The effective separation and utilization of photo-generated carriers are of great significance for promoting the development of photocatalysis,especially in the coupled process of photocatalytic H_(2)production and va...The effective separation and utilization of photo-generated carriers are of great significance for promoting the development of photocatalysis,especially in the coupled process of photocatalytic H_(2)production and valueadded chemicals synthesis.To realize this goal,a sandwichstructured MnO_(2)@ZnIn_(2)S_(4)@Ti_(3)C_(2)hollow sphere was designed and synthesized,in which MnO_(2)and Ti_(3)C_(2)were loaded on the inner and outer surfaces of ZnIn_(2)S_(4),respectively.In the photocatalytic system,MnO_(2)as oxidation cocatalyst and Ti_(3)C_(2)as reduction cocatalyst can serve as photo-generated holes and electrons collectors,respectively,which boost the photo-generated carrier separation and create a spatially separated redox reaction.Furthermore,the unique hollow structure integrated into the photocatalytic system further endows a significant enhancement in light-harvesting ability.Remarkably,the optimal MnO_(2)@ZnIn_(2)S_(4)@Ti_(3)C_(2)hollow sphere exhibits an outstanding the photocatalytic activity for coupled H_(2)production(6.29 mmol g^(-1)h^(-1))and selective benzyl alcohol oxidation to benzaldehyde(5.26 mmol g^(-1)h^(-1)),which is significantly superior to that of ZnIn_(2)S_(4),MnO_(2)@ZnIn_(2)S_(4),and ZnIn_(2)S_(4)@Ti_(3)C_(2).By the in situ irradiated X-ray photoelectron spectroscopy,the result reveals that the spatially separated redox dual-cocatalysts can effectively impel the photo-generated carrier separation.Simultaneously,the intermediates during the benzyl alcohol oxidation process have also been confirmed through in situ electron paramagnetic resonance spectroscopy and diffuse reflectance infrared Fourier transform spectroscopy.This work provides a reference and inspiration for constructing efficient photocatalysts that achieve an efficient coupling of photocatalytic H_(2)production and value-added chemicals synthesis.展开更多
Photosynthesis with the chloroplast works efficiently because of the envelope structure that serves to carry enzymes and to simultaneously maintain the spatial separation of photosynthesis and cellular respiration.Ins...Photosynthesis with the chloroplast works efficiently because of the envelope structure that serves to carry enzymes and to simultaneously maintain the spatial separation of photosynthesis and cellular respiration.Inspired by the spatially separated architecture,a chloroplast-like structured photocatalyst(PdS@CdS@MoS_(2)),in which the PdS and MoS_(2) function as enzymes in the chloroplast and CdS shell functions as the chloroplast envelope,was developed to improve the photocatalytic H_(2) evolution.In this unique nanoscale bionic structure,the poriferous CdS shell enhances light absorption,generates photoinduced carriers,and separates oxidation and reduction reactions.Meanwhile,PdS and MoS_(2) dual cocatalysts enhance the charge separation efficiency through forming a built-in electric field with CdS.We demonstrate that the separation efficiency of carriers,carrier lifetime,and the yield of H_(2) are both higher than that of CdS nanoparticles,evidencing the feasibility of the chloroplast-like structure in enhancing the photocatalyst activity.This work emphasizes the synergism of the three key processes of the photocatalytic reaction by simulating the chloroplast structure and provides a general synthesis strategy,the synthesis of novel structured for photocatalysts for diverse applications in the energy field.展开更多
Narrowband photodetectors conventionally rely on optical structure design orbandpass filters to achieve the narrowband regime. Recently, a strategy forfilterless narrowband photoresponse based on the charge collection...Narrowband photodetectors conventionally rely on optical structure design orbandpass filters to achieve the narrowband regime. Recently, a strategy forfilterless narrowband photoresponse based on the charge collection narrowing(CCN) mechanism was reported. However, the CCN strategy requires an electrically and optically “thick” photoactive layer, which poses challenges in controlling the narrowband photoresponse. Here we propose a novel strategy forconstructing narrowband photodetectors