A novel Eu^(3+)-doped fluorapatite red phosphor Ca_(2)Y_(8)(BO_(4))_(2)(SiO_(4))_(4)F_(2)Eu^(3+)with pure phase was synthesized in this study.Density functional theory(DFT)calculation and diffuse reflection spectrum a...A novel Eu^(3+)-doped fluorapatite red phosphor Ca_(2)Y_(8)(BO_(4))_(2)(SiO_(4))_(4)F_(2)Eu^(3+)with pure phase was synthesized in this study.Density functional theory(DFT)calculation and diffuse reflection spectrum analysis reveal its potential as a matrix for phosphors excited by ultraviolet light.Eu^(3+)has a^(7)F_(0)→^(5)L_(6)transition at 394 nm,and the prepared phosphor exhibits a high emission intensity at 614 nm,which may be attributed to the^(5)D_(0)-^(7)F_(2)energy transition at the lower symmetry site of Eu^(3+).The optimal doping concentration of the phosphor is determined to be 11 mol%,with concentration quenching attributed to the exchange interaction mechanism.The overall color purity of the phosphor is up to 99.88%,with an internal quantum efficiency as high as 91.15%.Notably,Ca_(2)Y_(8)(BO_(4))_(2)(SiO_(4))_(4)F_(2):11 mol%Eu^(3+)(CYBSF:11 mol%Eu^(3+))phosphors exhibit good thermal stability,with a thermal quenching temperature(T1/2)of 552 K and the intensity of emission at 423 K still at 88.89%of that at 298 K.The activation energy of the phosphor is up to 0.30287 eV.Its comprehensive luminescence performance surpasses that of commercial red phosphor,making it suitable for near ultraviolet excited warm white light emitting diode(NUV-WLED)with a high color rendering index(Ra=82)and a correlated color temperature(CCT)of 4339 K.Moreover,the phosphor achieves latent fingerprint visualization and anti-counterfeiting ink on different material surfaces:glass,aluminum foil,plastic and paper.Overall,the fluorapatite CYBSF:11 mol%Eu^(3+)phosphor holds great potential for multimodal applications due to its high quantum efficiency and good thermal stability.展开更多
Co_(3)V_(2)O_(8)/Co_(3)O_(4)/Ti_(3)C_(2)T_(x) composite was easily synthesized via one-step succinct-operated hydrothermal process.The interconnected Co_(3)V_(2)O_(8)/Co_(3)O_(4) nanowires network can in-situ grow and...Co_(3)V_(2)O_(8)/Co_(3)O_(4)/Ti_(3)C_(2)T_(x) composite was easily synthesized via one-step succinct-operated hydrothermal process.The interconnected Co_(3)V_(2)O_(8)/Co_(3)O_(4) nanowires network can in-situ grow and anchor on the surface of Ti_(3)C_(2)T_(x) via the strong Co-F bonds and contribute tremendously to depress Ti_(3)C_(2)T_(x) self-restacking.Profiting from the synergistically interplayed effect among the multiple interfaces and high conductivity of Ti_(3)C_(2)T_(x) as well as outstanding stability of the as-designed nanostructure,the optimum Co_(3)V_(2)O_(8)/Co_(3)O_(4)/Ti_(3)C_(2)T_(x)electrode reaches a commendable specific capacitance(up to 3800 mF·cm^(−2)),great rate capability(80%capacitance retention after 20-times current increasing),and preeminent cycling stability(95.4%/85.5%retention at 7000th/20,000th cycle).Moreover,the all-solid-state asymmetric supercapacitor based on Co_(3)V_(2)O_(8)/Co_(3)O_(4)/Ti_(3)C_(2)T_(x) and active carbon can deliver a high energy density of 84.0μWh·cm^(−2) at the power energy of 3.2 mW·cm^(−2),and excellent cycling durability with 87.0%of initial capacitance retention upon 20,000 loops.This work provides a practicable pathway to tailor MXene-based composites for high-performance supercapacitor.展开更多
The problem of water and sulfur poisoning in flue gas atmosphere remains a significant obstacle for low-temperature deNO_(x) catalysts.This study investigated the sulfation mechanism of the CoMn_(2)O_(4)/CeTiO_(x)(CMC...The problem of water and sulfur poisoning in flue gas atmosphere remains a significant obstacle for low-temperature deNO_(x) catalysts.This study investigated the sulfation mechanism of the CoMn_(2)O_(4)/CeTiO_(x)(CMCT)catalyst during the selective catalytic reduction of NO_(x) with NH3 under conditions containing H2O and SO_(2) at 150℃.Employing a comprehensive suite of time-resolved analysis and characterization techniques,the evolution of sulfate species was systematically