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Effect of conduction band potential on cocatalyst-free plasmonic H <sub/>2</sub> evolution over Au loaded on Sr <sup>2+</sup> -doped CeO <sub/>2</sub>
摘要： There is little information on the effect of the conduction band (CB) position on plasmonic hydrogen (H2) formation under visible light irradiation over gold (Au) nanoparticles supported on semiconductors because there were no appropriate materials for which the CB position gradually changes. In this study, we analyzed the flatband potential of strontium ion (Sr2+)-doped cerium(IV) oxide (CeO2:Sr) and found that the CB position gradually shifted negatively from +0.031 V to ?1.49 V vs. NHE with an increase in the Sr2+ mole fraction. Plasmonic photocatalysts consisting of Au nanoparticles, CeO2:Sr and a platinum (Pt) cocatalyst were prepared and characterized by using X-ray diffraction, UV-vis spectroscopy, and transmission electron spectroscopy. Photocatalytic reaction under visible light irradiation revealed that H2 was produced over Au nanoparticles supported on CeO2:Sr having the CB potential of ?0.61 V vs. NHE and that the negative limit of the CB position for electron injection from Au nanoparticles existed between ?0.61 V and ?1.49 V vs. NHE. We found that Au/CeO2:Sr plasmonic photocatalysts also produced H2 without the aid of a Pt cocatalyst due to the sufficiently negative potential of electrons injected into the CB of CeO2:Sr.
关键词： hydrogen evolution,visible light irradiation,gold nanoparticles,plasmonic photocatalysts,strontium-doped cerium oxide
更新于2025-11-19 16:51:07
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Dual Function of Graphene Oxide for Assisted Exfoliation of Black Phosphorus and Electron Shuttle in Promoting Visible and Near-Infrared Photocatalytic H2 Evolution
摘要： The search for suitable photocatalysts with broadband absorption in visible and near-infrared (NIR) region is recognized as one of the most challenging issues on solar energy utilization. Black phosphorous (BP) is demonstrated as an effective visible and NIR activated material in solar energy conversion. However, traditional liquid exfoliation yield is low and the rigid structure and insoluble properties of pristine BP hinder its high-yield of hybridization. Herein, a new and stable noble-metal-free ternary photocatalyst molybdenum disulfide (MoS2)-BP/graphene oxide (GO) was constructed for splitting water to H2, showing dual functions of GO in synthetic and photocatalytic processes. Under visible-NIR light irradiation, the H2 evolution rates of MoS2-BP/GO was enhanced to 3.47 μmol h-1. Rapid electron injection efficiency from excited BP to GO and to MoS2 was confirmed by femtosecond transient absorption spectroscopy. This study provides new insight into the design of nanomaterials, and offers a noble-metal-free protocol with noble-metal-free.
关键词： visible and NIR,hydrogen evolution,graphene oxide,black phosphorous,noble-metal-free
更新于2025-11-19 16:51:07
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Self-generating CeVO4 as conductive channel within CeO2/CeVO4/V2O5 to induce Z-scheme-charge-transfer driven photocatalytic degradation coupled with hydrogen production
摘要： The construction of highly efficient Z-scheme photocatalytic system is regarded as a hot research topic in the fields of environmental remediation and renewable energy production. In this work, a novel Z-scheme CeO2/CeVO4/V2O5 photocatalyst is successfully prepared by using solid phase reaction method. The photocatalytic degradation of organic pollutant (Methylene Blue) with simultaneous hydrogen production is efficiently realized over the prepared Z-scheme CeO2/CeVO4/V2O5 photocatalysts under visible-light irradiation. The effects of treatment temperatures and treatment times of CeO2/V2O5 composite on the photocatalytic performance of Z-scheme CeO2/CeVO4/V2O5 photocatalyst are studied. The as-prepared Z-scheme CeO2/CeVO4/V2O5 (550-3) photocatalyst heat-treated at 550 °C for 3.0 h exhibits the highest photocatalytic performance. It can be ascribed to a moderate amount of CeVO4 nanoparticles generated between CeO2 and V2O5. The generated CeVO4 nanoparticles can be used as effective conductive channel to transfer the photo-generated carriers. At the same time, as redox reaction centers it can further accelerate the transfer of photo-generated electrons, effectively enhancing the separation efficiency of photo-generated electron and hole pairs. Furthermore, cyclic test demonstrates that the as-prepared Z-scheme CeO2/CeVO4/V2O5 (550-3) photocatalyst still maintains a high level of photocatalytic activity within five periods under the same conditions. Moreover, the related photocatalytic mechanism for degradation of organic pollutants with simultaneous hydrogen evolution over the Z-scheme CeO2/CeVO4/V2O5 (550-3) photocatalyst is proposed. Perhaps, this study affords a simple and novel method to design and develop next generation of highly efficient Z-scheme photocatalysts.
