A controllable crystallization is of practical importance to produce high-quality perovskite thin films with reduced structural defects.Lewis bases as electron-pair donor chemicals can strongly coordinate to lead ions...A controllable crystallization is of practical importance to produce high-quality perovskite thin films with reduced structural defects.Lewis bases as electron-pair donor chemicals can strongly coordinate to lead ions and have been extensively employed to manipulate the growth of perovskite crystals.In this work,we demonstrate a series of Lewis-base amides,for morphological regulation of methylammonium lead triiodide(MAPbI3)thin films.The screened acetamide was demonstrated to decently improve the grain size,along with a spatial distribution at grain boundaries(GBs).The mesostructured solar cells of acetamide-modified absorbers yielded an optimized power conversion efficiency(PCE)of 20.04%with a mitigated open-circuit voltage(V_(OC))deficit of 0.39 V.This work provides a facile and cost-effective strategy toward controllable fabrication of high-performance MAPbI3 solar cells.展开更多
Organometal halide perovskites have recently emerged with a huge potential for photovoltaic applications. Moreover, preparation of high-quality perovskite crystals with controlled morphology is of great significance f...Organometal halide perovskites have recently emerged with a huge potential for photovoltaic applications. Moreover, preparation of high-quality perovskite crystals with controlled morphology is of great significance for the fundamental studies such as optical and electrical properties, as well as the applications. Here, we report a one-pot solvothermal process to synthesize sheet-shaped CH3NH3PbBr3 single crystals with the lateral size of 100 μm and the thickness of 3–8 μm. Furthermore, a controlled etching behavior on the crystalline surface was demonstrated, which could be the irregular collapse of the crystalline surface caused by the local accumulation of methylammonium cations. Using this technique,CH3NH3PbBr3 single crystal sheets could be used in the various optoelectronic devices, such as nanolaser,optical sensors, photodetectors and field effect transistors.展开更多
An amorphous ferric oxide layer was prepared on a bismuth vanadate photoanode.This resulted in improved charge carrier separation and surface catalytic performance compared with the photoanode without the oxide layer....An amorphous ferric oxide layer was prepared on a bismuth vanadate photoanode.This resulted in improved charge carrier separation and surface catalytic performance compared with the photoanode without the oxide layer.The photocurrent of the oxide‐layer‐containing photoanode was2.52mA/cm2at1.23V versus the reversible hydrogen electrode,in potassium phosphate buffer,(0.5mol/L,pH=7.0).The amorphous ferric oxide layer on the photoanode contained low‐valence‐state iron species(FeII),which enabled efficient hole extraction and transfer.展开更多
The development of a facile method to construct a high-performance electrode is of paramount importance to the application of alkaline water electrolysis. Here, we report that the activity of nickel foam （NF） toward...The development of a facile method to construct a high-performance electrode is of paramount importance to the application of alkaline water electrolysis. Here, we report that the activity of nickel foam （NF） towards the oxygen evolution reaction （OER） can be enhanced remarkably through simple immersion in a ferric nitrate （Fe（NOs）s） solution at room temperature. During this immersion process, the oxidation of the NF surface by NOs- ions increases the near-surface concentrations of OH- and Ni2＋, which results in the in situ deposition of a highly active amorphous Ni-Fe hydroxide （a-NiFeOxHy） layer. Specifically the OER overpotential of the NF electrode decreases from 371 mV （bare NF） to 270 mV （@10 mA-cm-2 in 0.1 M KOH） after immersion in a 20 mM Fe（NOs）s solution for just I min. A longer immersion time results in further increased OER activity （196 mV@10 mA,cm-2 in 1 M KOH）. The overall water splitting properties of the a-NiFeOxHy@NF electrode were evaluated using a two-electrode configuration. It is worth noting that the current density can reach 25 mA.cm-2 in 6 M KOH at an applied voltage of 1.5 V at room temperature.展开更多
Bismuth vanadate （BiVO4） has been identified as one of the excellent visible-light-responsive photoanode for use in the photoelectrochemical water splitting. Recently intense research efforts have been devoted to th...Bismuth vanadate （BiVO4） has been identified as one of the excellent visible-light-responsive photoanode for use in the photoelectrochemical water splitting. Recently intense research efforts have been devoted to the development of highly efficient BiVO4 photoanode. Herein, we reported a low-cost and scalable method for preparing nanostructured BiVO4 film. A much enhanced photocurrent （1.5 mAocm 2） was obtained for such film, which was 6.5 times higher than that of planar film at 1.23 V [vs. RHE （Reversible Hydrogen Electrode）]. The method provides an eco-friendly, reproducible and facile way to scale up on different substrates with attractive potential.展开更多
