A series of Bi2 S3-BiOCI composites with two-dimensional(2 D) square-like structures were prepared via a two-step anion exchange route.X-ray diffraction(XRD), scanning electron microscopy(SEM), transmission electron m...A series of Bi2 S3-BiOCI composites with two-dimensional(2 D) square-like structures were prepared via a two-step anion exchange route.X-ray diffraction(XRD), scanning electron microscopy(SEM), transmission electron microscopy(TEM), and diffuse reflectance spectra(DRS)were used to investigate the properties of the as-prepared Bi_2 S_3-BiOCI heterostructures. The coupling of BiOCl and Bi_2 S_3 induced enhanced photoabsorption efficiency and bandgap narrowing. A reactive brilliant red X-3 B dye was used as a contaminant to test the photocatalytic activity of the obtained Bi_2 S_3-BiOCl samples under visible light irradiation. The sample Bi_2 S_3-BiOCl with a mass ratio of 8:4 exhibited the highest photodegradation efficiency, which was six times higher than that of pure BiOCl. In addition, a mechanism for the enhancement of photocatalytic activity is proposed.展开更多
Graphitic carbon nitride(g-C_(3)N_(4)) is a fascinating photocatalyst for solar energy utilization in photo-catalysis.Nevertheless,it often suffers from moderate photo-catalytic activity due to its low specific surfac...Graphitic carbon nitride(g-C_(3)N_(4)) is a fascinating photocatalyst for solar energy utilization in photo-catalysis.Nevertheless,it often suffers from moderate photo-catalytic activity due to its low specific surface area and fast recombination rate of photogenerated electrons upon photo-excitation.Herein,we overcome the bottlenecks by constructing a porous g-C_(3)N_(4) nanosheet(PCNS)through a simple thermal oxidation etching method.Benefited from its porous layer structure,the obtained PCNS exhibits large specific surface area,efficient separation of photogenerated charge carriers,as well as high exposure of active sites.As a result,it is robust and universal in visible light-driven dehydrogenation of alcohols in water under oxidant-free condition.Almost quantitative yields(>99%)of various valuable carbonyl compounds were obtained over PCNS,while bulk g-C_(3)N_(4) was far less efficient.Moreover,the photo-catalyst was highly stable and could be facilely recovered from the aqueous system for efficient reuse.The easy preparation and excellent performance made PCNS a promising and competitive photocatalyst for the solar applications.展开更多
The redox active ionic liquid, 1-ethyl-4-(methoxycarbonyl)pyridinium bis(trifluoromethanesulfonyl)amide(RIL), was synthesized from its iodide form by an anion exchange reaction of Li(NTf_2) with viscos liquid(η= 122 ...The redox active ionic liquid, 1-ethyl-4-(methoxycarbonyl)pyridinium bis(trifluoromethanesulfonyl)amide(RIL), was synthesized from its iodide form by an anion exchange reaction of Li(NTf_2) with viscos liquid(η= 122 cP at 25C) and characterized by NMR, IR, and elemental analysis. The compound showed reversible redox couples at -0.65 V and -1.48 V vs. Ag/AgCl and worked as an electron mediator in the B_(12) complex/[Ru(bpy)_3]Cl_2 photosensitizer catalytic system under visible light irradiation. The catalytic efficiency in the RIL was higher than those in DMF, MeOH, and the redox inactive ionic liquid, 1-butyl-3-methyl imidazolium bis(trifluoromethylsulfonyl)amide.展开更多
S-doped Sb_2O_3 nanocrystals were synthesized using SbCl3 and thioacetamide（TAA） as starting materials by a hydrothermal method and the effects of TAA dosage on the composition and properties of resultant nanocrysta...S-doped Sb_2O_3 nanocrystals were synthesized using SbCl3 and thioacetamide（TAA） as starting materials by a hydrothermal method and the effects of TAA dosage on the composition and properties of resultant nanocrystals were determined.Their photocatalytic performance was evaluated using the degradation of methyl orange（MO） as a model reaction.The results suggest that TAA dosage can affect the preferential growth direction of Sb_2O_3,and further influences its photocatalytic activity.S doping can extend the optical absorption edge of Sb_2O_3 to the visible light religion,and thus endows its ability to photocatalyze the degradation of MO under visible light illumination.Based on these results,the correlations between the photocatalytic activity of S-doped Sb_2O_3 and the ratio between exposed facets,specific surface area and crystallographic defects were discussed.展开更多
Light-induced electron transfer can broaden the substrate range of metalloenzyme.However,the efficiency of photo-enzyme coupling is limited by the poor combination of photosensitizer or photocatalyst with enzyme.Herei...Light-induced electron transfer can broaden the substrate range of metalloenzyme.However,the efficiency of photo-enzyme coupling is limited by the poor combination of photosensitizer or photocatalyst with enzyme.Herein,we prepared the nano-photocatalyst MIL-125-NH_(2)@Ru(bpy)by in site embedding ruthenium pyridine-diimine complex[Ru(bpy)_(3)^(2+)into metal organic frameworks MIL-125-NH_(2)and associated it with multicopper oxidase(MCO)laccase.Compared to[Ru(bpy)_(3)]^(2+),the coupling efficiency of MIL-125-NH_(2)@Ru(bpy)_(3)for enzymatic oxygen reduction increased by 35.7%.A series of characterizations confirmed that the amino group of laccase formed chemical bonds with the surface defects or hydrophobic groups of MIL-125-NH_(2)@Ru(bpy)_(3).Consequently,the tight binding accelerated the quenching process and electron transfer between laccase and the immobilized ruthenium pyridine-diimine complex.This work would open an avenue for the synthesis of MOFs photocatalyst towards photo-enzyme coupling.展开更多
The heterogeneous photocatalysis for the oxidative cleavage of C-C bond is significant to the transformation of biomass feedstock.In this work,a heterojunction photocatalyst based on the conductor ZnS and C_(3)N_(4)(C...The heterogeneous photocatalysis for the oxidative cleavage of C-C bond is significant to the transformation of biomass feedstock.In this work,a heterojunction photocatalyst based on the conductor ZnS and C_(3)N_(4)(CN)material is prepared and employed in the aerobic oxidative cleavage reaction of vicinal diol under visible light irradiation.As a result,it is found that 3ZnS/CN catalyst obtained by a mechanical grinding method shows a high photocatalytic activity.In the photocatalytic oxidative cleavage process of 1-phenyl-1,2-glycol,more than 98.7% conversion of substrate with a 96.2% selectivity of benzaldehyde was attained using O_(2) as oxidant.In addition,the photocatalyst recycling experiments exhibited that the 3ZnS/CN catalyst still kept a good activity and stability even after being recycled for 5 times.Finally,the active reaction intermediates were investigated by the control experiments and the relative electron paramagnetic resonance(EPR)detection.According to the obtained results and photocatalytic principle,the mechanism for the selective oxidative transformatioin of 1-phenyl-1,2-glycol has been proposed.It gives a promising approach for the catalytic utilization of biomass-based lignin and cellulose.展开更多
