Hydrogen Production Rate Research Articles

Synergistic effects of MXene support and cobalt salts in dye-sensitized photocatalytic hydrogen generation

This study introduces an approach to photocatalytic hydrogen production through a dye-sensitized photocatalytic system employing MXene (Ti3C2Tx) and a non-noble cobalt metal catalyst. It was demonstrated that simple integration of eosin Y, Ti3C2Tx and cobalt salt (CoSO4) significantly enhances the photocatalytic hydrogen evolution, outperforming the corresponding system that does not include Ti3C2Tx. The key to this enhanced performance lies in the unique properties of MXene material, which facilitates effective electron transfer and acts as a support for dye and catalyst. The successful well-dispersed decoration of small (2–3 nm) cobalt-based nanoparticles on the Ti3C2Tx sheet via in situ photodeposition was confirmed by transmission electron microscopy (TEM) and X-ray Photoelectron Spectroscopy (XPS). The optimal hydrogen production rates were achieved with a Co to Ti3C2Tx mass ratio of 15%. This optimized interaction results in a hydrogen evolution rate of 40.1 mmol h−1 g−1 and an apparent quantum efficiency (AQE) of 35.4% at 505 nm. These findings highlight the potential of Ti3C2Tx as a versatile component in photocatalytic systems, particularly effective when paired with economically viable, earth-abundant catalysts like cobalt.

In situ Construction of Single‐Atom Electronic Bridge on COF to Enhance Photocatalytic H2 Production

AbstractPhotocatalytic hydrogen production is one of the most valuable technologies in the future energy system. Here, we designed a metal‐covalent organic frameworks (MCOFs) with both small‐sized metal clusters and nitrogen‐rich ligands, named COF‐Cu3TG. Based on our design, small‐sized metal clusters were selected to increase the density of active sites and shorten the distance of electron transport to active sites. While another building block containing nitrogen‐rich organic ligands acted as a node that could in situ anchor metal atoms during photocatalysis and form interlayer single‐atom electron bridges (SAEB) to accelerate electron transport. Together, they promoted photocatalytic performance. This represented the further utilization of Ru atoms and was an additional application of the photosensitizer. N2‐Ru‐N2 electron bridge (Ru‐SAEB) was created in situ between the layers, resulting in a considerable enhancement in the hydrogen production rate of the photocatalyst to 10.47 mmol g−1 h−1. Through theoretical calculation and EXAFS, the existence position and action mechanism of Ru‐SAEB were reasonably inferred, further confirming the rationality of the Ru‐SAEB configuration. A sufficiently proximity between the small‐sized Cu3 cluster and the Ru‐SAEB was found to expedite electron transfer. This work demonstrated the synergistic impact of small molecular clusters with Ru‐SAEB for efficient photocatalytic hydrogen production.

Strong Electron Coupling Effect of Prussian Blue Analogs Derived Ultrathin Nitrogen‐Doped Carbon Wrapped Fe‐CoP for Enhanced Wide Spectrum Photocatalytic H2 Evolution

AbstractWith the advantages of large specific surface area and high porosity of general metal‐organic frame materials, russian blue analogs have broad application prospects in catalysis. In this work, a series of ultra‐thin N‐doped carbon coated Fe‐CoP (Fe‐CoP@NC) are prepared by phosphating Fe‐Co‐Co Prussian blue analogs (Fe‐Co‐Co PBA) in different degrees for the broad‐spectrum photocatalytic hydrogen evolution. The results show that Fe‐CoP@NC‐3 has the highest photocatalytic hydrogen production rate of 16.6 mmol h−1 g−1, which is 83 times greater than that of Fe‐Co‐Co PBA. The excellent stability of Fe‐CoP@NC‐3 is proved by cyclic experiments. The outstanding photocatalytic H2 production activity of Fe‐CoP@NC‐3 can be ascribed to the strong electron coupling effect between Fe‐CoP and N‐doped carbon layer. The photogenerated electrons of Fe‐CoP are transferred to the N‐doped carbon layer, which is electron transport mediator accelerating the electron transfer and synergetic improving the hydrogen evolution efficiency. This work provides an effective strategy for designing an ultra‐thin N‐doped carbon layer coated phosphide photocatalyst with strong electron coupling effect.

