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Constructing an efficient photoelectron transfer channel to promote the charge carrier separation is a great challenge for enhancing photocatalytic hydrogen evolution from water. In this work, an ultrathin 2D/2D Ti3C2Tx/ZnIn2S4 heterostructure is rationally designed by coupling the ultrathin ZnIn2S4 with few‐layered Ti3C2Tx via the electrostatic self‐assembly strategy. The 2D/2D Ti3C2Tx/ZnIn2S4 heterostructure possesses larger contact area and strong electronic interaction to promote the charge carrier transfer at the interface, and the sulfur vacancy on the ZnIn2S4 acting as the electron trap further enhances the separation of the photoinduced electrons and holes. As a consequence, the optimal 2D/2D Ti3C2Tx/ZnIn2S4 composite exhibits a high photocatalytic hydrogen evolution rate of 148.4 µmol h−1, which is 3.6 times and 9.2 times higher than that of ZnIn2S4 nanosheet and flower‐like ZnIn2S4, respectively. Moreover, the stability of the ZnIn2S4 is significantly improved after coupling with the few‐layered Ti3C2Tx. The characterizations and density functional theory calculation demonstrate that the synergistic effect of the sulfur vacancy and Ti3C2Tx cocatalyst can greatly promote the electrons transfer from ZnIn2S4 to Ti3C2Tx and the separation of photogenerated charge carriers, thus enhancing the photocatalytic hydrogen evolution from water. 2D/2D Ti3C2Tx/ZnIn2S4 heterojunction is constructed to achieve high‐efficiency photocatalytic hydrogen evolution under visible light. The synergistic effect of sulfur vacancies and Ti3C2Tx cocatalyst promotes the efficient transfer of photogenerated electrons at the 2D/2D interface, thus greatly enhances the photocatalytic hydrogen evolution performance of 2D/2D Ti3C2Tx/ZnIn2S4 composites.

Rational design hybrid nanostructure photocatalysts with efficient charge separation and transfer, and good solar light harvesting ability have critical significance for achieving high solar‐to‐chemical conversion efficiency. Here a highly active and stable composite photocatalyst is reported by integrating ultrathin ZnIn2S4 nanosheets on surface of hollow CdS cube to form the cube‐in‐cube structure. Experimental results combined with density functional theory calculations confirm that the Z‐scheme ZnIn2S4/CdS heterojunction is formed, which highly boosts the charge separation and transfer under the local‐electric‐field at semiconductor/semiconductor interface, and thus prolongs their lifetimes. Moreover, such a structure affords the highly enhanced light‐harvesting property. The optimized ZnIn2S4/CdS nanohybrids exhibit superior H2 generation rate under visible‐light irradiation (λ ≥ 420 nm) with excellent photochemical stability during 20 h continuous operation. The stable composite photocatalyst integrated by ultrathin ZnIn2S4 nanosheets on surface of hollow CdS exhibits outstanding visible‐light‐driven photocatalytic H2 generation activity, due to that: i) the Z‐scheme charge transfer route facilitates charge separation, prolongs carrier lifetimes, and remains strong electron reduction capacity; ii) the unique cube‐in‐cube structure brings abundant active sites, improves light harvesting ability, shortens charge transfer distance.

Achieving structure optimizing and component regulation simultaneously in the ZnIn2S4‐based photocatalytic system is an enormous challenge in improving its hydrogen evolution performance. 3D hollow‐structured photocatalysts have been intensively studied due to their obvious advantages in solar energy conversion reactions. The synthesis of 3D hollow‐structured ZnIn2S4, however, is limited by the lack of suitable template or synthesis methods, thereby restricting the wide application of ZnIn2S4 in the field of photocatalysis. Herein, Ce‐doped ZnIn2S4 photocatalysts with hollow nanocages are obtained via one‐step hydrothermal method with an ordered large‐pore tetrakaidecahedron cerium‐based metal–organic frameworks (Ce‐MOFs) as template and Ce ion source. The doping of Ce and the formation of ZnIn2S4 tetrakaidecahedron hollow nanocages with ultrathin nanosheet subunits are simultaneously induced by the Ce‐MOFs, making this groundbreaking work. The Ce‐doped ZnIn2S4 with a nonspherical 3D hollow nanostructure inherit the tetrakaidecahedron shape of the Ce‐MOF templates, and the shell is composed of ultrathin nanosheet subunits. Both theoretical and experimental results indicate that the doping of Ce and the formation of hollow nanocages increase light capture and the separation of photogenerated charge carriers. Ce‐doped ZnIn2S4 photocatalysts with hollow nanocages are obtained via one‐step hydrothermal method with an ordered large‐pore tetrakaidecahedron cerium‐based metal–organic frameworks as template and Ce ion source.