This study developed a novel heterogeneous Vis-Photo+Fenton-like system by integrating visible-light-responsive Co_(3)O_(4)/TiO_(2) photocatalysis with peroxymonosulfate(PMS)activation for efficient atrazine(ATZ)degra...This study developed a novel heterogeneous Vis-Photo+Fenton-like system by integrating visible-light-responsive Co_(3)O_(4)/TiO_(2) photocatalysis with peroxymonosulfate(PMS)activation for efficient atrazine(ATZ)degradation.The synergistic process achieved complete ATZ removal within 60 min under near-neutral pH(6.9),outperform-ing individual Fenton-like(39%)and photocatalytic(24%)processes.Key factors influencing the degradation efficiency included light sources(UV>visible),pH(optimal at 6.9),catalyst dosage(0.01 g Co_(3)O_(4)/TiO_(2)),and PMS:ATZ molar ratio(1:2).The system exhibited a synergistic coefficient of 5.03(degradation)and 1.97(miner-alization),attributed to enhanced radical generation and accelerated Co^(3+)/Co^(2+)redox cycling through photoin-duced electron transfer.Intermediate analysis revealed dealkylation,dechlorination,and oxidation pathways,with reduced toxicity of by-products(e.g.,CEAT,CIAT)confirmed by ecotoxicity assessments.The mineralization efficiency(Vis-Photo+Fenton-like)reached 83.1%,significantly higher than that of standalone processes(Fenton-like:43.2%;photocatalysis:30.5%).The catalyst demonstrated excellent stability(nearly 90%recov-ery,<1μg/L Co leaching)and practical applicability.This study provides an efficient,sludge-free,and solar-compatible strategy for eliminating persistent herbicides in water treatment.展开更多
In the image fusion field,fusing infrared images(IRIs)and visible images(VIs)excelled is a key area.The differences between IRIs and VIs make it challenging to fuse both types into a high-quality image.Accordingly,eff...In the image fusion field,fusing infrared images(IRIs)and visible images(VIs)excelled is a key area.The differences between IRIs and VIs make it challenging to fuse both types into a high-quality image.Accordingly,efficiently combining the advantages of both images while overcoming their shortcomings is necessary.To handle this challenge,we developed an end-to-end IRI andVI fusionmethod based on frequency decomposition and enhancement.By applying concepts from frequency domain analysis,we used the layering mechanism to better capture the salient thermal targets from the IRIs and the rich textural information from the VIs,respectively,significantly boosting the image fusion quality and effectiveness.In addition,the backbone network combined Restormer Blocks and Dense Blocks;Restormer blocks utilize global attention to extract shallow features.Meanwhile,Dense Blocks ensure the integration between shallow and deep features,thereby avoiding the loss of shallow attributes.Extensive experiments on TNO and MSRS datasets demonstrated that the suggested method achieved state-of-the-art(SOTA)performance in various metrics:Entropy(EN),Mutual Information(MI),Standard Deviation(SD),The Structural Similarity Index Measure(SSIM),Fusion quality(Qabf),MI of the pixel(FMI_(pixel)),and modified Visual Information Fidelity(VIF_(m)).展开更多
Image fusion technology aims to generate a more informative single image by integrating complementary information from multi-modal images.Despite the significant progress of deep learning-based fusion methods,existing...Image fusion technology aims to generate a more informative single image by integrating complementary information from multi-modal images.Despite the significant progress of deep learning-based fusion methods,existing algorithms are often limited to single or dual-dimensional feature interactions,thus struggling to fully exploit the profound complementarity between multi-modal images.To address this,this paper proposes a parallel multidimensional complementary fusion network,termed PMCFusion,for the task of infrared and visible image fusion.The core of this method is its unique parallel three-branch fusion module,PTFM,which pioneers the parallel synergistic perception and efficient integration of three distinct dimensions:spatial uncorrelation,channel-wise disparity,and frequency-domain complementarity.Leveraging meticulously designed cross-dimensional attention interactions,PTFM can selectively enhance multi-dimensional features to achieve deep complementarity.Furthermore,to enhance the detail clarity and structural integrity of the fused image,we have designed a dedicated multi-scale high-frequency detail enhancement module,HFDEM.It effectively improves the clarity of the fused image by actively extracting,enhancing,and injecting high-frequency components in a residual manner.The overall model employs a multi-scale architecture and is constrained by corresponding loss functions to ensure efficient and robust fusion across different resolutions.Extensive experimental results demonstrate that the proposed method significantly outperforms current state-of-the-art fusion algorithms in both subjective visual effects and objective evaluation metrics.展开更多
We investigate theoretically and experimentally the chaotic dynamics of visible-wavelength all-fiber ring laser.The100-m 630 HP fibers are used to ensure high non-linearity.A 4-m Pr^(3+)/Yb^(3+)-co-doped ZBLAN fiber p...We investigate theoretically and experimentally the chaotic dynamics of visible-wavelength all-fiber ring laser.The100-m 630 HP fibers are used to ensure high non-linearity.A 4-m Pr^(3+)/Yb^(3+)-co-doped ZBLAN fiber provides the gain.The chaotic laser was pumped by the laser diodes with the maximum power of 150 mW at the wavelength of 850 nm.The peak fluorescence spectrum of Pr^(3+)/Yb^(3+)-co-doped ZBLAN fiber at the wavelength of 635 nm shows that the visiblewavelength fiber laser can be achieved by synergistic energy transfer between Pr~(3+)and Yb^(3+)ions.The chaotic fiber laser is generated by adjusting the pump power,polarization controller and the auto-correlation,permutation entropy,skewness,and kurtosis were used to analyze the characteristics of chaotic laser.The noise-like time series and delta-like auto-correlation curve indicate the chaotic output.The complexity and randomness of time series are analyzed by the permutation entropy,skewness,and kurtosis.The result shows that chaotic dynamics is stable when the pump power exceeds a certain value.The visible chaotic all-fiber laser has high stability and can be applied for real-time monitoring and sensing.We believe that this approach may also be feasible for other materials for emission in the visible range.展开更多
