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The Artificial Leaf: Recent Progress and Remaining Challenges
摘要: The prospect of a device that uses solar energy to split water into H2 and O2 is highly attractive in terms of producing hydrogen as a carbon-neutral fuel. In this mini review, key research milestones that have been reached in this field over the last two decades will be discussed, with special focus on devices that use earth-abundant materials. Finally, the remaining challenges in the development of such “artificial leaves” will be highlighted.
关键词: water splitting,hydrogen production,sustainable hydrogen,artificial photosynthesis,electrochemistry
更新于2025-09-10 09:29:36
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An efficient tandem photoelectrochemical cell composed of FeOOH/TiO2/BiVO4 and Cu2O for self-driven solar water splitting
摘要: An integrated solar water splitting tandem cell without external bias was designed using a FeOOH modified TiO2/BiVO4 photoanode as a photoanode and p-Cu2O as a photocathode in this study. An apparent photocurrent (0.37 mA/cm2 at operating voltage of +0.36 VRHE) for the tandem cell without applied bias was measured, which is corresponding to a photoconversion efficiency of 0.46%. Besides, the photocurrent of FeOOH modified TiO2/BiVO4 and Cu2O photocathode (~0.07 mA/cm2 at +0.42 VRHE). Then we established a FeOOH modified TiO2/BiVO4-Cu2O two-electrode system and measured the current density-voltage curves under AM 1.5G illumination. The unassisted photocurrent density is 0.12 mA/cm2 and the corresponding amounts of hydrogen and oxygen evolved by the tandem PEC cell without bias are 2.36 mmol/cm2 and 1.09 mmol/cm2 after testing for 2.5 h. The photoelectrochemical (PEC) properties of the FeOOH modified TiO2/BiVO4 photoanode were further studied to demonstrate the electrons transport process of solar water splitting. This aspect provides a fundamental challenge to establish an unbiased and stabilized photoelectrochemical (PEC) solar water splitting tandem cell with higher solar-to-hydrogen efficiency.
关键词: Self-driven water splitting,PEC tandem cell,Solar hydrogen,Cu2O-BiVO4
更新于2025-09-10 09:29:36
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Hybrid microwave annealing for fabrication of more efficient semiconductor photoanodes for solar water splitting
摘要: Hybrid microwave annealing (HMA) is proposed as an alternative to conventional thermal annealing (CTA) in a furnace to fabricate efficient semiconductor photoelectrodes for solar water splitting. Thus the effects of HMA are investigated in comparison with CTA using spinel zinc ferrite as an example. The ZnFe2O4 photoanodes fabricated by HMA with a graphite susceptor provide less defective surface, better structural ordering and smaller feature size than photoanodes prepared by CTA. Besides, HMA does not impair conductivity of the F:SnO2 glass substrate. All these positive factors of HMA leads to ~4 times higher photocurrents at 1.23 VRHE and lowered onset potential by ~100 mV under 1-sun irradiation of an optimized ZnFe2O4 photoanode relative to that fabricated by CTA. The HMA could be an effective generic method to fabricate efficient photoelectrodes based on refractory semiconductors replacing incumbent CTA.
关键词: Conventional thermal annealing,ZnFe2O4,Hybrid microwave annealing,Photoelectrochemical water splitting
更新于2025-09-10 09:29:36
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A New Class of Zn <sub/>1</sub><i> <sub/>-x</sub></i> Fe <i> <sub/>x</sub></i> -Oxyselenide and Zn <sub/>1-</sub><i> <sub/>x</sub></i> Fe <i> <sub/>x</sub></i> -LDH Nanostructured Material with Remarkable Bifunctional Oxygen and Hydrogen Evolution Electrocatalytic Activities for Overall Water Splitting
摘要: The scalable and cost-effective H2 fuel production via electrolysis demands an efficient earth-abundant oxygen and hydrogen evolution reaction (OER, and HER, respectively) catalysts. In this work, for the first time, the synthesis of a sheet-like Zn1-xFex–oxyselenide and Zn1-xFex–LDH on Ni-foam is reported. The hydrothermally synthesized Zn1-xFex–LDH/Ni-foam is successfully converted into Zn1-xFex–oxyselenide/Ni-foam through an ethylene glycol-assisted solvothermal method. The anionic regulation of electrocatalysts modulates the electronic properties, and thereby augments the electrocatalytic activities. The as-prepared Zn1-xFex–LDH/Ni-foam shows very low OER and HER overpotentials of 263 mV at a current density of 20 mA cm?2 and 221 mV at 10 mA cm?2, respectively. Interestingly, this OER overpotential is decreased to 256 mV after selenization and the HER overpotential of Zn1-xFex–oxyselenide/Ni-foam is decreased from 238 to 202 mV at 10 mA cm?2 after a stability test. Thus, the Zn1-xFex–oxyselenide/Ni–foam shows superior bifunctional catalytic activities and excellent durability at a very high current density of 50 mA cm?2. More importantly, when the Zn1-xFex–oxyselenide/Ni-foam is used as the anode and cathode in an electrolyzer for overall water splitting, Zn1-xFex–oxyselenide/Ni-foam(+)∥Zn1-xFex–oxyselenide/Ni-foam(-) shows an appealing potential of 1.62 V at 10 mA cm?2. The anionic doping/substitution methodology is new and serves as an effective strategy to develop highly efficient bifunctional electrocatalysts.
