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A comparative study on photocatalytic hydrogen evolution activity of synthesis methods of CDs/ZnIn2S4 photocatalysts
摘要： The introduction of carbon materials in photocatalytic systems can significantly enhance the photocatalytic hydrogen evolution activity. Here, we proposed and fabricated carbon nanodots/ZnIn2S4 (CDs/ZIS) samples via three methods. The morphology, chemical elements and valence, and photoelectric properties of CDs/ZIS samples were systematically characterized by SEM, TEM, XPS, UV and PL. The photocatalytic H2 production experiments indicate that the photocatalytic performance of all CDs/ZIS samples has been significantly improved, which could be attributed to the fact that serving as an excellent electron acceptor, CDs can accelerate the separation efficiency of photogenerated electrons and holes. The samples prepared via one-pot hydrothermal method exhibit the optimal photocatalytic activity and the corresponding H2 production rate of 4.15 mmol g?1 h?1 under visible light irradiation (λ > 420 nm), which is about 2.92 times higher than pure ZIS. Our work presented the influence of synthetic method on photoelectric performance and photocatalytic activity of CDs/ZIS nanocomposites, and provided a reliable idea for improving the photocatalytic performance of photocatalyst toward practical applications.
关键词： Synthesis methods,ZnIn2S4,Photocatalytic hydrogen evolution,Carbon dots
更新于2025-11-14 15:29:11
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Stable Hybrid Perovskite MAPb(I1?Br )3 for Photocatalytic Hydrogen Evolution
摘要： Hybrid organic-inorganic perovskites have been pursuing for solar/visible-driven H2 evolution from hydrohalic acid (HX) splitting, but their inherent structural stability and performance are still challenging. Herein, we report on a stable hybrid perovskite MAPb(I1?xBrx)3 (x = 0 – 0.20) obtained by one-pot crystallization in a mixed halide parent solution and its implementation as a newcomer photocatalyst for H2 evolution in aqueous HX solution. MAPb(I1?xBrx)3 is demonstrated to be a superior visible-light-driven photocatalyst for H2 evolution in aqueous HI/HBr solution with no Pt as a cocatalyst. An optimized MAPb(I1?xBrx)3 (x = 0.10) shows a highest H2 evolution rate of 1471 μmol h?1 g?1 under visible light (λ ≥ 420 nm) illumination, which is ~ 40 times higher than that of pure MAPbI3, and the dual-halide perovskite is rather stable showing no obvious decrease in the photocatalytic activity over 60 runs (252 h). The perovskite inherent structural stability is further evidenced by XRD, UV-vis spectra and EDS elemental mapping of MAPb(I1?xBrx)3 measured after cycled photocatalytic reaction. The solar HI splitting efficiency of MAPb(I1?xBrx)3 (x = 0.10) is determined as 1.42%. The mechanism behind photocatalytic H2 evolution enhancement is elucidated by the experimental and computational methods.
关键词： photocatalyst,MAPb(I1?xBrx)3,hydrogen evolution,perovskite,visible light
更新于2025-11-14 15:28:36
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Direct Observation of Structural Evolution of Metal Chalcogenide in Electrocatalytic Water Oxidation
摘要： As one of the most remarkable oxygen evolution reaction (OER) electrocatalysts, metal chalcogenides have been intensively reported due to their high OER activities during the past few decades. It has been reported that electron-chemical conversion of metal chalcogenides into oxides/hydroxides would take place after OER. However, the transition mechanism of such unstable structures, as well as the real active sites and catalytic activity during OER for these electrocatalysts, has not been understood yet, which urgently needs a direct observation for the electrocatalytic water oxidation process, especially at nano or even angstrom scale. In this research, by employing advanced Cs-corrected transmission electron microscopy (TEM), a step by step oxidational evolution of amorphous electrocatalyst CoSx into crystallized CoOOH in OER has been in situ captured: irreversible conversion of CoSx to crystallized CoOOH is initiated on the surface of electrocatalysts with a morphology change via Co(OH)2 intermediate during OER measurement, where CoOOH is confirmed as the real active species. Besides, this transition process has also been confirmed by multiple applications of X-ray photoelectron spectroscopy (XPS), in situ Fourier-transform infrared spectroscopy (FTIR) and other ex situ technologies. Moreover, based on this discovery, a high-efficiency electrocatalyst of a nitrogen-doped graphene foam (NGF) coated by CoSx has been explored through a thorough structure transformation of CoOOH. We believe this in situ and in-depth observation of structural evolution in OER measurement can provide insights into the fundamental understanding of the mechanism for OER catalysts, thus enabling the more rational design of low-cost and high-efficient electrocatalysts for water splitting.