Cross-band camouflage technology is a critical necessity,enabling personnel and equipment to evade detection across evolving surveillance systems,thereby enhancing survivability and mission success.Herein,this work de...Cross-band camouflage technology is a critical necessity,enabling personnel and equipment to evade detection across evolving surveillance systems,thereby enhancing survivability and mission success.Herein,this work develops a layer-structured composite system based on carbon nanotube(CNT)film comprising ionic liquid(IL)interlayer for infrared(IR)modulation and surface-engineered Cu_(2)O nanoparticles for visible camouflage.The CNT/IL/CNT architecture enables reversible IR emissivity switching(Δε≈0.55)through electrically driven ion intercalation/deintercalation within 2 s,while spray-coated Cu_(2)O nanoparticles(100~400 nm diameter)on the top CNT film layer generate rich structure colors with 90%IR transmittance.This spectral-decoupling design overcomes the traditional trade-off between color visibility and IR transmittance observed in pigment-based systems.Remarkably,due to physical interface coupling,the Cu_(2)O-coated layer-structured system maintains exceptional electrical conductivity,enabling simultaneous electromagnetic interference shielding and electrothermal energy conversion.The integrated system demonstrates long-term operational stability.By unifying visible-IR camouflage,electromagnetic protection,and energy management in a lightweight platform,this work provides an important paradigm for cross-band camouflage technologies.展开更多
Light-driven artificial molecular machines[1,2]are a class of functional small molecules powered by photochemical reactions,broadly divided into molecular motors and molecular photoswitches.Molecular motors[3,4],owing...Light-driven artificial molecular machines[1,2]are a class of functional small molecules powered by photochemical reactions,broadly divided into molecular motors and molecular photoswitches.Molecular motors[3,4],owing to their intrinsic point chirality and dynamic axial chirality,undergo unidirectional rotation about a carbon–carbon double bond when irradiated with light.In nature,biological molecular motors and pumps are ubiquitous:driving vision,intracellular transport,energy conversion,signal transduction,muscle contraction,and locomotion.展开更多
In recent years, visible light-driven organic photochemical synthesis has attracted wide research interest from academic and industrial communities due to its features of green and sustainable chemistry. In this flour...In recent years, visible light-driven organic photochemical synthesis has attracted wide research interest from academic and industrial communities due to its features of green and sustainable chemistry. In this flourishing area, Chinese chemists have devoted great efforts to different aspects of synthetic chemistry. This review will summarize their representative work according to the following categories: C–H functionalization, synthesis of aromatic aza-heterocycles, asymmetric organic photochemical synthesis, transformations of small molecules and biomolecule-compatible reactions.展开更多
A visible-light-enabled method for the synthesis ofα-azidoketones has been developed via oxo-azidation of alkenyl silanes with trimethylsilylazide and molecular oxygen under mild conditions.The reaction could be carr...A visible-light-enabled method for the synthesis ofα-azidoketones has been developed via oxo-azidation of alkenyl silanes with trimethylsilylazide and molecular oxygen under mild conditions.The reaction could be carried out in gram scale.Various radical sources,including trifluoromethyl radical,thiocyanate radical,bromide radical,chlorine radical could partici-pate effectively instead of azide radical in the reaction.展开更多
A template-free hydrothermal-assisted thermal polymerization method has been developed for the large-scale synthesis of one-dimensional （1D） graphitic carbon nitride （g-C3N4） microtubes. The g-C3N4 microtubes were...A template-free hydrothermal-assisted thermal polymerization method has been developed for the large-scale synthesis of one-dimensional （1D） graphitic carbon nitride （g-C3N4） microtubes. The g-C3N4 microtubes were obtained by simple thermal polymerization of melamine-cyanuric acid complex microrods under N2 atmosphere, which were synthesized by hydrothermal treatment of melamine solution at 180℃ for 24 h. The as-obtained g-C3N4 microtubes exhibited a large surface area and a unique one-dimensional tubular structure, which provided abundant active sites for proton reduction and also facilitated the electron transfer processes. As such, the g-C3N4 microtubes showed enhanced photocatalytic H2 production activity in lactic acid aqueous solutions under visible light irradiation （A 〉 420 nm）, which was - 3.1 times higher than that of bulk g-C3N4 prepared by direct thermal polymerization of the melamine precursor under the same calcination conditions.展开更多
Several nanoporous Fe2 O3-xSx/S-doped g-C3 N4（CNS） Z-scheme hybrid heterojuctions have been successfully synthesized by one-pot in situ growth of the Fe2O3-xSx particles on the surface of CNS. The characterization r...Several nanoporous Fe2 O3-xSx/S-doped g-C3 N4（CNS） Z-scheme hybrid heterojuctions have been successfully synthesized by one-pot in situ growth of the Fe2O3-xSx particles on the surface of CNS. The characterization results show that S-doping in the g-C3 N4 backbone can greatly enhance the charge mobility and visible light harvesting capability. In addition, porous morphology of hybrid composite provides available open pores for vip molecules and also improves light absorbing property due to existence of multiple scattering effects. More importantly, the Fe2 O3-xSx nanoparticles formed intimate heterojunction with CNS and developed the efficient charge transfer by extending interfacial interactions occurred at the interfaces of both components. It has been found that the Fe2 O3-xSx/CNS composites have an enhanced photocatalytic activity under visible light irradiation compared with isolated Fe2 O3 and CNS components toward the photocatalytic degradation of methylene blue（MB）. The optimal loaded Fe2 O3-xSx value obtained is equal to 6.6 wt% that provided 82% MB photodegradation after 150 min with a reaction rate constant of 0.0092 min（-1） which was faster than those of the pure Fe2 O3（0.0016 min（-1））and CNS（0.0044 min（-1）） under the optimized operating variables acquired by the response surface methodology. The specific surface area and the pore volume of Fe2 O3（6.6）/CNS hybrid are 33.5 m2/g and0.195 cm3/g, which are nearly 3.8 and 7.5 times greater compared with those of the CNS, respectively. The TEM image of Fe2 O3（6.6）/CNS nanocomposite exhibits a nanoporous morphology with abundant uniform pore sizes of around 25 nm. Using the Mott-Schottky plot, the conduction and valence bands of the CNS are measured（at pH = 7） equal to-1.07 and 1.48 V versus normal hydrogen electrode（NHE）, respectively.Trapping tests prove that ·OH-and ·O2-radicals are major active species in the photocatalytic reaction.It has been established that formation of the Z-scheme Fe2 O3（6.6）/CNS heterojunction between CNS and Fe2 O3 directly produces ·OH as well as ·O2-radicals which is consistent with the results obtained from trapping experiments.展开更多
