Solar Hydrogen Generation Research Articles

Photothermal-assisted S-scheme heterojunction of NiPS3 nanosheets modified ZnIn2S4 microspheres for promoting photocatalytic hydrogen evolution

Exploring high-efficiency photocatalysts for solar hydrogen (H2) generation through water splitting is of great significance for addressing both energy shortage and environmental contamination. In this work, a facile self-assembly strategy was developed to couple NiPS3 nanosheets (NPS NSs) with ZnIn2S4 (ZIS) microspheres to synthesize NPS NSs/ZIS (NPS/ZIS) composites, featuring a characteristic of S-scheme charge transfer mechanism. The NPS/ZIS composites possess broad-spectrum light absorption property, improved photothermal effect and efficient charge transfer, showcasing exceptional solar-to-chemical energy conversion capability for visible-light-driven photocatalytic hydrogen evolution (PHE). The photothermal effect derived from NPS NSs loading can facilitate charge carrier transfer across the interfaces and surface reaction kinetics. By carefully adjusting the mass ratio of NPS NSs, the optimized 4-NPS/ZIS exhibits excellent stability and significantly improved PHE activity (1827.6 μmol⋅g−1⋅h−1) in water, which is 18.4 times higher than that of bare ZIS (99.4 μmol⋅g−1⋅h−1). Furthermore, the 4-NPS/ZIS also shows the high PHE efficiency of 312.2 μmol⋅g−1⋅h−1 in seawater. Diverse characterization results reveal that the remarkably enhanced PHE performance primarily arises from the synergistic effect of S-scheme heterostructure, heightened light harvesting capacity, and enhanced photothermal effect. On the basis of density functional theory (DFT) simulations and experimental verifications, a possible PHE mechanism via the S-scheme heterojunction with photothermal assistance in NPS/ZIS is proposed. This study serves as inspiration for the development of novel photothermal-assisted S-scheme photocatalysts, paving the way for efficient and sustainable green energy production.

Precise solar radiation forecasting for sustainable energy integration: A hybrid CEEMD-SCM-GA-LGBM model for day-ahead power and hydrogen production

In response to the critical need for sustainable energy solutions, this study introduces a groundbreaking hybrid model for enhancing solar radiation forecasting, which is crucial for optimizing solar power integration and hydrogen production. Leveraging a sophisticated amalgamation of Ensemble Empirical Mode Decomposition (EEMD), Sample Entropy-based System Clustering Method (SCM), Genetic Algorithms (GA), and Light Gradient Boosting Machine (LGBM), the model sets a new benchmark in forecasting accuracy. Tested across diverse seasonal data from Jiangsu province, China, it outperforms conventional models like Multi-Layer Perceptron (MLP) and Long Short-Term Memory (LSTM) networks, achieving exceptional accuracy with an average coefficient of determination (R2) of 0.99, root mean square error (RMSE) of 31.17, and mean absolute error (MAE) of 24.03. The model's practical efficacy was validated through a simulated system comprising a photovoltaic array, a DC-DC converter, and an Alkaline electrolyzer, demonstrating a peak hydrogen production of 0.25 kg at 2:30 p.m. on June 18. This indicates the model's superior capability to forecast solar irradiance accurately, which is essential for enhancing the efficiency of solar energy systems and hydrogen generation. The CEEMD-SCM-GA-LGBM hybrid model's adoption is advocated for solar radiation forecasting, promising significant advancements in the integration of solar energy and the optimization of hydrogen production, aligning with global sustainability objectives.

A noise resilient multi-step ahead deep learning forecasting technique for solar energy centered generation of green hydrogen

Generation of green hydrogen based on solar energy is significantly dependent upon photovoltaic (PV) panel energy, which is reliant on the stochastic and intermittent global horizontal irradiance (GHI). Further, if inconsistent power output from PV panels due to influence of noise interferes with continuous supply of energy needed for electrolysis process, then reliable generation of green hydrogen may be impacted. Therefore, in this study, preliminary fast fourier transform (FFT) technique for noise removal is utilized and thereafter, singular spectrum analysis (SSA) algorithm is integrated with Gated Recurrent Unit (GRU) in order to enhance the accuracy during forecasting of green hydrogen reliant on GHI at multiple time steps. The suggested methodology is assessed using GHI dataset for Jaipur site (Rajasthan, India) obtained from National Institute of Wind Energy (NIWE) portal. The monthly average prediction for solar energy centered green hydrogen generation by employing the proposed methodology at Jaipur location corresponds between 0.010 kg/m2 (10 × 103 kg/km2) to 0.020 kg/m2 (20 × 103 kg/km2) in diverse circumstances. The suggested forecasting algorithm provides a reliable and precise methodology that will significantly supports low-carbon economy goals.