关键词： structural evolution,XPS,in situ TEM,water oxidation,cobalt chalcogenide
更新于2025-11-14 15:27:09
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Construction of dual defect mediated Z-scheme photocatalysts for enhanced photocatalytic hydrogen evolution
摘要： The construction of Z-scheme system is a promising approach for photocatalytic hydrogen evolution (PHE). In this study, we fabricated a direct Z-scheme system consisting of defect-rich g-C3N4 nanosheets (DR-CNNS) crumpled nanosheets with defect-rich TiO2 (DR-TiO2) nanoparticles via a dual defective strategy. The optimized dual-defective rich TiO2/CNNS composite showed a superior PHE rate of ?651.79 μmol/h with a turnover frequency of ?419.3 h?1 as well as high stability and recyclability, which presented the highest value in single defective TiO2 or g-C3N4-based photocatalysts families reported previously. Furthermore, this protocol could also be extended to synthesize other dual defective g-C3N4/oxides (ZnO, SnO2, etc.) heterostructures. The improved photocatalytic performances could be ascribed to the following aspects: (1) rich dual defect, narrowing the band gap and providing more reactive sites for PHE; (2) intimate interface, facilitating interfacial migration and utilization of photogenerated charges; (3) Z-scheme structure, accelerating photogenerated electron-hole pair separation and thus leading to more e?cient PHE. Our work highlights the critical role of defects in construction of Z-scheme system and provides the possibility of utilizing dual defective g-C3N4-based systems for other photocatalytic applications including CO2 reduction and water puri?cation.
关键词： Photocatalytic hydrogen evolution,Dual defect,Oxides/g-C3N4,Heterojunction,Direct Z-scheme
更新于2025-11-14 15:27:09
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Cadmium sulfide nanostructures: Influence of morphology on the photocatalytic degradation of erioglaucine and hydrogen generation
摘要： Size and shape of inorganic materials are known to have great effects on their physical and chemical properties. Here, for the first time we report the visible light driven photocatalytic degradation of erioglaucine – a stable organic dye molecule in the presence of chemically synthesized nanoscale CdS with 1D (nanorods), 2D (nanosheets) and 3D (hierarchical) morphology. Visible light driven photocatalytic degradation efficiency of both 1D and 3D CdS in the removal of erioglaucine are identical. Surprisingly, with 5 min of sonication, the highly crystalline 3D CdS stacked with many thin nanowires containing numerous active surface sites exhibited four-fold enhanced photodegradation efficiency in comparison to 1D and 2D CdS. Scavenger studies revealed that electrons and superoxide radicals are primary reactive species involved in the photodegradation of erioglaucine, while cyclic photodegradation studies revealed the good stability of 3D CdS against photocorrosion. Further, the photocatalytic hydrogen evolution studies also revealed the excellent activity of 3D CdS in comparison to 1D and 2D CdS. Thus, we find that the morphology indeed influences the photocatalytic activity. These results reveal that 3D CdS nanostructures investigated in the present work are efficient photocatalysts that could be fine-tuned for both environmental remediation and hydrogen generation applications.
关键词： erioglaucine,nanostructures,photocatalysis,hydrogen evolution,Cadmium sulfide
更新于2025-11-14 14:48:53
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Gold doping induced strong enhancement of carbon quantum dots fluorescence and oxygen evolution reaction catalytic activity of amorphous cobalt hydroxide
摘要： Gold doping induced strong enhancement of carbon quantum dots fluorescence and oxygen evolution reaction catalytic activity of amorphous cobalt hydroxide. Water splitting using electrocatalysts is expected to provide an alternative green energy source to meet increasing energy demands as well as addressing environmental concerns related to fossil fuels. Herein, we report one-step synthesis of sulfur, nitrogen and Au-doped carbon quantum dots (Au-SCQDs) and strong enhancement of fluorescence intensity and oxygen evolution reaction (OER) catalytic activity of amorphous Co(OH)2 nanoparticles compared to pure Co(OH)2 as well as commercial RuO2 and Pt/C catalysts. Au doping into sulfur and nitrogen co-doped CQDs showed over seventy times enhanced fluorescence. OER studies of amorphous-Co(OH)2 incorporated Au-SCQDs produced current density of 178 mA cm?2 at the applied potential of 2.07 V whereas un-doped Co(OH)2 showed current density of 59 mA cm?2. To produce geometric current density of 10 mA cm?2, amorphous Co(OH)2-Au-SCQDs (CSA) required 388–456 mV overpotential depending on the Au ion concentration used for preparing the Au-SCQDs, which is equal to or lower than overpotential required by commercial electrocatalysts. The strongly enhanced OER activity of Co(OH)2-Au-SCQDs (CSA) was attributed to the presence of electronegative metallic conducting Au atoms along with the high catalytic surface area of amorphous Co(OH)2. The present studies demonstrate a new method of exploiting amorphous Co(OH)2NPs electrocatalysts that could provide more catalytically active sites by integrating an electronegative conducting Au atom doped SCQDs matrix.