Pathogenic viruses in drinking water are great threats to public health. Visible-lightdriven photocatalysis is a promising technology for virus inactivation. However, the existing photocatalytic antiviral research stu...Pathogenic viruses in drinking water are great threats to public health. Visible-lightdriven photocatalysis is a promising technology for virus inactivation. However, the existing photocatalytic antiviral research studies have mostly been carried out in single-component systems, neglecting the effect of natural organic matter, which exists widely in actual water bodies. In this paper, electrospun Cu-TiO2 nanofibers were prepared as photocatalysts, and their photocatalytic antiviral performance in the presence of humic acid(HA) was comprehensively studied for the first time. The properties of the reaction mixture were measured during the reaction. In addition, the safety, reliability and stability of photocatalytic disinfection in the mixed system were evaluated. The results showed that the virus removal efficiency decreased with the increase of the HA concentration. The type of reaction solution, such as PBS buffer solution or water, did not affect the removal efficiency noticeably. Under acidic conditions, the electrostatic forces between photocatalysts and viruses were strengthened, leading to higher virus removal efficiency. As the reaction time went on, the pH value in the solution increased first and then tended to be stable, the conductivity remained stable, and the dissolved oxygen increased first and then decreased. The safety test showed that the concentration of Cu ions released into the solution was lower than specified by the international standards. No photoreactivation was observed, and the addition of HA significantly reduced the reutilization efficiency of the photocatalysts.展开更多
The existence form and effect of La on the phase composition,morphology,recombination of photocarriers,and optical absorptivity of La-F codoped TiO2 were investigated.Experimental results indicate that all the phase c...The existence form and effect of La on the phase composition,morphology,recombination of photocarriers,and optical absorptivity of La-F codoped TiO2 were investigated.Experimental results indicate that all the phase composition of samples is anatase TiO2,the grain sizes decrease with the increasing of La content The catalysts have a well-defined spherical structure with an average size of 12-14 nm,and the doping elements are uniformly dispersed.Compared with pure TiO2,the absorption edge of La1.5F5-TiO2 red shifts from 388 to 437 nm,accordingly the energy gap(Eg) reduces from 32 to 2.84 eV,Besides,the recombination rate of electron-holes in La1.5F5-TiO2 is the weakest among the prepared samples,and the specific surface area of La1.5F5-TiO2 reaches 105.27 m2/g.The apparent reaction rate constant k of La1.5F5-TiO2 for methylene blue(MB) degradation under visible light obtained from the apparent first-order model achieves 0.0166±0.52 min-1,which is greater than 0.0033±0.09 min 1 of TiO2.Moreover,high-resolution transmission electron microscopy(HRTEM) observation reveals that there coexist La2O3 particles in the co-doped TiO2.展开更多
We demonstrate a bottom-up approach to fabricating a visible light-driven titania photocatalyst device bearing an embeddedtwo-dimensional (2D) array of gold nanoparticles (AuNPs) as a near-field light-generating layer...We demonstrate a bottom-up approach to fabricating a visible light-driven titania photocatalyst device bearing an embeddedtwo-dimensional (2D) array of gold nanoparticles (AuNPs) as a near-field light-generating layer. The device is a layered structureprepared by depositing a 2D array of AuNPs on a transparent conductive substrate (10 nm indium tin oxide (ITO) layer on quartz),coating the 2D array of AuNPs with a monolayer of trimethoxyoctylsilane (TMOS), and depositing titania nanocrystals on the anchoringmolecule (TMOS) layer. The visible light activity of the device was tested using photocatalytic degradation of methylene blue (MB) byilluminating the device with visible light (700 nm light) and ultraviolet (UV) light (250–380 nm). The localized surface plasmonresonance peak of the 36 nm AuNP 2D array is around 700 nm with a full-width at half-maximum of 350 nm. In comparison with othercontrol samples, the device showed the highest photocatalytic activity with visible irradiation, which was 1.7 times higher than that oftitania with UV irradiation. The origin of the visible light activity was confirmed by both quadratic incident light power dependency andaction spectrum to be plasmon-induced (near-field enhancement by AuNPs) two-photon absorption.展开更多
W, N co-doped TiO2 nanoparticles were synthesized by a sol-gel method. The prepared samples were characterized by X-ray diffraction （XRD）, field emission scanning electron microscopy （FE-SEM）, trans- mission elect...W, N co-doped TiO2 nanoparticles were synthesized by a sol-gel method. The prepared samples were characterized by X-ray diffraction （XRD）, field emission scanning electron microscopy （FE-SEM）, trans- mission electron microscopy （TEM）, Fourier transform infrared spectroscopy （FT-1R）, X-ray photoelectron spectroscopy （XPS） and diffuse reflectance spectrophotometry （DRS）. The results showed that the co- doped photocatalysts were essentially uniform spherical particles with the smallest particle size of 22.5 nm. Compared to un-doped TiO2, N-TiO2 and P-25, the absorption edge of the W, N co-doped TiO2 shifted to longer wavelength and its photocatalytic activity for degradation of methyl orange （MO） under Xe-lamp （350W） was higher.展开更多
基金supported by the Natural Science Foundation of Jiangsu Province(Grant No.BK2012464)the Research Fellowship from the Jiangsu Overseas Research and Training Programfunded by the Priority Academic Program Development of Jiangsu Higher Education Institutions(PAPD)
文摘A series of Bi2 S3-BiOCI composites with two-dimensional(2 D) square-like structures were prepared via a two-step anion exchange route.X-ray diffraction(XRD), scanning electron microscopy(SEM), transmission electron microscopy(TEM), and diffuse reflectance spectra(DRS)were used to investigate the properties of the as-prepared Bi_2 S_3-BiOCI heterostructures. The coupling of BiOCl and Bi_2 S_3 induced enhanced photoabsorption efficiency and bandgap narrowing. A reactive brilliant red X-3 B dye was used as a contaminant to test the photocatalytic activity of the obtained Bi_2 S_3-BiOCl samples under visible light irradiation. The sample Bi_2 S_3-BiOCl with a mass ratio of 8:4 exhibited the highest photodegradation efficiency, which was six times higher than that of pure BiOCl. In addition, a mechanism for the enhancement of photocatalytic activity is proposed.
