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Double Perovskite Cobaltites Integrated in a Monolithic and Noble Metal-Free Photoelectrochemical Device for Efficient Water Splitting.

ABSTRACT: Water photoelectrolysis has the potential to produce renewable hydrogen fuel, therefore addressing the intermittent nature of sunlight. Herein, a monolithic, photovoltaic (PV)-assisted water electrolysis device of minimal engineering and of low (in the μg range) noble-metal-free catalysts loading is presented for unassisted water splitting in alkaline media. An efficient double perovskite cobaltite catalyst, originally developed for high-temperature proton-conducting ceramic electrolyzers, possesses high activity for the oxygen evolution reaction in alkaline media at room temperatures too. Ba_1-xGd_1-yLa_x+yCo₂O_6-δ (BGLC) is combined with a NiMo cathode, and a solar-to-hydrogen efficiency of 6.6% in 1.0 M NaOH, under 1 sun simulated illumination for 71 h, is demonstrated. This work highlights how readily available earth-abundant materials and established PV methods can achieve high performance and stable and monolithic photoelectrolysis devices with potential for full-scale applications.

SUBMITTER: Zhu J

PROVIDER: S-EPMC8289171 | biostudies-literature |

REPOSITORIES: biostudies-literature

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Efficient Photoelectrochemical Water Splitting by Tailoring MoS2/CoTe Heterojunction in a Photoelectrochemical Cell.

Project description:Solar energy conversion through photoelectrochemical water splitting (PEC) is an upcoming promising technique. MoS2/CoTe heterostructures were successfully prepared and utilized for PEC studies. MoS2 and CoTe were prepared by a hydrothermal method which were then ultrasonicated with wt. % ratios of 1:3, 1:1 and 3:1 to prepare MoS2/CoTe (1:3), MoS2/CoTe (1:1) and MoS2/CoTe (3:1) heterostructure, respectively. The pure materials and heterostructures were characterized by XRD, UV-vis-DRS, SEM, XPS, PL and Raman spectroscopy. Photoelectrochemical measurements were carried out by linear sweep voltammetry and electrochemical impedance spectroscopic measurements. A maximum photocurrent density of 2.791 mA/cm2 was observed for the MoS2/CoTe (1:1) heterojunction which is about 11 times higher than the pristine MoS2. This current density was obtained at an applied bias of 0.62 V vs. Ag/AgCl (1.23 V vs. RHE) under the light intensity of 100 mW/cm2 of AM 1.5G illumination. The enhanced photocurrent density may be attributed to the efficient electron-hole pair separation. The solar to hydrogen conversion efficiency was found to be 0.84% for 1:1 MoS2/CoTe, signifying the efficient formation of the p-n junction. This study offers a novel heterojunction photocatalyst, for PEC water splitting.

| S-EPMC7760392 | biostudies-literature

Metal-Organic Frameworks as Promising Photosensitizers for Photoelectrochemical Water Splitting.

Project description:Ti-based metal-organic frameworks (MOFs) are demonstrated as promising photosensitizers for photoelectrochemical (PEC) water splitting. Photocurrents of TiO2 nano wire photoelectrodes can be improved under visible light through sensitization with aminated Ti-based MOFs. As a host, other sensitizers or catalysts such as Au nanoparticles can be incorporated into the MOF layer thus further improving the PEC water splitting efficiency.

| S-EPMC5063145 | biostudies-literature

Upscaling of integrated photoelectrochemical water-splitting devices to large areas.

Project description:Photoelectrochemical water splitting promises both sustainable energy generation and energy storage in the form of hydrogen. However, the realization of this vision requires laboratory experiments to be engineered into a large-scale technology. Up to now only few concepts for scalable devices have been proposed or realized. Here we introduce and realize a concept which, by design, is scalable to large areas and is compatible with multiple thin-film photovoltaic technologies. The scalability is achieved by continuous repetition of a base unit created by laser processing. The concept allows for independent optimization of photovoltaic and electrochemical part. We demonstrate a fully integrated, wireless device with stable and bias-free operation for 40 h. Furthermore, the concept is scaled to a device area of 64 cm(2) comprising 13 base units exhibiting a solar-to-hydrogen efficiency of 3.9%. The concept and its successful realization may be an important contribution towards the large-scale application of artificial photosynthesis.

| S-EPMC5023961 | biostudies-literature

Solar Water Splitting with a Hydrogenase Integrated in Photoelectrochemical Tandem Cells.

