Sodium with low cost and high abundance is considered as a substitute element of lithium for batteries and supercapacitors,which need the appropriate host materials to accommodate the relatively large Na^(+) ions.Comp...Sodium with low cost and high abundance is considered as a substitute element of lithium for batteries and supercapacitors,which need the appropriate host materials to accommodate the relatively large Na^(+) ions.Compared to Li^(+) storage,Na^(+) storage makes higher demands on the structural optimization of perovskite bismuth ferrite(BiFeO_(3)).We propose a novel strategy of defect engineering on BiFeO_(3) through Na and V codoping for high-efficiency Na^(+) storage,to reveal the roles of oxygen vacancies and V ions played in the enhanced electrochemical energy storage performances of Na-ion capacitors.The formation of the oxygen vacancies in the Na and V codoped BiFeO_(3)(denoted as NV-BFO),is promoted by Na doping and suppressed by V doping,which can be demonstrated by XPS and EPR spectra.By the first-principles calculations,the oxygen vacancies and V ions in NV-BFO are confirmed to substantially lower the Na^(+)migration energy barriers through the space and electric field effects,to effectively promote the Na^(+) transport in the crystals.Electrochemical kinetic analysis of the NV-BFO//NV-BFO capacitors indicates the dominant capacitive-controlled capacity,which depends on fast Na^(+) deintercalation-intercalation process in the NV-BFO electrode.The NV-BFO//NV-BFO capacitors open up a new avenue for developing highperformance Na-ion capacitors.展开更多
The activation of H_(2)O is a key step of the COS hydrolysis,which may be tuned by oxygen vacancy defects in the catalysts.Herein,we have introduced Cu into Co_(3)O_(4) to regulate the oxygen vacancy defect content of...The activation of H_(2)O is a key step of the COS hydrolysis,which may be tuned by oxygen vacancy defects in the catalysts.Herein,we have introduced Cu into Co_(3)O_(4) to regulate the oxygen vacancy defect content of the catalysts.In situ DRIFTS and XPS spectra reveal that COS and H_(2)O are adsorbed and activated by oxygen vacancy.The 10 at%Cu doped Co_(3)O_(4) sample(10Cu-Co_(3)O_(4))exhibits the optimal activity,100%of COS conversion at 70℃.The improved oxygen vacancies of CueCo_(3)O_(4) accelerate the activation of H_(2)O to form active -OH.COS binds with hydroxyl to form the intermediate HSCO^(-)_(2),and then the activated-OH on the oxygen vacancy reacts with HSCO^(-)_(2) to form HCO^(-)_(3).Meanwhile,the catalyst exhibits high catalytic stability because copper species(Cu+/Cu^(2+))redox cycle mitigate the sulfation of Co_(3)O_(4)(Co^(2+)/Co^(3+)).Our work offers a promising approach for the rational design of cobalt-related catalysts in the highly efficient hydrolysis COS process.展开更多
A ratiometric fluorescent probe for hypoxanthine(Hx)detection was established based on the mimic enzyme and fluorescence characteristics of cobalt-doped graphite-phase carbon nitride(Co doped g-C_(3)N_(4)).In addition...A ratiometric fluorescent probe for hypoxanthine(Hx)detection was established based on the mimic enzyme and fluorescence characteristics of cobalt-doped graphite-phase carbon nitride(Co doped g-C_(3)N_(4)).In addition to emitting strong fluorescence,the peroxidase activity of Co doped g-C_(3)N_(4)can catalyze the reaction of O-phenylenediamine and H_(2)O_(2)to produce diallyl phthalate which can emit yellow fluorescence at 570 nm.Through the decomposition of Hx by xanthine oxidase,Hx can be indirectly detected by the generating hydrogen peroxide based on the measurement of fluorescent ratio I(F_(570)/F_(370)).The linear range was 1.7-272.2 mg/kg(R^(2)=0.997),and the detection limit was 1.52 mg/kg(3σ/K,n=9).The established method was applied to Hx detection in bass,grass carp,and shrimp,and the data were verified by HPLC.The result shows that the established probe is sensitive,accurate,and reliable,and can be used for Hx detection in aquatic products.展开更多