categorized into three stages:initial rapid surface sulfate accumulation,the transformation of surface sulfates to bulk metal sulfates,and partial sulfates decomposition after the removal of H2O and SO_(2).These findings indicate that bulk metal sulfates irreversibly deactivate the catalyst by distorting active component lattices and consuming oxygen vacancies,whereas surface sulfates(including ammonium sulfates and surface-coordinated metal sulfates)cause reversible performance loss through decomposition.Furthermore,the competitive adsorption of H2O and SO_(2) significantly influences the catalytic efficiency,with H2O suppressing SO_(2) adsorption while simultaneously enhancing the formation of Brönsted acid sites.This research underscores the critical role of sulfate dynamics on catalyst performance,revealing the enhanced SO_(2) resistance of the Eley-Rideal mechanism facilitated by the Ce-Ti support relative to the Langmuir-Hinshelwood pathway.Collectively,the study unravels the complex interplay of sulfate dynamics influencing catalyst performance and provides potential approaches to mitigate deactivation in demanding atmospheric conditions.展开更多
Here we report that the presence of MgCO_(3) stimulates the extracellular polymeric substance (EPS) secretion of Microcystis Aeruginosa (M. Aeruginosa). This stimulation led to a significant reduction in the total con...Here we report that the presence of MgCO_(3) stimulates the extracellular polymeric substance (EPS) secretion of Microcystis Aeruginosa (M. Aeruginosa). This stimulation led to a significant reduction in the total concentration of NH_(4)^(+)‒N by more than 86%, and effective recovery of PO_(4)^(3-)‒P within three days from concentrated wastewater (WW), although the secreted EPS inhibited the conversion of MgCO_(3) to specific crystal forms (MgNH4PO4.6H2O or MgHPO4.7H2O). Moreover, with an increase in PO_(4)^(3-) concentration in WW, these crystals appeared, thus the removal of NH_(4)^(+)‒N and PO_(4)^(3-)‒P nutrients can be attributed to the combined effect of M. Aeruginosa and MgCO_(3). We used Surface-Enhanced Raman Spectroscopy (SERS) combined with X-ray Diffraction (XRD), Field Emission Scanning Electron Microscopy with Energy-Dispersive X-ray Spectroscopy (FESEM-EDS), and X-ray Photoelectron Spectroscopy (XPS) to investigate the mechanism for competitive interactions between M. Aeruginosa and MgCO_(3) in removing NH_(4)^(+)‒N and PO_(4)^(3-)‒P. We identified that the bound EPS accumulated amorphous Mg–P–O dense particles on M. Aeruginosa, while soluble EPS, containing –COOH groups of humic-like substances decreased the pH of the solution and coordinated with Mg^(2+) ions. Therefore, both secreted bound and soluble EPS play a vital role in hindering the transformation of Mg^(2+) ions or MgCO_(3) to MgNH4PO4.6H2O or MgHPO4.7H2O crystals within WW, and they enhanced M. Aeruginosa 's ability in absorbing nutrients of NH_(4)^(+)‒N and PO_(4)^(3-)‒P. This mechanism plays a crucial role in the efficient recovery of NH_(4)^(+)‒N and PO_(4)^(3-)‒P from concentrated wastewater sources such as aerobically or anaerobically digested effluent from various sources like agriculture, livestock, and domestic wastewaters.展开更多
Solubilities and properties (density, conductivity and pH value) of solutions in the quaternary system Li +,K +//CO 2- 3,B 4O 2- 7-H 2O at 288 K were experimentally studied with the isothermal equilibrium method. The ...Solubilities and properties (density, conductivity and pH value) of solutions in the quaternary system Li +,K +//CO 2- 3,B 4O 2- 7-H 2O at 288 K were experimentally studied with the isothermal equilibrium method. The phase diagram of the system consisted of two invariant points E and F, five univariant curves, and four crystallization fields that belonged to K 2CO 3·3/2H 2O,Li 2 B 4O 7·3H 2O, K 2 B 4O 7 ·4H 2O and Li 2CO 3. The composition of the solution corresponding to E was w(CO 2- 3)=2.27 %, w(B 4O 2- 7) =6.05 %, w(K + ) =4.30%,w(Li + )=0.30 % and the equilibrium solids were Li 2 B 4O 7· 3H 2O+K 2 B 4O 7·4H 2O+Li 2CO 3;The composition of the solution for F was w(CO 2- 3) =22.45%,w(B 4O 2- 7)=1.88%,w(K + )=29.96%,w(Li + )=0.03% and the equilibrium solids were K 2CO 3·3/2H 2O+ K 2 B 4O 7·4H 2O+Li 2CO 3. K 2CO 3 possesses strong salting-out effect on K 2 B 4O 7,Li 2CO 3 and Li 2 B 4O 7.展开更多