Solar Hydrogen Production and Storage in Solid Form: Prospects for Materials and Methods.

Climatic changes are reaching alarming levels globally, seriously impacting the environment. To address this environmental crisis and achieve carbon neutrality, transitioning to hydrogen energy is crucial. Hydrogen is a clean energy source that produces no carbon emissions, making it essential in the technological era for meeting energy needs while reducing environmental pollution. Abundant in nature as water and hydrocarbons, hydrogen must be converted into a usable form for practical applications. Various techniques are employed to generate hydrogen from water, with solar hydrogen production-using solar light to split water-standing out as a cost-effective and environmentally friendly approach. However, the widespread adoption of hydrogen energy is challenged by transportation and storage issues, as it requires compressed and liquefied gas storage tanks. Solid hydrogen storage offers a promising solution, providing an effective and low-cost method for storing and releasing hydrogen. Solar hydrogen generation by water splitting is more efficient than other methods, as it uses self-generated power. Similarly, solid storage of hydrogen is also attractive in many ways, including efficiency and cost-effectiveness. This can be achieved through chemical adsorption in materials such as hydrides and other forms. These methods seem to be costly initially, but once the materials and methods are established, they will become more attractive considering rising fuel prices, depletion of fossil fuel resources, and advancements in science and technology. Solid oxide fuel cells (SOFCs) are highly efficient for converting hydrogen into electrical energy, producing clean electricity with no emissions. If proper materials and methods are established for solar hydrogen generation and solid hydrogen storage under ambient conditions, solar light used for hydrogen generation and utilization via solid oxide fuel cells (SOFCs) will be an efficient, safe, and cost-effective technique. With the ongoing development in materials for solar hydrogen generation and solid storage techniques, this method is expected to soon become more feasible and cost-effective. This review comprehensively consolidates research on solar hydrogen generation and solid hydrogen storage, focusing on global standards such as 6.5 wt% gravimetric capacity at temperatures between -40 and 60 °C. It summarizes various materials used for efficient hydrogen generation through water splitting and solid storage, and discusses current challenges in hydrogen generation and storage. This includes material selection, and the structural and chemical modifications needed for optimal performance and potential applications.

Optimization of a hybrid renewable energy system for off-grid residential communities using numerical simulation, response surface methodology, and life cycle assessment

This paper presents an optimized hybrid renewable energy system tailored for off-grid residential communities, integrating wind, solar, and hydrogen technologies to meet electricity, cooling, heating, and water needs. The proposed optimization methodology combines numerical simulation, response surface methodology (RSM), and life cycle assessment (LCA), ensuring robust performance across diverse conditions. Key components include fuel cells, reverse osmosis systems, heat pumps, photovoltaic/thermal solar collectors, wind turbines, and hydrogen generation systems. The optimization process targets critical variables such as PVT panel area, the number of wind turbines, and fuel cell power. The optimal configuration was found to include 24 small-scale wind turbines, 159.46 m2 of PVT collectors, and 79.73 kW of fuel cell power. This configuration generated surplus electricity with net electricity usage (NEU) values of −123084.27 kWh/year in New York, −224245.29 kWh/year in Forks, and −215949.30 kWh/year in Santa Barbara. Additionally, the optimized systems achieved a significant reduction in life cycle cost (LCC), with Forks showing the lowest LCC at 304428.97 USD. The environmental impact was also minimized using the novel optimization approach, with the optimized systems achieving negative 100-year global warming potential (GWP100) values, indicating a net reduction in greenhouse gas emissions.

