Engineering an efficient interface is a trustworthy strategy for designing advanced photocatalytic systems for solar energy conversion.Herein,oxygen-deficient Bi_(2)WO_(6)atomic layers without organic residues were su...Engineering an efficient interface is a trustworthy strategy for designing advanced photocatalytic systems for solar energy conversion.Herein,oxygen-deficient Bi_(2)WO_(6)atomic layers without organic residues were successfully fabricated via a facile solvothermal strategy by the multifunctional regulatory mechanism of introduced chloridion.Both DFT calculations and speciation determination revealed that chloridion displayed a more pronounced effect in the controllable synthesis of oxygen-deficient Bi_(2)WO_(6)atomic layers without organic residues:ultrathinning and defect-engineering.This built-in multi-cooperative interface endowed Bi_(2)WO_(6)with intriguing photoelectrochemical properties,O_(2) activation ability,and ultrahigh activity in visible-light powered deep oxidation of NO.A reasonable photocatalytic mechanism was proposed based on in situ infrared spectroscopy analysis and theoretical calculations.We believe that this multi-cooperative interface engineering of oxygen-deficient Bi_(2)WO_(6)atomic layers without organic residues could provide new insights into the design of two-dimensional(2D)layered materials with efficient active sites and pave the way for efficient NO photooxidation systems.展开更多
Cubic phase CsPbBr_(3)perovskite nanocrystals(PNCs)was prepared by a high-temperature hot-injection method.The high photoluminescence quantum yield(PLQY)of as-prepared CsPbBr_(3)PNCs was 87%,which can be used for the ...Cubic phase CsPbBr_(3)perovskite nanocrystals(PNCs)was prepared by a high-temperature hot-injection method.The high photoluminescence quantum yield(PLQY)of as-prepared CsPbBr_(3)PNCs was 87%,which can be used for the determination of chloridion in domestic water samples based on their wavelength-shift characteristics via halide exchange.The proposal approach for the determination of chloridion reveals a linear correlation ranged from 10 to 200μM of the chloridion concentration and the wavelength shift of CsPbBr_(3)PNCs with a correlation coe fficient of R^(2)=0.9956.The as-mentioned method reveals neglectable responses towards those co-existing ions in the water aside from chloridion,due to the quick exchange between Cl and Br and the outstanding color change caused by wavelength shift.The strategy has been applied to the determination of chloridion in water samples with the recoveries of 98.9–104.2%and the limit of detection(LOD)of 4μM.These results show that the suggested approach is promising for the development of novel fluorescence detection for chloridion in water.展开更多
Photoelectrochemical(PEC)seawater splitting is a promising method for the direct utilization of solar energy and abundant seawater resources for hydrogen production.Photoelectrodes are susceptible to various ions in s...Photoelectrochemical(PEC)seawater splitting is a promising method for the direct utilization of solar energy and abundant seawater resources for hydrogen production.Photoelectrodes are susceptible to various ions in seawater and complicated competitive reactions,resulting in the failure of photoelectrodes.This paper proposes the design and fabrication of diff erent sputtered stainless steel(SS)fi lms deposited on silicon photoanodes,completely isolating the electrolytes and semiconductor substrate.Upon coupling with the PEC flow cell,the back-illuminated photoanode coated with 316 SS cocatalyst achieves stable operation for 70 h in natural seawater with a highly alkaline KOH(30 wt.%,7.64 mol/L)electrolyte due to the remarkable protection eff ect of the substrate from stainless steel,while the PEC seawater splitting system achieves a record hydrogen production rate of 600μmol/(h·cm^(2)).An appropriate Ni/Fe ratio in the SS ensures remarkable oxygen evolution activity,while chromic oxide ensures the effective anticorrosion effect by adjusting the microenvironment of the photoanodes.Moreover,fabricating PEC flow cells with photoanodes coated with SS cocatalysts are a viable strategy for PEC seawater splitting.展开更多
文摘Engineering an efficient interface is a trustworthy strategy for designing advanced photocatalytic systems for solar energy conversion.Herein,oxygen-deficient Bi_(2)WO_(6)atomic layers without organic residues were successfully fabricated via a facile solvothermal strategy by the multifunctional regulatory mechanism of introduced chloridion.Both DFT calculations and speciation determination revealed that chloridion displayed a more pronounced effect in the controllable synthesis of oxygen-deficient Bi_(2)WO_(6)atomic layers without organic residues:ultrathinning and defect-engineering.This built-in multi-cooperative interface endowed Bi_(2)WO_(6)with intriguing photoelectrochemical properties,O_(2) activation ability,and ultrahigh activity in visible-light powered deep oxidation of NO.A reasonable photocatalytic mechanism was proposed based on in situ infrared spectroscopy analysis and theoretical calculations.We believe that this multi-cooperative interface engineering of oxygen-deficient Bi_(2)WO_(6)atomic layers without organic residues could provide new insights into the design of two-dimensional(2D)layered materials with efficient active sites and pave the way for efficient NO photooxidation systems.