A more feasibly convergent synthesis of selective estrogen receptor degrading agent(S)-8-(4-((1-(3-fluoropropyl)-pyrrolidin-3-yl)oxy)phenyl)-7-(4-hydroxyphenyl)-5,6-dihydronaphthalen-2-ol was reported,featured with co...A more feasibly convergent synthesis of selective estrogen receptor degrading agent(S)-8-(4-((1-(3-fluoropropyl)-pyrrolidin-3-yl)oxy)phenyl)-7-(4-hydroxyphenyl)-5,6-dihydronaphthalen-2-ol was reported,featured with concise work up and absence of regioselectivity dilemma.展开更多
基金supported by the National Natural Science Foundation of China(52372013)Natural Science Foundation of Shanghai(22ZR1460600)。
文摘A novel Eu^(3+)-doped fluorapatite red phosphor Ca_(2)Y_(8)(BO_(4))_(2)(SiO_(4))_(4)F_(2)Eu^(3+)with pure phase was synthesized in this study.Density functional theory(DFT)calculation and diffuse reflection spectrum analysis reveal its potential as a matrix for phosphors excited by ultraviolet light.Eu^(3+)has a^(7)F_(0)→^(5)L_(6)transition at 394 nm,and the prepared phosphor exhibits a high emission intensity at 614 nm,which may be attributed to the^(5)D_(0)-^(7)F_(2)energy transition at the lower symmetry site of Eu^(3+).The optimal doping concentration of the phosphor is determined to be 11 mol%,with concentration quenching attributed to the exchange interaction mechanism.The overall color purity of the phosphor is up to 99.88%,with an internal quantum efficiency as high as 91.15%.Notably,Ca_(2)Y_(8)(BO_(4))_(2)(SiO_(4))_(4)F_(2):11 mol%Eu^(3+)(CYBSF:11 mol%Eu^(3+))phosphors exhibit good thermal stability,with a thermal quenching temperature(T1/2)of 552 K and the intensity of emission at 423 K still at 88.89%of that at 298 K.The activation energy of the phosphor is up to 0.30287 eV.Its comprehensive luminescence performance surpasses that of commercial red phosphor,making it suitable for near ultraviolet excited warm white light emitting diode(NUV-WLED)with a high color rendering index(Ra=82)and a correlated color temperature(CCT)of 4339 K.Moreover,the phosphor achieves latent fingerprint visualization and anti-counterfeiting ink on different material surfaces:glass,aluminum foil,plastic and paper.Overall,the fluorapatite CYBSF:11 mol%Eu^(3+)phosphor holds great potential for multimodal applications due to its high quantum efficiency and good thermal stability.
基金This study was financially supported by the National Science Foundation of China(No.52201254)the National Science Foundation of Shandong Province(Nos.ZR2020MB090 and ZR2020QE012)+1 种基金the Project of“20 Items of University”of Jinan(No.202228046)Taishan Scholar Project of Shandong Province.
文摘Co_(3)V_(2)O_(8)/Co_(3)O_(4)/Ti_(3)C_(2)T_(x) composite was easily synthesized via one-step succinct-operated hydrothermal process.The interconnected Co_(3)V_(2)O_(8)/Co_(3)O_(4) nanowires network can in-situ grow and anchor on the surface of Ti_(3)C_(2)T_(x) via the strong Co-F bonds and contribute tremendously to depress Ti_(3)C_(2)T_(x) self-restacking.Profiting from the synergistically interplayed effect among the multiple interfaces and high conductivity of Ti_(3)C_(2)T_(x) as well as outstanding stability of the as-designed nanostructure,the optimum Co_(3)V_(2)O_(8)/Co_(3)O_(4)/Ti_(3)C_(2)T_(x)electrode reaches a commendable specific capacitance(up to 3800 mF·cm^(−2)),great rate capability(80%capacitance retention after 20-times current increasing),and preeminent cycling stability(95.4%/85.5%retention at 7000th/20,000th cycle).Moreover,the all-solid-state asymmetric supercapacitor based on Co_(3)V_(2)O_(8)/Co_(3)O_(4)/Ti_(3)C_(2)T_(x) and active carbon can deliver a high energy density of 84.0μWh·cm^(−2) at the power energy of 3.2 mW·cm^(−2),and excellent cycling durability with 87.0%of initial capacitance retention upon 20,000 loops.This work provides a practicable pathway to tailor MXene-based composites for high-performance supercapacitor.