Potassium-ion batteries(PIBs)offer a cost-effective and resource-abundant solution for large-scale energy storage.However,the progress of PIBs is impeded by the lack of high-capacity,long-life,and fast-kinetics anode ...Potassium-ion batteries(PIBs)offer a cost-effective and resource-abundant solution for large-scale energy storage.However,the progress of PIBs is impeded by the lack of high-capacity,long-life,and fast-kinetics anode electrode materials.Here,we propose a dual synergic optimization strategy to enhance the K^(+)storage stability and reaction kinetics of Bi_(2)S_(3) through two-dimensional compositing and cation doping.Externally,Bi_(2)S_(3) nanoparticles are loaded onto the surface of three-dimensional interconnected Ti_(3)C_(2)T_(x) nanosheets to stabilize the electrode structure.Internally,Cu^(2+)doping acts as active sites to accelerate K^(+)storage kinetics.Various theoretical simulations and ex situ techniques are used to elucidate the external–internal dual synergism.During discharge,Ti_(3)C_(2)T_(x) and Cu^(2+)collaboratively facilitate K+intercalation.Subsequently,Cu^(2+)doping primarily promotes the fracture of Bi2S3 bonds,facilitating a conversion reaction.Throughout cycling,the Ti_(3)C_(2)T_(x) composite structure and Cu^(2+)doping sustain functionality.The resulting Cu^(2+)-doped Bi2S3 anchored on Ti_(3)C_(2)T_(x)(C-BT)shows excellent rate capability(600 mAh g^(-1) at 0.1 A g^(–1);105 mAh g^(-1) at 5.0 A g^(-1))and cycling performance(91 mAh g^(-1) at 5.0 A g^(-1) after 1000 cycles)in half cells and a high energy density(179 Wh kg–1)in full cells.展开更多
Sn doping is an effective way to improve the response rate of Ga_(2)O_(3) film based solar-blind detectors. In this paper,Sn-doped Ga_(2)O_(3) films were prepared on a sapphire substrate by radio frequency magnetron s...Sn doping is an effective way to improve the response rate of Ga_(2)O_(3) film based solar-blind detectors. In this paper,Sn-doped Ga_(2)O_(3) films were prepared on a sapphire substrate by radio frequency magnetron sputtering. The films were characterized by X-ray diffraction, scanning electron microscopy, X-ray photoelectron spectroscopy and ultraviolet visible spectroscopy, and the effect of annealing atmosphere on the properties of films was studied. The Ga_(2)O_(3) films changed from amorphous to β-Ga_(2)O_(3) after annealing at 900 °C. The films were composed of micro crystalline particles with a diameter of about 5–20 nm.The β-Ga_(2)O_(3) had high transmittance for wavelengths above 300 nm, and obvious absorption for solar-blind signals at 200–280 nm.The metal semiconductor metal type solar-blind detectors were prepared. The detector based on Sn-doped β-Ga_(2)O_(3) thin film annealed in N_2 has the best response performance to 254 nm light. The photo-current is 10 μA at 20 V, the dark-current is 5.76 pA,the photo dark current ratio is 1.7 × 10~6, the response rate is 12.47 A/W, the external quantum efficiency is 6.09 × 10~3%, the specific detection rate is 2.61 × 10~(12) Jones, the response time and recovery time are 378 and 90 ms, respectively.展开更多
Pr3＋ doped ZnO quantum dots （QDs） were successfully synthesized by sol-gel process. X-ray diffraction （XRD） and X-ray Phtoelectron spectroscopy （XPS） were used to analyze the microstructure variation of ZnO QDs...Pr3＋ doped ZnO quantum dots （QDs） were successfully synthesized by sol-gel process. X-ray diffraction （XRD） and X-ray Phtoelectron spectroscopy （XPS） were used to analyze the microstructure variation of ZnO QDs and the chemical environment of Pr3＋ with increasing Pr3＋ doping concentrations. Most of Pr3＋ ions distribute on the surface ofZnO QDs while a few of them penetrate into the ZnO lattice to substitute Zn2＋ which causes the lattice distortion and the change of the crystal size. With increasing concentration of Pr3＋ ions, the crystal size of ZnO QDs firstly increases and then decreases meanwhile the amorphization gradually increases. New Pr-O-Zn bonds formed after Pr3＋ doping and Pr3＋ ions have at least two chemical bonding environments： one is Pr-O-Zn bond and the other is Pr-O bond surrounded by oxygen vacancies.展开更多