The electrocatalytic reduction of CO_(2) presents a promising strategy in addressing environmental and energy crisis.Significant progress has been achieved via CO_(2) gas diffusion electrolysis,to react at high select...The electrocatalytic reduction of CO_(2) presents a promising strategy in addressing environmental and energy crisis.Significant progress has been achieved via CO_(2) gas diffusion electrolysis,to react at high selectivity and high rate.However,the gas diffusion layer(GDL)of the gas diffusion electrode(GDE)still suffers from low tolerance and limited active sites.Here,the hydrophobic 1-octadecanethiol molecular was functionalized over the Cu catalyst layer of the GDE,which simultaneously stabilizes the GDL and exposes abundant active solid-liquid-gas three-phase interfaces.The resultant GDE exhibits multi-carbon(C_(2+))product selectivity over faradaic efficiency(FE)of 70.0%in the range of 100 to 800 mA·cm^(-2),with the peak FE^(c2+)of 85.2%at 800 mA·cm^(-2).Notably,the strengthened GDE could continuously drive high-current electrolysis for more than 100 h without flooding.This work opens a new way to improve CO_(2) gas diffusion electrolysis via surface molecular engineering.展开更多
The activity and durability of electrocatalysts are important factors in their practical applications, such as electrocatalytic oxygen evolution reactions （OERs） used in water splitting cells and metal-air batteries...The activity and durability of electrocatalysts are important factors in their practical applications, such as electrocatalytic oxygen evolution reactions （OERs） used in water splitting cells and metal-air batteries. In this study, a novel electrocatalyst, comprising few-layered graphitic carbon （-5 atomic layers） encapsulated heazlewoodite （Ni3S2@C） nanoparticles （NPs）, was designed and synthesized using a one-step solid phase pyrolysis method. In the OER test, the Ni3S2@C catalyst exhibited an overpotential of 298 mV at a current density of 10 mA·cm^-2, a Tafel slope of 51.3 mV·dec^-1, and charge transfer resistance of 22.0 Ω, which were better than those of benchmark RuO2 and most nickel- sulfide-based catalysts previously reported. This improved performance was ascribed to the high electronic conductivity of the graphitic carbon encapsulating layers. Moreover, the encapsulation of graphitic carbon layers provided superb stability without noticeable oxidation or depletion of Ni3S2 NPs within the nanocomposite. Therefore, the strategy introduced in this work can benefit the development of highly stable metal sulfide electrocatalysts for energy conversion and storage applications, without sacrificing electrocatalytic activity.展开更多
Metal-organic frameworks(MOFs) possess the features of highly porosity-tunable and electronic-tunable structures,. Taking advantages of these merits, we successfully installed high-valence W6+ions onto the Ti-oxo clus...Metal-organic frameworks(MOFs) possess the features of highly porosity-tunable and electronic-tunable structures,. Taking advantages of these merits, we successfully installed high-valence W6+ions onto the Ti-oxo clusters of MIL-125(Ti)(W-MIL-125). The installed W^(6+) ions which form a W–O–Ti structure trigger the metal-to-cluster charge transfer(MCCT), together with an enhanced light absorption.Structural and spectroscopic characterizations reveal that the MCCT process optimizes the charge transfer process and efficiently separates the photogenerated electron-hole spatially.The as-obtained sample of 3.45 W-MIL-125 with optimized electronic structure demonstrates an enhanced photocatalytic hydrogen evolution performance of 1110.7 ± 63.7 μmol g^(-1)h^(-1) under light irradiation, which is 4.0 times that of the pristine MIL-125(Ti). This work will open up a new avenue for local structural modification of MOFs to boost photocatalytic performance.展开更多
Anatase TiO2 as a promising photocatalyst has been widely employed in the decontamination treatment of polluted water, air purification and water splitting. Coupling TiO2 with other semiconductor materials could furth...Anatase TiO2 as a promising photocatalyst has been widely employed in the decontamination treatment of polluted water, air purification and water splitting. Coupling TiO2 with other semiconductor materials could further enhance the photocatalytic activity. Here, we successfully synthesized the SnOz/TiO2 catalyst by depositing SnO2 particles on the anatase TiO2 {105} facets through a gas phase oxidation process. The SnOz/TiO2 catalyst shows higher photocatalytic activity for decomposition of MB than that of the pure YiO2 catalyst. The enhanced photo- catalytic activity can be attributed to the efficient charge separation since TiO2 and SnO2 catalyst have staggered energy level.展开更多