Enhanced PEC generation of hydrogen from seawater driven by efficient and stable Ti-Fe2O3 photoanode

Incorporation of Ti4+ ions into the hematite (α-Fe2O3) photoanodes has garnered significant consideration for the photoelectrochemical water splitting process since it improves the charge transport and optical properties of pristine hematite material. Herein, we have approached a facile route to fabricate the thin films of Ti-Fe2O3 by spray pyrolysis treatment. The Ti-Fe2O3 photocurrent density delivers 1.34 mA/cm2 at 1.23 V RHE in an alkaline seawater environment, showing its excellent performance for photoelectrochemical water- splitting applications. Moreover, it offers outstanding stability in seawater (0.5 M NaCl + 1 M KOH) at applied 1.23 V for 20 h and produces 21.79 µmol/cm2.h of hydrogen. Hence, it will hold a tremendously promising electrode within this area for efficient solar hydrogen generation.

Copper/ cerium metal organic frame work as highly efficient structures for solar power-induced hydrogen generation through the process of water splitting

Increased dependence on fossil fuels as energy sources strongly contributes in both global warming and environmental pollution, leading to serious impacts on human-beings and societies. Therefore, shift from hydrocarbon-based energy to alternative green, sustainable and renewable sources of energy has been globally stimulated in past decades. In an agreement with this context, hydrogen is counted as one of these sources which has been paid strong attention recently due to its high energy content and no harmful emissions. Consequently, this study introduces production of clean green hydrogen through the process of photocatalytic water splitting which is a cost-effective route and releases zero emissions. A series of copper/ or cerium based metal–organic frameworks were successfully prepared via one-pot solvothermal technique and were presented as three novel photocatalysts for hydrogen production from water. The photocatalytic performances of these structures were investigated under visible light irradiation, revealing the highest activity for copper doped cerium metal–organic framework. It exhibited a maximum pure hydrogen productivity of 465 mmol per hour/ gram which was much higher than those the detected productivity by copper and cerium metal–organic frameworks (289 and 375 mmol per hour/ gram respectively). Heterojunction between the two central metals as well as effective charge separation in copper doped cerium metal–organic framework are reasons of its superiority in hydrogen evolution exploit, compared to the other two structures. The recyclability of copper doped cerium metal–organic framework demonstrated high reliability since it showed nearly stable yields of hydrogen over ten cycles of photocatalytic reuse. Therefore, the presented binary metals organic framework establishes new platform for photocatalysts in process of hydrogen production through water splitting.

(Invited) Photoelectrode Design for Photoelectrocatalytic Hydrogen Production

Semiconductor nanomaterials hold the keys for efficient solar energy harvesting and conversion processes like photocatalysis and photoelectrochemical reactions. In this talk, we will give a brief overview of our recent progress in designing semiconductor nanomaterials for photoelectrochemical energy conversion including solar hydrogen generation and low-cost solar cells. In more details, we have been focusing on a few aspects; 1) photocatalysis mechanism, light harvesting, charge separation and transfer and surface reaction engineering of low-cost metal oxide based semiconductors including TiO2, BiVO4 as efficient photoelectrode for photoelectrochemical hydrogen production; 2). The design of ultra-stable composites of perovskite-MOF with improved light emitting and photocatalytic performance.1-5 The resultant material systems exhibited efficient photocatalytic performance and improved power conversion efficiency in solar cells, which underpin sustainable development of solar-energy conversion application. References ： 1. Adv. Mater., 2018, doi:10.1002/adma.201705666.2. Angew. Chem, 2019, doi/10.1002/anie.2018105833. Nature Commun, 2020, (2020) 11:21294. Science, 2021, 374, 621.5. Adv. Mater., 2022, 34 (10), 2106776.

Photocatalytic Solar Hydrogen Generation by SWCNT-Supported Nickel Oxide Nanoparticles Wrapped by Polypyrrole

Photocatalytic Solar Hydrogen Generation by SWCNT-Supported Nickel Oxide Nanoparticles Wrapped by Polypyrrole

Materials Advances in Photocatalytic Solar Hydrogen Production: Integrating Systems and Economics for a Sustainable Future.

