In this work,we synthesized LaFeO_3–xwt%Ni(x=0,5,10,15)composites via a solid-state reaction method by adding Ni to the reactants,La_2O_3 and Fe_2O_3.Field-emission scanning electron microscopy(FE-SEM)and energy-disp...In this work,we synthesized LaFeO_3–xwt%Ni(x=0,5,10,15)composites via a solid-state reaction method by adding Ni to the reactants,La_2O_3 and Fe_2O_3.Field-emission scanning electron microscopy(FE-SEM)and energy-dispersive X-ray spectroscopy(EDS)results revealed that Ni powders evenly dispersed among the LaFeO_3 particles and apparently reduced their aggregation,which imparted the composites with a loose structure.Moreover,the Ni formed a conductive network,thus improving the conductivity of the composites.The maximum discharge capacity of the LaFeO_3 electrodes remarkably increased from 266.8 mAh·g^(–1)(x=0)to 339.7 mAh·g^(–1)(x=10).In particular,the high-rate dischargeability of the LaFeO_3–10wt%Ni electrode at a discharge current density of 1500 mA·g^(-1) reached 54.6%,which was approximately 1.5 times higher than that of the pure LaFeO_3.Such a Ni-modified loose structure not only increased the charge transfer rate on the surface of the LaFeO_3 particles but also enhanced the hydrogen diffusion rate in the bulk LaFeO_3.展开更多
CO_(2) is the most cost-eff ective and abundant carbon resource,while the reverse water-gas reaction(rWGS)is one of the most eff ective methods of CO_(2) utilization.This work presents a comparative study of rWGS acti...CO_(2) is the most cost-eff ective and abundant carbon resource,while the reverse water-gas reaction(rWGS)is one of the most eff ective methods of CO_(2) utilization.This work presents a comparative study of rWGS activity for perovskite systems based on AFeO_(3)(where A=Ce,La,Y).These systems were synthesized by solution combustion synthesis(SCS)with diff erent ratios of fuel(glycine)and oxidizer(φ),diff erent amounts of NH 4 NO_(3),and the addition of alumina or silica as supports.Various techniques,including X-ray diff raction analysis,thermogravimetric analysis,Fourier transform infrared spectroscopy(FTIR),scanning electron microscopy,energy-dispersive X-ray spectroscopy,N 2-physisorption,H_(2) temper-ature-programmed reduction,temperature-programmed desorption of H_(2) and CO_(2),Raman spectroscopy,and in situ FTIR,were used to relate the physicochemical properties with the catalytic performance of the obtained composites.Each specifi c perovskite-containing system(either bulk or supported)has its own optimalφand NH_(4) NO_(3) amount to achieve the highest yield and dispersion of the perovskite phase.Among all synthesized systems,bulk SCS-derived La-Fe-O systems showed the highest resistance to reducing environments and the easiest hydrogen desorption,outperforming La-Fe-O produced by solgel combustion(SGC).CO_(2) conversion into CO at 600°C for bulk ferrite systems,depending on the A-cation type and preparation method,follows the order La(SGC)<Y<Ce<La(SCS).The diff erences in properties between La-Fe-O obtained by the SCS and SGC methods can be attributed to diff erent ratios of oxygen and lanthanum vacancy contributions,hydroxyl coverage,morphology,and free iron oxide presence.In situ FTIR data revealed that CO_(2) hydrogenation occurs through formates generated under reaction conditions on the bulk system based on La-Fe-O,obtained by the SCS method.γ-Al_(2)O_(3) improves the dispersion of CeFeO_(3) and LaFeO_(3) phases,the specifi c surface area,and the quantity of adsorbed H_(2) and CO_(2).This led to a signifi cant increase in CO_(2) conversion for supported CeFeO_(3) but not for the La-based system compared to bulk and SiO_(2)-supported perovskite catalysts.However,adding alumina increased the activity per mass for both Ce-and La-based perovskite systems,reducing the amount of rare-earth components in the catalyst and thereby lowering the cost without substantially compromising stability.展开更多
基金financially supported by the National Natural Science Foundation of China(Nos.51771164,51571173,and 51701175)the National Postdoctoral Program for Innovative Talents of China(No.BX201700204)the Innovation Fund for the Graduate Students of Hebei Province(No.CXZZBS2017057)
文摘In this work,we synthesized LaFeO_3–xwt%Ni(x=0,5,10,15)composites via a solid-state reaction method by adding Ni to the reactants,La_2O_3 and Fe_2O_3.Field-emission scanning electron microscopy(FE-SEM)and energy-dispersive X-ray spectroscopy(EDS)results revealed that Ni powders evenly dispersed among the LaFeO_3 particles and apparently reduced their aggregation,which imparted the composites with a loose structure.Moreover,the Ni formed a conductive network,thus improving the conductivity of the composites.The maximum discharge capacity of the LaFeO_3 electrodes remarkably increased from 266.8 mAh·g^(–1)(x=0)to 339.7 mAh·g^(–1)(x=10).In particular,the high-rate dischargeability of the LaFeO_3–10wt%Ni electrode at a discharge current density of 1500 mA·g^(-1) reached 54.6%,which was approximately 1.5 times higher than that of the pure LaFeO_3.Such a Ni-modified loose structure not only increased the charge transfer rate on the surface of the LaFeO_3 particles but also enhanced the hydrogen diffusion rate in the bulk LaFeO_3.
