Efficient Photocatalytic System Research Articles

Distinct Pathways Determined by Photocatalytic C─H or O─H Bond Activation for Hydroxyl Compounds Conversion Paired With Hydrogen Production

AbstractSelective control of C─H or O─H bond activation in photocatalytic conversion coupled with hydrogen production is a promising yet challenging goal. Here, an efficient photocatalytic system is reported that can produce high‐valued tartaric acid or formaldehyde and simultaneous producing hydrogen. At optimized conditions, the directional conversion of glycolic acid into tartaric acid is achieved with a selectivity of 76.24%, and the selectivity of methanol oxidation into formaldehyde reaches 88.21%. A high hydrogen production rate of 21.43 mmol·g−1·h−1 is obtained using glycolic acid as substrate. Mechanism studies reveal that α‐C─H bond is preferentially activated in glycolic acid adsorbed on the photocatalyst, while O─H bond is preferentially activated in methanol, forming carbon‐centered radical (•CH(OH)COOH) or oxygen‐centered radical (CH3O•) for subsequent coupling or oxidation reactions. This work demonstrates the selective control of the photocatalytic conversion process of different hydroxyl compounds, providing a new perspective for achieving organic compounds selective activation coupled with hydrogen production.

Mitochondria‐Targeted Photoredox Catalysis Activates Pyroptosis for Effective Tumor Therapy

AbstractThe development of biocompatible and efficient photocatalytic redox systems to mimic bio‐photoreactors in living cells holds great potential for manipulating intracellular biochemical reaction processes and thus advancing tumor therapy. In this study, a mitochondria‐targeted photoredox catalyst, 2D vacancy‐rich molybdenum oxide nanosheets (Mt‐VR‐MoO3) is presented. These nanosheets possess a high density of oxygen vacancies (19.2%) and exhibit strong photocatalytic redox activity under near‐infrared (NIR) light. Following a two‐step functionalization, Mt‐VR‐MoO3 effectively disrupts mitochondrial electron flow in an oxygen‐independent manner upon irradiation with second near‐infrared (NIR‐II) light. This targeted disruption leads to on‐demand induction of substantial damage to tumor cell mitochondria, characterized by increased production of mitochondrial reactive oxygen species (mtROS) and the release of cytochrome c (Cyt c), which collectively trigger the pyroptosis of cancer cells. The approach achieved tumor‐targeted photocatalytic eradication with high efficacy (tumor growth inhibition rate of 86.9%) in an orthotopic breast 4T1 murine tumor model, with no observable harm to normal organs. These findings provide inspiration for manipulating intracellular biochemical reactions using artificial photocatalytic materials, paving the way for pyroptosis activation as a promising approach in tumor therapy.

Generation of Triplet States by Host‐Stabilized Through‐Space Conjugation for the Construction of Efficient Supramolecular Photocatalysts

AbstractPromoting the generation of triplet states is essential for developing efficient photocatalytic systems. This research presents a novel approach of host‐stabilized through‐space conjugation via the combination of covalent and non‐covalent methods. The designed building block, 4,4′‐(1,4(1,4)‐dibenzene cyclohexaphane‐1,4‐diyl)bis(1‐phenylpyridinium) chloride, features inherently stable through‐space conjugation. When this block forms a 1 : 1 host–guest complex with cucurbit[8]uril, the through‐space conjugation is further stabilized within the confined cavity. Both the generation and lifetime of triplet state are significantly increased, resulting from the host‐stabilized through‐space conjugation. Additionally, the ultrahigh binding constant of 6.58×1014 M−1 ensures the persistence of host‐stabilization effect. As a result, the host–guest complex acts as a highly efficient catalyst in the photocatalytic oxidation of thioether and aromatic alcohol. In the photodegradation of lignin, a complex natural product, the host–guest complex also exhibits high efficiency, demonstrating its robustness. This line of research is anticipated to enrich the toolbox of supramolecular photochemistry and provide a strategy for fabricating efficient supramolecular photocatalysts.