Photocatalytic solar hydrogen generation, encompassing both overall water splitting and organic reforming, presents a promising avenue for green hydrogen production. This technology holds the potential for reduced capital costs in comparison to competing methods like photovoltaic-electrocatalysis and photoelectrocatalysis, owing to its simplicity and fewer auxiliary components. However, the current solar-to-hydrogen efficiency of photocatalytic solar hydrogen production has predominantly remained low at ≈1-2% or lower, mainly due to curtailed access to the entire solar spectrum, thus impeding practical application of photocatalytic solar hydrogen production. This review offers an integrated, multidisciplinary perspective on photocatalytic solar hydrogen production. Specifically, the review presents the existing approaches in photocatalyst and system designs aimed at significantly boosting the solar-to-hydrogen efficiency, while also considering factors of cost and scalability of each approach. In-depth discussions extending beyond the efficacy of material and system design strategies are particularly vital to identify potential hurdles in translating photocatalysis research to large-scale applications. Ultimately, this review aims to provide understanding and perspective of feasible pathways for commercializing photocatalytic solar hydrogen production technology, considering both engineering and economic standpoints.

Penternary Wurtzitic Nitrides Li1-xZnxGe2-xGaxN3: Powder Synthesis, Crystal Structure, and Potentiality as a Solar-Active Photocatalyst.

We developed a new penternary wurtzitic nitride system Li1-xZnxGe2-xGaxN3 (0 ≤ x ≤ 1) by hybridizing LiGe2N3 and ZnGeGaN3. Fairly stoichiometric fine powder samples were synthesized by the reduction-nitridation process at 900 °C. While the end member LiGe2N3 possessed a relatively large band gap of 4.16 eV, the band gap of the developed penternary system varied in a broad range of 3.81 to 3.10 eV, showing promising responsivity to the solar spectrum. The crystal structure of LiGe2N3 was precisely determined by time-of-flight neutron powder diffraction for the first time, revealing the complete ordering of Li and Ge in the Cmc21 structure. The structural evolution from completely ordered LiGe2N3 to fully disordered ZnGeGaN3 was quantitatively analyzed by Rietveld refinement based on a partially disordered Cmc21 model, and the obtained results were also supported by 71Ga solid-state NMR spectroscopy. The synthesized Li1-xZnxGe2-xGaxN3 powder samples exhibited photocatalytic activities for the water reduction and oxidation reactions under solar light irradiation, with the H2 evolution rate of 0.3-59.0 μmol/h and the O2 evolution rate of 3.1-296.2 μmol/h, depending on the composition. Stable solar hydrogen generation of up to 48 h was demonstrated by the x = 0.80 sample, with the total amount of H2 evolved over 1.6 mmol and an external quantum efficiency of 2.1%.

Reversible photo-electrochemical device for solar hydrogen and power generation

Reversible photo-electrochemical device for solar hydrogen and power generation

Local Ordering, Distortion, and Redox Activity in (La0.75Sr0.25)(Mn0.25Fe0.25Co0.25Al0.25)O3 Investigated by a Computational Workflow for Compositionally Complex Perovskite Oxides.

Mixing multiple cations can result in a significant configurational entropy, offer a new compositional space with vast tunability, and introduce new computational challenges. For applications such as the two-step solar thermochemical hydrogen (STCH) generation techniques, we demonstrate that using density functional theory (DFT) combined with Metropolis Monte Carlo method (DFT-MC) can efficiently sample the possible cation configurations in compositionally complex perovskite oxide (CCPO) materials, with (La0.75Sr0.25)(Mn0.25Fe0.25Co0.25Al0.25)O3 as an example. In the presence of oxygen vacancies (VO), DFT-MC simulations reveal a significant increase of the local site preference of the cations (short-range ordering), compared to a more random mixing without VO. Co is found to be the redox-active element and the VO is the preferentially generated next to Co due to the stretched Co-O bonds. A clear definition of the vacancy formation energy (Evf) is proposed for CCPO in an ensemble of structures evolved in parallel from independent DFT-MC paths. By combining the distribution of Evf with VO interactions into a statistical model, the oxygen nonstoichiometry (δ), under the STCH thermal reduction and oxidation conditions, is predicted and compared with the experiments. Similar to the experiments, the predicted δ can be used to extract the enthalpy and entropy of reduction using the van't Hoff method, providing direct comparisons with the experimental results. This procedure provides a full predictive workflow for using DFT-MC to obtain possible local ordering or fully random structures, understand the redox activity of each element, and predict the thermodynamic properties of CCPOs, for computational screening and design of these CCPO materials at STCH conditions.

