number of surficial metal-doped sites between nanometal and the support. Herein, we propose a mild reduction process using dry methane (CH4/CO2) gas that suppresses the aggregation of nanoparticles and increases the exposed interface between the metal and support, Ni and cerium oxide. The effects of mild reduction on the chemical state of Ni-cerium oxide nanocatalysts were specifically investigated in this study. As a result, mild reduction led to form large amounts of the Ni3+ phase at the catalyst surface of which SMSI was significantly enhanced. It can be easily fabricated while the dry reforming of methane (DRM) reaction is on stream. The superior performance of the catalyst achieved a considerably high CH4 conversion rate of approximately 60% and stable operation up to 550 h at a low temperature, 600 degrees C.

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