Engineered self-assembled protein nanosheets for in situ biosynthesis of peptide anchored protein-semiconductor hybrids for efficient hydrogen production

Catalytic hydrogen production using solar energy is of great significance in addressing the global energy crisis. Herein, an efficient artificial photocatalytic hydrogen production system based on hierarchical protein self-assembly is designed and developed by in situ biosynthesis of peptide-anchored protein-semiconductor hybrids. The self-grown protein-CdS quantum dot hybrids stabilize and array orderly by the predesigned bioengineered proteins assembled into monolayer nanosheets, perfectly mimicking both the structure and function of the natural photosynthetic system. By mild deposition of Pt nanoparticles, the photocatalytic hydrogen production performance of the system is further enhanced to 69100 μmolh−1 (Cd2+) g −1, 80 times the catalytic activity of free CdS. Remarkably, the protein 2D network effectively enhances the water solubility, dispersibility, and solution stability of the inorganic catalytic centers, affording efficient photocatalytic hydrogen evolution. The system maintains 91.2 % catalytic efficiency after 30 days. Furthermore, its hydrogen production rate can be artificially regulated between 69100 and 52100 μmolh−1 (per g Cd2+) by the assembly-disassembly process of the protein templates. Thus, our work showcases the importance of the protein template and its assembly in maintaining the structural stability and high catalytic performance of the photocatalytic system and provides promising ideas for the simulation of natural photosynthetic systems.

Facts and Fictions About Photocatalytic CO2 Reduction to C2+ Products.

In response to carbon neutrality, photocatalytic reduction of CO2 has been the subject of growing interest for researchers over the past few years. Multi-carbon products (C2+) with higher energy density and larger market value produced from photocatalytic reduction of CO2 are still very limited owing to the low photocatalytic productivity and poor selectivity of products. This review focuses on the recent progress on photocatalytic reduction of CO2 towards C2+ products from the perspective of performance evaluation and mechanistic understanding. We first provide a systematic description of the entire fundamental procedures of photocatalytic reduction of CO2. An in-depth strategy analysis for improving the selectivity of photocatalytic reduction of CO2 to C2+ products is then addressed. Then the focus was on summarizing the ways to improve C2+ selectivity. The intrinsic mechanisms of photocatalytic reduction of CO2 to C2+ products are summarized in the final. Combining the foundation of photocatalysis with promising catalyst strategies, this review will offer valuable guidance for the development of efficient photocatalytic systems for the synthesis of C2+ products.

Single-Particle Fluorescence Spectroscopy for Elucidating Charge Transfer and Catalytic Mechanisms on Nanophotocatalysts.

Photocatalysis is a cost-effective approach to producing renewable energy. A thorough comprehension of carrier separation at the micronano level is crucial for enhancing the photochemical conversion capabilities of photocatalysts. However, the heterogeneity of photocatalyst nanoparticles and complex charge migration processes limit the profound understanding of photocatalytic reaction mechanisms. By establishing the precise interrelationship between microscopic properties and photophysical behaviors of photocatalysts, single-particle fluorescence spectroscopy can elucidate the carrier separation and catalytic mechanism of the photocatalysts in situ, which provides perspectives for improving the photocatalytic efficiency. This Review primarily focuses on the basic principles and advantages of single-particle fluorescence spectroscopy and its progress in the study of plasmonic and semiconductor photocatalysis, especially emphasizing its importance in understanding the charge separation and photocatalytic reaction mechanism, which offers scientific guidance for designing efficient photocatalytic systems. Finally, we summarize and forecast the future development prospects of single-particle fluorescence spectroscopy technology, especially the insights into its technological upgrading.

Photocatalytic Ammonia Decomposition Using Dye-Encapsulated Single-Walled Carbon Nanotubes

The photocatalytic decomposition of ammonia to produce N2 and H2 was achieved using single-walled carbon nanotube (SWCNT) nanohybrids. The physical modification of ferrocene-dye-encapsulated CNTs by amphiphilic C60-dendron yielded nanohybrids with a dye/CNT/C60 coaxial heterojunction. Upon irradiation with visible light, an aqueous solution of NH3 and dye@CNT/C60-dendron nanohybrids produced both N2 and H2 in a stoichiometric ratio of 1/3. The action spectra of this reaction clearly demonstrated that the encapsulated dye acted as the photosensitizer, exhibiting an apparent quantum yield (AQY) of 0.22% at 510 nm (the λmax of the dye). This study reports the first example of dye-sensitized ammonia decomposition and provides a new avenue for developing efficient and sustainable photocatalytic hydrogen production systems.

