Kinetics of steam regeneration of SAPO-34 zeolite catalyst in methanol-to-olefins(MTO) process

Methanol-to-olefins(MTO)is industrially applied to produce ethylene and propylene using methanol converted from coal,synthetic gas,and biomass.SAPO-34 zeolites,as the most efficient catalyst in MTO process,are subject to the rapid deactivation due to coke deposition.Recent work shows that steam regeneration can provide advantages such as low carbon dioxide emission and enhanced light olefins yield in MTO process,compared to that by air regeneration.A kinetic study on the steam regeneration of spent SAPO-34 catalyst has been carried out in this work.In doing so,we first investigated the effect of temperature on the regeneration performance by monitoring the crystal structure,acidity,residual coke properties and other structural parameters.The results show that with the increase of regeneration temperature,the compositions of residual coke on the catalyst change from pyrene and phenanthrene to naphthalene,which are normally considered as active hydrocarbon pool species in MTO reaction.However,when the regeneration temperature is too high,nitrogen oxides can be found in the residual coke.Meanwhile,as the regeneration temperature increases,the quantity of residual coke reduces and the acidity,BET surface area and pore structure of the regenerated samples can be better recovered,resulting in prolonging catalyst lifetime.We have further derived the kinetics of steam regeneration,and obtained an activation energy of about 177.8 kJ·mol^(-1).Compared that with air regeneration,the activation energy of steam regeneration is higher,indicating that the steam regeneration process is more difficult to occur.

Scalable Jet-Based Fabrication of PEI-Hydrogel Particles for CO_(2) Capture

The capture,regeneration,and conversion of CO_(2) from ambient air and flue gas streams are critical aspects of mitigating global warming.Solid sorbents for CO_(2) absorption are very promising as they have high mass transfer areas without energy input and reduce emissions and minimize corrosion as compared to liquid sorbents.However,precisely tunable solid CO_(2) sorbents are difficult to produce.Here,we demonstrate the high-throughput production of hydrogel-based CO_(2)-absorbing particles via liquid jetting.By wrapping a liquid jet consisting of an aqueous solution of cross-linkable branched polyethylenimine(PEI)with a layer of suspension containing hydrophobic silica nanoparticles,monodisperse droplets with a silica nanoparticle coating layer was formed in the air.A stable Pickering emulsion containing PEI droplets was obtained after these ejected droplets were collected in a heated oil bath.The droplets turn into mm-sized particles after thermal curing in the bath.The diameter,PEI content,and silica content of the particles were systematically varied,and their CO_(2) absorption was measured as a function of time.Steam regeneration of the particles enabled cyclic testing,revealing a CO_(2) absorption capacity of 6.5±0.5 mol kg^(−1)solid PEI in pure CO_(2) environments and 0.7±0.3 mol kg^(−1)solid PEI for direct air capture.Several thousands of particles were produced per second at a rate of around 0.5 kg per hour,with a single nozzle.This process can be further scaled by parallelization.The complete toolbox for the design,fabrication,testing,and regeneration of functional hydrogel particles provides a powerful route toward novel solid sorbents for regenerative CO_(2) capture.