Correction: Stabilization of Catalytically Active Surface Defects on Ga-doped La–Sr–Mn Perovskites for Improved Solar Thermochemical Generation of Hydrogen

Correction: Stabilization of Catalytically Active Surface Defects on Ga-doped La–Sr–Mn Perovskites for Improved Solar Thermochemical Generation of Hydrogen

Stabilization of Catalytically Active Surface Defects on Ga-doped La–Sr–Mn Perovskites for Improved Solar Thermochemical Generation of Hydrogen

Stabilization of Catalytically Active Surface Defects on Ga-doped La–Sr–Mn Perovskites for Improved Solar Thermochemical Generation of Hydrogen

Enhancing the solar hydrogen generation performance of nickel-oxide nanostructured thin films doped with molybdenum

Using technology to store solar energy as hydrogen fuel (H2) on a scale corresponding to global energy use is a viable way to alleviate the energy crisis and environmental deterioration. This research deals with the manufacture of thin films prepared from nickel oxide (NiO) and their use in the photoelectrochemical (PEC) water-splitting process to produce green H2 as a clean energy fuel. Herein, pure and Mo-doped NiO thin films were successfully prepared using a straightforward sputtering method at different radio frequency (RF) power for the Mo target from 0 to 50 watt. x-ray diffraction (XRD), atomic force microscopy (AFM), x-ray photoelectron spectroscopy (XPS), energy dispersive x-ray spectroscopy (EDX), and UV–vis spectroscopy techniques were used to analyze the structural, morphological, chemical composition, and optical characterization of the prepared films. The PEC behaviours for green H2 production and the impedance spectroscopy measurements were also investigated for all samples. In PEC measurements, the 50 W sample showed the highest PEC performance. At −0.4V versus RHE, the 50 W sample verified the highest value for the photocurrent density of about 1.7 mA cm−2 which was approximately four times more than the pure NiO sample. The applied biased photon-to-current conversion efficiency and incident photon-to-current conversion efficiency were also estimated. This research provided a fresh viewpoint on the design of highly active NiO-based photo-catalysts for the production of green H2 powered by solar light.

Impressive efficiency of zinc oxide-manganese oxide/MAX composite in two-electrode system for photovoltaic-electrolyzer water splitting

The improvement and use of affordable and efficient electrocatalysts for complete water splitting are crucial for the future of energy supply. Here, a hybrid zinc oxide (ZnO)–manganese oxide (Mn3O4)/Ti3AlC2 (MAX) composite produced by a facile hydrothermal synthesis is utilized as a dual-function electrocatalyst for the hydrogen and oxygen evolution reactions (HER and OER, respectively). Its well-organized surfaces and bulky porous framework provide numerous catalytically active sites during electrochemical reactions, leading to significant improvement in the HER and OER activities. In particular, the ZnO and Mn3O4 phases increase the catalytic activity of the electrode, while the MAX phase enhances the conductivity and promotes low overpotential Ni sites through charge transfer effects. Consequently, the optimized ZnO-Mn3O4/MAX/Ni foam electrode exhibits relatively low overpotentials (η) of 244 and 340 mV at 20 mA cm−2 for the HER and OER at 1.0 M KOH, respectively. The electrodes also demonstrate exceptional long-term stability during cycling for both the HER and OER. A fully homemade water splitter, using these electrodes as anode and cathode, achieves a current density of 10 mA cm−2 at a cell voltage of only 1.62 V. When integrated with commercially available silicon-based solar cells, combined PV-EC water splitting devices enable increased hydrogen generation from stimulated sunlight. This study presents a typical demonstrated and proven strategy for real large-scale solar hydrogen generation using cost-effective PV-EC technology.