Enhanced photocatalytic oxidation of gaseous acetaldehyde using Fe-grafted ZnO nanocomposites in a continuous flow reactor

The purification of indoor air is a crucial application of photocatalysis, emphasizing the urgent need for more efficient photocatalytic systems. While photocatalytic oxidation of volatile organic compounds (VOCs) has been extensively studied in the liquid phase, effective removal of VOCs in the gaseous state in indoor air remains a significant challenge. This study focuses on the continuous gas-phase oxidation of gaseous acetaldehyde using ZnO and different weight percentage of Fe-grafted ZnO catalysts under light irradiation. The surface analysis using XPS and HR-TEM confirmed the presence of Fe(III) species, and UV–Vis-DRS analysis demonstrated a shift in the absorption edge towards the visible region. Real-time gas FTIR monitoring of acetaldehyde oxidation revealed that the 0.7% Fe(III)-grafted ZnO composite catalyst achieved a higher removal efficiency (74%) compared to bare ZnO and other Fe(III)-grafted ZnO ratios. The enhanced photocatalytic efficiency of acetaldehyde by Fe(III)-grafted ZnO supports indicated direct interfacial charge transfer (IFCT) from ZnO to Fe(III) species. Additionally, the Fe(III) cluster effectively improved the separation of electrons and holes, preventing their recombination and accelerating O₂ activation to generate O₂•⁻ radicals, which lead to high photocatalytic performance. The 0.7% Fe(III)-grafted ZnO also maintained its performance over a prolonged period of 360 min, showing excellent structural stability and durability across multiple cycles. This study highlights the possible synergistic effect of the ZnO and Fe systems, offering a new perspective on the photocatalytic decomposition of gaseous acetaldehyde in indoor environments.

Efficient photocatalytic H2O2 production and green oxidation of glycerol over a SrCoO3-incorporated catalyst

Photocatalysis for H2O2 production suffers from low carrier utilization and slow reaction kinetics. Herein, a photocatalytic system supported by a SrCoO3-MoS2 (SCOS) heterojunction, which possessed a unique S-O electron transport channel, was proposed to facilitate H2O2 production under condition where glycerol served as a sacrificial agent. The SCOS heterojunction achieved a remarkable yield of 15.90 mmol g−1 h−1 H2O2 production, 3.7 times higher than the base component SCO. The construction of the heterojunction enriched the oxygen vacancies on the catalyst surface, facilitated photogenerated charge separation, and promoted the adsorption of O2, reducing the oxygen reduction reaction (ORR) energy barrier. Besides, glycerol served as a unique proton donor, efficiently captured holes to enhance H2O2 production, and generated valuable by-products including glyceric acid and dihydroxyacetone. Furthermore, SCOS exhibited excellent stability over repeated cycles with consistent H2O2 yields. This study offers an efficient photocatalytic system and demonstrates glycerol’s potential in green oxidation processes.

Ferroelectric polarization synergism boosting CdS/PbTiO3 S-scheme heterostructures for efficiently bifunctional environmental applications

It is of great significance and challenges to construct physical field-enhanced photocatalysts for energy and environmental applications. Herein, an artificial-photosynthesized CdS/PbTiO3 S-scheme heterostructures with the enhancement of polarization electric field have been developed to promote the bifunctionally catalytic efficiencies for Cr(VI) photoreduction degradation of heavy metal pollution and Tetracycline (TC) photooxidation degradation of antibiotic. In our work, CdS nanoparticles are selectively grown on the positive polarization planes of PbTiO3 microplates to form the same direction for both the ferroelectric polarization field of PbTiO3 and the built-in electric field of S-scheme heterojunction. In this case, the stable heterostructures of PTO(00−1)/CdS(010) are obtained, and the greatly improved photocatalytic performances of redox degradation are achieved. The charge transfer mechanism and the synergetic effect between the spontaneous ferroelectric polarization and S-scheme heterojunction have been revealed by DFT calculations and experimental verifications. This interesting finding provides new insight into the design of efficient artificial-photosynthesized photocatalytic systems and we hope our work could serve as a valuable reference for our colleagues.

Modeling sustainable photocatalytic degradation of acidic dyes using Jordanian nano-Kaolin–TiO2 and solar energy: Synergetic mechanistic insights

