Defect and charge transfer efficiency of nano-photocatalysts are important factors which influence their photocatalytic performance.In this work,oxygen vacancies are successfully introduced in the synthesis process of...Defect and charge transfer efficiency of nano-photocatalysts are important factors which influence their photocatalytic performance.In this work,oxygen vacancies are successfully introduced in the synthesis process of Bi_(2)Al_(4)O_(9)/β-Bi_(2)O_(3)heterojunctions through one-step in situ selfcombustion method.High-resolution transmission electron microscopy (HRTEM),UV-Vis diffuse reflectance spectra (UV-Vis DRS),and electron spin resonance (ESR) measurements confirm the existence of oxygen vacancies.In addition,by controlling the ratio of reactants of Bi(NO_(3))_(3)to Al(NO_(3))_(3),the ratio of Bi_(2)Al_(4)O_(9)and β-Bi_(2)O_(3)in the heterojunction can be easily adjusted.Photocurrent responses and surface photovoltage spectroscopy (SPV) indicate that the construction of the Bi_(2)Al_(4)O_(9)/β-Bi_(2)O_(3)heterostructure improves the separation efficiency of the photo-generated electrons and holes.CO_(2)-TPD results imply that the amounts and stability of heterojunctions are enhanced compared with their counterparts.The Bi_(2)Al_(4)O_(9)/β-Bi_(2)O_(3)heterojunction with 14 mol%Bi_(2)Al_(4)O_(9)shows the highest photocatalytic ability for reduction of CO_(2)into CO.The enhanced photoreduction of CO_(2)performance can be ascribed to the synergistic effects of the heterojunction for electron separation and oxygen vacancies for CO_(2)activation.展开更多
采用传统的高温固相法制备一种新型的红色荧光粉Ba_(6)Gd_(2)Ti_(4)O_(17):Sm^(3+),并通过X射线衍射(X-ray diffraction,XRD)、扫描电子显微镜(scanning electron microscope,SEM)、荧光(photoluminescence,PL)光谱及色坐标表征系列样...采用传统的高温固相法制备一种新型的红色荧光粉Ba_(6)Gd_(2)Ti_(4)O_(17):Sm^(3+),并通过X射线衍射(X-ray diffraction,XRD)、扫描电子显微镜(scanning electron microscope,SEM)、荧光(photoluminescence,PL)光谱及色坐标表征系列样品的物相、形貌和发光性能.PL光谱表明该荧光粉可以被近紫外光有效激发,在407 nm近紫外光激发下,发射光谱由四个发射峰组成,最强发射峰位于616 nm处,归结为Sm^(3+)的^(4)G_(5/2)→^(6)H_(7/2)跃迁.随着Sm^(3+)掺杂量的增加,荧光粉的发光强度先增大后减小,最佳掺杂比例(物质的量分数)为3%.系列掺杂比例荧光粉的色坐标基本不变,均位于红光区.研究结果表明,该荧光粉是一种具有应用前景的新型白光发光二极管(light-emitting diode,LED)用红色荧光粉.展开更多
Lanthanide(Ln^(3+))oxysulfide nanocrystals(NCs)have great prospect in many advanced technologies;however,they suffer from a low photoluminescence efficiency due to the volatility of sulfur and deleterious surface quen...Lanthanide(Ln^(3+))oxysulfide nanocrystals(NCs)have great prospect in many advanced technologies;however,they suffer from a low photoluminescence efficiency due to the volatility of sulfur and deleterious surface quenching effect.Herein,we report a novel sandwiched luminescent heterostructure based on Ln^(3+)-doped Gd_(2)O_(2)S@NaYF_(4)core/shell NCs with tunable sulfur content in the sandwich layer.By means of Eu^(3+)as the sensitive structural probes,we unravel the ligand-mediated structure control of the NCs from Gd_(2)O_(3):Ln^(3+)@NaYF_(4)to Gd_(2)O_(2)S:Ln^(3+)@NaYF_(4)with tailored S2–deficiency.Such a sandwich-type core/shell heterostructure enables us to achieve efficient and multicolor downshifting and upconversion luminescence(UCL),with up to 208.8 folds of enhancement in UCL intensity as compared to that of their core-only counterparts.These findings provide a general approach for the controlled synthesis of lanthanide oxysulfide@fluoride heterostructure,which offers a new way for the materials design towards diverse emerging applications.展开更多
Piezocatalytic activation of persulfate(PS) has great application potential in environmental remediation;however,the relationship between piezocatalyst thickness and catalytic activity is not clear,limiting the furthe...Piezocatalytic activation of persulfate(PS) has great application potential in environmental remediation;however,the relationship between piezocatalyst thickness and catalytic activity is not clear,limiting the further improvement of catalytic activity and application of the technology.Herein,the Bi_(2)Fe_(4)O_(9)(BFO) piezocatalysts with tunable thickness were prepared through a facile hydrothermal method by tuning the molar ratio of Bi(NO_(3)),5H_(2)O and FeCl_(3)·6H_(2)O for piezocatalytic activation of peroxydisulfate(PDS).The BFO with the smallest thickness exhibits excellent catalytic activity,and the SO_(4)^(·-)and ·OH are the major reactive oxygen species for degrading organic pollutants.Further XPS investigations and finite element analyses demonstrate that the decreased thickness of BFO not only exposes more Fe^(2+)sites for PDS activation,but also improve the piezoelectric effect to accelerate the regeneration of Fe^(2+),thus enabling an enhanced synergy effect between PDS activation and piezocatalysis for outstanding catalytic activity.This work provides an understanding of the relationship between thickness of piezocatalysts and its catalytic activity over PDS activation,facilitating the development of more efficient piezocatalysts and PS-based advanced oxidation processes.展开更多
