La_(0.8)A_(0.2)NiO_(3) (A=K,Ba,Y) catalysts supported on the microwave-absorbing ceramic heating carrier were prepared by the sol-gel method.The crystalline phase and the catalytic activity of the La_(0.8)A_(0.2)NiO_(...La_(0.8)A_(0.2)NiO_(3) (A=K,Ba,Y) catalysts supported on the microwave-absorbing ceramic heating carrier were prepared by the sol-gel method.The crystalline phase and the catalytic activity of the La_(0.8)A_(0.2)NiO_(3)catalysts were characterized by XRD and H_(2) temperature-programmed reduction (TPR).The effects of reaction temperature,oxygen concentration,and gas flow rate on the direct decomposition of nitric oxide over the synthesized catalysts were studied under microwave irradiation (2.45 GHz).The XRD results indicated that the La_(0.8)A_(0.2)NiO_(3) catalysts formed an ABO_(3) perovskite structure,and the H_(2)-TPR results revealed that the relative reducibility of the catalysts increased in the order of La_(0.8)K_(0.2)NiO_(3)>La_(0.8)Ba_(0.2)NiO_(3)>La_(0.8)Y_(0.2)Ni O_(3).Under microwave irradiation,the highest NO conversion amounted to 98.9%,which was obtained with the La_(0.8)K_(0.2)NiO_(3) catalyst at 400℃.The oxygen concentration did not inhibit the NO decomposition on the La_(0.8)A_(0.2)NiO_(3) catalysts,thus the N_(2) selectivity exceeded 99.8%under excess oxygen at 550℃.The NOconversion of the La_(0.8)A_(0.2)NiO_(3) catalysts decreased linearly with the increase in the gas flow rate.展开更多
Plastic waste management has emerged as a critical environmental issue due to the exponential increase in plastic consumption worldwide.Polyethylene terephthalate(PET)is extensively used in the production of water bot...Plastic waste management has emerged as a critical environmental issue due to the exponential increase in plastic consumption worldwide.Polyethylene terephthalate(PET)is extensively used in the production of water bottles,which constitutes a significant fraction of the plastic waste.PET recycling is a challenging task due to the lack of efficient and cost-effective depolymerization methods.In this study,we developed a microwave(MW)catalytic depolymerization method for PET recycling using modified zinc oxide loaded with manganese oxide as a cocatalyst.The modified Mn_(3)O_(4)/ZnO catalyst presents high efficiency in depolymerizing PET into its monomers with only 0.4 wt% ratio of the catalyst to PET at 175℃ for 5 min,resulting in 100% conversion of PET and 88% selectivity toward bis-hydroxyethyl terephthalate monomers.It is believed that Mn_(3)O_(4)provides additional Lewis acid sites,promoting the dissociation of glycol from PET,and the MW irradiation plays a crucial role in rapidly heating the ethylene glycol and the catalyst,thereby accelerating the PET depolymerization process.In addition,the heterogeneous nature of the catalyst facilitates its easy separation from the reaction mixture for reuse,simplifying the catalyst recovery process and enabling costeffective and sustainable PET recycling.Thus,this study provides an innovative and sustainable solution for PET recycling,contributing toward the circular economy and mitigating the environmental impact of plastic waste.展开更多
文摘La_(0.8)A_(0.2)NiO_(3) (A=K,Ba,Y) catalysts supported on the microwave-absorbing ceramic heating carrier were prepared by the sol-gel method.The crystalline phase and the catalytic activity of the La_(0.8)A_(0.2)NiO_(3)catalysts were characterized by XRD and H_(2) temperature-programmed reduction (TPR).The effects of reaction temperature,oxygen concentration,and gas flow rate on the direct decomposition of nitric oxide over the synthesized catalysts were studied under microwave irradiation (2.45 GHz).The XRD results indicated that the La_(0.8)A_(0.2)NiO_(3) catalysts formed an ABO_(3) perovskite structure,and the H_(2)-TPR results revealed that the relative reducibility of the catalysts increased in the order of La_(0.8)K_(0.2)NiO_(3)>La_(0.8)Ba_(0.2)NiO_(3)>La_(0.8)Y_(0.2)Ni O_(3).Under microwave irradiation,the highest NO conversion amounted to 98.9%,which was obtained with the La_(0.8)K_(0.2)NiO_(3) catalyst at 400℃.The oxygen concentration did not inhibit the NO decomposition on the La_(0.8)A_(0.2)NiO_(3) catalysts,thus the N_(2) selectivity exceeded 99.8%under excess oxygen at 550℃.The NOconversion of the La_(0.8)A_(0.2)NiO_(3) catalysts decreased linearly with the increase in the gas flow rate.
基金UK EPSRC project(EP/S018204/2)Royal Society Leverhulme Trust Senior Research Fellowship(SRF\R1\21000153).
文摘Plastic waste management has emerged as a critical environmental issue due to the exponential increase in plastic consumption worldwide.Polyethylene terephthalate(PET)is extensively used in the production of water bottles,which constitutes a significant fraction of the plastic waste.PET recycling is a challenging task due to the lack of efficient and cost-effective depolymerization methods.In this study,we developed a microwave(MW)catalytic depolymerization method for PET recycling using modified zinc oxide loaded with manganese oxide as a cocatalyst.The modified Mn_(3)O_(4)/ZnO catalyst presents high efficiency in depolymerizing PET into its monomers with only 0.4 wt% ratio of the catalyst to PET at 175℃ for 5 min,resulting in 100% conversion of PET and 88% selectivity toward bis-hydroxyethyl terephthalate monomers.It is believed that Mn_(3)O_(4)provides additional Lewis acid sites,promoting the dissociation of glycol from PET,and the MW irradiation plays a crucial role in rapidly heating the ethylene glycol and the catalyst,thereby accelerating the PET depolymerization process.In addition,the heterogeneous nature of the catalyst facilitates its easy separation from the reaction mixture for reuse,simplifying the catalyst recovery process and enabling costeffective and sustainable PET recycling.Thus,this study provides an innovative and sustainable solution for PET recycling,contributing toward the circular economy and mitigating the environmental impact of plastic waste.