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research article

Investigating active phase loss from supported ruthenium catalysts during supercritical water gasification

Hunston, Christopher
•
Baudouin, David
•
Tarik, Mohamed
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October 14, 2021
Catalysis Science & Technology

Active phase loss mechanisms from Ru/AC catalysts were studied in continuous supercritical water gasification (SCWG) for the first time by analysing the Ru content in process water with low limit-of-detection time-resolved ICP-MS. Ru loss was investigated alongside the activity of commercial and in-house Ru-based catalysts, showing very low Ru loss rates compared to Ru/metal-oxides (0.2-1.2 vs. 10-24 mu g g(Ru)(-1) h(-1), respectively). Furthermore, AC-supported Ru catalysts showed superior long-term SCWG activity to their oxide-based analogues. The impact on Ru loss of several parameters relevant for catalytic SCWG (temperature, feed concentration or feed rate) was also studied and was shown to have no effect on the Ru concentration in the process water, as it systematically stabilised to 0.01-0.2 mu g(Ru) L-1 for Ru/AC. Looking into the type of Ru loss in steady-state operation, time-resolved ICP-MS confirmed a high probability of finding Ru in the ionic form, suggesting that leaching is the main steady-state Ru loss mechanism. In non-steady-state operation, abrupt changes in the pressure and flow rate induced important Ru losses, which were assigned to catalyst fragments. This is directly linked to irreversible mechanical damage to the catalyst. Taking the different observations into consideration, the following Ru loss mechanisms are suggested: 1) constant Ru dissolution (leaching) until solubility equilibrium is reached; 2) minor nanoparticle uncoupling from the support (both at steady state); 3) support disintegration leading to the loss of larger amounts of Ru in the form of catalyst fragments (abrupt feed rate or pressure variations). The very low Ru concentrations detected in process water at steady state (0.01-0.2 mu g(Ru) L-1) are close to the thermodynamic equilibrium and indicated that leaching did not contribute to Ru/AC deactivation in SCWG.

  • Details
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Type
research article
DOI
10.1039/D1CY00379H
Web of Science ID

WOS:000707139600001

Author(s)
Hunston, Christopher
Baudouin, David
Tarik, Mohamed
Kröcher, Oliver
Vogel, Frédéric
Date Issued

2021-10-14

Published in
Catalysis Science & Technology
Volume

11

Issue

22

Start page

7431

End page

7444

Subjects

pressure aqueous environments

•

synthetic natural-gas

•

hydrothermal gasification

•

biomass gasification

•

heterogeneous catalysts

•

hydrogen-production

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chemical-reactions

•

high-temperature

•

metal-catalysts

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ru/c catalysts

Editorial or Peer reviewed

REVIEWED

Written at

EPFL

EPFL units
GR-LUD  
GR-KRO  
FunderGrant Number

FNS

200021_184817

FNS

200021_172624/1

CTI/Innosuisse

SCCER BIOSWEET

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Available on Infoscience
January 17, 2022
Use this identifier to reference this record
https://infoscience.epfl.ch/handle/20.500.14299/184606
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