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Band structure tuning and charge separation of MNX monolayers and MNX/GaS van der Waals heterostructures
摘要： Efficient charge separation and band structure tuning are very important for application to photoelectric device. Here, based on first-principles calculations, we propose two-dimensional (2D) MNX (M=Zr, Hf; X=Cl, Br, I) monolayers which can be exfoliated from the corresponding layered bulk phase due to the low cleavage energy. The phonon band structure and the mechanical analysis indicate that 2D MNX monolayers can form free-standing membranes. The calculated results suggest that 2D MNX monolayers are indirect band gap semiconductors with band gaps in the range of 1.55-3.37 eV. Among them, MNI (M=Zr, Hf) monolayers with effective charge separation and moderate band gaps would have potential application to photocatalytic water splitting. In order to realize the effective charge separation for the other MNX monolayers, MNX/GaS (X=Cl, Br) heterostructures are investigated. Our calculations reveal that MNX/GaS heterostructures are typical type-II band alignment, facilitating the separation of photogenerated carriers where electrons and holes are localized in MNX and GaS monolayers, respectively. Furthermore, the band gaps of the MNX/GaS heterostructures are obviously narrowed compared to those of the isolated constituent monolayers. In addition, the band gaps and band edge positions of MNX/GaS heterostructures can further be tuned by biaxial strain to match better with the redox potentials of water. These findings in this study not only enrich the family of 2D materials, but also demonstrate that MNI (M=Zr, Hf) monolayers and MNX/GaS heterostructures are promising candidates for photocatalytic materials.
关键词： van der Waals heterostructures,photocatalytic water splitting,band structure tuning,MNX monolayers,charge separation
更新于2025-09-04 15:30:14
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The Middle Road Less Taken: Electronic-Structure-Inspired Design of Hybrid Photocatalytic Platforms for Solar Fuel Generation
摘要： The development of efficient solar energy conversion to augment other renewable energy approaches is one of the grand challenges of our time. Water splitting, or the disproportionation of H2O into energy-dense fuels, H2 and O2, is undoubtedly a promising strategy. Solar water splitting involves the concerted transfer of four electrons and four protons, which requires the synergistic operation of solar light harvesting, charge separation, mass and charge transport, and redox catalysis processes. It is unlikely that individual materials can mediate the entire sequence of charge and mass transport as well as energy conversion processes necessary for photocatalytic water splitting. An alternative approach, emulating the functioning of photosynthetic systems, involves the utilization of hybrid systems wherein different components perform the various functions required for solar water splitting. The design of such hybrid systems requires the multiple components to operate in lockstep with optimal thermodynamic driving forces and interfacial charge transfer kinetics.
关键词： hybrid systems,water splitting,photocatalytic,charge transfer,solar energy conversion
更新于2025-09-04 15:30:14
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A porous Ni-O/Ni/Si photoanode for stable and efficient photoelectrochemical water splitting
摘要： Excellent photoelectrochemical activity was demonstrated for an easily prepared porous Ni-O/Ni/Si photoanode with an onset potential of 0.93 VRHE, a photocurrent of 39.7 mA cm?2 at 1.23 VRHE, an energy conversion efficiency of 3.2% and a stability above 100 h.
关键词： stability,water splitting,porous Ni-O/Ni/Si photoanode,energy conversion efficiency,photoelectrochemical
更新于2025-09-04 15:30:14
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<i>In situ</i> topotactic fabrication of direct Z-scheme 2D/2D ZnO/Zn <sub/>x</sub> Cd <sub/>1?x</sub> S single crystal nanosheet heterojunction for efficient photocatalytic water splitting
摘要： Direct Z-scheme heterojunction can effectively enhance the photocatalytic activity due to its low carrier recombination rate and high redox ability. In this study, a 2D/2D ZnO/ZnxCd1?xS single crystal nanosheet heterojunction is synthesized in situ by topotactic sulfurization/oxidization pyrolysis of Zn/Cd/Al layer double hydroxides (LDHs). Its unique structure provides not only numerous intimate interfaces but also a direct Z-scheme junction. The in situ topotactic fabrication of ZnO by the oxidation process causes some Zn ions to dissolve out from the Zn0.67Cd0.33S solid solution nanosheets with increase in annealing temperature and time. The longer the time for oxidation, the more ZnO is obtained. The formation of ZnO yields 2D/2D ZnO/ZnxCd1?xS single crystal nanosheet heterojunction, which increases the visible light absorption and boosts the separation of photogenerated carriers. The ZnO/ZnxCd1?xS-4 single crystal nanosheet heterojunction presents the highest photocatalytic activity under visible light irradiation (38.93 mmol h?1 g?1), which is nearly 16.93 times higher than that of Zn0.67Cd0.33S-300, and an external quantum efficiency of 40.97% at λ = 420 nm. The proposed synthetic route for the construction of 2D/2D ZnO/ZnxCd1?xS single crystal nanosheet provides a direct Z-scheme structure with highly efficient photocatalytic hydrogen evolution activity.