A series of Zr-doped CaTiO3 powders were prepared with the mild co-precipitation method and calcined at 850℃ for 3 h. The as-prepared Zr-doped CaTiO3 samples were characterized by scanning electron microscopy （SEM）...A series of Zr-doped CaTiO3 powders were prepared with the mild co-precipitation method and calcined at 850℃ for 3 h. The as-prepared Zr-doped CaTiO3 samples were characterized by scanning electron microscopy （SEM）, X-ray diffraction （XRD）, UV-Vis diffuse reflectance spectra （DRS） and X-ray photoelectron spectra （XPS）. XRD result revealed the presence of single perovskite phase of CaTiO3. UV-Vis diffusive reflection spectra of Zr-doped CaTiO3 indicated that the absorbance obviously increased in the visible light irradiation. XPS analysis showed that two types of oxygen existed on the photocatalyst surface, including lattice oxygen and absorbed oxygen. Their photocatalytic activity in the case of the degradation of methyl orange in water and photoelectrochemical activity were also tested. The 5%Zr-doped （mole fraction） CaTiO3 sample showed the highest photocatalytic activity. The enhanced photocatalytic activity was ascribed to the change of the lattice structure, existence of oxygen vacancies and increase of the photogenerated charge separation efficiency.展开更多
基金financial supports from National Natural Science Foundation of China(22005174 and 52271133)。
文摘Sodium with low cost and high abundance is considered as a substitute element of lithium for batteries and supercapacitors,which need the appropriate host materials to accommodate the relatively large Na^(+) ions.Compared to Li^(+) storage,Na^(+) storage makes higher demands on the structural optimization of perovskite bismuth ferrite(BiFeO_(3)).We propose a novel strategy of defect engineering on BiFeO_(3) through Na and V codoping for high-efficiency Na^(+) storage,to reveal the roles of oxygen vacancies and V ions played in the enhanced electrochemical energy storage performances of Na-ion capacitors.The formation of the oxygen vacancies in the Na and V codoped BiFeO_(3)(denoted as NV-BFO),is promoted by Na doping and suppressed by V doping,which can be demonstrated by XPS and EPR spectra.By the first-principles calculations,the oxygen vacancies and V ions in NV-BFO are confirmed to substantially lower the Na^(+)migration energy barriers through the space and electric field effects,to effectively promote the Na^(+) transport in the crystals.Electrochemical kinetic analysis of the NV-BFO//NV-BFO capacitors indicates the dominant capacitive-controlled capacity,which depends on fast Na^(+) deintercalation-intercalation process in the NV-BFO electrode.The NV-BFO//NV-BFO capacitors open up a new avenue for developing highperformance Na-ion capacitors.
基金the National Natural Science Foundation of China (92034301,22078063 and 22022804)Major Program of Qingyuan Innovation Laboratory (00121003)the Natural Science Foundation of Fujian Province (2020H6007)。
文摘The activation of H_(2)O is a key step of the COS hydrolysis,which may be tuned by oxygen vacancy defects in the catalysts.Herein,we have introduced Cu into Co_(3)O_(4) to regulate the oxygen vacancy defect content of the catalysts.In situ DRIFTS and XPS spectra reveal that COS and H_(2)O are adsorbed and activated by oxygen vacancy.The 10 at%Cu doped Co_(3)O_(4) sample(10Cu-Co_(3)O_(4))exhibits the optimal activity,100%of COS conversion at 70℃.The improved oxygen vacancies of CueCo_(3)O_(4) accelerate the activation of H_(2)O to form active -OH.COS binds with hydroxyl to form the intermediate HSCO^(-)_(2),and then the activated-OH on the oxygen vacancy reacts with HSCO^(-)_(2) to form HCO^(-)_(3).Meanwhile,the catalyst exhibits high catalytic stability because copper species(Cu+/Cu^(2+))redox cycle mitigate the sulfation of Co_(3)O_(4)(Co^(2+)/Co^(3+)).Our work offers a promising approach for the rational design of cobalt-related catalysts in the highly efficient hydrolysis COS process.
