Heterojunction construction,especially S-scheme heterojunction,represents an efficient universal strategy to achieve high-performance photocatalytic materials.For further performance stimulation of these well-designed...Heterojunction construction,especially S-scheme heterojunction,represents an efficient universal strategy to achieve high-performance photocatalytic materials.For further performance stimulation of these well-designed heterojunctions,modulating the interfacial internal electric field(IEF)to steer dynamic charge transfer represents a promising approach.Herein,we realized the precise regulation of Fermi level(E_(F))of the oxidation semiconductor(mesoporous WO_(3-x))by tailoring the concentration of oxygen vacancies(V_(O)),maximizing the IEF intensity in Cs_(2)CuBr_(4)@WO_(3-x)(CCB@WO_(3-x))S-scheme heterojunction.The augmented IEF affords a robust driving force for directional electron delivery,leading to boosted charge separation.Hence,the developed CCB@WO_(3-x)S-scheme heterojunction demonstrated outstanding photocatalytic CO_(2)reduction performance,with the electron consumption rate(Relectron)up to 390.34μmol g^(-1)h^(-1),which is 3.28 folds higher than that of pure CCB.An in-depth analysis of the S-scheme electron transfer mode was presented via theoretical investigations,electron spin resonance(ESR),photo-irradiated Kelvin probe force microscopy(KPFM),and in-situ X-ray photoelectron spectroscopy(XPS).Finally,the CO_(2)photoconversion route was explored in detail using in-situ diffuse reflectance infrared Fourier transform spectroscopy(DRIFTS)and DFT theoretical calculations.展开更多
YBa2Cu3O7-x(YBCO) films with co-doping BaTiO3(BTO) and Y2O3 nanostructures were prepared by metal organic deposition using trifluoroacetates(TFA-MOD). The properties of the BTO/Y2O3co-doped YBCO films with diffe...YBa2Cu3O7-x(YBCO) films with co-doping BaTiO3(BTO) and Y2O3 nanostructures were prepared by metal organic deposition using trifluoroacetates(TFA-MOD). The properties of the BTO/Y2O3co-doped YBCO films with different excess yttrium have been systematically studied by x-ray diffraction(XRD), Raman spectra, and scanning electron microscope(SEM). The optimized content of yttrium excess in the BTO/Y2O3co-doped YBCO films is 10 mol.%, and the critical current density is as high as - 17 mA/cm^2(self-field, 65 K) by the magnetic signal. In addition, the Y2Cu2O5 was formed when the content of yttrium excess increases to 24 mol.%, which may result in the deterioration of the superconducting properties and the microstructure. The unique combination of the different types of nanostructures of BTO and Y2O3 in the doped YBCO films, compared with the pure YBCO films and BTO doped YBCO films, enhances the critical current density(JC) not only at the self-magnetic field, but also in the applied magnetic field.展开更多
All-solid-state Z-scheme photocatalysts for overall water splitting to evolve H_(2) is a promising strategy for efficient conversion of solar energy.However,most of these strategies require redox mediators.Herein,a di...All-solid-state Z-scheme photocatalysts for overall water splitting to evolve H_(2) is a promising strategy for efficient conversion of solar energy.However,most of these strategies require redox mediators.Herein,a direct Z-scheme photoelectrocatalytic electrode based on a WO_(3-x)nanowire-bridged TiO_(2)nanorod array heterojunction is constructed for overall water splitting,producing H_(2).The as-prepared WO_(3-x)/TiO_(2)nanorod array heterojunction shows photoelectrochemical(PEC)overall water splitting activity evolving both H_(2) and O_(2)under UV-vis light irradiation.An optimum PEC activity was achieved over a 1.67-WO_(3-x)/TiO_(2)photoelectrode yielding maximum H_(2) and O_(2)evolution rates roughly 11 times higher than that of pure TiO_(2)nanorods without any sacrificial agent or redox mediator.The role of oxygen vacancy in WO_(3-x)in affecting the H_(2) production rate was also comprehensively studied.The superior PEC activity of the WO_(3-x)/TiO_(2)electrode for overall water splitting can be ascribed to an efficient Z-scheme charge transfer pathway between the WO_(3-x)nanowires and TiO_(2)nanorods,the presence of oxygen vacancies in WO_(3-x),and a bias potential applied on the photoelectrode,resulting in effective spatial charge separation.This study provides a novel strategy for developing highly efficient PECs for overall water splitting.展开更多
Y_(1-x)Ho_xBa_2Cu_3O_(7-δ)(0<x<1) sinsle crystal thin films oriented with the caxis perpendicular to the sur-face were grown by DC magnetron sputtering technique. Target was pieced together with half of YBa_2Cu...Y_(1-x)Ho_xBa_2Cu_3O_(7-δ)(0<x<1) sinsle crystal thin films oriented with the caxis perpendicular to the sur-face were grown by DC magnetron sputtering technique. Target was pieced together with half of YBa_2Cu_3O_(7-δ)(YBCO) and half of HoBa_2Cu_3O_(7-δ)(HBCO) superconducting materials. As the distance between HBCO targetmaterial and substrate is varied , the Ho content in material is changed respectively. When the content of Ho is0. 7 (atom ratio) , the T_c>83K.展开更多
基金This work was financially supported by the National Natural Science Foundation of China(51972213)Natural Science Foundation of Shanghai(22ZR1460700).