Search on stable binary and ternary compounds of two-dimensional transition metal halides

Ab initio driven density functional theory-based high throughput simulations have been conducted to search for stable two-dimensional (2D) structures based on transition metal halides. Binary MeX2 and MeXY (Me—transition element, X and Y–Cr, Br, I, where X ≠ Y) 2D structures in two structural polymorphic modifications, which are 1T-phase and 1H-phase, have been studied. The main structural stability criteria, such as heat formation energy, elasticity constants, and phonon spectra and the following ab initio molecular dynamics simulations have been used to determine the stability of studied compounds. It has been shown that 35 MeX2 and 32 MeXY 2D structures comply with given stability criteria. Photocatalytic properties of these stable 2D MeX2 and 2D MeXY have been investigated. Based on the calculated band gap size E g, work function Ф and electron affinity χ, it has been found that among all stable compounds 13 MeX2 and 16 MeXY 2D structures are promising photocatalysts for water splitting. However, only 7 compounds have solar-to-hydrogen (STH) efficiency overcome the 10% threshold, which is a critical parameter for solar hydrogen generation to be an economically viable resource. Among MeX2 2D structures 1T-CdI2 and 1H-VBr2 possess a STH efficiency of 11.58% and 17.23%. In the case of 2D MeXY, STH efficiencies are 22.79% (1T-ZnClI), 15.20% (1T-CdClI), 22.13% (1T-ZnBrI), 12.11% (1T-CdBrI) and 19.76% (1H-VClBr). Moreover, as a result of this work, a comprehensive publicly available database, containing detailed calculation parameters and fundamental properties of the discovered 2D transition metal halides, has been created.

Ternary Oxides of s - and p -Block Metals for Photocatalytic Solar-to-Hydrogen Conversion

Oxides containing metals or metalloids from the p block of the periodic table (e.g., In, Sn, Sb, Pb, and Bi) are of technological interest as transparent conductors and light absorbers for solar-energy conversion due to the tunability of their electronic conductivity and optical absorption. Comparatively, these oxides have found limited applications in hydrogen photoelectrolysis, primarily due to their high electronegativity, which impedes electron transfer for reducing protons into hydrogen. We have shown recently that inserting s-block cations into p-block metal oxides is effective at lowering electronegativities while affording further control of band gaps. Here, we explain the origins of this dual tunability by demonstrating the mediator role of s-block cations in modulating orbital hybridization while not contributing to frontier electronic states. From this result, we carry out a comprehensive computational study of 109 ternary oxides of s- and p-block metal elements as candidate photocatalysts for solar hydrogen generation. We down-select the most desirable materials using band gaps and band edges obtained from Hubbard-corrected density-functional theory, with Hubbard parameters computed entirely from first principles, evaluate the stability of these oxides in aqueous conditions, and characterize experimentally four of the remaining materials, synthesized with high phase uniformity, to validate and further develop the computational models. We thus propose nine oxide semiconductors, including CsIn3O5, Sr2In2O5, and KSbO2, which, to the extent of our literature review, have not been previously considered as water-splitting photocatalysts. Published by the American Physical Society 2024

Dual interfacing with metallic cobalt boosts the electron shuttle of CdS-carbide nanoassemblies

Harnessing accelerated interfacial redox, thus boosting charge separation, is of great importance in photocatalytic solar hydrogen generation. In effect, nanoassembling non-noble metallic phases in CdS-based systems and elucidating their role in photocatalysis hold the key to eventually boosting electron shuttle in the field. Here we combine an efficient in-situ exsoluted metallic Co0 nanoparticles on a carbides matrix (CMG) with CdS (CdS@CoCMG) for photogeneration of hydrogen. The metallic cobalt phase exhibits strong binding at the CdS-carbide dual interfaces, forming the accelerated “electron converter” mechanism validated by charge transfer kinetics and achieving two orders of magnitude faster hydrogen production (44.42 mmol g−1 h−1) relative to CdS (0.43 mmol g−1 h−1). We propose that the unique catalyst configuration enable the directional electron-relay photocatalysis via harnessing interfaces between Co0 phase, carbides, and CdS clusters, which eventually boosts the redox process and charge separation of the integrated system, leading to high H2 production rates in the suspension.