ZnIn2S4 (ZIS) is widely used in the field of photocatalytic hydrogen production due to its unique photoelectric properties. Nonetheless, the photocatalytic performance of ZIS usually faces problems of poor conductivity and rapid recombination of charge carriers. Heteroatom doping is often regarded as one of the effective strategies for improving the catalytic activity of photocatalysts. Herein, phosphorus (P)-doped ZIS was prepared by hydrothermal method, whose photocatalytic hydrogen production performance and energy band structure were fully studied. The band gap of P-doped ZIS is about 2.51 eV, which is slightly smaller than that of pure ZIS. Moreover, due to the upward shift of its energy band, the reduction ability of P-doped ZIS is enhanced, and P-doped ZIS also exhibits stronger catalytic activity than pure ZIS. The optimized P-doped ZIS exhibits a hydrogen production rate of 1566.6 μmol g−1 h−1, which is 3.8 times that of the pristine ZIS (411.1 μmol g−1 h−1). This work provides a broad platform for the design and synthesis of phosphorus-doped sulfide-based photocatalysts for hydrogen evolution.

Photocatalytic H2 evolution technology is regarded as a promising and green route for the urgent requirement of efficient H2 production. At present, low efficiency is a major bottleneck that limits the practical application of photocatalytic H2 evolution. The construction of high-activity photocatalysts is highly crucial for achieving advanced hydrogen generation. Herein, a new S-scheme FeS2@ZnIn2S4 (FeS2@ZIS) heterostructure as the photocatalyst was developed for enhanced photocatalytic H2 evolution. Density function theory (DFT) calculation results strongly demonstrated that FeS2@ZIS generates a giant interface electric field (IEF), thus promoting the separation efficiency of photogenerated charge carriers for efficient visible-light-driven hydrogen evolution. At optimal conditions, the H2 production rate of the 8%FeS2@ZIS is 5.3 and 3.6 times higher than that of the pure FeS2 and ZIS, respectively. The experimental results further indicate that the close contact between FeS2 and ZIS promotes the formation of the S-scheme heterojunction, where the interfacial charge transfer achieves spatial separation of charge carriers. This further broadens the light absorption range of the FeS2@ZIS and improves the utilization rate of photogenerated charge carriers. This work thus offers new insights that the FeS2-based co-catalyst can enrich the research on S-scheme heterojunction photocatalysts and improve the transfer and separation efficiency of photogenerated carriers for photocatalytic hydrogen production.

Hydrogen production technology has triggered a research boom in order to alleviate the problems of environmental pollution and the pressure on non-renewable energy sources. The key factor of this technology is the use of an efficient photocatalyst. g-C3N4 is a typical semiconductor photocatalytic material that is non-toxic and environmentally friendly and does not cause any serious harm to human beings. Therefore, it can be applied to drug degradation and the photocatalytic production of H2. Combined with ZnIn2S4, this semiconductor photocatalytic material, with a typical lamellar structure, has become one of the most promising catalysts for research due to its suitable bandgap structure and excellent photoelectric properties. In this study, 10% g-C3N4/ZnIn2S4 nano-heterojunction composite photocatalytic materials were successfully prepared by compounding ZnIn2S4 and g-C3N4 semiconductor materials with good visible-light-trapping ability. Under visible light irradiation, the photocatalytic activity of the composites was significantly better than that of pure g-C3N4 and ZnIn2S4. This is attributed to the formation of a heterojunction structure, which effectively inhibited the recombination of photogenerated carriers through the interfacial contact between the two semiconducting materials, and then improved the separation efficiency of the photogenerated electron–hole pairs, thus enhancing the catalytic activity. In this study, pure g-C3N4 and ZnIn2S4 were prepared using calcination and hydrothermal methods, and then, the composites were synthesized using ultrasonic and hydrothermal means. The differences in the structure, morphology, and hydrogen production performance of the materials before and after recombination were analyzed in detail using XRD, SEM, and FTIR characterization, which further verified that the 10% g-C3N4/ZnIn2S4 nano-heterojunction composites possessed excellent photocatalytic activity and stability, providing new possibilities for the optimization and application of photocatalytic hydrogen production technology.