基金The research was carried out within the State Assignment of the Ministry of Science and Higher Education of the Russian Federation(project No.FFUG-2024-0036)。
文摘CO_(2) is the most cost-eff ective and abundant carbon resource,while the reverse water-gas reaction(rWGS)is one of the most eff ective methods of CO_(2) utilization.This work presents a comparative study of rWGS activity for perovskite systems based on AFeO_(3)(where A=Ce,La,Y).These systems were synthesized by solution combustion synthesis(SCS)with diff erent ratios of fuel(glycine)and oxidizer(φ),diff erent amounts of NH 4 NO_(3),and the addition of alumina or silica as supports.Various techniques,including X-ray diff raction analysis,thermogravimetric analysis,Fourier transform infrared spectroscopy(FTIR),scanning electron microscopy,energy-dispersive X-ray spectroscopy,N 2-physisorption,H_(2) temper-ature-programmed reduction,temperature-programmed desorption of H_(2) and CO_(2),Raman spectroscopy,and in situ FTIR,were used to relate the physicochemical properties with the catalytic performance of the obtained composites.Each specifi c perovskite-containing system(either bulk or supported)has its own optimalφand NH_(4) NO_(3) amount to achieve the highest yield and dispersion of the perovskite phase.Among all synthesized systems,bulk SCS-derived La-Fe-O systems showed the highest resistance to reducing environments and the easiest hydrogen desorption,outperforming La-Fe-O produced by solgel combustion(SGC).CO_(2) conversion into CO at 600°C for bulk ferrite systems,depending on the A-cation type and preparation method,follows the order La(SGC)<Y<Ce<La(SCS).The diff erences in properties between La-Fe-O obtained by the SCS and SGC methods can be attributed to diff erent ratios of oxygen and lanthanum vacancy contributions,hydroxyl coverage,morphology,and free iron oxide presence.In situ FTIR data revealed that CO_(2) hydrogenation occurs through formates generated under reaction conditions on the bulk system based on La-Fe-O,obtained by the SCS method.γ-Al_(2)O_(3) improves the dispersion of CeFeO_(3) and LaFeO_(3) phases,the specifi c surface area,and the quantity of adsorbed H_(2) and CO_(2).This led to a signifi cant increase in CO_(2) conversion for supported CeFeO_(3) but not for the La-based system compared to bulk and SiO_(2)-supported perovskite catalysts.However,adding alumina increased the activity per mass for both Ce-and La-based perovskite systems,reducing the amount of rare-earth components in the catalyst and thereby lowering the cost without substantially compromising stability.
文摘用柠檬酸法合成了钙钛矿型复合氧化物 La Fe O3,并按不同比例进行掺杂 ,制备了L a1-x Srx Fe O3( x=0 .0 1、0 .0 2、0 .0 3、0 .0 4、0 .0 5) .以荧光汞灯为光源测定了样品对不同染料的光催化降解活性 ,根据红外、紫外、光声光谱等技术对催化剂的分析结果 ,讨论了光催化性能及掺杂Sr2 +对其活性的影响 ,结果表明 ,掺杂后 L a Fe