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Ternary Hierarchical Cu <sub/>7</sub> S <sub/>4</sub> /TiO <sub/>2</sub> /CoCr-LDH Heterostructured Nanorod Arrays with Multiphase Reaction Interfaces for More Efficient Photoelectrochemical Water Splitting
摘要： Fabricating hierarchical and highly matched heterostructure with large surface areas and multiple interfaces is an effective approach to enhancing the photoelectrochemical performance. Here, well-aligned hierarchical Cu7S4/TiO2/CoCr-layered double hydroxide (LDH) nanorod arrays are reported, aiming at accelerating charge separation and transfer kinetics. The modifications of Cu7S4 and CoCr-LDH based on TiO2 have endowed the photoanode a surprising enhancement in both ultraviolet light absorption and charge separation efficiency due to highly matched band alignment. The formation of heterojunction is an effective strategy to prevent photocorrosion of Cu7S4 by attaching protective layers on Cu7S4. Moreover, other than the hierarchical morphology with enlarged active surface areas would provide sufficient active sites for the water oxidation processes and pore channels for the gas escaping, owing to the special band alignment of three components, multiple reaction interfaces are produced and involved in the water splitting process, since the photoinduced holes for water oxidation are simultaneously distributed in CoCr-LDH and Cu7S4. As expected, this synergistic effect in this ternary Cu7S4/TiO2/CoCr-LDH heterogeneous photoanode gives rise to a largely enhanced photoconversion efficiency (0.58% at 0.6 V) and photocurrent density (2.04 mA cm?2 at 1.23 V).
关键词： 3D hierarchical nanorod arrays,Cu7S4/TiO2/CoCr-LDH,ternary heterostructure,highly matched band alignment,photoelectrochemical water splitting
更新于2025-09-23 15:21:01
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Strong Lighta??matter Interaction in Au Plasmonic Nanoantennas Coupled with Prussian Blue Catalyst on BiVO4 for Photoelectrochemical Water Splitting
摘要： We establish a facial and large scale compatible fabrication route affording a high performance heterogeneous plasmonic-based photoelectrode for water oxidation that incorporates a CoFe-Prussian blue analog (PBA) structure as the water oxidation catalytic center. For this purpose, an angled deposition of gold (Au) was used to selectively coat the tips of the bismuth vanadate (BiVO4) nanostructures, yielding Au capped BiVO4 (Au-BiVO4). The formation of multiple size/dimension Au capping islands provides strong light-matter interaction at nanoscale dimensions. These plasmonic particles not only enhance light absorption in the bulk BiVO4 (through the excitation of Fabry-Perot (FP) modes) but also contribute to photocurrent generation via the injection of sub-bandgap hot electrons. To substantiate the activity of the photoanodes, the interfacial electron dynamics is significantly improved using a PBA water oxidation catalyst (WOC) resulting in Au-BiVO4/PBA assembly. At 1.23 V vs RHE, the photocurrent value for a bare BiVO4 photoanode was obtained as 190 μA cm?2, while it was boosted to 295 μA cm?2, and 1,800 μA cm?2 for Au-BiVO4, and Au-BiVO4/PBA, respectively. Our results suggest that this simple and facial synthetic approach paves the way for plasmonic-based solar water splitting, in which a variety of common metals and semiconductors can be employed in conjunction with catalyst designs.