Nitrogen-oxygen defect engineering enhanced intrinsic electric field in CoFe2O4/g-C3N4 heterojunctions for photocatalytic tetracycline degradation and H2 evolution

A range of efficient g-C3N4/CoFe2O4 heterojunction with nitrogen deficiencies (NDs) and oxygen deficiencies (ODs) were successfully synthesized through doping-melting and hydrothermal methods. Nitrogen-oxygen defect engineering effectively enhanced the active sites on the catalyst surface and regulated the optical bandgap, band structure, and work function (Φ) of g-C3N4 and CoFe2O4, regulating the strength of the intrinsic electric field (IEF) and promoting the separation of photo-generated carriers at the heterojunction interface. Among the series of samples, CH-H2@CFO-A5 (properly oxalate-doped g-C3N4/CoFe2O4 heterojunctions treated with prolonged annealing) demonstrated remarkable optical properties due to its narrowest optical band gap, while the strongest IEF and redox potential make it has strong carrier dynamics and photocatalytic efficiency. Under visible light, the mineralization rate of tetracycline (TC) on CH-H2@CFO-A5 and the photocatalytic hydrogen production rate were 4.51 times and 2.72 times higher than that of unmodified CN-H0@CFO-A1, respectively. This study aimed to provide an efficient strategy for regulating the IEF within the heterojunction, by altering the Fermi level through multi-element defect engineering.

Plasmon-induced efficient solar-driven H2 production using bimetallic core-shell Cu@Ag:TiO2 nanocomposite photocatalyst

The nano-interface formed by bimetallic Cu@Ag nanoparticles (NPs) on a TiO2 surface enhances charge separation through plasmonic heterojunctions. These bimetallic Cu@Ag NPs were synthesized via the a galvanic replacement reaction (GRR) involving Ag+ in an aqueous medium and metallic Cu NPs on TiO2. During the GRR, Cuδ+ and Agδ+ charge pairs are generated by electron transfer from the catalyst surface. These charge pairs act as active sites, significantly enhancing photocatalytic hydrogen production. Additionally, the cubic crystalline phase of metallic Cu NPs is maintained after the GRR process with Ag ions, while the size of bimetallic Cu@Ag NPs remains constant. Consequently, Cu@Ag NPs supported on TiO2 (Cu@Ag:TiO2) exhibit increased donor charge density of 1.66 × 1020 cm−3 and facilitate rapid charge transfer. As a result, the photocatalytic hydrogen production rate of Cu@Ag:TiO2 is 20 times higher than that of pristine TiO2. Moreover, the visible-light responsive photocatalytic activity of Cu@Ag:TiO2 NPs reaches 3.4 mmol g−1 over 5 hours, which is 78 times higher than that of pristine TiO2. This remarkable enhancement is attributed to the formation of a plasmonic heterojunction with close contact between Cu@Ag and TiO2, enabling efficient charge carrier separation.

Investigation into the hydrogen inhibition mechanism of Platycladus orientalis leaf extract as a biodegradation inhibitor for waste aluminum-silicon alloy dust in wet dust collectors

This study investigates the risk of hydrogen explosion caused by waste metal dust encountering water in wet dust collectors. It proposes using renewable plant extracts to suppress hydrogen evolution from aluminum-silicon (Al-Si) alloy dust, aiming to achieve intrinsically safer production. Platycladus orientalis leaf extract (POLE) was prepared using water as a solvent. Hydrogen inhibition experiments, material characterization, and theoretical calculations were conducted to evaluate the effect of POLE on waste Al-Si dust. The inhibition experiments demonstrated that POLE exhibits excellent inhibitory performance. At a POLE concentration of 2.0 g/L, the hydrogen inhibition efficiency reaches 97.71 % after 22 h, with a reaction rate constant of 8.9708 × 10−5, approaching zero. This efficiency remained stable over 5 days. POLE formed a uniform, dense protective film on the Al-Si dust surface, with a contact angle of 99.23°. FTIR spectra revealed absorption peaks corresponding to POLE functional groups and Al-O bonds, indicating that successfully adsorption of POLE through both physical and chemical interactions. Finally, theoretical calculations were performed to further explain the hydrogen inhibition mechanism of POLE, supplementing and confirming the characterization data. This study inhibited hydrogen production from waste dust, offering a new approach to enhancing the hydrogen production rate from recycled Al scraps.

Hedgehog Zinc Oxide-Graphene Quantum Dot Heterostructures as Photocatalysts for Visible-Light-Driven Water Splitting.