文摘The problem of water and sulfur poisoning in flue gas atmosphere remains a significant obstacle for low-temperature deNO_(x) catalysts.This study investigated the sulfation mechanism of the CoMn_(2)O_(4)/CeTiO_(x)(CMCT)catalyst during the selective catalytic reduction of NO_(x) with NH3 under conditions containing H2O and SO_(2) at 150℃.Employing a comprehensive suite of time-resolved analysis and characterization techniques,the evolution of sulfate species was systematically categorized into three stages:initial rapid surface sulfate accumulation,the transformation of surface sulfates to bulk metal sulfates,and partial sulfates decomposition after the removal of H2O and SO_(2).These findings indicate that bulk metal sulfates irreversibly deactivate the catalyst by distorting active component lattices and consuming oxygen vacancies,whereas surface sulfates(including ammonium sulfates and surface-coordinated metal sulfates)cause reversible performance loss through decomposition.Furthermore,the competitive adsorption of H2O and SO_(2) significantly influences the catalytic efficiency,with H2O suppressing SO_(2) adsorption while simultaneously enhancing the formation of Brönsted acid sites.This research underscores the critical role of sulfate dynamics on catalyst performance,revealing the enhanced SO_(2) resistance of the Eley-Rideal mechanism facilitated by the Ce-Ti support relative to the Langmuir-Hinshelwood pathway.Collectively,the study unravels the complex interplay of sulfate dynamics influencing catalyst performance and provides potential approaches to mitigate deactivation in demanding atmospheric conditions.
基金supported by Cultivating Fund Project of Hubei Hongshan Laboratory(2022hspy002).
文摘Here we report that the presence of MgCO_(3) stimulates the extracellular polymeric substance (EPS) secretion of Microcystis Aeruginosa (M. Aeruginosa). This stimulation led to a significant reduction in the total concentration of NH_(4)^(+)‒N by more than 86%, and effective recovery of PO_(4)^(3-)‒P within three days from concentrated wastewater (WW), although the secreted EPS inhibited the conversion of MgCO_(3) to specific crystal forms (MgNH4PO4.6H2O or MgHPO4.7H2O). Moreover, with an increase in PO_(4)^(3-) concentration in WW, these crystals appeared, thus the removal of NH_(4)^(+)‒N and PO_(4)^(3-)‒P nutrients can be attributed to the combined effect of M. Aeruginosa and MgCO_(3). We used Surface-Enhanced Raman Spectroscopy (SERS) combined with X-ray Diffraction (XRD), Field Emission Scanning Electron Microscopy with Energy-Dispersive X-ray Spectroscopy (FESEM-EDS), and X-ray Photoelectron Spectroscopy (XPS) to investigate the mechanism for competitive interactions between M. Aeruginosa and MgCO_(3) in removing NH_(4)^(+)‒N and PO_(4)^(3-)‒P. We identified that the bound EPS accumulated amorphous Mg–P–O dense particles on M. Aeruginosa, while soluble EPS, containing –COOH groups of humic-like substances decreased the pH of the solution and coordinated with Mg^(2+) ions. Therefore, both secreted bound and soluble EPS play a vital role in hindering the transformation of Mg^(2+) ions or MgCO_(3) to MgNH4PO4.6H2O or MgHPO4.7H2O crystals within WW, and they enhanced M. Aeruginosa 's ability in absorbing nutrients of NH_(4)^(+)‒N and PO_(4)^(3-)‒P. This mechanism plays a crucial role in the efficient recovery of NH_(4)^(+)‒N and PO_(4)^(3-)‒P from concentrated wastewater sources such as aerobically or anaerobically digested effluent from various sources like agriculture, livestock, and domestic wastewaters.
文摘Solubilities and properties (density, conductivity and pH value) of solutions in the quaternary system Li +,K +//CO 2- 3,B 4O 2- 7-H 2O at 288 K were experimentally studied with the isothermal equilibrium method. The phase diagram of the system consisted of two invariant points E and F, five univariant curves, and four crystallization fields that belonged to K 2CO 3·3/2H 2O,Li 2 B 4O 7·3H 2O, K 2 B 4O 7 ·4H 2O and Li 2CO 3. The composition of the solution corresponding to E was w(CO 2- 3)=2.27 %, w(B 4O 2- 7) =6.05 %, w(K + ) =4.30%,w(Li + )=0.30 % and the equilibrium solids were Li 2 B 4O 7· 3H 2O+K 2 B 4O 7·4H 2O+Li 2CO 3;The composition of the solution for F was w(CO 2- 3) =22.45%,w(B 4O 2- 7)=1.88%,w(K + )=29.96%,w(Li + )=0.03% and the equilibrium solids were K 2CO 3·3/2H 2O+ K 2 B 4O 7·4H 2O+Li 2CO 3. K 2CO 3 possesses strong salting-out effect on K 2 B 4O 7,Li 2CO 3 and Li 2 B 4O 7.
文摘A more feasibly convergent synthesis of selective estrogen receptor degrading agent(S)-8-(4-((1-(3-fluoropropyl)-pyrrolidin-3-yl)oxy)phenyl)-7-(4-hydroxyphenyl)-5,6-dihydronaphthalen-2-ol was reported,featured with concise work up and absence of regioselectivity dilemma.