基金financial support provided by the National Natural Science Foundation of China(21676078)the Natural Science Foundation of Hunan Province for Distinguished Young Scholar(2016JJ1013)+1 种基金Scientific Research Fund of Hunan Provincial Education Department(19A323)Science and Technology Planning Project of Hunan Province(2018TP1017)。
文摘Graphitic carbon nitride(g-C_(3)N_(4)) is a fascinating photocatalyst for solar energy utilization in photo-catalysis.Nevertheless,it often suffers from moderate photo-catalytic activity due to its low specific surface area and fast recombination rate of photogenerated electrons upon photo-excitation.Herein,we overcome the bottlenecks by constructing a porous g-C_(3)N_(4) nanosheet(PCNS)through a simple thermal oxidation etching method.Benefited from its porous layer structure,the obtained PCNS exhibits large specific surface area,efficient separation of photogenerated charge carriers,as well as high exposure of active sites.As a result,it is robust and universal in visible light-driven dehydrogenation of alcohols in water under oxidant-free condition.Almost quantitative yields(>99%)of various valuable carbonyl compounds were obtained over PCNS,while bulk g-C_(3)N_(4) was far less efficient.Moreover,the photo-catalyst was highly stable and could be facilely recovered from the aqueous system for efficient reuse.The easy preparation and excellent performance made PCNS a promising and competitive photocatalyst for the solar applications.
基金partially supported by JSPS KAKENHI Grant Number 18H04265 in Precisely Designed Catalysts with Customized Scaffolding and Grant Number JP16H04119by JSPS and PAN under the Research Cooperative Program Grant Number AJ180081 (30-0004-04)a Grant from the Nippon Sheet Glass Foundation (HAKF541800)
文摘The redox active ionic liquid, 1-ethyl-4-(methoxycarbonyl)pyridinium bis(trifluoromethanesulfonyl)amide(RIL), was synthesized from its iodide form by an anion exchange reaction of Li(NTf_2) with viscos liquid(η= 122 cP at 25C) and characterized by NMR, IR, and elemental analysis. The compound showed reversible redox couples at -0.65 V and -1.48 V vs. Ag/AgCl and worked as an electron mediator in the B_(12) complex/[Ru(bpy)_3]Cl_2 photosensitizer catalytic system under visible light irradiation. The catalytic efficiency in the RIL was higher than those in DMF, MeOH, and the redox inactive ionic liquid, 1-butyl-3-methyl imidazolium bis(trifluoromethylsulfonyl)amide.
基金supported by the National Natural Science Foundation of China(21307012)Educational Commission of Fujian Province(JK2013007,2014J01035,JA15138)
文摘S-doped Sb_2O_3 nanocrystals were synthesized using SbCl3 and thioacetamide（TAA） as starting materials by a hydrothermal method and the effects of TAA dosage on the composition and properties of resultant nanocrystals were determined.Their photocatalytic performance was evaluated using the degradation of methyl orange（MO） as a model reaction.The results suggest that TAA dosage can affect the preferential growth direction of Sb_2O_3,and further influences its photocatalytic activity.S doping can extend the optical absorption edge of Sb_2O_3 to the visible light religion,and thus endows its ability to photocatalyze the degradation of MO under visible light illumination.Based on these results,the correlations between the photocatalytic activity of S-doped Sb_2O_3 and the ratio between exposed facets,specific surface area and crystallographic defects were discussed.
基金supported by the National Natural Science Foundation of China (No.21906078)the Central Public-Interest Scientific Institution Basal Research Fund of China (No.PM-zx703–202204–104)the Gusu Innovation and Entrepreneurship Leading Talent Plan (No.ZXL2022500)。
文摘Light-induced electron transfer can broaden the substrate range of metalloenzyme.However,the efficiency of photo-enzyme coupling is limited by the poor combination of photosensitizer or photocatalyst with enzyme.Herein,we prepared the nano-photocatalyst MIL-125-NH_(2)@Ru(bpy)by in site embedding ruthenium pyridine-diimine complex[Ru(bpy)_(3)^(2+)into metal organic frameworks MIL-125-NH_(2)and associated it with multicopper oxidase(MCO)laccase.Compared to[Ru(bpy)_(3)]^(2+),the coupling efficiency of MIL-125-NH_(2)@Ru(bpy)_(3)for enzymatic oxygen reduction increased by 35.7%.A series of characterizations confirmed that the amino group of laccase formed chemical bonds with the surface defects or hydrophobic groups of MIL-125-NH_(2)@Ru(bpy)_(3).Consequently,the tight binding accelerated the quenching process and electron transfer between laccase and the immobilized ruthenium pyridine-diimine complex.This work would open an avenue for the synthesis of MOFs photocatalyst towards photo-enzyme coupling.
基金financially supported by the General Program of NSFC(21878235).