Project description:Hydrogenases (H2 ases) are benchmark electrocatalysts for H2 production, both in biology and (photo)catalysis in?vitro. We report the tailoring of a p-type Si photocathode for optimal loading and wiring of H2 ase through the introduction of a hierarchical inverse opal (IO) TiO2 interlayer. This proton-reducing Si|IO-TiO2 |H2 ase photocathode is capable of driving overall water splitting in combination with a photoanode. We demonstrate unassisted (bias-free) water splitting by wiring Si|IO-TiO2 |H2 ase to a modified BiVO4 photoanode in a photoelectrochemical (PEC) cell during several hours of irradiation. Connecting the Si|IO-TiO2 |H2 ase to a photosystem?II (PSII) photoanode provides proof of concept for an engineered Z-scheme that replaces the non-complementary, natural light absorber photosystem?I with a complementary abiotic silicon photocathode.

| S-EPMC6100105 | biostudies-literature

Modified Nanopillar Arrays for Highly Stable and Efficient Photoelectrochemical Water Splitting.

Project description:Atomically modified graphitic carbon nitride quantum dots (QDs), characterized by strongly increased reactivity and stability, are developed. These are deposited on arrays of TiO2 nanopillars used as a photoanode for the photoelectrochemical water splitting. This photoanode shows excellent stability, with 111 h of continuous work without any performance loss, which outperforms the best-reported results by a factor of 10. Remarkably, our photoanode produces hydrogen even at zero bias. The excellent performance is attributed to the enhancement of photoabsorption, as well as to the promotion of charge separation between TiO2 nanopillars and the QDs.

| S-EPMC6436580 | biostudies-literature

Thickness-Dependent Photoelectrochemical Water Splitting Properties of Self-Assembled Nanostructured LaFeO3 Perovskite Thin Films.

Project description:Tuning the intrinsic structural and stoichiometric properties by different means is used for increasing the green energy production efficiency of complex oxide materials. Here, we report on the formation of self-assembled nanodomains and their effects on the photoelectrochemical (PEC) properties of LaFeO3 (LFO) epitaxial thin films as a function of layer's thickness. The variation with the film's thickness of the structural parameters such as in-plane and out-of-plane crystalline coherence length and the coexistence of different epitaxial orientation-<100>SrTiO3//<001> LFO, <100>SrTiO3//<110> LFO and [110] LFO//[10] STO, as well as the appearance of self-assembled nanodomains for film's thicknesses higher than 14 nm, is presented. LFO thin films exhibit different epitaxial orientations depending on their thickness, and the appearance of self-assembled nanopyramids-like domains after a thickness threshold value has proven to have a detrimental effect on the PEC functional properties. Using Nb:SrTiO3 as conductive substrate and 0.5 M NaOH aqueous solution for PEC measurements, the dependence of the photocurrent density and the onset potential vs. RHE on the structural and stoichiometric features exhibited by the LFO photoelectrodes are unveiled by the X-ray diffraction, high-resolution transmission electron microscopy, ellipsometry, and Rutherford backscattering spectroscopy results. The potentiodynamic PEC analysis has revealed the highest photocurrent density Jphotocurrent values (up to 1.2 mA/cm2) with excellent stability over time, for the thinnest LFO/Nb:SrTiO3 sample, both cathodic and anodic behavior being noticed. Noticeably, the LFO thin film shows unbiased hydrogen evolution from water, as determined by gas chromatography in aqueous 0.5 M NaOH solution under constant illumination.

| S-EPMC8224280 | biostudies-literature

Design of SnO2:Ni,Ir Nanoparticulate Photoelectrodes for Efficient Photoelectrochemical Water Splitting.