by leveraging the inherent ion migration in perovskites, which we term “band modulation narrowing” (BMN). Bymanipulating the ion migration with external stimuli such as illumination,temperature, and bias voltage, we can regulate in situ the energy-band structure of perovskite photodetectors (PPDs) and hence their spectral response.Combining the Fermi energy levels obtained by the Kelvin probe force microscopy, the internal potential profiles from solar cell capacitance simulator simulation, and the anion accumulation revealed by the transient ion-drifttechnique, we discover two critical mechanisms behind our BMN strategy: theextension of an optically active but electronically dead region proximal to the top electrode and the down-bending energy bands near the electron transportlayer. Our findings offer a case for harnessing the often-annoying ionmigration for developing advanced narrowband PPDs.展开更多
The advantage of spatial phase-shifting shearography is its ability to extract the phase from a single speckle pattern;however,it often faces spectrum overlapping,which seriously affects phase quality.In this paper,we...The advantage of spatial phase-shifting shearography is its ability to extract the phase from a single speckle pattern;however,it often faces spectrum overlapping,which seriously affects phase quality.In this paper,we propose a shearography phase-extraction method based on windowed Fourier ridges,which can effectively extract phase information even in the presence of severe spectrum overlapping.A simple and efficient method was applied to determine the parameters of the windowed Fourier ridges,and a linear variation window was used to match the phase-extraction requirements for different frequency coordinates.A numerical simulation was quantitatively conducted to compare the phase-extraction results of the proposed method with those of the conventional method for various cases,and a shearography system was built with two types of objects to demonstrate the feasibility of the proposed method.展开更多
基金supported by the National Natural Science Foundation of China(52202102,52472215)Key Innovation Project of the Science-Education-Industry Integration Pilot Engineering of Qilu University of Technology(Shandong Academy of Sciences)(2025ZDZX08)+1 种基金Key Research&Development Project of Shandong Province(2024TSGC0222)Interdisciplinary Innovation Guidance Program from Qilu University of Technology(Shandong Academy of Sciences)(2025XKJC0103)。
文摘The effective separation and utilization of photo-generated carriers are of great significance for promoting the development of photocatalysis,especially in the coupled process of photocatalytic H_(2)production and valueadded chemicals synthesis.To realize this goal,a sandwichstructured MnO_(2)@ZnIn_(2)S_(4)@Ti_(3)C_(2)hollow sphere was designed and synthesized,in which MnO_(2)and Ti_(3)C_(2)were loaded on the inner and outer surfaces of ZnIn_(2)S_(4),respectively.In the photocatalytic system,MnO_(2)as oxidation cocatalyst and Ti_(3)C_(2)as reduction cocatalyst can serve as photo-generated holes and electrons collectors,respectively,which boost the photo-generated carrier separation and create a spatially separated redox reaction.Furthermore,the unique hollow structure integrated into the photocatalytic system further endows a significant enhancement in light-harvesting ability.Remarkably,the optimal MnO_(2)@ZnIn_(2)S_(4)@Ti_(3)C_(2)hollow sphere exhibits an outstanding the photocatalytic activity for coupled H_(2)production(6.29 mmol g^(-1)h^(-1))and selective benzyl alcohol oxidation to benzaldehyde(5.26 mmol g^(-1)h^(-1)),which is significantly superior to that of ZnIn_(2)S_(4),MnO_(2)@ZnIn_(2)S_(4),and ZnIn_(2)S_(4)@Ti_(3)C_(2).By the in situ irradiated X-ray photoelectron spectroscopy,the result reveals that the spatially separated redox dual-cocatalysts can effectively impel the photo-generated carrier separation.Simultaneously,the intermediates during the benzyl alcohol oxidation process have also been confirmed through in situ electron paramagnetic resonance spectroscopy and diffuse reflectance infrared Fourier transform spectroscopy.This work provides a reference and inspiration for constructing efficient photocatalysts that achieve an efficient coupling of photocatalytic H_(2)production and value-added chemicals synthesis.