基金National Natural Science Foundation of China(12175254,U1832119)National Key R&D Program of China(2021YFE0104800)+2 种基金International Partnership Program of Chinese Academy of Sciences(121631KYSB20200039)International Cooperation Project of Shanghai Science and Technology Commission(20520750200)National Centre for Research and Development(WPC2/1/SCAPOL/2021)。
基金financial support from the National Natural Science Foundation of China(21776059,21376061)the Natural Science Foundation for Distinguished Young Scholars of Hebei Province(B2015208010)the Research Foundation of Hebei Province Education Department(No.ZC2016007)。
文摘Defect and charge transfer efficiency of nano-photocatalysts are important factors which influence their photocatalytic performance.In this work,oxygen vacancies are successfully introduced in the synthesis process of Bi_(2)Al_(4)O_(9)/β-Bi_(2)O_(3)heterojunctions through one-step in situ selfcombustion method.High-resolution transmission electron microscopy (HRTEM),UV-Vis diffuse reflectance spectra (UV-Vis DRS),and electron spin resonance (ESR) measurements confirm the existence of oxygen vacancies.In addition,by controlling the ratio of reactants of Bi(NO_(3))_(3)to Al(NO_(3))_(3),the ratio of Bi_(2)Al_(4)O_(9)and β-Bi_(2)O_(3)in the heterojunction can be easily adjusted.Photocurrent responses and surface photovoltage spectroscopy (SPV) indicate that the construction of the Bi_(2)Al_(4)O_(9)/β-Bi_(2)O_(3)heterostructure improves the separation efficiency of the photo-generated electrons and holes.CO_(2)-TPD results imply that the amounts and stability of heterojunctions are enhanced compared with their counterparts.The Bi_(2)Al_(4)O_(9)/β-Bi_(2)O_(3)heterojunction with 14 mol%Bi_(2)Al_(4)O_(9)shows the highest photocatalytic ability for reduction of CO_(2)into CO.The enhanced photoreduction of CO_(2)performance can be ascribed to the synergistic effects of the heterojunction for electron separation and oxygen vacancies for CO_(2)activation.
基金National Key R&D Program of China,Grant/Award Number:2022YFB3503700NSFC,Grant/Award Numbers:12074379,12174391,U22A20398,22135008+1 种基金the Youth Innovation Promotion Association of CAS,Grant/Award Number:2020305Natural Science Foundation of Fujian Province,Grant/Award Numbers:2020I0037,2021L3024,2022H0040。
文摘Lanthanide(Ln^(3+))oxysulfide nanocrystals(NCs)have great prospect in many advanced technologies;however,they suffer from a low photoluminescence efficiency due to the volatility of sulfur and deleterious surface quenching effect.Herein,we report a novel sandwiched luminescent heterostructure based on Ln^(3+)-doped Gd_(2)O_(2)S@NaYF_(4)core/shell NCs with tunable sulfur content in the sandwich layer.By means of Eu^(3+)as the sensitive structural probes,we unravel the ligand-mediated structure control of the NCs from Gd_(2)O_(3):Ln^(3+)@NaYF_(4)to Gd_(2)O_(2)S:Ln^(3+)@NaYF_(4)with tailored S2–deficiency.Such a sandwich-type core/shell heterostructure enables us to achieve efficient and multicolor downshifting and upconversion luminescence(UCL),with up to 208.8 folds of enhancement in UCL intensity as compared to that of their core-only counterparts.These findings provide a general approach for the controlled synthesis of lanthanide oxysulfide@fluoride heterostructure,which offers a new way for the materials design towards diverse emerging applications.
基金financially supported by the National Natural Science Foundation of China (Nos.52170155 and 52100084)。
文摘Piezocatalytic activation of persulfate(PS) has great application potential in environmental remediation;however,the relationship between piezocatalyst thickness and catalytic activity is not clear,limiting the further improvement of catalytic activity and application of the technology.Herein,the Bi_(2)Fe_(4)O_(9)(BFO) piezocatalysts with tunable thickness were prepared through a facile hydrothermal method by tuning the molar ratio of Bi(NO_(3)),5H_(2)O and FeCl_(3)·6H_(2)O for piezocatalytic activation of peroxydisulfate(PDS).The BFO with the smallest thickness exhibits excellent catalytic activity,and the SO_(4)^(·-)and ·OH are the major reactive oxygen species for degrading organic pollutants.Further XPS investigations and finite element analyses demonstrate that the decreased thickness of BFO not only exposes more Fe^(2+)sites for PDS activation,but also improve the piezoelectric effect to accelerate the regeneration of Fe^(2+),thus enabling an enhanced synergy effect between PDS activation and piezocatalysis for outstanding catalytic activity.This work provides an understanding of the relationship between thickness of piezocatalysts and its catalytic activity over PDS activation,facilitating the development of more efficient piezocatalysts and PS-based advanced oxidation processes.