The abstract highlights the global issue of environmental contamination caused by organic compounds and the exploration of various methods for its resolution. One such approach involves the utilization of titanium dioxide (TiO2) as a photocatalyst in conjunction with natural adsorption materials like kaolin. The study employed a modeling-based approach to investigate the sustainable photocatalytic degradation of acidic dyes using a Jordanian nano-kaolin–TiO2 composite material and solar energy. Mechanistic insights were gained through the identification of the dominant reactive oxygen species (ROS) involved in the degradation process, as well as the synergetic effect between adsorption and photocatalysis. The Jordanian nano-kaolin–TiO2 composite was synthesized using the sol-gel method and characterized. The nanocomposite photocatalyst exhibited particle sizes ranging from 27 to 41 nm, with the TiO2 nanoparticles well-dispersed within the kaolin matrix. The efficacy of this nanocomposite in removing Congo-red dye was investigated under various conditions, including pH, initial dye concentration, and photocatalyst amount. The optimal conditions for dye removal were found to be at pH 5, with an initial dye concentration of 20 ppm, and using 0.1 g of photocatalyst, resulting in a 95 % removal efficiency. The mechanistic insights gained from this study indicate that the hydroxyl radicals (•OH) generated during the photocatalytic process play a dominant role in the degradation of the acidic dye. Furthermore, the synergetic effect between the adsorption of the dye molecules onto the photocatalyst surface and the subsequent photocatalytic degradation by the ROS was found to enhance the overall removal efficiency. These findings contribute to the fundamental understanding of the photodegradation mechanisms and guide the development of more efficient photocatalytic systems for the treatment of acidic dye-containing wastewater. The use of solar power during the purification procedure also leads to cost reduction and strengthens sustainability efforts.

Triangle CeO2/g-C3N4 heterojunctions: Enhanced light-driven photocatalytic degradation of methylparaben

In this work, an efficient photocatalytic system for methylparaben (MP) removal, using solar (λ > 360 nm) and visible (λ > 420 nm) light-driven CeO2/g-C3N4 (CeO2/CN) heterojunctions is reported for the first time. The physicochemical properties of pure CeO2, CN, and CeO2/CN composites were investigated using characterization techniques, such as XRD, FESEM-EDS, TEM, UV–Vis, PL, XPS, and electrochemical spectroscopy. Among the catalysts with different mass ratios of CeO2, 10 %CeO2/CN showed the best photocatalytic performance. This is attributed to the enhanced charge carrier’s separation because of the proper band-edge alignment between CN and CeO2 components, and the strong visible light absorbance. The photocatalytic degradation of MP followed the first-order kinetics, and the 10 %CeO2/CN catalyst exhibited a 3.8- and 11.3-times higher reaction rate (k) constant than that of pure CN, investigated under solar and visible light illumination, respectively. Further, scavenger trapping experiments confirmed that hydroxyl radicals (OH.) and dissolved oxygen are the predominant active species in MP oxidation over 10 %CeO2/CN composite catalyst. 1H NMR and LCMS-HPLC results and observations showed complete degradation of MP (0.1 g/L) to CO2 and H2O after 7 h of solar irradiation, due to the absence of the representative peaks of MP and its organic degradation products (e.g. phenols, benzoates).

Enhanced photocatalytic performance of CdZnS nanoparticles and attapulgite/carbon nitride composites by carbon quantum dots mediated facilitated charge separation/transfer: Cr(VI) reduction and H2O2 production

In this work, CdZnS@carbon quantum dots/amino-modified attapulgite/carbon nitride (CdZnS@CQDs/M-ATP/PCN), function as Z-scheme heterojunction photocatalysts, have been successfully prepared by the hydrothermal method. CdZnS@CQDs-1/M-ATP/PCN-1 was optimized toward reduction of Cr(VI) and production of H2O2 under visible light, showing significantly improved photocatalytic performance. After coupling of M-ATP/PCN-1 with CdZnS and a moderate addition of CQDs, the synergistic formation of Z-scheme heterojunctions photocatalytic system effectively enhanced the photocatalytic properties of the composites. The results revealed that the CdZnS@CQDs/M-ATP/PCN catalysts contain rich active centers and suitable energy band structures, which enable them to produce more OH and O2−. Additionally, they also absorb visible light strongly and thus effectively improves the photocatalytic activity. Specifically, the reduction of Cr(VI) by CdZnS@CQDs-1/M-ATP/PCN-1 catalyst was achieved greater than 97.6 %, along with the production of 719.32 μmol·L−1 H2O2. Combining density functional theory (DFT) calculations, experimental test results and characterizations, we find that the excellent photocatalytic performance is attributed to the incorporation of CQDs and the formation of Z-scheme heterojunctions. We have developed a non-precious metal-based efficient Z-scheme photocatalytic system using simple hydrothermal synthesis method, which has a very high potential for energy production, environmentally sustainable remediation, and water purification.