基金supported by the National Natural Science Foundation of China(21804050)the National Key R and D Program of China(2018YFD0901003)+2 种基金the Science and Technology Planning Project of Xiamen,China(3502Z20183031)the Fujian Provincial Fund Project(2018J01432)the Xiamen Science and Technology Planning Project,China(3502Z20183031)。
文摘A ratiometric fluorescent probe for hypoxanthine(Hx)detection was established based on the mimic enzyme and fluorescence characteristics of cobalt-doped graphite-phase carbon nitride(Co doped g-C_(3)N_(4)).In addition to emitting strong fluorescence,the peroxidase activity of Co doped g-C_(3)N_(4)can catalyze the reaction of O-phenylenediamine and H_(2)O_(2)to produce diallyl phthalate which can emit yellow fluorescence at 570 nm.Through the decomposition of Hx by xanthine oxidase,Hx can be indirectly detected by the generating hydrogen peroxide based on the measurement of fluorescent ratio I(F_(570)/F_(370)).The linear range was 1.7-272.2 mg/kg(R^(2)=0.997),and the detection limit was 1.52 mg/kg(3σ/K,n=9).The established method was applied to Hx detection in bass,grass carp,and shrimp,and the data were verified by HPLC.The result shows that the established probe is sensitive,accurate,and reliable,and can be used for Hx detection in aquatic products.
基金This work received financial support from the National Natural Science Foundation of China(Grant Nos.U23A20574,52250010,and 52201242)the 261 Project MIIT,the Young Elite Scientists Sponsorship Program by CAST(Grant No.2021QNRC001)+1 种基金the Fundamental Research Funds for the Central Universities(Grant No.2242022R40018)the Jiangsu Funding Program for Excellent Postdoctoral Talent(Grant No.2022ZB75).
文摘Potassium-ion batteries(PIBs)offer a cost-effective and resource-abundant solution for large-scale energy storage.However,the progress of PIBs is impeded by the lack of high-capacity,long-life,and fast-kinetics anode electrode materials.Here,we propose a dual synergic optimization strategy to enhance the K^(+)storage stability and reaction kinetics of Bi_(2)S_(3) through two-dimensional compositing and cation doping.Externally,Bi_(2)S_(3) nanoparticles are loaded onto the surface of three-dimensional interconnected Ti_(3)C_(2)T_(x) nanosheets to stabilize the electrode structure.Internally,Cu^(2+)doping acts as active sites to accelerate K^(+)storage kinetics.Various theoretical simulations and ex situ techniques are used to elucidate the external–internal dual synergism.During discharge,Ti_(3)C_(2)T_(x) and Cu^(2+)collaboratively facilitate K+intercalation.Subsequently,Cu^(2+)doping primarily promotes the fracture of Bi2S3 bonds,facilitating a conversion reaction.Throughout cycling,the Ti_(3)C_(2)T_(x) composite structure and Cu^(2+)doping sustain functionality.The resulting Cu^(2+)-doped Bi2S3 anchored on Ti_(3)C_(2)T_(x)(C-BT)shows excellent rate capability(600 mAh g^(-1) at 0.1 A g^(–1);105 mAh g^(-1) at 5.0 A g^(-1))and cycling performance(91 mAh g^(-1) at 5.0 A g^(-1) after 1000 cycles)in half cells and a high energy density(179 Wh kg–1)in full cells.
