The fabrication of monolithic ZSM-5 catalysts via extrusion is pivotal for industrial catalytic processes;nevertheless,the addition of adhesives might affect their catalytic performance.Herein,the rice husk-derived bi...The fabrication of monolithic ZSM-5 catalysts via extrusion is pivotal for industrial catalytic processes;nevertheless,the addition of adhesives might affect their catalytic performance.Herein,the rice husk-derived bio-SiO_(2),serving as a silicon source and natural adhesive,was introduced in the synthesis and extrusion of ZSM-5 catalysts denoted as BioZSM-5,thereby enhancing their industrial viability and catalytic performance.The f-n-BioZSM-5(obtained by extrusion of n-BioZSM-5)showcased enhanced butene and pentene selectivity,exhibiting robust stability,achieving an impressive 84.8%olefin selectivity(over 10 cycles).The biomass template significantly improved porosity,acidity,and anti-coking properties.Moreover,the f-n-BioZSM-5 exhibited a compressive strength 4.3 times superior to that of f-n-ZSM-5 without using bio-template,achieving better abrasion resistance and enhanced mechanical properties even using 1/3 of the adhesive dosage.These results will provide valuable guidance for developing shaped zeolite catalysts for industrial catalytic pyrolysis applications,especially for the production of olefin from fatty acids.展开更多
Artificial photosynthesis is an ideal method for solar-to-chemical energy conversion,wherein solar energy is stored in the form of chemical bonds of solar fuels.In particular,the photocatalytic reduction of CO_(2)has ...Artificial photosynthesis is an ideal method for solar-to-chemical energy conversion,wherein solar energy is stored in the form of chemical bonds of solar fuels.In particular,the photocatalytic reduction of CO_(2)has attracted considerable attention due to its dual benefits of fossil fuel production and CO_(2)pollution reduction.However,CO_(2)is a comparatively stable molecule and its photoreduction is thermodynamically and kinetically challenging.Thus,the photocatalytic efficiency of CO_(2)reduction is far below the level of industrial applications.Therefore,development of low-cost cocatalysts is crucial for significantly decreasing the activation energy of CO_(2)to achieving efficient photocatalytic CO_(2)reduction.Herein,we have reported the use of a Ni_(2)P material that can serve as a robust cocatalyst by cooperating with a photosensitizer for the photoconversion of CO_(2).An effective strategy for engineering Ni_(2)P in an ultrathin layered structure has been proposed to improve the CO_(2)adsorption capability and decrease the CO_(2)activation energy,resulting in efficient CO_(2)reduction.A series of physicochemical characterizations including X-ray diffraction(XRD),X-ray photoelectron spectroscopy(XPS),transmission electron microscopy(TEM),high-resolution transmission electron microscopy(HRTEM),and atomic force microscopy(AFM)were used to demonstrate the successful preparation of ultrathin Ni_(2)P nanosheets.The XRD and XPS results confirm the successful synthesis of Ni_(2)P from Ni(OH)2 by a low temperature phosphidation process.According to the TEM images,the prepared Ni_(2)P nanosheets exhibit a 2D and near-transparent sheet-like structure,suggesting their ultrathin thickness.The AFM images further demonstrated this result and also showed that the height of the Ni_(2)P nanosheets is ca 1.5 nm.The photoluminescence(PL)spectroscopy results revealed that the Ni_(2)P material could efficiently promote the separation of the photogenerated electrons and holes in[Ru(bpy)3]Cl2?6H2O.More importantly,the Ni_(2)P nanosheets could more efficiently promote the charge transfer and charge separation rate of[Ru(bpy)3]Cl2?6H2O compared with the Ni_(2)P particles.In addition,the electrochemical experiments revealed that the Ni_(2)P nanosheets,with their high active surface area and charge conductivity,can provide more active centers for CO_(2)conversion and accelerate the interfacial reaction dynamics.These results strongly suggest that the Ni_(2)P nanosheets are a promising material for photocatalytic CO_(2)reduction,and can achieve a CO generation rate of 64.8μmol·h^(-1),which is 4.4 times higher than that of the Ni_(2)P particles.In addition,the XRD and XPS measurements of the used Ni_(2)P nanosheets after the six cycles of the photocatalytic CO_(2)reduction reaction demonstrated their high stability.Overall,this study offers a new function for the 2D transition-metal phosphide catalysts in photocatalytic CO_(2)reduction.展开更多