The development of efficient photocatalysts for sustainable hydrogen production via water splitting is vital for advancing renewable energy technologies. In this study, we present the synthesis and characterization of a novel visible-light-active photocatalyst comprising hedgehog-shaped zinc oxide (ZnO) nanostructures coupled with graphene quantum dots (GQDs). Optical properties assessed by UV-visible and photoluminescence (PL) spectroscopy revealed that the ZnO/GQDs heterostructure possessed a reduced band gap (2.86 eV) compared with pristine ZnO (3.10 eV), resulting in improved light absorption and charge separation. Electrochemical analyses indicated a significantly higher photocurrent response and lower charge transfer resistance for the ZnO/GQDs heterostructure compared with the pristine ZnO nanostructure. Photocatalytic tests demonstrated that the ZnO/GQDs heterostructure achieved over 3-fold higher hydrogen (H2) production rates, with an apparent quantum yield (AQY) of 1.51% at 440 nm, and maintained stable activity over prolonged reaction periods. These results highlight the enhanced photocatalytic efficiency and stability of the ZnO/GQDs heterostructure, underscoring its potential as a high-performance photocatalyst for sustainable hydrogen generation. The synergistic effects between ZnO nanostructures and GQDs offer valuable insights into the design of advanced photocatalytic materials for renewable energy applications.

Nitrogen-doped ZnIn2S4 and TPA multi-dimensional synergistically enhance photocatalytic hydrogen production

To alleviate the environmental pollution and energy crisis caused by the excessive use of fossil fuels, photocatalytic water splitting to produce hydrogen is an important way to solve energy and environmental problems. Here, Nitrogen-doped ZnIn2S4 (N-ZIS) composite tungsten-based polyoxometalate (TPA) composites (denoted as N-ZIS/TPA) were synthesized by a one-step solvothermal method. The introduction of N3– instead of S2− in ZIS changes the internal electron arrangement of ZIS, improves the electronegativity of ZIS, and is conducive to the surface adsorption of positively charged H*. At the same time, the impurity energy level is generated at the valence band position, which narrows the band gap and broadens the light absorption range, thereby promoting photocatalytic hydrogen production. After compounding, due to the adjustable redox properties of TPA itself, the internal W6+ part is reduced to W4+, resulting in the coexistence of W6+ and W4+ in the composite material, which fully verifies the flow of interface electrons from N-ZIS to TPA. The close contact between N-ZIS and TPA and the built-in electric field’s driving force help achieve efficient interfacial charge transfer. At the same time, W6+/W4+ redox pairs were introduced to accelerate the separation of photogenerated electrons and holes. The photocatalytic hydrogen production rate of the best sample 1N-ZIS/TPA-15 is as high as 17345.53 μmol·g−1·h−1, which is 2.92 times that of N-ZIS (5940.08 μmol·g−1·h−1) and 8.03 times that of ZIS (2159.22 μmol·g−1·h−1). This study explores the design and construction of efficient s-type heterojunctions by adjusting the energy band position of ZnIn2S4 as a new strategy in the field of photocatalytic hydrogen production.

Insight into the unique role of silver single-atom in atomic-thickness ZnIn2S4/g-C3N4 Van der Waals heterojunction for photocatalytic hydrogen evolution

The construction of ultra-close 2D atomic-thickness Van der Waals heterojunctions with high-speed charge transfer still faces challenges. Here, we synthesized single-layer ZnIn2S4 and g-C3N4, and introduced silver single atoms to regulate Van der Waals heterojunctions at the atomic level to optimize charge transfer and catalytic activity. At the atomic scale, the impact of detailed structural differences between the two characteristic surfaces of ZnIn2S4 ([Zn-S4] and [In-S4]) on catalytic performance has been first proposed. Experiments combined with the DFT study demonstrate that single atom Ag not only acts as a charge transfer bridge but also regulates the energy band and intrinsic catalytic activity. Benefiting from the enhanced electron delocalization, the synthesized catalyst ZIS/Ag@CN exhibits excellent photocatalytic performance, with a hydrogen production rate of 5.50 mmol·g−1·h−1, which is much higher than the reported Ag-based single-atom catalysts so far. This work provides a new understanding of atomic-level heterojunction interface regulation and modification.