文摘Heterojunction construction,especially S-scheme heterojunction,represents an efficient universal strategy to achieve high-performance photocatalytic materials.For further performance stimulation of these well-designed heterojunctions,modulating the interfacial internal electric field(IEF)to steer dynamic charge transfer represents a promising approach.Herein,we realized the precise regulation of Fermi level(E_(F))of the oxidation semiconductor(mesoporous WO_(3-x))by tailoring the concentration of oxygen vacancies(V_(O)),maximizing the IEF intensity in Cs_(2)CuBr_(4)@WO_(3-x)(CCB@WO_(3-x))S-scheme heterojunction.The augmented IEF affords a robust driving force for directional electron delivery,leading to boosted charge separation.Hence,the developed CCB@WO_(3-x)S-scheme heterojunction demonstrated outstanding photocatalytic CO_(2)reduction performance,with the electron consumption rate(Relectron)up to 390.34μmol g^(-1)h^(-1),which is 3.28 folds higher than that of pure CCB.An in-depth analysis of the S-scheme electron transfer mode was presented via theoretical investigations,electron spin resonance(ESR),photo-irradiated Kelvin probe force microscopy(KPFM),and in-situ X-ray photoelectron spectroscopy(XPS).Finally,the CO_(2)photoconversion route was explored in detail using in-situ diffuse reflectance infrared Fourier transform spectroscopy(DRIFTS)and DFT theoretical calculations.
基金Project supported by the National Natural Science Foundation of China(Grant No.51272250)the National Basic Research Program of China(Grant No.2011CBA00105)+1 种基金the National High Technology Research and Development Program of China(Grant No.2014AA032702)the Natural Science Foundation of Beijing,China(Grant No.2152035)
文摘YBa2Cu3O7-x(YBCO) films with co-doping BaTiO3(BTO) and Y2O3 nanostructures were prepared by metal organic deposition using trifluoroacetates(TFA-MOD). The properties of the BTO/Y2O3co-doped YBCO films with different excess yttrium have been systematically studied by x-ray diffraction(XRD), Raman spectra, and scanning electron microscope(SEM). The optimized content of yttrium excess in the BTO/Y2O3co-doped YBCO films is 10 mol.%, and the critical current density is as high as - 17 mA/cm^2(self-field, 65 K) by the magnetic signal. In addition, the Y2Cu2O5 was formed when the content of yttrium excess increases to 24 mol.%, which may result in the deterioration of the superconducting properties and the microstructure. The unique combination of the different types of nanostructures of BTO and Y2O3 in the doped YBCO films, compared with the pure YBCO films and BTO doped YBCO films, enhances the critical current density(JC) not only at the self-magnetic field, but also in the applied magnetic field.
基金supported by the National Key Research and Development Program of China(2019YFA0705400 and 2019YFD0901100)the National Natural Science Foundation of China(21991151,21925404,and 21775127)+1 种基金the“111”Project(B17027)Guangdong Basic and Applied Basic Research Foundation(2020A1515010510)。
文摘All-solid-state Z-scheme photocatalysts for overall water splitting to evolve H_(2) is a promising strategy for efficient conversion of solar energy.However,most of these strategies require redox mediators.Herein,a direct Z-scheme photoelectrocatalytic electrode based on a WO_(3-x)nanowire-bridged TiO_(2)nanorod array heterojunction is constructed for overall water splitting,producing H_(2).The as-prepared WO_(3-x)/TiO_(2)nanorod array heterojunction shows photoelectrochemical(PEC)overall water splitting activity evolving both H_(2) and O_(2)under UV-vis light irradiation.An optimum PEC activity was achieved over a 1.67-WO_(3-x)/TiO_(2)photoelectrode yielding maximum H_(2) and O_(2)evolution rates roughly 11 times higher than that of pure TiO_(2)nanorods without any sacrificial agent or redox mediator.The role of oxygen vacancy in WO_(3-x)in affecting the H_(2) production rate was also comprehensively studied.The superior PEC activity of the WO_(3-x)/TiO_(2)electrode for overall water splitting can be ascribed to an efficient Z-scheme charge transfer pathway between the WO_(3-x)nanowires and TiO_(2)nanorods,the presence of oxygen vacancies in WO_(3-x),and a bias potential applied on the photoelectrode,resulting in effective spatial charge separation.This study provides a novel strategy for developing highly efficient PECs for overall water splitting.
文摘Y_(1-x)Ho_xBa_2Cu_3O_(7-δ)(0<x<1) sinsle crystal thin films oriented with the caxis perpendicular to the sur-face were grown by DC magnetron sputtering technique. Target was pieced together with half of YBa_2Cu_3O_(7-δ)(YBCO) and half of HoBa_2Cu_3O_(7-δ)(HBCO) superconducting materials. As the distance between HBCO targetmaterial and substrate is varied , the Ho content in material is changed respectively. When the content of Ho is0. 7 (atom ratio) , the T_c>83K.