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

ABSTRACT: 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 μg gRu -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 μgRu 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 μgRu L-1) are close to the thermodynamic equilibrium and indicated that leaching did not contribute to Ru/AC deactivation in SCWG.

SUBMITTER: Hunston C

PROVIDER: S-EPMC8591986 | biostudies-literature |

REPOSITORIES: biostudies-literature

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Project description:Hydrogen production from biomass, a renewable resource, has been attracting attention in recent years. We conduct a detailed process design for cellulose-derived hydrogen production via glucose using supercritical water gasification technology. Gasification of biomass in supercritical water offers advantages over conventional biomass conversion methods, including high gasification efficiency, elevated hydrogen molar fractions, and the minimization of drying process for wet biomass. In the process design, a continuous tank reactor is employed because the reaction in the glucose production process involves solids, and using a tube-type reactor may clog the reactor with solids. In the glucose separation process, glucose and levulinic acid, which cannot be separated by boiling point difference, are separated by using an extraction column. In the hydrogen separation process, the hydrogen purity, which could not be sufficiently increased with a single pressure swing adsorption (PSA) process, is increased to the target value by employing two sets of PSA columns. The overall utility cost is significantly reduced by $0.020/mol-H2 through heat integration. Our economic evaluation for this process results in a deficit of $0.015/mol-H2, as a price to be paid by the human for renewable hydrogen production from biomass at the present stage. By simply adopting the reported experimental condition, our process contains a large amount of water and sulfuric acid, which requires an enormous cost for the neutralizer, drying utility, and extractant. To improve the economic performance of the process, it is necessary to consider the reaction of cellulose solution at a higher concentration to reduce the burden of glucose separation. In addition, the effective use of the wasted hydrogen with a purity of about 95 vol% from the second PSA column may also improve the process economics. Whilst, the required energy cost for hydrogen production for our process is calculated to be significantly lower than those for other various representative hydrogen production methods: 0.37 (0.44) times less than that of steam reforming of methane with (without) CO2 capture, 0.15 times less than that of the water electrolysis by the electric power system, and 0.073 times less than that of electrolysis of water by wind power. This result implies the practical potential of our cellulose-based green hydrogen production scheme.

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

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