Unveiling the Role of Boron on Nickel‐Based Catalyst for Efficient Urea Oxidation Assisted Hydrogen Production

AbstractUrea oxidation reaction (UOR) is an ideal alternative to oxygen evolution reaction (OER) for efficient hydrogen production but is immensely plagued by slow kinetics. Herein, a multilayer hole amorphous boron‐nickel catalyst (a‐NiBx) is fabricated through a simple chemical plating method, which displays intriguing catalytic activity toward UOR, demanding a low working potential of 1.4 V to reach 100 mA cm−2. The high performance is credited to the formation of metaborate (BO2−), which can promote the formation of high‐oxidation‐state NiOOH active phase and optimize the adsorption of urea molecules. This can be confirmed by the operando spectroscopy characteristics and density functional theory calculations. Consequently, the assembled electrolyzer utilizing NiBx as bifunctional catalysts exhibited splendid catalytic activity, requiring an evidently lower voltage of 1.66 V to reach a current density of 100 mA cm−2 and 1.57 V when using Pt/C as a cathode catalyst. Moreover, the assembled electrolyzer secured a robust stability of over 200 h, as well as a four times higher hydrogen production rate than traditional water electrolysis.

Photoelectrolysis of glucose and fructose containing solution in PGM-free cells for hydrogen and valuable chemicals production

This study investigates the reforming of glucose and fructose by photoelectrolyis, employing TiO2 NTs photoanodes for the selective oxidation of the carbohydrates and Ni foam as cathode. TiO2 NTs with different structural features were grown on Ti felt via anodizing and annealing to promote their crystallization.These electrodes were tested in aqueous solutions at three different pH values (i.e., 2, 7, and 12) both without and with the addition of biomass. When biomass was present, the hydrogen production rate increased, reaching faradic efficiencies (FEs) ∼ 100% in spite of the use of undivided cell, allowing the simultaneous production of valuable partial oxidation compounds, such as gluconic acid (GA) and formic acid (FA), with FEs of 24% and 55% respectively, and overall quantum yields of 5.67% and 4.36% respectively. The photoanodes used demonstrated high mechanical and chemical stability under all the tested conditions, with electrode performance remaining consistent over time, allowing the reuse of the same electrode for a not limited number of runs after a mild cleaning step.The results demonstrated that this photoelectrocatalytic (PEC) process is promising for both biomass valorization and H2 production.

Oxygen vacancies promoted hydrogen production from methanol aqueous phase reforming over MgAl−LDHs supported plasmonic Ru nanoparticles catalyst

Catalytic aqueous phase reforming of methanol is a promising process for the sustainable hydrogen production. The search for highly efficient heterogeneous catalyst is a topic of interest. Herein, we report oxygen vacancies enriched MgAl−LDHs supported plasmonic Ru nanoparticles catalyst exhibit excellent photocatalytic performance for efficient hydrogen production at 150 ºC under light irradiation. Characterizations demonstrate abundant oxygen vacancies are introduced into MgAl−LDHs via “memory effect”. The local electron transfer from oxygen vacancies of the MgAl−LDHs to the Ru nanoparticles leading the formation of electron-rich Ru species, which promote the dehydrogenation of methanol under light irradiation. In situ DRIFTS demonstrated a redox mechanism of water-gas shift reaction due to the existence of oxygen vacancies, which resulted a faster hydrogen production rate. This work displays a facile strategy for synthesis of oxygen vacancies rich LDH supported metal nanoparticles catalysts and deep understanding into the pathway and mechanism toward the effective hydrogen production.

Improvement in the Photocatalytic Hydrogen Production of Flower-Shaped ZnIn2S4 by Surface Modification with Amino Silane

ZnIn2S4 has attracted extensive attention in the field of photocatalytic hydrogen production because of its suitable band gap and excellent photoelectrochemical properties. However, its lower photogenerated carrier separation efficiency and high degree of photocorrosion severely restricts its photocatalytic activity. In this work, the photocatalytic hydrogen production performance of ZnIn2S4 modified with 3-aminopropylmethoxysilane was studied. Surface modification by amino silane not only regulated the band gap and enhanced the light absorption of ZnIn2S4 but it also increased the colloidal stability of the ZnIn2S4 suspension and enhanced the adsorption of H+ on the active surface sites, thereby improving the photocatalytic hydrogen production performance. Compared with that of unmodified ZnIn2S4, the photocatalytic hydrogen production rate of surface-modified ZnIn2S4 increased by 1.46 times, and after four cycles for 12 h, the hydrogen production efficiency remained at 75.14%.