Here we report a hydrothermal approach to build and tailor the hierarchical structure of brookite TiO_2 crystal under multiple hierarchical scales. Benefiting from the hierarchical structure and the existence of oxyge...Here we report a hydrothermal approach to build and tailor the hierarchical structure of brookite TiO_2 crystal under multiple hierarchical scales. Benefiting from the hierarchical structure and the existence of oxygen vacancy,these as-prepared hierarchical brookite TiO_2 crystals can not only enhance photocatalytic activity, but also demonstrate their potential in the treatment of superficial malignant tumor.展开更多
基金financially supported by the National Natural Science Funds for Distinguished Young Scholar(51725201)the National Natural Science Foundation of China(51972111,51902185,51602103)+4 种基金Young Elite Scientists Sponsorship Program by CAST(2017QNRC001)International(Regional)Cooperation and Exchange Projects of the National Natural Science Foundation of China(51920105003)Innovation Program of Shanghai Municipal Education Commission(E00014)the Fundamental Research Funds for the Central Universities(JKD012016025,JKD012016022)Shanghai Engineering Research Center of Hierarchical Nanomaterials(18DZ2252400)。
文摘A controllable crystallization is of practical importance to produce high-quality perovskite thin films with reduced structural defects.Lewis bases as electron-pair donor chemicals can strongly coordinate to lead ions and have been extensively employed to manipulate the growth of perovskite crystals.In this work,we demonstrate a series of Lewis-base amides,for morphological regulation of methylammonium lead triiodide(MAPbI3)thin films.The screened acetamide was demonstrated to decently improve the grain size,along with a spatial distribution at grain boundaries(GBs).The mesostructured solar cells of acetamide-modified absorbers yielded an optimized power conversion efficiency(PCE)of 20.04%with a mitigated open-circuit voltage(V_(OC))deficit of 0.39 V.This work provides a facile and cost-effective strategy toward controllable fabrication of high-performance MAPbI3 solar cells.
基金financially supported by the National Natural Science Foundation of China (51602103)the National Natural Science Funds for Distinguished Young Scholar (51725201)+4 种基金Young Elite Scientists Sponsorship Program by CAST (2017QNRC001)Shanghai Pujiang Program (18PJD009)“Chen Guang” Project supported by Shanghai Municipal Education Commission and Shanghai Education Development Foundation (15CG26)Fundamental Research Funds for the Central Universities (222201718002)the Major Research plan of National Natural Science Foundation of China (91534202)
文摘Organometal halide perovskites have recently emerged with a huge potential for photovoltaic applications. Moreover, preparation of high-quality perovskite crystals with controlled morphology is of great significance for the fundamental studies such as optical and electrical properties, as well as the applications. Here, we report a one-pot solvothermal process to synthesize sheet-shaped CH3NH3PbBr3 single crystals with the lateral size of 100 μm and the thickness of 3–8 μm. Furthermore, a controlled etching behavior on the crystalline surface was demonstrated, which could be the irregular collapse of the crystalline surface caused by the local accumulation of methylammonium cations. Using this technique,CH3NH3PbBr3 single crystal sheets could be used in the various optoelectronic devices, such as nanolaser,optical sensors, photodetectors and field effect transistors.
基金supported by the National Natural Science Foundation of China(21373083,21573068)Program of Shanghai Subject Chief Scientist(15XD1501300)+1 种基金the Scientific Research Foundation for the Returned Overseas Chinese Scholars,State Education MinistryScience Technology Commission of Shanghai Municipality(14JC1490900)~~
文摘An amorphous ferric oxide layer was prepared on a bismuth vanadate photoanode.This resulted in improved charge carrier separation and surface catalytic performance compared with the photoanode without the oxide layer.The photocurrent of the oxide‐layer‐containing photoanode was2.52mA/cm2at1.23V versus the reversible hydrogen electrode,in potassium phosphate buffer,(0.5mol/L,pH=7.0).The amorphous ferric oxide layer on the photoanode contained low‐valence‐state iron species(FeII),which enabled efficient hole extraction and transfer.