基金financially supported by the National Natural Science Foundation of China(U21A20324,22278167,22350410389 and 22322806)the Fujian Provincial Natural Science Foundation of China(2024J01100)。
文摘The fabrication of monolithic ZSM-5 catalysts via extrusion is pivotal for industrial catalytic processes;nevertheless,the addition of adhesives might affect their catalytic performance.Herein,the rice husk-derived bio-SiO_(2),serving as a silicon source and natural adhesive,was introduced in the synthesis and extrusion of ZSM-5 catalysts denoted as BioZSM-5,thereby enhancing their industrial viability and catalytic performance.The f-n-BioZSM-5(obtained by extrusion of n-BioZSM-5)showcased enhanced butene and pentene selectivity,exhibiting robust stability,achieving an impressive 84.8%olefin selectivity(over 10 cycles).The biomass template significantly improved porosity,acidity,and anti-coking properties.Moreover,the f-n-BioZSM-5 exhibited a compressive strength 4.3 times superior to that of f-n-ZSM-5 without using bio-template,achieving better abrasion resistance and enhanced mechanical properties even using 1/3 of the adhesive dosage.These results will provide valuable guidance for developing shaped zeolite catalysts for industrial catalytic pyrolysis applications,especially for the production of olefin from fatty acids.
文摘Artificial photosynthesis is an ideal method for solar-to-chemical energy conversion,wherein solar energy is stored in the form of chemical bonds of solar fuels.In particular,the photocatalytic reduction of CO_(2)has attracted considerable attention due to its dual benefits of fossil fuel production and CO_(2)pollution reduction.However,CO_(2)is a comparatively stable molecule and its photoreduction is thermodynamically and kinetically challenging.Thus,the photocatalytic efficiency of CO_(2)reduction is far below the level of industrial applications.Therefore,development of low-cost cocatalysts is crucial for significantly decreasing the activation energy of CO_(2)to achieving efficient photocatalytic CO_(2)reduction.Herein,we have reported the use of a Ni_(2)P material that can serve as a robust cocatalyst by cooperating with a photosensitizer for the photoconversion of CO_(2).An effective strategy for engineering Ni_(2)P in an ultrathin layered structure has been proposed to improve the CO_(2)adsorption capability and decrease the CO_(2)activation energy,resulting in efficient CO_(2)reduction.A series of physicochemical characterizations including X-ray diffraction(XRD),X-ray photoelectron spectroscopy(XPS),transmission electron microscopy(TEM),high-resolution transmission electron microscopy(HRTEM),and atomic force microscopy(AFM)were used to demonstrate the successful preparation of ultrathin Ni_(2)P nanosheets.The XRD and XPS results confirm the successful synthesis of Ni_(2)P from Ni(OH)2 by a low temperature phosphidation process.According to the TEM images,the prepared Ni_(2)P nanosheets exhibit a 2D and near-transparent sheet-like structure,suggesting their ultrathin thickness.The AFM images further demonstrated this result and also showed that the height of the Ni_(2)P nanosheets is ca 1.5 nm.The photoluminescence(PL)spectroscopy results revealed that the Ni_(2)P material could efficiently promote the separation of the photogenerated electrons and holes in[Ru(bpy)3]Cl2?6H2O.More importantly,the Ni_(2)P nanosheets could more efficiently promote the charge transfer and charge separation rate of[Ru(bpy)3]Cl2?6H2O compared with the Ni_(2)P particles.In addition,the electrochemical experiments revealed that the Ni_(2)P nanosheets,with their high active surface area and charge conductivity,can provide more active centers for CO_(2)conversion and accelerate the interfacial reaction dynamics.These results strongly suggest that the Ni_(2)P nanosheets are a promising material for photocatalytic CO_(2)reduction,and can achieve a CO generation rate of 64.8μmol·h^(-1),which is 4.4 times higher than that of the Ni_(2)P particles.In addition,the XRD and XPS measurements of the used Ni_(2)P nanosheets after the six cycles of the photocatalytic CO_(2)reduction reaction demonstrated their high stability.Overall,this study offers a new function for the 2D transition-metal phosphide catalysts in photocatalytic CO_(2)reduction.