基金supported by the Gansu Provincial Development and Reform Commission(NDRC,No.2013-1336).
文摘Photosynthesis with the chloroplast works efficiently because of the envelope structure that serves to carry enzymes and to simultaneously maintain the spatial separation of photosynthesis and cellular respiration.Inspired by the spatially separated architecture,a chloroplast-like structured photocatalyst(PdS@CdS@MoS_(2)),in which the PdS and MoS_(2) function as enzymes in the chloroplast and CdS shell functions as the chloroplast envelope,was developed to improve the photocatalytic H_(2) evolution.In this unique nanoscale bionic structure,the poriferous CdS shell enhances light absorption,generates photoinduced carriers,and separates oxidation and reduction reactions.Meanwhile,PdS and MoS_(2) dual cocatalysts enhance the charge separation efficiency through forming a built-in electric field with CdS.We demonstrate that the separation efficiency of carriers,carrier lifetime,and the yield of H_(2) are both higher than that of CdS nanoparticles,evidencing the feasibility of the chloroplast-like structure in enhancing the photocatalyst activity.This work emphasizes the synergism of the three key processes of the photocatalytic reaction by simulating the chloroplast structure and provides a general synthesis strategy,the synthesis of novel structured for photocatalysts for diverse applications in the energy field.
基金National Natural Science Foundation of China,Grant/Award Numbers:21972006,22275180,U2001217,22261160370,52202182Shenzhen Peacock plan,Grant/Award Number:KQTD2016053015544057+1 种基金Shenzhen Innovation Fund,Grant/Award Number:JCYJ20220818101018038Natural Sciences and Engineering Research Council of Canada,Grant/Award Number:RGPIN-2020-04239。
文摘Narrowband photodetectors conventionally rely on optical structure design orbandpass filters to achieve the narrowband regime. Recently, a strategy forfilterless narrowband photoresponse based on the charge collection narrowing(CCN) mechanism was reported. However, the CCN strategy requires an electrically and optically “thick” photoactive layer, which poses challenges in controlling the narrowband photoresponse. Here we propose a novel strategy forconstructing narrowband photodetectors by leveraging the inherent ion migration in perovskites, which we term “band modulation narrowing” (BMN). Bymanipulating the ion migration with external stimuli such as illumination,temperature, and bias voltage, we can regulate in situ the energy-band structure of perovskite photodetectors (PPDs) and hence their spectral response.Combining the Fermi energy levels obtained by the Kelvin probe force microscopy, the internal potential profiles from solar cell capacitance simulator simulation, and the anion accumulation revealed by the transient ion-drifttechnique, we discover two critical mechanisms behind our BMN strategy: theextension of an optically active but electronically dead region proximal to the top electrode and the down-bending energy bands near the electron transportlayer. Our findings offer a case for harnessing the often-annoying ionmigration for developing advanced narrowband PPDs.
基金supported by the National Key Research and Development Program of China(No.2016YFF0101803)Hefei Municipal Natural Science Foundation(No.2021017).
文摘The advantage of spatial phase-shifting shearography is its ability to extract the phase from a single speckle pattern;however,it often faces spectrum overlapping,which seriously affects phase quality.In this paper,we propose a shearography phase-extraction method based on windowed Fourier ridges,which can effectively extract phase information even in the presence of severe spectrum overlapping.A simple and efficient method was applied to determine the parameters of the windowed Fourier ridges,and a linear variation window was used to match the phase-extraction requirements for different frequency coordinates.A numerical simulation was quantitatively conducted to compare the phase-extraction results of the proposed method with those of the conventional method for various cases,and a shearography system was built with two types of objects to demonstrate the feasibility of the proposed method.
