Abstract
Environmental problems associated with the use of fossil fuels and increase in energy demands due to rise in population and rapid industrialisation, are the driving forces for energy. Catalytic conversion of biomass to renewable energies is among the promising approaches to materialize the above. This requires development of robust catalysts to suppress deactivation due to carbon deposition and agglomeration. In this work, surface properties and chemistry such as exsolution of B-site metal catalyst nanoparticles, particle size and distribution, as well as catalyst-support interactions were tailored through the use of alkaline dopants to enhance catalytic behaviour in valorisation of glycerol. The incorporation of alkaline metals into the lattice of an A-site deficient perovskite modified the surface basic properties and morphology with a consequent robust catalyst-support interaction. This resulted in promising catalytic behaviour of the materials where hydrogen selectivity of over 30% and CO selectivity of over 60% were observed. The catalyst ability to reduce fouling of the catalyst surface as a result of carbon deposition during operation was also profound due to the robust catalyst-support interaction occurring at the exsolved nanoparticles due to their socketing and the synergy between the dopant metals in the alloy in perovskite catalyst systems. In particular, one of the designed systems, La0.4Sr0.2Ca0.3Ni0.1Ti0.9O3±δ, displayed almost 100% resistance to carbon deposition. Therefore, lattice rearrangement using exsolution and choice of suitable dopant could be tailored to improve catalytic performance.
Highlights
Fouling of the used catalysts surface due to carbon deposition during catalysis was characterized using temperature programmed oxidation (TPO) on NETZSCH STA 449C thermogravimetric analyser equipped with Thermostar mass spectrometer
The crystallographic data obtained at room temperature was used to ascertain the phase purity of the synthesised catalyst systems
The catalysts systems were tested for several hours to further analyse their activity as well as stability to deactivation as a result of carbon deposition, catalyst sintering, or poisoning due to prolonged usage in gaseous stream
Summary
Catalytic steam reforming of pure glycerol was performed in a fixed bed quartz tube reactor (8 mm internal diameter (ID), 10 mm outer diameter (OD) and 24 cm long) at 700 oC and atmospheric pressure. Syringe Harvard apparatus 22 infusions pump supplied the glycerol-water mixture (steam/carbon ratio 3:1) at the flow rate of 0.019 mL/min and weight hourly space velocity (WHSV) of 28 h-1 to a stainless-steel pipe wrapped with heating tape at 250 oC for vaporisation and mixing. The vaporised reactant mixture was introduced into the reactor by high purity carrier Helium gas at flow rate of 40 mL/min and was controlled by mass flow controllers. The stability test was carried out at constant temperature of 700 oC at a heating of 5 oC under the helium gas carrier. The system was allowed to attain the required temperature and stabilised before the glycerol feedstock began to flow continuously for 10 h
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