文摘The development of a facile method to construct a high-performance electrode is of paramount importance to the application of alkaline water electrolysis. Here, we report that the activity of nickel foam （NF） towards the oxygen evolution reaction （OER） can be enhanced remarkably through simple immersion in a ferric nitrate （Fe（NOs）s） solution at room temperature. During this immersion process, the oxidation of the NF surface by NOs- ions increases the near-surface concentrations of OH- and Ni2＋, which results in the in situ deposition of a highly active amorphous Ni-Fe hydroxide （a-NiFeOxHy） layer. Specifically the OER overpotential of the NF electrode decreases from 371 mV （bare NF） to 270 mV （@10 mA-cm-2 in 0.1 M KOH） after immersion in a 20 mM Fe（NOs）s solution for just I min. A longer immersion time results in further increased OER activity （196 mV@10 mA,cm-2 in 1 M KOH）. The overall water splitting properties of the a-NiFeOxHy@NF electrode were evaluated using a two-electrode configuration. It is worth noting that the current density can reach 25 mA.cm-2 in 6 M KOH at an applied voltage of 1.5 V at room temperature.
基金This work was financially supported by the National Natural Science Foundation of China （Nos. 21373083 and 21573068）, the Program of Shanghai Subject Chief Scientist （No. 15XD 1501300）, the Specialized Research Fund for the Doctoral Program of Higher Education, the Scientific Research Foundation for the Returned Overseas Chinese Scholars, State Education Ministry Fundamental Research Funds for the Central Universities （No. WD1313009）, 111 Project （No. B14018） and the Science and Technology Commission of Shanghai Municipality （No. 14JC 1490900）.
文摘Bismuth vanadate （BiVO4） has been identified as one of the excellent visible-light-responsive photoanode for use in the photoelectrochemical water splitting. Recently intense research efforts have been devoted to the development of highly efficient BiVO4 photoanode. Herein, we reported a low-cost and scalable method for preparing nanostructured BiVO4 film. A much enhanced photocurrent （1.5 mAocm 2） was obtained for such film, which was 6.5 times higher than that of planar film at 1.23 V [vs. RHE （Reversible Hydrogen Electrode）]. The method provides an eco-friendly, reproducible and facile way to scale up on different substrates with attractive potential.
基金supported by the International(Regional)Cooperation and Exchange Projects of the National Natural Science Foundation of China(No.51920105003)the National Natural Science Funds for Distinguished Young Scholars(No.51725201)+5 种基金the Innovation Program of Shanghai Municipal Education Commission(No.E00014)the National Natural Science Foundation of China(Nos.51902105 and 22072045)the Shanghai Engineering Research Center of Hierarchical Nanomaterials(No.18DZ2252400)the Shanghai Sailing Program(No.19YF1411600)support by Shanghai Rising-star and Shuguang Programs(Nos.20QA1402400 and 17SG30)the Program for Professor of Special Appointment(Eastern Scholar)at Shanghai Institutions of Higher Learning.
文摘The electrocatalytic reduction of CO_(2) presents a promising strategy in addressing environmental and energy crisis.Significant progress has been achieved via CO_(2) gas diffusion electrolysis,to react at high selectivity and high rate.However,the gas diffusion layer(GDL)of the gas diffusion electrode(GDE)still suffers from low tolerance and limited active sites.Here,the hydrophobic 1-octadecanethiol molecular was functionalized over the Cu catalyst layer of the GDE,which simultaneously stabilizes the GDL and exposes abundant active solid-liquid-gas three-phase interfaces.The resultant GDE exhibits multi-carbon(C_(2+))product selectivity over faradaic efficiency(FE)of 70.0%in the range of 100 to 800 mA·cm^(-2),with the peak FE^(c2+)of 85.2%at 800 mA·cm^(-2).Notably,the strengthened GDE could continuously drive high-current electrolysis for more than 100 h without flooding.This work opens a new way to improve CO_(2) gas diffusion electrolysis via surface molecular engineering.
基金Acknowledgements This work was financially supported by Australian Research Council （ARC） Discovery Project and the National Natural Science Foundation of China （Nos. 51372248 and 51432009）.