Hierarchical Bi2Fe4O9/BiOI S-scheme heterojunctions with exceptional hydraulic shear induced photo-piezoelectric catalytic activity

Hierarchical Bi2Fe4O9/BiOI S-scheme nanoflower heterostructures are prepared by hydrothermal method, which exhibit exceptional photo-piezoelectric catalytic performance. The tight binding between the sheets ensures the efficient electron transport, and provides a large interface area and adequate reaction sites for photo-piezoelectric catalytic reactions. At the same time, because the water flow in the water body produces hydraulic shear force on the material, the material produces piezoelectric effect. Bi2Fe4O9/BiOI exhibit a remarkable degradation efficiency of 99.4% for tetracycline and a hydrogen production rate of 4089.36 µmol h−1 g−1. The observed behavior can be explained by the combined influence of the formation of S-scheme structure and the process of photo-piezoelectric catalysis, confirmed by in-situ XPS, transient/steady-state fluorescence and piezoelectric response force test. The excellent stability of the material suggests its possible use in the sectors of energy and environment. This work introduces novel concepts for the future advancement of photo-piezoelectric synergistic catalysis.

Prediction of hydrogen production in proton exchange membrane water electrolysis via neural networks

Advancements in water electrolysis technologies are crucial for green hydrogen production. Proton exchange membrane water electrolysis (PEMWE) is characterized by its efficiency and environmental benefits. The prediction and optimization of hydrogen production rates (HPRs) in PEMWE systems is difficult and still challenging because of the complexity of the system as well as the operational parameters. The integration of artificial intelligence (AI) and machine learning (ML) appears to be effective in optimization within the energy sector. Hence, this work employs the artificial neural network (ANN) to develop a model that accurately predicts HPR in PEMWE setups. A novel approach is introduced by employing the Levenberg–Marquardt backpropagation (LMBP) algorithm for training the ANN. This model is designed to predict HPR based on critical operational parameters, including anode and cathode areas (mm2), cell voltage (V) and current (A), water flow rate (mL/min), power (W), and temperature (K). The optimized ANN configuration features an architecture with 7 input nodes, two hidden layers of 64 neurons each, and a single output node. The performance of the ANN model was evaluated against conventional regression models using key metrics: mean squared error (MSE), coefficient of determination (R2), and mean absolute error (MAE). The findings of this study reveal that the developed ANN model significantly outperforms traditional models, achieving an R2 value of 0.9989 and an MAE of 0.012. In comparison, random forest (R2 = 0.9795), linear regression (R2 = 0.9697), and support vector machines (R2 = − 0.4812) show lower predictive accuracy, underscoring the ANN model's superior performance. This work demonstrates the efficiency of the LMBP in enhancing hydrogen production forecasts and sets a foundation for future improvements in PEMWE efficiency. By enabling precise control and optimization of operational parameters, this study contributes to the broader goal of advancing green hydrogen production as a viable and scalable alternative to fossil fuels, offering both immediate and long-term benefits to sustainable energy initiatives.

Hydrogen production with a novel coaxial cylindrical electrolyser: A CFD study

This study introduces a unique coaxial cylindrical electrode design for Alkaline Water Electrolysers (AWEs) that is analyzed to show possible enhancements over the traditional stacked plate design. It investigates the performance of the proposed coaxial AWE for enhanced hydrogen production. Through comprehensive computational simulations, key performance indicators, such as current density and hydrogen volume fraction, are analyzed across various operating parameters. The results of this study indicate that the production rate of hydrogen achieves its highest level at a volume percentage of 3.4 %. This rate is significantly influenced by the concentration of the electrolyte, the distance between the cathode and anode rings, and, to a lesser degree, the porosity of the separator. Consequently, the optimized conditions demonstrate a promising increase in current densities, reaching 1000 mA/cm2 at an operating voltage of 2 V, showcasing the potential for developing more efficient and cost-effective AWE systems. This study further contributes valuable insights into the design and operational improvements needed for the advancement of large-scale hydrogen production technologies.

Preparation of Bi@Ho3+:TiO2/Composite Fiber Photocatalytic Materials and Hydrogen Production via Visible Light Decomposition of Water

Using electrospun nanofibers doped with TiO2 and rare-earth ion Ho3+ as the matrix, and sodium gluconate as the reducing agent, Bi(NO3)3 was reduced using hydrothermal technology to produce Bi@Ho3+:TiO2 composite fiber materials. The materials’ phase, morphology, and photoelectric properties were characterized using various analytical testing methods, including X-ray diffraction (XRD), scanning electron microscopy (SEM), transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS), ultraviolet-visible diffuse reflectance spectroscopy (UV-Vis DRS), and transient photocurrent (IP). During the hydrothermal process, it was confirmed that Bi3+ was reduced by sodium gluconate to form pure Bi nanoparticles, which combined with Ho3+:TiO2 nanofibers to form heterojunctions. By leveraging the surface plasmon resonance (SPR) effect of metallic Bi and the abundant energy level structure and 4f electron transition properties of rare-earth Ho3+, the TiO2 nanofibers underwent dual modification, effectively enhancing the photocatalytic activity and stability of TiO2. Under visible light irradiation, the rate of hydrogen production through water decomposition reached 43.6 μmol·g−1·h−1.