关键词： 2D/2D ZnO/ZnxCd1?xS,photocatalytic water splitting,Zn/Cd/Al layer double hydroxides,Direct Z-scheme heterojunction,topotactic sulfurization/oxidization pyrolysis
更新于2025-09-04 15:30:14
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Nanorods Array of SnO2 Quantum Dots Interspersed Multiphase TiO2 Heterojunctions with Highly Photocatalytic Water Splitting and Self-Rechargeable Battery-Like Applications
摘要： Facing an ever-growing demand for sustainable and renewable power sources, it has detonated the development of novel materials for photocatalytic water splitting, but how to enhance the photocatalytic efficiency remains a core problem. Herein, we reported a conceptual effective and experimental confirmed strategy in SnO2 quantum dots (QD) interspersed multiphase (Rutile, Anatase) TiO2 nanorods arrays (SnO2/RA@TiO2 NRs) to immensely enhance the carrier separation for highly efficient water splitting by merging simultaneously the QD, multiphase, and heterojunction approaches. Under this synergistic effect, a doping ratio of 25% SnO2 QD interspersed into multiphase TiO2 NRs exhibited a superior optical adsorption and excellent photocurrent density (2.45 mA/cm2 at 1.0 V), giving rise to a largely enhanced incident light to current efficiency (IPCE) in the UV region (45~50 %). More importantly, this material-based device can act as power supply with a voltage of ~2.8 V after illumination, which can automatically self-recharging by reacting with oxygen vacancy and water molecule to realize reusing. The current study provide a new paradigm about heightening the carrier separation extent of QD interspersed multiphase heterojunctions, fabricate a new solar energy converting material/device, and achieve a highly photocatalytic water splitting/self-charging battery-like application.
关键词： Photocatalytic,Water splitting,Titanium Dioxide,Heterojunction
更新于2025-09-04 15:30:14
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Ta <sub/>3</sub> N <sub/>5</sub> /Co(OH) <sub/>x</sub> composites as photocatalysts for photoelectrochemical water splitting
摘要： Ta3N5 nanotubes (NTs) were obtained from nitridation of Ta2O5 NTs, which were grown directly on Ta foil through a 2-step anodization procedure. With Co(OH)x decoration, a photocurrent density as high as 2.3 mA cm?2 (1.23 V vs. NHE) was reached under AM1.5G simulated solar light; however, the electrode suffered from photocorrosion. More stable photoelectrochemical (PEC) performance was achieved by first loading Co(OH)x, followed by loading cobalt phosphate (Co–Pi) as double co-catalysts. The Co(OH)x/Co–Pi double co-catalysts may act as a hole storage layer that slows down the photocorrosion caused by the accumulated holes on the surface of the electrode. A “waggling” appearance close to the “mouth” of Ta2O5 NTs was observed, and may indicate structural instability of the “mouth” region, which breaks into segments after nitridation and forms a top layer of broken Ta3N5 NTs. A unique mesoporous structure of the walls of the Ta3N5 NTs, which is reported here the first time, is also a result of the nitridation process. We believe that the mesoporous structure makes it difficult for the nanotubes to be fully covered by the co-catalyst layer, hence rationalizing the remaining degradation by photocorrosion.
关键词： photoelectrochemical water splitting,photocorrosion,Co–Pi,Co(OH)x,mesoporous structure,Ta3N5 nanotubes
更新于2025-09-04 15:30:14
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Efficient synthesis of BiFeO3 by the microwave-assisted sol-gel method: “A” site influence on the photoelectrochemical activity of perovskites
摘要： BiFeO3 (BF) and LaFeO3 (LF) perovskites were synthesized using a microwave-assisted (MW) and sol-gel (SG) methods. XRD, XPS, TEM, UV-DRS techniques were applied to study physicochemical properties of perovskites. In addition, Incident Photon-to-Current Efficiency (IPCE) measurements, Linear Sweep Voltammetry (LSV) and impedance spectroscopy were used to characterize electrochemical properties of the material. The band gap energy increases in the following way: BF-MW (2.05 eV), LF-MW (2.18 eV), BF-SG (2.26 eV) and LF-SG (2.54 eV), demonstrating a remarkable influence of the synthesis method on the optical and electronic properties of the materials. Furthermore, XRD showed a significant impact of the synthesis methods on the crystal structure. Perovskites synthesized under WM irradiation showed a pure crystal structure compared to the perovskites prepared by SG method, which contained some admixtures. IPCE shows that LF-MW has a better charge separation ability compared to BF-MW. However, BF-SG showed the highest activity. Temperature programmed reduction tests (TPR) revealed a better ability of BiFeO3 to adsorb/desorb oxygen, compared to LaFeO3. XPS measurements pointed at the presence of Fe4+. Finally, the photocatalytic activity of the perovskites was tested in solar water-splitting as a function of the synthesis method and presence of Bi and La in “A” sites of the ABO3 perovskites. We postulate, that the Jahn-Teller distortion effect in LF-MW increases its catalytic activity by decreasing the binding energy compared to BF-MW.
关键词： Microwave-assisted synthesis,Jahn-Teller distortion,Photocatalysts,Photoelectrochemical water splitting,Perovskites
更新于2025-09-04 15:30:14
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Efficient bifunctional vanadium doped Ni3S2 nanorod array for overall water splitting
摘要： Electrochemical water splitting, allowing energy conversion from renewable resources into non-polluting chemical fuels, is vital in the future sustainable energy system, and great efforts have been paid on developing efficient and cheap bifunctional electrocatalysts. Herein we report a bifunctional vanadium doped Ni3S2 nanorod array electrode for overall water splitting in alkaline media. To afford a catalytic current of 10 mA cm-2, the designed V-Ni3S2 electrode only requires the overpotentials of 133 mV for hydrogen evolution and 148 mV for oxygen generation, meanwhile showing high long-term stability. The excellent catalytic properties are assigned to the V dopants and geometric advantages of nanorod array. The V-Ni3S2 electrodes are simultaneously utilized as cathode and anode in one two-electrode cell to function overall water splitting, exhibiting a cell voltage of 1.421 V at 10 mA cm-2. The water splitting in this cell can also be feasibly driven by a single-cell AA battery (1.5 V). Our report shows substantial advancement in the exploration of efficient bifunctional electrocatalysts for water splitting.
关键词： bifunctional electrocatalysts,water splitting,nanorod array,alkaline media,vanadium doped Ni3S2
更新于2025-09-04 15:30:14