基金supported by the National Natural Science Foundation of China (Grant No. 62204203)the Shaanxi Natural Science Basic Research Program (Grant No. 2022JQ-701)。
文摘Sn doping is an effective way to improve the response rate of Ga_(2)O_(3) film based solar-blind detectors. In this paper,Sn-doped Ga_(2)O_(3) films were prepared on a sapphire substrate by radio frequency magnetron sputtering. The films were characterized by X-ray diffraction, scanning electron microscopy, X-ray photoelectron spectroscopy and ultraviolet visible spectroscopy, and the effect of annealing atmosphere on the properties of films was studied. The Ga_(2)O_(3) films changed from amorphous to β-Ga_(2)O_(3) after annealing at 900 °C. The films were composed of micro crystalline particles with a diameter of about 5–20 nm.The β-Ga_(2)O_(3) had high transmittance for wavelengths above 300 nm, and obvious absorption for solar-blind signals at 200–280 nm.The metal semiconductor metal type solar-blind detectors were prepared. The detector based on Sn-doped β-Ga_(2)O_(3) thin film annealed in N_2 has the best response performance to 254 nm light. The photo-current is 10 μA at 20 V, the dark-current is 5.76 pA,the photo dark current ratio is 1.7 × 10~6, the response rate is 12.47 A/W, the external quantum efficiency is 6.09 × 10~3%, the specific detection rate is 2.61 × 10~(12) Jones, the response time and recovery time are 378 and 90 ms, respectively.
基金Funded by the Science and Technology Planning Project of Wuhan City(No.2013010501010135)the Science and Technology Planning Project of Hubei Province(Nos.2013BAA095,2014BAA136)National Natural Science Foundation of China(No.51372179)
文摘Pr3＋ doped ZnO quantum dots （QDs） were successfully synthesized by sol-gel process. X-ray diffraction （XRD） and X-ray Phtoelectron spectroscopy （XPS） were used to analyze the microstructure variation of ZnO QDs and the chemical environment of Pr3＋ with increasing Pr3＋ doping concentrations. Most of Pr3＋ ions distribute on the surface ofZnO QDs while a few of them penetrate into the ZnO lattice to substitute Zn2＋ which causes the lattice distortion and the change of the crystal size. With increasing concentration of Pr3＋ ions, the crystal size of ZnO QDs firstly increases and then decreases meanwhile the amorphization gradually increases. New Pr-O-Zn bonds formed after Pr3＋ doping and Pr3＋ ions have at least two chemical bonding environments： one is Pr-O-Zn bond and the other is Pr-O bond surrounded by oxygen vacancies.
基金Projects(5070202051402100+5 种基金81171461)supported by the National Natural Science Foundation of ChinaProject(11JJ4013)supported by the Natural Science Foundation of Hunan Province,ChinaProject(2013GK3155)supported by Science&Technology Project of Hunan Province,ChinaProject supported by the Youth 1000 Talent Program of ChinaProject supported by the Interdisciplinary Research Program of Hunan University,ChinaProject supported by the Young Teacher Promotion Fund by Hunan University,China
文摘A series of Zr-doped CaTiO3 powders were prepared with the mild co-precipitation method and calcined at 850℃ for 3 h. The as-prepared Zr-doped CaTiO3 samples were characterized by scanning electron microscopy （SEM）, X-ray diffraction （XRD）, UV-Vis diffuse reflectance spectra （DRS） and X-ray photoelectron spectra （XPS）. XRD result revealed the presence of single perovskite phase of CaTiO3. UV-Vis diffusive reflection spectra of Zr-doped CaTiO3 indicated that the absorbance obviously increased in the visible light irradiation. XPS analysis showed that two types of oxygen existed on the photocatalyst surface, including lattice oxygen and absorbed oxygen. Their photocatalytic activity in the case of the degradation of methyl orange in water and photoelectrochemical activity were also tested. The 5%Zr-doped （mole fraction） CaTiO3 sample showed the highest photocatalytic activity. The enhanced photocatalytic activity was ascribed to the change of the lattice structure, existence of oxygen vacancies and increase of the photogenerated charge separation efficiency.