Fabricating FeS2/Mn0.3Cd0.7S S-scheme heterojunction for enhanced photothermal-assisted photocatalytic H2 evolution under full-spectrum light

To effectively harness solar energy, the rational construction and development of full-spectrum photocatalysts has become an appealing challenge. In this study, a novel full-spectrum responsive FeS2/Mn0.3Cd0.7S (FS/MCS) S-scheme photocatalyst was obtained by attaching FeS2 nanoparticles with excellent photothermal properties on Mn0.3Cd0.7S nanorods. The photocatalytic hydrogen production rate of the optimal FS/MCS composite was 52.017 mmol·g−1·h−1 under full-spectrum irradiation, which was 3.88 times that of pure MCS. Based on the experimental results and density functional theory (DFT) calculations, the enhanced photoactivity of FS/MCS was attributed to the synergetic effects of photothermal and S-scheme heterojunction. The photothermal effect of FeS2 could convert the near infrared light to heat, which elevated the local temperature of photocatalyst particles, thereby promoting the photocatalytic reaction. Meanwhile, the S-scheme heterojunction between FeS2 and Mn0.3Cd0.7S accelerated the charge transfer and suppressed the recombination of electron-hole pairs, thereby enabling efficient charge separation while maintaining high redox potentials. This work offers a novel perspective on constructing a full-spectrum-driven photothermal-assisted photocatalytic H2 evolution system though the dual effects of photothermal and heterojunction.

Assessing PEM fuel cell performance in a geothermal Cogeneration system for peak-time energy storage

In this investigation, a novel geothermal power plant was designed, combining absorption chiller units, PEMFC, EPEM, and ORC. We conducted a comprehensive case study across four continents—Asia, Oceania, Europe, and America—leveraging weather data from various cities to evaluate the system's efficacy. Our modeling utilized EES (Engineering Equation Solver) software, optimizing the setup via the RSM with three key objective functions: exergy efficiency, hydrogen production, and cost rate. The primary focus was on delivering electricity to residential properties during peak demand periods. Exploring six scenarios for organic fluids in organic Rankine cycles, we gauged energy, exergy, and overall system performance. The TOPSIS method led us to select scenario 3, employing R123 and R134a refrigerants, as the optimal choice. The results of the optimization showcased impressive figures: an exergy efficiency of 81.816%, a hydrogen production rate of 25.119 kg/h, and a cost rate of 15.967 $/h for the system's most efficient configuration. Economic analysis highlighted the organic Rankine cycle units 1 and 2 as the components with the highest costs. Our evaluation extended to various cities—Aomori, Grosseto, Lhasa, Wellington, and San Diego—assessing the electricity, heating, and cooling needs of residential complexes based on the system's performance.

Construction of ZnAl LDH-Derived Sulfides with Etching Modification to Trigger Photocatalytic H2 Production and Degradation Oxidation.

Constructing novel functional photocatalysts represents a promising approach to optimize the energy band structure and facilitate the separation of photogenerated carriers. Layered double hydroxides (LDHs) exhibit notable advantages in photocatalysis due to the exceptional photoelectrochemical properties and elevated number of active surface atoms. However, an unsuitable band gap and limited carrier migration have inhibited their development in photocatalysis. Herein, we propose a novel in situ topological vulcanization strategy for optimizing the photocatalytic activity of ZnAl LDH-derived sulfides (ZnAlSx). The subsequent etching process via a 1 M NaOH solution was introduced to construct the ZnSx photocatalysts. Then, the crystallinity of the crystals was enhanced by etching to further improve the catalytic activity and stability of ZnSx. The as-synthesized ZnSx shows an excellent photocatalytic hydrogen production rate (11.89 mmol/g/h) and tetracycline degradation efficiency (91.94%) under light illumination, and its hydrogen evolution efficiency is approximately 176 and 2 times greater than that of ZnAl LDH and ZnAlSx, respectively. The characterization and density functional theory (DFT) analysis confirmed that the surface electronic properties and energy band structure of ZnAl LDH were significantly optimized after experimental treatment, resulting in enhanced carrier separation and photooxidative reduction capacity. Combining in situ topological vulcanization and etching to realize the functional conversion of ZnAl LDH provides promising insights into the construction of high-performance, low-cost photocatalysts.