关键词： amorphous cobalt hydroxide,fluorescence,water splitting,Gold doping,carbon quantum dots,oxygen evolution reaction,electrocatalysts
更新于2025-10-22 19:40:53
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Surface-to-volume ratio drives photoelelectron injection from nanoscale gold into electrolyte
摘要： Hot charge carriers from plasmonic nanomaterials currently receive increased attention due to their promising potential in important applications such as solar water splitting. While a number of important contributions were made on plasmonic charge carrier generation and their transfer into the metal’s surrounding in the last decades, the local origin of those carriers is still unclear. With our study employing a nanoscaled bicontinous network of nanoporous gold, we take a comprehensive look at both subtopics in one approach and give unprecedented insights into the physical mechanisms controlling the broadband optical absorption and the generation and injection of hot electrons into an adjacent electrolyte where they enhance electrocatalytic hydrogen evolution. This absorption behavior is very different from the well-known localized surface plasmon resonance effects observed in metallic nanoparticles. For small ligament sizes the plasmon decay in our network is strongly enhanced via surface collisions of electrons. These surface collisions are responsible for the energy transfer to the carriers, thus, the creation of hot electrons from a broad spectrum of photon energies. As we reduce the gold ligament sizes below 30 nm, we demonstrate an occurring transition from absorption that is purely exciting 5d-electrons from deep below the Fermi level to an absorption which significantly excites “free” 6sp-electrons to be emitted. We differentiate these processes via assessing the internal quantum efficiency of the gold network photoelectrode as a function of the feature size providing a size-dependent understanding of the hot electron generation and injection processes in nanoscale plasmonic systems. We demonstrate that the surface effect - compared to the volume effect – becomes dominant and leads to significantly improved efficiencies. The most important fact to recognize is that in the surface photoeffect presented here, absorption and electron transfer are both part of the same quantum mechanical event.
关键词： Hot electron,Photoemission,Water splitting,Hydrogen evolution,Carrier injection,Surface damping,Nanoporous Au
更新于2025-10-22 19:40:53
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Zinc ions modified InP quantum dots for enhanced photocatalytic hydrogen evolution from hydrogen sulfide
摘要： Through direct addition of inorganic zinc ions into the solution of indium phosphide quantum dots (InP QDs) at ambient environment, we here present a facile but effective method to modify InP QDs for photocatalytic hydrogen evolution from hydrogen sulfide (H2S). X-ray diffraction patterns and transmission electron microscopic images demonstrate that zinc ions have no significant influence on the crystal structure and morphology of InP QDs, while X-ray photoemission spectra and UV–Vis diffuse and reflectance spectra indicate that zinc ions mainly adsorbed on the surface of InP QDs. Photocatalytic results show the average hydrogen evolution rate has been enhanced to 2.9 times after modification and H2S has indeed involves in the hydrogen evolution process. Steady-state and transient photoluminescence spectra prove that zinc ions could effectively eliminate the surface traps on InP QDs, which is crucial to suppress the recombination of charge carriers. In addition, the electrostatic interaction between zinc ions and the surface sulfide from InP QDs could mitigate the repulsion between QDs and sulfide/hydrosulfide, which may promote the surface oxidative reaction during photocatalysis. This work avoids the traditional harsh and complicated operations required for surface passivation of QDs, which offers a convenient way for optimization of QDs in photocatalysis.
关键词： Hydrogen sulfide,Photocatalytic hydrogen evolution,InP quantum dots,Surface modification
更新于2025-10-22 19:38:57
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Anomalous shape evolution of Ag2O2 nanocrystals modulated by surface adsorbates during electron beam etching
摘要： An understanding of nanocrystal shape evolution is significant for the design, synthesis and applications of nanocrystals with surface-enhanced properties such as catalysis or plasmonics. Surface adsorbates that are selectively attached to certain facets may strongly affect the atomic pathways of nanocrystal shape development. However, it is a great challenge to directly observe such dynamic processes in situ with high spatial resolution. Here, we report the anomalous shape evolution of Ag2O2 nanocrystals modulated by the surface adsorbates of Ag clusters during electron beam etching, which is revealed through in situ transmission electron microscopy (TEM). In contrast to the Ag2O2 nanocrystals without adsorbates, which display the near-equilibrium shape throughout the etching process, Ag2O2 nanocrystals with Ag surface adsorbates show distinct facet development during etching by electron beam irradiation. Three stages of shape changes are observed: a sphere-to-a cube transformation, side etching of a cuboid, and bottom etching underneath the surface adsorbates. We find that the Ag adsorbates modify the Ag2O2 nanocrystal surface configuration by selectively capping the junction between two neighboring facets. They prevent the edge atoms from being etched away and block the diffusion path of surface atoms. Our findings provide critical insights into the modulatory function of surface adsorbates on shape control of nanocrystals.
关键词： surface adsorbates,Ag2O2 nanocrystal,shape evolution,In situ TEM,electron beam etching
更新于2025-09-23 15:23:52
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A heterobimetallic Au(III)?Pt(II) photocatalyst for water reduction to hydrogen
摘要： A supramolecular complex, [Au(C^N^C)(C≡CC6H4C≡C)Pt(terpy)]+, has been synthesized as a photocatalyst for water reduction. This compound consists of a cyclometalated alkyngold(III) photosensitizer and a platinum(II) terpyridine complex bridged through a central phenylethynyl group.
关键词： heterobimetallic system,hydrogen evolution,photocatalyst
更新于2025-09-23 15:23:52