关键词： photoelectrochemical water splitting,Prussian blue,plasmonics,hot electron,cyanide chemistry
更新于2025-09-23 15:19:57
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Plasmonic Enhanced Gold Nanoclusters-Based Photoelectrochemical Biosensor for Sensitive Alkaline Phosphatase Activity Analysis
摘要： Low-toxicity gold nanoclusters-decorated Ag@SiO2 (Au NCs-Ag@SiO2) nanocomposites modified plasmonic photoelectrodes were firstly fabricated to improve the photoelectric properties of Au NCs and practical application in biological detection. Through adjusting distance between Au NCs and plasmonic silver nanoparticles (Ag NPs), the photocurrent intensity of Au NCs enhanced by 3.8 times attributed to strong competition between enhancement functions of hot electron transfer, local electric field, light scattering effects and quenching functions of nonradiative energy transfer. Further comparison between experimental results and theoretical simulations were conducted to gain a deeper understanding toward the photoelectric enhancement mechanism. Moreover, Au NCs-Ag@SiO2 nanocomposites was successfully applied to the construction of photoelectrochemical (PEC) biosensors for sensitively detecting alkaline phosphatase activity. This proposed PEC biosensor showed a wide linear range from 0.04 to 400 U·L-1, and a low detection limit of 0.022 U·L-1.
关键词： Alkaline phosphatase,Gold nanoclusters,Photoelectrochemical,Ag@SiO2
更新于2025-09-23 15:19:57
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Bias-Free In Situ H <sub/>2</sub> O <sub/>2</sub> Generation in a Photovoltaic-Photoelectrochemical Tandem Cell for Biocatalytic Oxyfunctionalization
摘要： Peroxygenases catalyze selective oxyfunctionalization of hydrocarbons with high conversion efficiencies using H2O2 as a key cosubstrate. Here, we report an unbiased photoelectrochemical (PEC) tandem structure consisting of a FeOOH/BiVO4 photoanode, a Cu(In,Ga)Se2 solar absorber, and a graphitic carbon nitride/reduced graphene oxide hybrid cathode for light-driven peroxygenase catalysis. Powered by sufficient photovoltage generated by the solar absorber, the PEC platform generates H2O2 in situ through reductive activation of molecular oxygen using water as an electron donor in the absence of external bias. The peroxygenase from Agrocybe aegerita catalyzed the stereoselective hydroxylation of ethylbenzene to (R)-1-phenylethanol with total turnover numbers over 43 300 and high enantioselectivity (ee > 99%) in the unbiased PEC tandem system.
关键词： photoelectrochemical cells,peroxygenases,photovoltaics,biocatalysis,oxyfunctionalization
更新于2025-09-23 15:19:57
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Probing the Advantageous Photosensitization Effect of Metal Nanoclusters over Plasmonic Metal Nanocrystals in Photoelectrochemical Water Splitting
摘要： Atomically precise metal nanoclusters (NCs)-based photocatalytic systems have garnered enormous attention owing to the fascinating merits including unique physicochemical properties, quantum confinement effect and photosensitization effect, which are distinct from conventional metal nanocrystals (NYs). Nevertheless, systematic comparison between electrons photoexcited from metal NCs and hot electrons from surface plasmonic resonance (SPR) effect of metal NYs in boosting photoelectrochemical water splitting reaction remains blank. Here, we report the strict and comprehensive comparison on the capability of electrons photoexcited from glutathione-capped gold nanoclusters (Aux@GSH) and hot electrons from plasmonic excitation of gold nanoparticles (Au NYs) self-transformed from Aux@GSH to trigger the PEC water splitting reaction under visible light irradiation. The results indicate photoelectrons of Aux NCs trigger more efficient charge transport rate than hot electrons of plasmonic Au NYs in terms of light harvesting and conversion efficiency under the identical conditions. Moreover, charge transfer characteristics in Aux NCs and Au NYs-based PEC systems were established. This work would reinforce our deep understanding on these two pivotal sectors of metal nanomaterials for solar energy conversion.