关键词： Conductive channel,Z-scheme CeO2/CeVO4/V2O5 photocatalyst,Solid phase reaction method,Simultaneous hydrogen evolution,Visible-light photocatalytic degradation
更新于2025-11-19 16:51:07
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An anti-symmetric dual (ASD) Z-scheme photocatalytic system: (ZnIn2S4/Er3+:Y3Al5O12@ZnTiO3/CaIn2S4) for organic pollutants degradation with simultaneous hydrogen evolution
摘要： An anti-symmetric dual (ASD) Z-scheme ZnIn2S4/Er3+:Y3Al5O12@ZnTiO3/CaIn2S4 photocatalyst was prepared by isoelectric point and calcination methods. The photocatalytic activity is estimated via degradation of Acid Orange II as a target organic contaminant with simultaneous hydrogen evolution under simulated solar-light irradiation. The prepared ASD Z-scheme ZnIn2S4/Er3+:Y3Al5O12@ZnTiO3/CaIn2S4 photocatalyst has a high photocatalytic activity, which can be assigned to the enlarged photoresponse range, increased reduction surface and enhanced separation efficiency of photo-induced carriers. Furthermore, the cyclic experiment proves that the prepared ASD Z-scheme ZnIn2S4/Er3+:Y3Al5O12@ZnTiO3/CaIn2S4 photocatalyst still maintains a high photocatalytic activity within five repetitive cycles. Moreover, the mechanism on photocatalytic degradation of organic pollutants with simultaneous hydrogen evolution caused by ASD Z-scheme ZnIn2S4/Er3+:Y3Al5O12@ZnTiO3/CaIn2S4 photocatalyst is proposed. It is wished that this study could provide a promising pathway for effective degradation and rapid hydrogen production.
关键词： Simultaneous hydrogen evolution,Organic contaminants,Anti-symmetric dual (ASD) Z-scheme photocatalytic system,ZnIn2S4/Er3+:Y3Al5O12@ZnTiO3/CaIn2S4 composite,Up-conversion luminescence agent,Photocatalytic degradation
更新于2025-11-19 16:51:07
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Ultra-small colloidal heavy-metal-free nanoplatelets for efficient hydrogen generation
摘要： Metal chalcogenide semiconducting nanoplatelets exhibit a broad absorption spectrum, as well as thickness-dependent optical and electronic properties. As such, they may be used as building blocks in a variety of optoelectronic devices. The direct synthesis of heavy-metal-free ultra-small sized nanoplatelets is still challenging, due to the inherent limits in existing synthetic approaches. Here, we report an efficient template-assisted cation-exchange route to synthesize heavy metal free metal chalcogenide nanoplatelets that are optically active in the near infrared. The SnSe nanoplatelets, whose lateral dimension is 6-10 nm, exhibit a quantum yield of 20%. The nanoplatelets are applied as light absorbers in a photoelectrochemical (PEC) system for hydrogen generation, leading to a saturated photocurrent density of 7.4 mA/cm2, which is a record for PEC devices using heavy metal-free colloidal quantum dots or nanoplatelets under identical measurement conditions. Our results indicate that quasi-zero-dimensional SnSe nanoplatelets hold great potential as efficient light absorbers for emerging optoelectronic technologies.