文摘The activity and durability of electrocatalysts are important factors in their practical applications, such as electrocatalytic oxygen evolution reactions （OERs） used in water splitting cells and metal-air batteries. In this study, a novel electrocatalyst, comprising few-layered graphitic carbon （-5 atomic layers） encapsulated heazlewoodite （Ni3S2@C） nanoparticles （NPs）, was designed and synthesized using a one-step solid phase pyrolysis method. In the OER test, the Ni3S2@C catalyst exhibited an overpotential of 298 mV at a current density of 10 mA·cm^-2, a Tafel slope of 51.3 mV·dec^-1, and charge transfer resistance of 22.0 Ω, which were better than those of benchmark RuO2 and most nickel- sulfide-based catalysts previously reported. This improved performance was ascribed to the high electronic conductivity of the graphitic carbon encapsulating layers. Moreover, the encapsulation of graphitic carbon layers provided superb stability without noticeable oxidation or depletion of Ni3S2 NPs within the nanocomposite. Therefore, the strategy introduced in this work can benefit the development of highly stable metal sulfide electrocatalysts for energy conversion and storage applications, without sacrificing electrocatalytic activity.
基金financially supported by the National Natural Science Funds for Distinguished Young Scholars (51725201)the International (Regional) Cooperation and Exchange Projects of the National Natural Science Foundation of China (51920105003)+6 种基金the Innovation Program of Shanghai Municipal Education Commission (E00014)China Postdoctoral Science Foundation Funded Project (2020M681201)Shanghai Engineering Research Center of Hierarchical Nanomaterials (18DZ2252400)the Fundamental Research Funds for the Central Universities (JKD01211519)the support by Shanghai Rising-star Program (20QA1402400)the Program for Professor of Special Appointment (Eastern Scholar) at Shanghai Institutions of Higher Learningprovided by the Feringa Nobel Prize Scientist Joint Research Center。
文摘Metal-organic frameworks(MOFs) possess the features of highly porosity-tunable and electronic-tunable structures,. Taking advantages of these merits, we successfully installed high-valence W6+ions onto the Ti-oxo clusters of MIL-125(Ti)(W-MIL-125). The installed W^(6+) ions which form a W–O–Ti structure trigger the metal-to-cluster charge transfer(MCCT), together with an enhanced light absorption.Structural and spectroscopic characterizations reveal that the MCCT process optimizes the charge transfer process and efficiently separates the photogenerated electron-hole spatially.The as-obtained sample of 3.45 W-MIL-125 with optimized electronic structure demonstrates an enhanced photocatalytic hydrogen evolution performance of 1110.7 ± 63.7 μmol g^(-1)h^(-1) under light irradiation, which is 4.0 times that of the pristine MIL-125(Ti). This work will open up a new avenue for local structural modification of MOFs to boost photocatalytic performance.
基金This work was financially supported by National Natural Science Foundation of China，SRF for ROCS,SEM,Programme for Professor of Special Appointment (Eastern Scholar) at Shanghai Institutions of Higher Learning,Major Basic Research Programme of Science and Technology Commission of Shanghai Municipality，Australian Research Council's Future Fellowships，Shanghai Municipal Natural Science Foundation
文摘Anatase TiO2 as a promising photocatalyst has been widely employed in the decontamination treatment of polluted water, air purification and water splitting. Coupling TiO2 with other semiconductor materials could further enhance the photocatalytic activity. Here, we successfully synthesized the SnOz/TiO2 catalyst by depositing SnO2 particles on the anatase TiO2 {105} facets through a gas phase oxidation process. The SnOz/TiO2 catalyst shows higher photocatalytic activity for decomposition of MB than that of the pure YiO2 catalyst. The enhanced photo- catalytic activity can be attributed to the efficient charge separation since TiO2 and SnO2 catalyst have staggered energy level.
基金supported by the National Natural Science Foundation of China (21573068)Program of Shanghai Subject Chief Scientist (15XD1501300)+1 种基金the Scientific Research Foundation for the Returned Overseas Chinese Scholars, State Education Ministrythe Fundamental Research Funds for the Central Universities (WD1313009)
文摘Here we report a hydrothermal approach to build and tailor the hierarchical structure of brookite TiO_2 crystal under multiple hierarchical scales. Benefiting from the hierarchical structure and the existence of oxygen vacancy,these as-prepared hierarchical brookite TiO_2 crystals can not only enhance photocatalytic activity, but also demonstrate their potential in the treatment of superficial malignant tumor.