关键词： photosensitization effect,plasmonic metal nanocrystals,charge transfer,photoelectrochemical water splitting,metal nanoclusters
更新于2025-09-23 15:19:57
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Metal-Reduced WO3a??x Electrodes with Tunable Plasmonic Resonance for Enhanced Photoelectrochemical Water Splitting
摘要： Photoelectrochemical (PEC) water splitting is one of the most promising green technologies for producing renewable clean hydrogen energy. Developing plasmonic semiconductors with tunable plasmonic resonance to visible light has drawn increasing attention in view of utilizing abundant low-energy photons for solar-to-chemical conversion. Herein, we demonstrate for the first time that the WO3 electrode can be partly reduced by various metal foils in acid solution, showing strong localized surface plasmon resonance (LSPR) in the visible-to-near-infrared (Vis–NIR) region. The LSPR can be precisely tuned by using metal foils with different standard electrode potentials for different reaction times, and the LSPR peak position strongly depends on the concentration of W5+ in the WO3?x electrodes. A photocurrent density of 0.79 mA·cm?2 at 1.23 VRHE, which is twice that of pristine one, is obtained over an optimally reduced WO3?x electrode. The enhanced PEC water splitting performance is ascribed to the increased light absorption, conductivity and charge carrier concentration.
关键词： photoelectrochemical water splitting,semiconductor,plasmonic resonance,metal foil,tungsten oxide
更新于2025-09-23 15:19:57
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High-Performance Silicon Photoanode Enabled by Oxygen Vacancy Modulation on NiOOH Electrocatalyst for Water Oxidation
摘要： Silicon (Si) is an attractive photoanode material for photoelectrochemical (PEC) water splitting. However, Si photoanode is highly challenging due to its poor stability and catalytic inactivity toward oxygen evolution reaction (OER). Integration of highly active electrocatalysts with Si photoanodes has been considered as an effective strategy to improve OER performance through accelerates reaction kinetics and inhibits Si photocorrosion. In this work, ultra-small NiFe nanoparticles are deposited onto n-Si/Ni/NiOOH surface to improve the activity and stability of Si photoanode by engineering the electrocatalyst and Si interface. Ultra-small NiFe can introduce oxygen vacancies via modulating the local electronic structure of Ni hosts in NiOOH electrocatalyst for fast charge separation and transfer. Besides, NiFe nanoparticles also can serve as co-catalyst exposure more active sites and as protection layer prevents Si photocorrosion. The as-prepared n-Si/Ni/NiOOH/NiFe photoanode exhibits excellent OER activity with an onset potential of 1.0 V versus reversible hydrogen electrode (RHE) and a photocurrent density of ～25.2 mA cm-2 at 1.23 V versus RHE. This work provides a promising approach to design high-performance Si photoanodes by surface electrocatalyst engineering.
关键词： photoelectrochemical water splitting,oxygen vacancies,OER activity,NiFe nanoparticles,Silicon photoanode
更新于2025-09-23 15:19:57
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Dual-photocathode array propelled lab-on-paper ratiometric photoelectrochemical sensing platform for ultrasensitive microRNA bioassay
摘要： In this work, a dual-photocathode array propelled lab-on-paper ratiometric photoelectrochemical (PEC) sensing platform integrated with DNA bridge nanostructure mediated electron-transfer tunneling distance regulation strategy was engineered for ultrasensitive assay of microRNA-141 (miRNA-141). Specifically, the spatial-resolved dual-photocathode array were comprised of a working electrode (PCE1) and internal reference electrode (PCE2), which were responsible for producing independent working signal (Iw) and internal reference signal (Ir). The dual-photocathode array was assembled with cascading multiple photosensitive structures enhanced rigidity remarkably increased the electron-transfer tunneling distance DNA probes from various concentrations of miRNA-141 induced duplex specific output DNA probes produced with a constant concentration of miRNA-141 were (NPs). With the proximity regulation of DNA hairpins H1 and H2, the amplified nanostructures on PCE1 and PCE2. Those formed DNA bridge nanostructures with consisting of pyramid-shaped Cu2O, graphene quantum dots, and AgI nanoparticles introduced onto PCE2, resulting in the formation of different amounts of DNA bridge photocurrent signals were obtained on PCE1 and PCE2. When target existed, the output nuclease-catalyzed target recycling reactions were introduced onto PCE1, while the Iw and constant Ir were ultimately collected. By monitoring the ratio of Iw and Ir, the different amounts of target-induced output DNA probes on PCE1 and PCE2, the variable between the sensing interface and AgI NPs immobilized on the terminals of H1 and H2, leading to noticeably decreased photocurrent signals. Based on the introduction of ultrasensitive bioassay of miRNA-141 was realized with high accuracy, selectivity, and practicability.