Zinc indium sulfide (ZnIn2S4), as a significant visible-light-responsive photocatalyst, has become a research hotspot to tackle energy demand and environmental issues owing to its excellent properties of high stability, easy fabrication, and remarkable catalytic activity. However, its drawbacks, including low utilization of solar light and fast photoinduced charge carriers, limit its applications. Promoting the response for near-infrared (NIR) light (~52% solar light) of ZnIn2S4-based photocatalysts is the primary challenge to overcome. In this review, various modulation strategies of ZnIn2S4 have been described, which include hybrid with narrow optical gap materials, bandgap engineering, up-conversion materials, and surface plasmon materials for enhanced NIR photocatalytic performance in the applications of hydrogen evolution, pollutants purification, and CO2 reduction. In addition, the synthesis methods and mechanisms of NIR light-driven ZnIn2S4-based photocatalysts are summarized. Finally, this review presents perspectives for future development of efficient NIR photon conversion of ZnIn2S4-based photocatalysts.

New surface coordination photocatalytic systems that are inspired by natural photosynthesis have significant potential to boost fuel denitrification. Despite this, the direct synthesis of efficient surface coordination photocatalysts remains a major challenge. Herein, it is verified that a coordination photocatalyst can be constructed by coupling Pd and CTAB-modified ZnIn2S4 semiconductors. The optimized Pd/ZnIn2S4 showed a superior degradation rate of 81% for fuel denitrification within 240 min, which was 2.25 times higher than that of ZnIn2S4. From the in situ FTIR and XPS spectra of 1% Pd/ZnIn2S4 before and after pyridine adsorption, we find that pyridine can be selectively adsorbed and form Zn⋅⋅⋅C-N or In⋅⋅⋅C-N on the surface of Pd/ZnIn2S4. Meanwhile, the superior electrical conductivity of Pd can be combined with ZnIn2S4 to promote photocatalytic denitrification. This work also explains the surface/interface coordination effect of metal/nanosheets at the molecular level, playing an important role in photocatalytic fuel denitrification.

The gradual depletion of fossil fuel reserves that contribute to ~85% of global energy production and release of toxic effluents urges the transformation toward renewable fuels. Thus, the sustainable utilization of sunlight for water splitting and CO2 reduction with heterogeneous photocatalysts has come to light. As a semiconductor photocatalyst, ZnIn2S4 has hit the limelight owing to its narrow bandgap and visible‐light‐responsive properties. However, the limitations of ZnIn2S4 include limited active sites, fast charge‐carrier recombination, and low photoconversion efficiency. Beginning from the fundamental photocatalytic mechanism, this review then provides in‐depth insights into several modification strategies of ZnIn2S4, extending from defect engineering, facet engineering, cocatalyst loading to junction engineering, enabling the synergistic construction of high‐performance ZnIn2S4‐based systems. Subsequently, the structure‐performance relation of ZnIn2S4‐based photocatalysts for hydrogen evolution (HER), overall water splitting (OWS), and CO2 reduction applications in the last 4 years will be discussed and concluded by the future perspectives of this frontier. ZnIn2S4 has triggered great interest in the realm of artificial photosynthesis attributed to its narrow bandgap and visible‐light‐responsive properties. Concerning the shortcomings of pristine ZnIn2S4, a series of modification strategies has been proposed. This review discusses the surface and heterostructure engineering of ZnIn2S4 toward photocatalytic hydrogen evolution, overall water splitting, and CO2 reduction, with the challenges and recommendations prospected.

Effective charge separation and migration pose a critical challenge in the field of solar-driven hydrogen production. In this work, a Z-scheme structured CuInS2/ZnIn2S4 heterojunction was successfully fabricated through a two-step hydrothermal synthesis method to significantly enhance the efficiency of solar-to-hydrogen energy conversion. Structural characterization revealed that the lattice-matched CuInS2/ZnIn2S4 heterojunction exhibits an enlarged interfacial contact area, which facilitates the transfer and separation of photogenerated charges. Microscopic analysis indicated that the CuInS2/ZnIn2S4 composite material has a tightly interwoven interface and a morphology resembling small sugar cubes. Photoelectrochemical spectroscopy analysis demonstrated that the heterojunction structure effectively enhances visible light absorption and charge separation efficiency, leading to an improvement in photocatalytic activity. Hydrogen production experimental data indicated that the CuInS2/ZnIn2S4 heterojunction photocatalyst prepared with a CuInS2 content of 20 wt% exhibits the highest hydrogen evolution rate, reaching 284.9 μmol·g−1·h−1. Moreover, this photocatalyst maintains robust photocatalytic stability even after three consecutive usage cycles. This study demonstrated that the Z-scheme CuInS2/ZnIn2S4 heterojunction photocatalyst exhibits enhanced hydrogen evolution efficiency, offering an effective structural design for harnessing solar energy to obtain hydrogen fuel. Therefore, this heterojunction photocatalyst is a promising candidate for practical applications in solar hydrogen production.