关键词： nanoplatelets,cation exchange,optoelectronic technologies,SnSe,hydrogen generation
更新于2025-11-19 16:51:07
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Black phosphorous sensitized TiO <sub/>2</sub> mesocrystals photocatalyst for hydrogen evolution with visible and near-infrared light irradiation
摘要： Wide absorption from ultraviolet (UV) to near-infrared (NIR) region and enhanced charge separation are two main requirements for promising semiconductor photocatalysts. Here, we studied visible-NIR driven photocatalytic hydrogen evolution over black phosphorus nanosheets/TiO2 mesocrystals loaded with Pt heterostructure (BP NS/ Pt (3 wt%)/TMC TMC). BP NS/Pt (3 wt%)/TMC can harvest photons from UV to NIR and simultaneously has enhanced charge separation to increase the generation of electrons for photocatalytic reduction of water. BP NS/Pt (3 wt%)/TMC exhibited photocatalytic H2 evolution rates of 1.9 and 0.41 μmol h-1 under visible (λ> 420 nm (420-1800 nm)) and NIR (λ> 780 nm (780-1800 nm) irradiation, respectively, compared with 0.3 and 0.10 μmol h-1 for BP NS/Pt (3 wt%)/P25. Moreover, a comparative study was made to examine the effect of thickness of BP NS on the photocatalytic H2 evolution. Femtosecond time-resolved diffused reflectance spectroscopy (fs-TRDRS) was integrated together with photoelectrochemical measurement to shed the light on the importance of charge transfer and separation, confirming that decreasing the thickness of BP NS enhances electron injection from BP NS to TMC to increase the photocatalytic activity.
关键词： hydrogen evolution,Black phosphorus,visible-light photocatalyst,charge carriers dynamics,TiO2 mesocrystals,femtosecond time-resolved diffuse reflectance
更新于2025-11-19 16:51:07
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Thiourea-assisted coating of dispersed copper electrocatalysts on Si photocathodes for solar hydrogen production
摘要： Photoelectrochemical water splitting can convert solar energy into clean hydrogen energy for storage. It is desirable to explore non-precious electrocatalysts for practical applications of a photoelectrode in a large scale. Here, we developed a facile spin-coating and in-situ photoelectrochemical reduction method to prepare a dispersed Cu electrocatalyst on a Si photocathode, which improves the performance remarkably. We find that thiourea in the precursor solution for spin-coating plays an important role in obtaining dispersed Cu particles on the surface of a Si photoelectrode. With thiourea in the precursor, the Cu/Si photocathode shows higher performance than the one without thiourea. Moreover, the Cu/Si photocathode also indicates good stability after 16 h illumination.
关键词： In-situ photoelectrochemical reduction,Cu electrocatalyst,Thiourea,Hydrogen evolution reaction
更新于2025-11-19 16:51:07
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A Red Emitting Fluorescent Probe for Imaging Mitochondrial Hydrogen Polysulfide in Living Cells and Tissues
摘要： Hydrogen polysulfide (H2Sn) has attracted increasing attention since H2Sn instead of H2S has been shown to be the actual signaling molecule in physiological and pathological processes. Thus, developing accurate and sensitive assays for H2Sn detection is urgently needed in biological science. In this work, we developed a red emitting mitochondria-targeting fluorescent probe, HQO-PSP, that is capable of tracking H2Sn. With low cytotoxicity, good selectively and high sensitively, HQO-PSP was able to detect H2Sn in living cells. Furthermore, we also demonstrated that HQO-PSP could also be successfully applied to recognize H2Sn in living tissues.