文摘The heterogeneous photocatalysis for the oxidative cleavage of C-C bond is significant to the transformation of biomass feedstock.In this work,a heterojunction photocatalyst based on the conductor ZnS and C_(3)N_(4)(CN)material is prepared and employed in the aerobic oxidative cleavage reaction of vicinal diol under visible light irradiation.As a result,it is found that 3ZnS/CN catalyst obtained by a mechanical grinding method shows a high photocatalytic activity.In the photocatalytic oxidative cleavage process of 1-phenyl-1,2-glycol,more than 98.7% conversion of substrate with a 96.2% selectivity of benzaldehyde was attained using O_(2) as oxidant.In addition,the photocatalyst recycling experiments exhibited that the 3ZnS/CN catalyst still kept a good activity and stability even after being recycled for 5 times.Finally,the active reaction intermediates were investigated by the control experiments and the relative electron paramagnetic resonance(EPR)detection.According to the obtained results and photocatalytic principle,the mechanism for the selective oxidative transformatioin of 1-phenyl-1,2-glycol has been proposed.It gives a promising approach for the catalytic utilization of biomass-based lignin and cellulose.
基金supported by the Financial Supports of the National Natural Science Foundation of China(Nos.51508056,52370030 and 42007352)the Chongqing Postgraduate Joint Training Base Project(No.JDLHPYJD2022005)the special fund of Henan Key Labora-tory of Water Pollution Control and Rehabilitation Technology(No.CJSZ2024001).
文摘This study developed a novel heterogeneous Vis-Photo+Fenton-like system by integrating visible-light-responsive Co_(3)O_(4)/TiO_(2) photocatalysis with peroxymonosulfate(PMS)activation for efficient atrazine(ATZ)degradation.The synergistic process achieved complete ATZ removal within 60 min under near-neutral pH(6.9),outperform-ing individual Fenton-like(39%)and photocatalytic(24%)processes.Key factors influencing the degradation efficiency included light sources(UV>visible),pH(optimal at 6.9),catalyst dosage(0.01 g Co_(3)O_(4)/TiO_(2)),and PMS:ATZ molar ratio(1:2).The system exhibited a synergistic coefficient of 5.03(degradation)and 1.97(miner-alization),attributed to enhanced radical generation and accelerated Co^(3+)/Co^(2+)redox cycling through photoin-duced electron transfer.Intermediate analysis revealed dealkylation,dechlorination,and oxidation pathways,with reduced toxicity of by-products(e.g.,CEAT,CIAT)confirmed by ecotoxicity assessments.The mineralization efficiency(Vis-Photo+Fenton-like)reached 83.1%,significantly higher than that of standalone processes(Fenton-like:43.2%;photocatalysis:30.5%).The catalyst demonstrated excellent stability(nearly 90%recov-ery,<1μg/L Co leaching)and practical applicability.This study provides an efficient,sludge-free,and solar-compatible strategy for eliminating persistent herbicides in water treatment.
基金funded by Anhui Province University Key Science and Technology Project(2024AH053415)Anhui Province University Major Science and Technology Project(2024AH040229)+3 种基金Talent Research Initiation Fund Project of Tongling University(2024tlxyrc019)Tongling University School-Level Scientific Research Project(2024tlxyptZD07)TheUniversity Synergy Innovation Programof Anhui Province(GXXT-2023-050)Tongling City Science and Technology Major Special Project(Unveiling and Commanding Model)(200401JB004).
文摘In the image fusion field,fusing infrared images(IRIs)and visible images(VIs)excelled is a key area.The differences between IRIs and VIs make it challenging to fuse both types into a high-quality image.Accordingly,efficiently combining the advantages of both images while overcoming their shortcomings is necessary.To handle this challenge,we developed an end-to-end IRI andVI fusionmethod based on frequency decomposition and enhancement.By applying concepts from frequency domain analysis,we used the layering mechanism to better capture the salient thermal targets from the IRIs and the rich textural information from the VIs,respectively,significantly boosting the image fusion quality and effectiveness.In addition,the backbone network combined Restormer Blocks and Dense Blocks;Restormer blocks utilize global attention to extract shallow features.Meanwhile,Dense Blocks ensure the integration between shallow and deep features,thereby avoiding the loss of shallow attributes.Extensive experiments on TNO and MSRS datasets demonstrated that the suggested method achieved state-of-the-art(SOTA)performance in various metrics:Entropy(EN),Mutual Information(MI),Standard Deviation(SD),The Structural Similarity Index Measure(SSIM),Fusion quality(Qabf),MI of the pixel(FMI_(pixel)),and modified Visual Information Fidelity(VIF_(m)).
基金supported in part by the Funds for Central-Guided Local Science&Technology Development(Grant No.202407AC110005)Key Technologies for the Construction of a Whole-Process Intelligent Service System for Neuroendocrine Neoplasmin part by the Xingdian Talent Project of Yunnan Province.The key technology research and application of cross-domain automatic business collaboration in smart tourism(XYYC-CYCX-2022-0005)in part by the Yunnan Province Zhangjun ExpertWorkstation(No.202205AF150081).
文摘Image fusion technology aims to generate a more informative single image by integrating complementary information from multi-modal images.Despite the significant progress of deep learning-based fusion methods,existing algorithms are often limited to single or dual-dimensional feature interactions,thus struggling to fully exploit the profound complementarity between multi-modal images.To address this,this paper proposes a parallel multidimensional complementary fusion network,termed PMCFusion,for the task of infrared and visible image fusion.The core of this method is its unique parallel three-branch fusion module,PTFM,which pioneers the parallel synergistic perception and efficient integration of three distinct dimensions:spatial uncorrelation,channel-wise disparity,and frequency-domain complementarity.Leveraging meticulously designed cross-dimensional attention interactions,PTFM can selectively enhance multi-dimensional features to achieve deep complementarity.Furthermore,to enhance the detail clarity and structural integrity of the fused image,we have designed a dedicated multi-scale high-frequency detail enhancement module,HFDEM.It effectively improves the clarity of the fused image by actively extracting,enhancing,and injecting high-frequency components in a residual manner.The overall model employs a multi-scale architecture and is constrained by corresponding loss functions to ensure efficient and robust fusion across different resolutions.Extensive experimental results demonstrate that the proposed method significantly outperforms current state-of-the-art fusion algorithms in both subjective visual effects and objective evaluation metrics.