Hetero-integration of cadmium sulfide nanorod arrays on graphite substrates to guide electron pathways for effective photocatalytic and photoelectrochemical activities

One-dimensional (1D) cadmium sulfide (CdS) nanostructures in photosynthetic systems have attracted attention because of their effective transport pathways for charge extraction which are essential for efficient photocatalytic and photoelectrochemical systems. Despite the numerous benefits of aligned 1D CdS nanostructures in photosynthetic systems, limited attention has been paid to hetero-integrating 1D CdS arrays on substrates with rapid charge extraction capabilities and practical applicability. Herein, we report the fabrication of vertically aligned CdS nanorod arrays on graphite substrates, in which electron transport pathways are rationally designed for effective photocatalysts and photoanodes. Specifically, CdS nanorod arrays integrated on graphite substrates exhibited photocatalytic reactions with excellent reusability and photostability owing to their superior bifacial properties compared to the control free-standing nanostructures. The proposed system also demonstrated excellent photoelectrochemical performance relative to control CdS nanorod arrays integrated on fluorine-doped tin oxide substrates because of the enhanced separation and extraction of photogenerated electrons combined with curvilinear surfaces.

Interfacial linkage modulated amorphous molybdenum sulfide/bismuth halide perovskite heterojunction for enhanced visible-light-driven photocatalytic hydrogen evolution

Photocatalytic hydrogen evolution is a promising approach for direct solar-to-fuel conversion. Although significant research efforts have been put on the development of lead-free metal halide perovskites to reach excellent optoelectronic properties, their rational design for efficient heterojunction photocatalytic systems still poses challenges. Here, we report a new strategy to tailor the interface of hybrid tri(dimethylammonium) hexaiodobismuthate (DMA3BiI6) and amorphous molybdenum sulfide (a-MoSx) heterojunctions. Specifically, a-MoSx was prepared with abundant apical S2– or bridging S22– ligands to allow coupling with DMA3BiI6 via an interfacial Mo–S–Bi linkage. The as-obtained heterostructures were found to show an improved visible-light-driven photocatalytic hydrogen evolution in hydroiodic acid splitting under mild conditions reaching a superior hydrogen evolution rate of around 750 µmol g−1 h−1 and an apparent quantum efficiency (AQE) of 13.0 % at 420 nm. The high activity was kept after a long-term performance test for 3 days.

Charge carrier controlled free radical construction efficient photocatalytic self-Fenton system

The photocatalytic self-Fenton technology has demonstrated unique advantages in the low-cost and efficient removal of environmental pollutants. Designing an efficient photocatalytic self-Fenton system (PSFs) to enhance the synergistic effect between photocatalytic H2O2 production and pollutant mineralization processes, as well as understanding the regulatory mechanism of free radical reactions in this process, are crucial for advancing this technology. In this study, an efficient PSFs was developed by coating COFs (TpPa-1) onto the surface of MXene (Ti3C2). Under visible light irradiation, the generation rate of H2O2 reached 983.9 μmol·g−1·h−1, which is 9 times that of pure TpPa-1. Additionally, this led to a significant increase in the removal rate of sulfamethoxazole (SMX) from 25 % to 92 % within 100 min. Photoelectrochemical tests and density functional theory (DFT) calculations confirmed that the incorporation of Ti3C2 not only facilitates efficient charge carrier transport but also enhances the generation of hydroxyl radicals (·OH) and the production of H2O2, thereby improving the photocatalytic self-Fenton removal efficiency of SMX. This research is expected to have a positive impact on the development of efficient PSFs.

Photonic crystal-assisted sub-bandgap photocatalysis via triplet-triplet annihilation upconversion for the degradation of environmental organic pollutants

This study explores novel approaches to enhance photocatalysis efficiency by introducing a photonic crystal (PC)-enhanced, multi-layered sub-bandgap photocatalytic reactor. The design aims to effectively utilize sub-bandgap photons that might otherwise go unused. The device consists of three types of layers: (1) two polymeric triplet-triplet annihilation upconversion (TTA-UC) layers converting low-energy green photons (λEx = 532 nm, 2.33 eV) to high-energy blue photons (λEm = 425 nm, 2.92 eV), (2) a platinum-decorated WO3 layer (Eg = 2.8 eV) serving as a visible-light photocatalyst, and (3) a PC layer optimizing both TTA-UC and photocatalysis. The integration of the PC layer resulted in a 1.9-fold increase in UC emission and a 7.9-fold enhancement in hydroxyl radical (•OH) generation, achieved under low-intensity sub-bandgap irradiation (17.6 mW cm–2). Consequently, the combined layered structure of TTA/Pt-WO3/TTA/PC achieved a remarkable 38.8-fold improvement in •OH production, leading to outstanding degradation capability for various organic pollutants (e.g., 4-chlorophenol, bisphenol A, and methylene blue). This multi-layered sub-bandgap photocatalytic structure, which uniquely combines TTA-UC and PC layers, offers valuable insights into designing efficient photocatalytic systems for future solar-driven environmental remediation.

