Development Of Catalysts Based On Ti₃AlC₂-derived Nanomaterials For High-value Conversion Of Bio-based Furfura

The global dilemma of fossil fuel depletion and environmental degradation fundamentally illustrates the fierce contradiction between traditional energy structure oriented economic growth and eco-environmental protection.Accelerated use of biomass centred renewable resources has become a common consensus and concerted action to tackle the overwhelming challenge of global climate change.In the biomass resource utilization road map,the catalytic escalation of biomass derived platform molecules holds a pivotal position in the synthesis of high value-added chemicals.The presence of aldehyde groups in furfural makes it possible to further synthesize higher value chemicals and polymer monomers,including furfuryl alcohol,Furfurylamine,cyclopentanone,and furfuric acid,among other molecules,by oxidation,hydrogenation,and hydrolysis.Therefore,high-value utilization of biomass derived furfural is critical for future sustainable development.Supported Pt catalysts play an important role in selective hydrogenation for such as valorization of bio-derived platform chemicals.Traditionally Pt catalysts were prepared by such as impregnation and deposition-precipitation,along with chemical reductionby such as NaBH₄ and H₂ under heated conditions.This study developed an in-situreduction method to produce supported Pt NPs on nanofibers,in which the typical MAX phase of Ti₃AlC₂ and chloroplatinic acid were employed as raw materials,using as-produced H₂ as the reductive agent under hydrothermal synthetic conditions.Over these newly developed Pt catalysts,the selective hydrogenation of furfural to furfuryl alcohol has been investigated systematically,and a high conversion of furfural（86.3%）and selectivity of furfuryl alcohol（98.1%）were obtained at 100°C and 1 MPa H₂ in 3h under aqueous media.Moreover,these fiberous catalysts exhibited strong reusability and recyclability in five runs without loss of activity and selectivity.Secondly,glucose was selected as the hydrothermal carbon source to be added into the catalyst generation process under the same synthesis conditions mentioned above.A Pt Glu/Ti₃Al_xC₂T_yseries catalyst with a surface wrapped hydrothermal carbon layer was successfully prepared.In the same furfural hydrogenation reaction process,the reaction activity was slightly reduced compared with that of the Pt/Ti₃Al_xC₂T_y series catalyst without wrapped hydrothermal carbon layer.On the one hand,the wrapping of hydrothermal char layer covered the platinum active sites on the surface of catalysts to some extent,and on the other hand,due to the one pot hydrothermal preparation process,part of platinum particles supported on the hydrothermal char layer without forming electronic interactions with the support,the electron rich platinum active sites were reduced.Finally,synthesis of ZnO/Ti₃Al_xC₂T_y series of catalysts for the oxidation of furfural using zinc acetate as precursor and Ti₃AlC₂ as starting material under hydrothermal synthesis conditions for the preparation of furfural based on the appeal synthesis method.In the presence of alkali,furfural conversion（96.8%）and furoic acid yield（64.7%）were obtained at 100 ℃ and 1 bar O₂ for 1 hour.It still showed strong stability in the cyclic experiment.