关键词: Zn1-xFex–oxyselenide,Zn1-xFex–LDH,overall water splitting,HER,OER
更新于2025-09-10 09:29:36
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[Energy, Environment, and Sustainability] Nano-Energetic Materials || Nanomaterials for Hydrogen Production Through Photocatalysis
摘要: In the last few decades, nanostructured materials have been of great interest worldwide due to their unique characteristics and their sub-driven reactivity. Furthermore, the unlimited applications of such materials in different fields and their associated success had added extra value for their importance. The combination between nanomaterials and photocatalytic processes has been recently given a great attention in different applications. It may enhance the viability of the nanotechnology principles. One of these applications is the usage of nanophotocatalytic materials in hydrogen production via water-splitting reaction. This chapter will cover the main concepts of photocatalysis and its associated terms. The main features of efficient photocatalysts and the ways of measuring such properties are illustrated in this chapter. Also, a brief presentation for the current methods that are utilized in the preparation of these catalysts is provided. An overview of the different types of semiconductors that are employed in the domain of photo-based hydrogen generation via splitting of water is introduced through this chapter too. A new approach in the water-splitting process by introducing noble metals attached magnetic nanoparticle (core/shell structure) as promising photomaterials is also described in this chapter. However, these materials are used in different fields such as bio-medical processes, water treatment, and energy storage. They are expected to be of high significance in field of catalysis, since they can be easily separated and recovered, due to their magnetic character, reactions. Implementation of a suitable magnetic force can enhance the hydrogen productivity during the water-splitting process. These materials are possessing magnetic properties which could reveal a new approach to their photocatalytic activity via quenching the radiation scattering.
关键词: Water-splitting processes,Magnetic materials,Photocatalysis,Hydrogen energy,Semiconductors
更新于2025-09-10 09:29:36
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Construction of Z-scheme MoSe2/CdSe Hollow Nanostructure with Enhanced Full Spectrum Photocatalytic Activity
摘要: For better use of solar energy, the development of full-spectrum photocatalysts has attracted most attentions. In this research, uniform hollow MoSe2/CdSe nanospheres (250 nm) were prepared by one-pot solvothermal strategy. It is the first time to synthesize hollow MoSe2 based nanostructure without any template/surfactant assistance. By varying reaction time, the formation mechanism was investigated, illuminating that the novel hollow structure is derived from the Kirkendall Effect. Both experimental and density functional theory (DFT) calculations reveal the Z-scheme mechanism of the charge transfer in the heterostructure. The hollow MoSe2/CdSe nanospheres (MC2) possess the remarkable photocatalytic activity in degradation of Cr(VI) (125 mg g-1, simulated sunlight), owing to the high harvest of full spectrum, porous hollow structure and effective charge separation/transfer. Furthermore, the photocatalytic process was further studied in detail, showing that the Langmuir single-layer adsorption behavior, low pH value condition, and thermal effect also benefit to the high photoreduction performance. Benefiting from the Z-scheme mechanism, the high redox activity make sure the water splitting capacity of MC2 (7120.0 and 348.0 μmol·h-1·g-1 of H2 and O2 evolution) under simulated sunlight irradiation and its AQY for H2 evolution at 670 nm reaches up to 27.2% (50 mg MC2).
关键词: Z-scheme,Water splitting,Cr(VI) photoreduction,Hollow MoSe2/CdSe nanospheres,Full Spectrum photocatalysis
更新于2025-09-10 09:29:36
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Excellent visible light photocatalytic H2 evolution activity of novel noble-metal-free Ni12P5/CdS composite
摘要: Novel noble-metal-free Ni12P5/CdS composite was designed and synthesized by a hydrothermal method. The photocatalytic H2 generation activity of the as-prepared Ni12P5/CdS is 1.93 fold of that of pure CdS under visible light (λ > 420 nm) irradiation. The enhanced activity of Ni12P5/CdS is ascribed to the improved separation e?ciency of photocarriers over a direct Z-scheme mechanism. It provides a potential strategy to improve the photocatalytic H2 evolution activity of CdS greatly by loading noble-metal-free Ni12P5 as electron co-catalyst via direct Z-scheme mechanism.