基金Project supported by the National Natural Science Foundation of China(Grant Nos.61975141,61575137,and61675144)。
文摘We investigate theoretically and experimentally the chaotic dynamics of visible-wavelength all-fiber ring laser.The100-m 630 HP fibers are used to ensure high non-linearity.A 4-m Pr^(3+)/Yb^(3+)-co-doped ZBLAN fiber provides the gain.The chaotic laser was pumped by the laser diodes with the maximum power of 150 mW at the wavelength of 850 nm.The peak fluorescence spectrum of Pr^(3+)/Yb^(3+)-co-doped ZBLAN fiber at the wavelength of 635 nm shows that the visiblewavelength fiber laser can be achieved by synergistic energy transfer between Pr~(3+)and Yb^(3+)ions.The chaotic fiber laser is generated by adjusting the pump power,polarization controller and the auto-correlation,permutation entropy,skewness,and kurtosis were used to analyze the characteristics of chaotic laser.The noise-like time series and delta-like auto-correlation curve indicate the chaotic output.The complexity and randomness of time series are analyzed by the permutation entropy,skewness,and kurtosis.The result shows that chaotic dynamics is stable when the pump power exceeds a certain value.The visible chaotic all-fiber laser has high stability and can be applied for real-time monitoring and sensing.We believe that this approach may also be feasible for other materials for emission in the visible range.
基金Financial support from the National Nature Science Foundation of China(No.:52373244)the Foundation of National Science and Technology Key Laboratory(No.:KZ571801)。
文摘Cross-band camouflage technology is a critical necessity,enabling personnel and equipment to evade detection across evolving surveillance systems,thereby enhancing survivability and mission success.Herein,this work develops a layer-structured composite system based on carbon nanotube(CNT)film comprising ionic liquid(IL)interlayer for infrared(IR)modulation and surface-engineered Cu_(2)O nanoparticles for visible camouflage.The CNT/IL/CNT architecture enables reversible IR emissivity switching(Δε≈0.55)through electrically driven ion intercalation/deintercalation within 2 s,while spray-coated Cu_(2)O nanoparticles(100~400 nm diameter)on the top CNT film layer generate rich structure colors with 90%IR transmittance.This spectral-decoupling design overcomes the traditional trade-off between color visibility and IR transmittance observed in pigment-based systems.Remarkably,due to physical interface coupling,the Cu_(2)O-coated layer-structured system maintains exceptional electrical conductivity,enabling simultaneous electromagnetic interference shielding and electrothermal energy conversion.The integrated system demonstrates long-term operational stability.By unifying visible-IR camouflage,electromagnetic protection,and energy management in a lightweight platform,this work provides an important paradigm for cross-band camouflage technologies.
文摘Light-driven artificial molecular machines[1,2]are a class of functional small molecules powered by photochemical reactions,broadly divided into molecular motors and molecular photoswitches.Molecular motors[3,4],owing to their intrinsic point chirality and dynamic axial chirality,undergo unidirectional rotation about a carbon–carbon double bond when irradiated with light.In nature,biological molecular motors and pumps are ubiquitous:driving vision,intracellular transport,energy conversion,signal transduction,muscle contraction,and locomotion.
基金supported by the National Natural Science Foundation of China(21772052,21772053,21772129,21801176,21672099,21732003)Chinese Academy of Sciences(XDB20020200)
文摘In recent years, visible light-driven organic photochemical synthesis has attracted wide research interest from academic and industrial communities due to its features of green and sustainable chemistry. In this flourishing area, Chinese chemists have devoted great efforts to different aspects of synthetic chemistry. This review will summarize their representative work according to the following categories: C–H functionalization, synthesis of aromatic aza-heterocycles, asymmetric organic photochemical synthesis, transformations of small molecules and biomolecule-compatible reactions.
文摘A visible-light-enabled method for the synthesis ofα-azidoketones has been developed via oxo-azidation of alkenyl silanes with trimethylsilylazide and molecular oxygen under mild conditions.The reaction could be carried out in gram scale.Various radical sources,including trifluoromethyl radical,thiocyanate radical,bromide radical,chlorine radical could partici-pate effectively instead of azide radical in the reaction.
文摘A template-free hydrothermal-assisted thermal polymerization method has been developed for the large-scale synthesis of one-dimensional （1D） graphitic carbon nitride （g-C3N4） microtubes. The g-C3N4 microtubes were obtained by simple thermal polymerization of melamine-cyanuric acid complex microrods under N2 atmosphere, which were synthesized by hydrothermal treatment of melamine solution at 180℃ for 24 h. The as-obtained g-C3N4 microtubes exhibited a large surface area and a unique one-dimensional tubular structure, which provided abundant active sites for proton reduction and also facilitated the electron transfer processes. As such, the g-C3N4 microtubes showed enhanced photocatalytic H2 production activity in lactic acid aqueous solutions under visible light irradiation （A 〉 420 nm）, which was - 3.1 times higher than that of bulk g-C3N4 prepared by direct thermal polymerization of the melamine precursor under the same calcination conditions.
基金financial supports from the Research Office of Amirkabir University of Technology (Tehran Polytechnic)
文摘Several nanoporous Fe2 O3-xSx/S-doped g-C3 N4（CNS） Z-scheme hybrid heterojuctions have been successfully synthesized by one-pot in situ growth of the Fe2O3-xSx particles on the surface of CNS. The characterization results show that S-doping in the g-C3 N4 backbone can greatly enhance the charge mobility and visible light harvesting capability. In addition, porous morphology of hybrid composite provides available open pores for vip molecules and also improves light absorbing property due to existence of multiple scattering effects. More importantly, the Fe2 O3-xSx nanoparticles formed intimate heterojunction with CNS and developed the efficient charge transfer by extending interfacial interactions occurred at the interfaces of both components. It has been found that the Fe2 O3-xSx/CNS composites have an enhanced photocatalytic activity under visible light irradiation compared with isolated Fe2 O3 and CNS components toward the photocatalytic degradation of methylene blue（MB）. The optimal loaded Fe2 O3-xSx value obtained is equal to 6.6 wt% that provided 82% MB photodegradation after 150 min with a reaction rate constant of 0.0092 min（-1） which was faster than those of the pure Fe2 O3（0.0016 min（-1））and CNS（0.0044 min（-1）） under the optimized operating variables acquired by the response surface methodology. The specific surface area and the pore volume of Fe2 O3（6.6）/CNS hybrid are 33.5 m2/g and0.195 cm3/g, which are nearly 3.8 and 7.5 times greater compared with those of the CNS, respectively. The TEM image of Fe2 O3（6.6）/CNS nanocomposite exhibits a nanoporous morphology with abundant uniform pore sizes of around 25 nm. Using the Mott-Schottky plot, the conduction and valence bands of the CNS are measured（at pH = 7） equal to-1.07 and 1.48 V versus normal hydrogen electrode（NHE）, respectively.Trapping tests prove that ·OH-and ·O2-radicals are major active species in the photocatalytic reaction.It has been established that formation of the Z-scheme Fe2 O3（6.6）/CNS heterojunction between CNS and Fe2 O3 directly produces ·OH as well as ·O2-radicals which is consistent with the results obtained from trapping experiments.