关键词： Hydrogen polysulfide,Fluorescent probe,Lung tissues,Living cells
更新于2025-11-19 16:46:39
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Novel BODIPY-based fluorescent probes with large Stokes shift for imaging hydrogen sulfide
摘要： Hydrogen sulfide has important biomedical significance because it plays a regulatory role in a variety of physiological processes. In our previous work, we investigated the effect of substituents on Stokes shift of BODIPY and found that methoxy groups on phenyl substituents at 3,5-positions could expand the Stokes shift of BODIPY-based probes. In this study, taking hydrogen sulfide (H2S) as analyte, we designed and synthesized 4,4-difluoro-8-{4-(2,4-dinitrophenoxy)phenyl}-3,5-bis(2,4-dimethoxyphenyl)-4-bora-3a,4a-diaza-s-indancene (DMOEPB) and 4,4-difluoro-8-(4-nitrophenyl)-3,5-bis(2,4-dimethoxyphenyl)-4-bora-3a,4a-diaza-s-indancene (DMONPB) according to the same strategy. As expected, Stokes shifts of 49 nm and 51 nm were obtained respectively, which demonstrate the feasibility of the strategy in the synthesis of other fluorescent probes for the detection of small biomolecules. DMONPB can react with H2S to form the derivative with a fluorescence quantum yield of 0.13. An excellent linear relationship was observed in the range of H2S concentrations from 0 μM to 800 μM and the detection limit was 1.3 μM. Furthermore, it can be successfully applied to imaging of H2S in cells and tissues. For DMOEPB, the presence of m-dinitrophenyl did not cause the expected fluorescence quenching, which makes it impossible to perform bioimaging. We speculate that the strong electron-withdrawing property of nitro group is obviously weaker when the two benzene rings are separated at 8-position and are not conjugated with the fluorophore. It provides experience and lessons for designing the same type of turn-on probe.
关键词： hydrogen sulfide,BODIPY,red fluorescence,bioimaging,large Stokes shift
更新于2025-11-19 16:46:39
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Bifunctional gold nanoclusters enable ratiometric fluorescence nanosensing of hydrogen peroxide and glucose
摘要： The accurate quantification of hydrogen peroxide (H2O2) and glucose is essential significance in clinical diagnosis. Herein a selective and sensitive ratiometric fluorescent nanosensor was developed for the determination of H2O2 and glucose by integrating peroxidase–like catalytic and fluorescent bifunctional properties of glutathione protected gold nanoclusters (GSH–AuNCs). The GSH–AuNCs exhibit inherent peroxidase–like activity and accelerate the decomposition of H2O2 into hydroxyl radicals. The produced hydroxyl radicals oxidize terephthalic acid (TA), a typical non–fluorescent substrate of peroxidase, to a highly fluorescent product hydroxyterephthalate (TAOH). Upon excitation with single–wavelength at 315 nm, dual–emission fluorescence peaks were recorded at 430 and 600 nm simultaneously. The fluorescence signal of TAOH at 430 nm continuously increased with increasing the concentration of H2O2 while the fluorescence signal of GSH–AuNCs at 600 nm remained unchangeable. Based upon on these facts, a ratiometric fluorescent nanosensor was fabricated for H2O2 assay with TAOH as response unit and GSH–AuNCs as reference, respectively. By converting glucose into H2O2 with catalytic oxidation of glucose oxidase (GOx), this nanosensor was further exploited for glucose assay. Under the optimum conditions, the detection limits of 10 nmol/L H2O2 and 20 nmol/L glucose were acquired. The relative standard deviations were less than 5% for both H2O2 and glucose (5.0 μmol/L solution, n = 11). The practicability of the nanosensor was verified by the determination of glucose in human serum samples. This nanosensor can be easily expanded as a general platform for the detection of other substances involving H2O2 produced or consumed.
关键词： Intrinsic peroxidase-like activity,Fluorescent gold nanoclusters,Hydrogen peroxide,Glucose,Ratiometric fluorescence,Nanosensor
更新于2025-11-14 17:03:37