基金financially supported by the National Natural Science Foundation of China(22004105)special project of the Marine and Fishery Department of Xiamen(No.19CZB001HJ03)the Training Program of the Outstanding Young Scientific Talents in Fujian(2018-47)
文摘Cubic phase CsPbBr_(3)perovskite nanocrystals(PNCs)was prepared by a high-temperature hot-injection method.The high photoluminescence quantum yield(PLQY)of as-prepared CsPbBr_(3)PNCs was 87%,which can be used for the determination of chloridion in domestic water samples based on their wavelength-shift characteristics via halide exchange.The proposal approach for the determination of chloridion reveals a linear correlation ranged from 10 to 200μM of the chloridion concentration and the wavelength shift of CsPbBr_(3)PNCs with a correlation coe fficient of R^(2)=0.9956.The as-mentioned method reveals neglectable responses towards those co-existing ions in the water aside from chloridion,due to the quick exchange between Cl and Br and the outstanding color change caused by wavelength shift.The strategy has been applied to the determination of chloridion in water samples with the recoveries of 98.9–104.2%and the limit of detection(LOD)of 4μM.These results show that the suggested approach is promising for the development of novel fluorescence detection for chloridion in water.
基金the National Key R&D Program of China(Nos.2021YFA1500804,2022YFA1505200)the National Natural Science Foundation of China(Nos.22121004,51861125104)+2 种基金the Natural Science Foundation of Tianjin City(Nos.18JCJQJC47500,21JCZXJC00060)Haihe Laboratory of Sustainable Chemical Transformations(No.CYZC202107)the Program of Introducing Talents of Discipline to Universities(No.BP0618007)and the Xplorer Prize for financial support。
文摘Photoelectrochemical(PEC)seawater splitting is a promising method for the direct utilization of solar energy and abundant seawater resources for hydrogen production.Photoelectrodes are susceptible to various ions in seawater and complicated competitive reactions,resulting in the failure of photoelectrodes.This paper proposes the design and fabrication of diff erent sputtered stainless steel(SS)fi lms deposited on silicon photoanodes,completely isolating the electrolytes and semiconductor substrate.Upon coupling with the PEC flow cell,the back-illuminated photoanode coated with 316 SS cocatalyst achieves stable operation for 70 h in natural seawater with a highly alkaline KOH(30 wt.%,7.64 mol/L)electrolyte due to the remarkable protection eff ect of the substrate from stainless steel,while the PEC seawater splitting system achieves a record hydrogen production rate of 600μmol/(h·cm^(2)).An appropriate Ni/Fe ratio in the SS ensures remarkable oxygen evolution activity,while chromic oxide ensures the effective anticorrosion effect by adjusting the microenvironment of the photoanodes.Moreover,fabricating PEC flow cells with photoanodes coated with SS cocatalysts are a viable strategy for PEC seawater splitting.