关键词: Water splitting,Photocatalysis,Semiconductors
更新于2025-09-10 09:29:36
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Titanate-based perovskites for photochemical and photoelectrochemical water splitting applications: A review
摘要: Recently, perovskites have been intensively studied for effective hydrogen production through photocatalytic water splitting reactions. The unique properties of perovskite materials are their tunable bandgap and high photocorrosion stability. Titanate-based perovskites are the most widely studied perovskites for activation under visible light and improvement in the hydrogen gas production rate by sunlight. Beneficial modifications were achieved through element doping, catalyst loading, heterojunction formation with other materials and surface modification. This review presents the progress over the last ten years in titanate perovskite modification and the increases achieved in the H2 production rate.
关键词: Water splitting,Photocatalyst,Hydrogen production,Titanate,Perovskite
更新于2025-09-10 09:29:36
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Janus Group-Ⅲ Chalcogenide Monolayers and Derivative Type-Ⅱ Heterojunctions as Water Splitting Photocatalysts with Strong Visible Light Absorbance
摘要: Search for two-dimensional (2D) water splitting photocatalysts is crucial to solve energy crises and environmental problems. In this research, we study the electronic and photocatalytic properties of single-layer Ga2X1X2 (Ga2SeTe, Ga2STe and Ga2SSe) and newly proposed α-Ga2S3/Ga2SSe-A, α-Ga2S3/Ga2SSe-B and α-Ga2S3/Ga2SSe-C van der Walls heterojunctions using first-principles calculations. Theoretical results indicate Ga2X1X2 monolayers present suitable band edges. 2D α-Ga2S3/Ga2SSe-B and α-Ga2S3/Ga2SSe-C belong to type-Ⅱ heterojunctions, and under biaxial strains embody suitable band edges. Comparisons of the valence band maximum (VBM) charge and electric dipole of α-Ga2S3/Ga2SSe-A and α-Ga2S3/Ga2SSe-B demonstrate it is possible to achieve suitable band edges for water splitting by switching electric dipoles. Especially, the three Ga2X1X2 monolayers, α-Ga2S3/Ga2SSe-B and α-Ga2S3/Ga2SSe-C heterojunctions absorb a large amount of visible light, promising they are photocatalysts for water splitting. More importantly, we find the optical absorption coefficients of 2D monolayers and heterojunctions in previous calculations are several times underestimated because the effective volume is not taken into consideration. To obtain reliable absorption coefficients, the real and imaginary parts of dielectric function must be renormalized.
关键词: visible light absorbance,van der Waals heterojunctions,two-dimensional (2D) materials,Janus group-Ⅲ chalcogenide monolayers,water splitting photocatalysts,first-principles calculations
更新于2025-09-10 09:29:36
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Enhanced Electrochemical Stability of TiO <sub/>2</sub> -Protected, Al-doped ZnO Transparent Conducting Oxide Synthesized by Atomic Layer Deposition
摘要: Transparent, conductive coatings on porous, three-dimensional materials are often used as the current collector for photoelectrode designs in photoelectrochemical applications. These structures allow for improved light trapping and absorption in chemically-synthesized, photoactive overlayers while minimizing parasitic absorption in the current collecting layer. Atomic layer deposition (ALD) is particularly useful for fabricating transparent conducting oxides (TCOs) like Sn-doped In2O3 (ITO) and Al-doped ZnO (AZO) for structured materials because the deposition is specific to exposed surfaces. Unlike line-of-site deposition methods (evaporation, spray pyrolysis, sputtering), ALD can access the entire complex interface to make a conformal transparent conductive layer. While ITO and AZO can be grown by ALD, they are intrinsically soluble in the acidic and basic environments common for electrochemical applications like water splitting. To take advantage of the unique characteristics of ALD in these applications, is important to develop strategies for fabricating TCO layers with enhanced chemical stability. Ultra-thin coatings of stable materials can be used to protect otherwise unstable electrochemical interfaces while maintaining the desired function. Here, we describe experiments to characterize the chemical and electrochemical stability of ALD-deposited AZO TCO thin films protected by a 10nm TiO2 overlayer. The addition of a TiO2 protection layer is demonstrated to improve the chemical stability of AZO by orders of magnitude compared to unprotected, yet otherwise identically prepared AZO films. The electrochemical stability is enhanced accordingly in both acidic and basic environments. We demonstrate that TiO2-protected AZO can be used as a TCO for both the cathodic hydrogen evolution (HER) and anodic water oxidation (OER) half-reactions of electrochemical water splitting in base and for HER in acid when the appropriate electrocatalysts are added. As a result, we show that ALD can be used to synthesize a chemically stable TCO heterostructure, expanding the range of materials and electrochemical environments available for building complex photoelectrode architectures.
关键词: Water splitting,Transparent conducting oxides,Atomic layer deposition,Electrochemical stability,Al-doped ZnO,TiO2 protection layer
更新于2025-09-10 09:29:36