基金supported by grants from the National Natural Science Foundation of China(Nos.51778618,51478460)
文摘Pathogenic viruses in drinking water are great threats to public health. Visible-lightdriven photocatalysis is a promising technology for virus inactivation. However, the existing photocatalytic antiviral research studies have mostly been carried out in single-component systems, neglecting the effect of natural organic matter, which exists widely in actual water bodies. In this paper, electrospun Cu-TiO2 nanofibers were prepared as photocatalysts, and their photocatalytic antiviral performance in the presence of humic acid(HA) was comprehensively studied for the first time. The properties of the reaction mixture were measured during the reaction. In addition, the safety, reliability and stability of photocatalytic disinfection in the mixed system were evaluated. The results showed that the virus removal efficiency decreased with the increase of the HA concentration. The type of reaction solution, such as PBS buffer solution or water, did not affect the removal efficiency noticeably. Under acidic conditions, the electrostatic forces between photocatalysts and viruses were strengthened, leading to higher virus removal efficiency. As the reaction time went on, the pH value in the solution increased first and then tended to be stable, the conductivity remained stable, and the dissolved oxygen increased first and then decreased. The safety test showed that the concentration of Cu ions released into the solution was lower than specified by the international standards. No photoreactivation was observed, and the addition of HA significantly reduced the reutilization efficiency of the photocatalysts.
基金Project supported by the Natural Science Foundation of China(21407084,51474133)
文摘The existence form and effect of La on the phase composition,morphology,recombination of photocarriers,and optical absorptivity of La-F codoped TiO2 were investigated.Experimental results indicate that all the phase composition of samples is anatase TiO2,the grain sizes decrease with the increasing of La content The catalysts have a well-defined spherical structure with an average size of 12-14 nm,and the doping elements are uniformly dispersed.Compared with pure TiO2,the absorption edge of La1.5F5-TiO2 red shifts from 388 to 437 nm,accordingly the energy gap(Eg) reduces from 32 to 2.84 eV,Besides,the recombination rate of electron-holes in La1.5F5-TiO2 is the weakest among the prepared samples,and the specific surface area of La1.5F5-TiO2 reaches 105.27 m2/g.The apparent reaction rate constant k of La1.5F5-TiO2 for methylene blue(MB) degradation under visible light obtained from the apparent first-order model achieves 0.0166±0.52 min-1,which is greater than 0.0033±0.09 min 1 of TiO2.Moreover,high-resolution transmission electron microscopy(HRTEM) observation reveals that there coexist La2O3 particles in the co-doped TiO2.
基金We thank the Japan Society for the Promotion of Science and the Ministry of Education,Culture,Sports,Science and Technology of Japan for financial supportGrant-in-Aid for Challenging Exploratory Research(KM,24656040)+4 种基金Grant-in-Aid for Scientific Research on Innovative Areas‘Integrated Organic Synthesis’(KM,22106545 and 24106746)Grant-inAid for Young Scientists(KI,30455274)Japan Science and Technology Agency for financial support of e-ASIA JRPsupported by the Research Foundation for Opto-Science and Technologyby Grant for Environmental Research Projects from The Sumitomo Foundation and the Collaborative Research Program of the Institute for Chemical Research,Kyoto University(grant 2012-14)
文摘We demonstrate a bottom-up approach to fabricating a visible light-driven titania photocatalyst device bearing an embeddedtwo-dimensional (2D) array of gold nanoparticles (AuNPs) as a near-field light-generating layer. The device is a layered structureprepared by depositing a 2D array of AuNPs on a transparent conductive substrate (10 nm indium tin oxide (ITO) layer on quartz),coating the 2D array of AuNPs with a monolayer of trimethoxyoctylsilane (TMOS), and depositing titania nanocrystals on the anchoringmolecule (TMOS) layer. The visible light activity of the device was tested using photocatalytic degradation of methylene blue (MB) byilluminating the device with visible light (700 nm light) and ultraviolet (UV) light (250–380 nm). The localized surface plasmonresonance peak of the 36 nm AuNP 2D array is around 700 nm with a full-width at half-maximum of 350 nm. In comparison with othercontrol samples, the device showed the highest photocatalytic activity with visible irradiation, which was 1.7 times higher than that oftitania with UV irradiation. The origin of the visible light activity was confirmed by both quadratic incident light power dependency andaction spectrum to be plasmon-induced (near-field enhancement by AuNPs) two-photon absorption.
文摘W, N co-doped TiO2 nanoparticles were synthesized by a sol-gel method. The prepared samples were characterized by X-ray diffraction （XRD）, field emission scanning electron microscopy （FE-SEM）, trans- mission electron microscopy （TEM）, Fourier transform infrared spectroscopy （FT-1R）, X-ray photoelectron spectroscopy （XPS） and diffuse reflectance spectrophotometry （DRS）. The results showed that the co- doped photocatalysts were essentially uniform spherical particles with the smallest particle size of 22.5 nm. Compared to un-doped TiO2, N-TiO2 and P-25, the absorption edge of the W, N co-doped TiO2 shifted to longer wavelength and its photocatalytic activity for degradation of methyl orange （MO） under Xe-lamp （350W） was higher.