Project description:Currently, hydrogen generation via photocatalytic water splitting using semiconductors is regarded as a simple environmental solution to energy challenges. This paper discusses the effects of the doping of noble metals, Ir (3.0 at.%) and Ni (1.5-4.5 at.%), on the structure, morphology, optical properties, and photoelectrochemical performance of sol-gel-produced SnO2 thin films. The incorporation of Ir and Ni influences the position of the peaks and the lattice characteristics of the tetragonal polycrystalline SnO2 films. The films have a homogeneous, compact, and crack-free nanoparticulate morphology. As the doping level is increased, the grain size shrinks, and the films have a high proclivity for forming Sn-OH bonds. The optical bandgap of the un-doped film is 3.5 eV, which fluctuates depending on the doping elements and their ratios to 2.7 eV for the 3.0% Ni-doped SnO2:Ir Photoelectrochemical (PEC) electrode. This electrode produces the highest photocurrent density (Jph = 46.38 mA/cm2) and PEC hydrogen production rate (52.22 mmol h-1cm-2 at -1V), with an Incident-Photon-to-Current Efficiency (IPCE% )of 17.43% at 307 nm. The applied bias photon-to-current efficiency (ABPE) of this electrode is 1.038% at -0.839 V, with an offset of 0.391% at 0 V and 307 nm. These are the highest reported values for SnO2-based PEC catalysts. The electrolyte type influences the Jph values of photoelectrodes in the order Jph(HCl) > Jph(NaOH) > Jph(Na2SO4). After 12 runs of reusability at -1 V, the optimized photoelectrode shows high stability and retains about 94.95% of its initial PEC performance, with a corrosion rate of 5.46 nm/year. This research provides a novel doping technique for the development of a highly active SnO2-based photoelectrocatalyst for solar light-driven hydrogen fuel generation.

| S-EPMC8839913 | biostudies-literature

Atomically dispersed iridium catalysts on silicon photoanode for efficient photoelectrochemical water splitting.

Project description:Stabilizing atomically dispersed single atoms (SAs) on silicon photoanodes for photoelectrochemical-oxygen evolution reaction is still challenging due to the scarcity of anchoring sites. Here, we elaborately demonstrate the decoration of iridium SAs on silicon photoanodes and assess the role of SAs on the separation and transfer of photogenerated charge carriers. NiO/Ni thin film, an active and highly stable catalyst, is capable of embedding the iridium SAs in its lattices by locally modifying the electronic structure. The isolated iridium SAs enable the effective photogenerated charge transport by suppressing the charge recombination and lower the thermodynamic energy barrier in the potential-determining step. The Ir SAs/NiO/Ni/ZrO2/n-Si photoanode exhibits a benchmarking photoelectrochemical performance with a high photocurrent density of 27.7 mA cm-2 at 1.23 V vs. reversible hydrogen electrode and 130 h stability. This study proposes the rational design of SAs on silicon photoelectrodes and reveals the potential of the iridium SAs to boost photogenerated charge carrier kinetics.

| S-EPMC9899270 | biostudies-literature

High-performance bifunctional porous non-noble metal phosphide catalyst for overall water splitting.

Project description:Water electrolysis is an advanced energy conversion technology to produce hydrogen as a clean and sustainable chemical fuel, which potentially stores the abundant but intermittent renewable energy sources scalably. Since the overall water splitting is an uphill reaction in low efficiency, innovative breakthroughs are desirable to greatly improve the efficiency by rationally designing non-precious metal-based robust bifunctional catalysts for promoting both the cathodic hydrogen evolution and anodic oxygen evolution reactions. We report a hybrid catalyst constructed by iron and dinickel phosphides on nickel foams that drives both the hydrogen and oxygen evolution reactions well in base, and thus substantially expedites overall water splitting at 10?mA?cm-2 with 1.42?V, which outperforms the integrated iridium (IV) oxide and platinum couple (1.57?V), and are among the best activities currently. Especially, it delivers 500?mA?cm-2 at 1.72?V without decay even after the durability test for 40 h, providing great potential for large-scale applications.

| S-EPMC6026163 | biostudies-literature

Metal-free organic sensitizers for use in water-splitting dye-sensitized photoelectrochemical cells.

Project description:Solar fuel generation requires the efficient capture and conversion of visible light. In both natural and artificial systems, molecular sensitizers can be tuned to capture, convert, and transfer visible light energy. We demonstrate that a series of metal-free porphyrins can drive photoelectrochemical water splitting under broadband and red light (λ > 590 nm) illumination in a dye-sensitized TiO2 solar cell. We report the synthesis, spectral, and electrochemical properties of the sensitizers. Despite slow recombination of photoinjected electrons with oxidized porphyrins, photocurrents are low because of low injection yields and slow electron self-exchange between oxidized porphyrins. The free-base porphyrins are stable under conditions of water photoelectrolysis and in some cases photovoltages in excess of 1 V are observed.

| S-EPMC4330777 | biostudies-literature

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