Ti-doped synergistic hollow thin-walled Bi2O3 nano-microspheres for efficient tetracycline hydrochloride photodegradation

Bismuth oxide (Bi2O3) has been extensively investigated in the fields of environmental photocatalysis, owing to its exceptional charge transport performance and remarkable resistance to photocorrosion. However, the limited absorption spectrum of light and rapid recombination of photogenerated charge results in a low quantum efficiency. Herein, an efficient photocatalytic system for tetracycline hydrochloride (TCH) photodegradation based on titanium (Ti)-doped hollow, thin-walled Bi2O3 with nano-microspheres is fabricated via a facile self-assembly strategy. It is shown that doping Ti in Bi2O3 can generate oxygen vacancies, in addition, the addition of Ti in the solvothermal process inhibits the conversion of Bi3+ to bismuth at high temperature, making the content of each component in the heterostructure controllable. The hybrid catalyst exhibits superior performance in visible-light-driven photocatalytic degradation of TCH (about 95.1 % degradation efficiency after 120 min) and excellent stability (up to 4 cycles) under visible light irradiation. The optimized catalyst exhibits excellent performance in visible light catalytic degradation, owing to the synergistic effect of high specific surface area, Bi plasma resonance effect and charge mobility. Moreover, the photocatalytic mechanism of Ti-Bi2O3 have been deeply analyzed through experimental investigation and DFT theoretical calculations. The findings contribute to the synthesis of efficient visible-light-driven Bi-based photocatalysts and to the understanding of photocatalytic degradation reactions.

Modulation of catalyst interfacial electric field and charge transfer promotes NiS-modified CoWO4/ZnIn2S4 S-scheme heterojunction for efficient photocatalytic hydrogen evolution

The strategic post-synthetic modification of engineered S-scheme heterojunctions represents a potent and manipulable approach to significantly enhance photocatalytic activity. This study details the synthesis of innovative photocatalysts via the deposition of NiS nanoparticles onto S-scheme heterojunctions of CoWO4/ZnIn2S4 (CWO/ZIS-NiS), facilitated by solvothermal and photochemical methodologies. Under visible light irradiation, the hydrogen production rate of CWO/ZIS-NiS was 22.304 mmol g−1 h−1, which 14.7 times higher than that of the ZnIn2S4. XPS, EPR, SPV and DFT calculations were used to analyze the charge transfer path and the reasons for the performance improvement of the catalyst. The construction of the S-scheme CoWO4/ZnIn2S4 heterojunction, along with NiS modification to enhance the interfacial electric field (IEF) and act as a reaction center, was identified as the primary reason for the enhanced hydrogen production activity. This work provides guidance for the design of efficient photocatalytic systems using the synergistic effect between cocatalysts and S-scheme heterojunctions.

Dual functional S-scheme ZnIn2S4/crystalline polymeric carbon nitride (ZIS/CPCN) heterojunction for efficient photocatalytic hydrogen evolution and degradation of levofloxacin

Developing dual functional catalysts for photocatalytic hydrogen evolution and pollutant degradation is one of the most ideal methods to address energy and environmental pollution. In the present study, an S-scheme ZnIn2S4/crystalline polymeric carbon nitride (ZIS/CPCN) heterojunction was synthesized using simple hydrothermal and calcination methods. The CPCN with a highly ordered heptazine-imide structure within the layer imparts a suitable band structure, while the widened interlayer spacing facilitates rapid electron transfer through surface engineering to construct heterojunctions. During the in-situ growth process, ZnIn2S4 uniformly distributes on the high surface area of CPCN as ultra-thin nanosheets. Under visible light irradiation, ZIS/CPCN-2 exhibited the highest hydrogen production activity (3492 μmol·g−1·h−1), which was 4 times and 112 times higher than ZIS and CPCN, respectively. Furthermore, the ZIS/CPCN catalyst demonstrated a certain degradation rate for quinolone antibiotics within 180 min, involving the •OH and •O2– radicals, and analyzed the degradation pathway of levofloxacin. The most stable configuration was obtained through theoretical calculations, and the density of states and work function of the sample were computed, proposing the S-scheme mechanism. This work contributes to the development of efficient photocatalytic systems with dual functions of hydrogen evolution and degradation.