关键词： Pyramid-shaped Cu2O,Dual-photocathode array,DNA bridge nanostructure,Photoelectrochemical,Ratiometric
更新于2025-09-23 15:19:57
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Au Quantum Dot/Nickel Tetraminophthalocyanainea??Graphene Oxide-Based Photoelectrochemical Microsensor for Ultrasensitive Epinephrine Detection
摘要： Owing to the importance of epinephrine as a neurotransmitter and hormone, sensitive methods are required for its detection. We have developed a sensitive photoelectrochemical (PEC) microsensor based on gold quantum dots (Au QDs) decorated on a nickel tetraminophthalocyanine?graphene oxide (NiTAPc-Gr) composite. NiTAPc was covalently attached to the surface of graphene oxide to prepare NiTAPc-Gr, which exhibits remarkable stability and PEC performance. In situ growth of Au QDs on the NiTAPc-Gr at room temperature. The synthesized materials were characterized by Fourier transform infrared spectroscopy, ultraviolet?visible spectroscopy, X-ray photoelectron spectroscopy, scanning electron microscopy, transmission electron microscopy, and electrochemical impedance spectroscopy. Au QDs@NiTAPc-Gr provided a much greater photocurrent than NiTAPc-Gr, making it suitable for the ultrasensitive PEC detection of epinephrine. The proposed PEC strategy exhibited a wide linear range of 0.12?243.9 nM with a low detection limit of 17.9 pM (S/N = 3). Additionally, the fabricated PEC sensor showed excellent sensitivity, remarkable stability, and good selectivity. This simple, fast, and low-cost strategy was successfully applied to the analysis of human serum samples, indicating the potential of this method for clinical detection applications.
关键词： photoelectrochemical,graphene oxide,gold quantum dots,epinephrine,nickel tetraminophthalocyanine,microsensor
更新于2025-09-23 15:19:57
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Laser-induced graphene hybrid photoelectrode for enhanced photoelectrochemical detection of glucose
摘要： The combination of electrocatalyst with semiconductor light-absorber is of great importance to increase the efficiency of photoelectrochemical (PEC) glucose detection. Here, in-situ and synchronous fabrication of Ni-based electrocatalyst (NiEC) and CdS semiconductor in laser-induced graphene (LIG) on indium?tin oxide glass is demonstrated via a one-step laser-induced solid phase transition. A series of component and structural characterizations suggest that the laser-induced NiEC uniformly disperses in the hybrid nanocomposite and exists mainly in the form of Ni0 and NiO state. Moreover, both electrochemical and PEC investigations confirm that the as-prepared hybrid photoelectrode exhibits excellent photoelectrocatalytic ability towards glucose, which is not only attributed to the strong synergistic interaction between CdS and NiEC, but also benefited from the high conductivity as well as 3D macroporous configuration of the simultaneously formed LIG, providing the key factor to achieve sensitive non-enzymatic PEC glucose sensors. Therefore, the laser-induced hybrid photoelectrode is then applied to the PEC detection of glucose, and a low detection limit of 0.4 μM is obtained with good stability, reproducibility, and selectivity. This study provides a promising paradigm for the facile and binder-free fabrication of electrocatalyst?semiconductor?graphene hybrid photoelectrode, which will find potential applications in sensitive PEC biosensing for a broad range of analytes.
关键词： nickel electrocatalyst,hybrid nanocomposite,cadmium sulfide,photoelectrochemical sensing,laser-induced graphene,glucose
更新于2025-09-23 15:19:57