As a fascinating visible‐light‐responsive photocatalyst, zinc indium sulfide (ZnIn2S4) has attracted extensive interdisciplinary interest and is expected to become a new research hotspot in the near future, due to its nontoxicity, suitable band gap, high physicochemical stability and durability, ease of synthesis, and appealing catalytic activity. This review provides an overview on the recent advances in ZnIn2S4‐based photocatalysts. First, the crystal structures and band structures of ZnIn2S4 are briefly introduced. Then, various modulation strategies of ZnIn2S4 are outlined for better photocatalytic performance, which includes morphology and structure engineering, vacancy engineering, doping engineering, hydrogenation engineering, and the construction of ZnIn2S4‐based composites. Thereafter, the potential applications in the energy and environmental area of ZnIn2S4‐based photocatalysts are summarized. Finally, some personal perspectives about the promises and prospects of this emerging material are provided.

ZnIn2S4-Based Photocatalysts for Energy and Environmental Applications

Understanding the site interaction nature of single-atom catalysts (SACs), especially densely populated SACs, is vital for their application to various catalytic reactions. Herein, we report a site distance effect, which emphasizes how well the distance of the adjacent copper atoms (denoted as dCu1-Cu1) matches with the reactant peroxydisulfate (PDS) molecular size determines the Fenton-like reaction reactivity on the carbon-supported SACs. The optimized dCu1-Cu1 in the range of 5-6 Å that matches the molecular size of PDS endows a nearly two times higher turnover frequency than that of dCu1-Cu1 beyond this range, accordingly achieving the record-breaking kinetics for emerging organic contaminant oxidation. Further studies suggest that this site distance effect originates from the alteration of PDS adsorption to a dual-site structure on Cu1-Cu1 sites when dCu1-Cu1 falls in 5-6 Å, significantly enhancing the interfacial charge transfer and consequently resulting in the most efficient catalyst for PDS activation so far.

A Site Distance Effect Induced by Reactant Molecule Matchup in Single-Atom Catalysts for Fenton-like Reactions.

Material-enhanced heterogonous peroxymonosulfate (PMS) activation on emerging organic pollutant degradation has attracted intensive attention, and a challenge is the electron transfer efficiency from material to PMS for radical production. Herein, an interface architecture of Co(OH)2 nanosheets growing on the KNbO3 perovskite [Co(OH)2/KNbO3] was developed, which showed high catalytic activity in PMS activation. A high reaction rate constant (k1) of 0.631 min-1 and complete removal of pazufloxacin within 5 min were achieved. X-ray photoelectron spectroscopy, X-ray absorption near edge structure spectra, and density functional theory (DFT) calculations revealed the successful construction of the material interface and modulated electronic structure for Co(OH)2/KNbO3, resulting in the hole accumulation on Co(OH)2 and electron accumulation on KNbO3. Bader topological analysis on charge density distribution further indicates that the occupations of Co-3d and O-2p orbitals in Co(OH)2/KNbO3 are pushed above the Fermi level to form antibonding states (σ*), leading to high chemisorption affinity to PMS. In addition, more reactive Co(II) with the closer d-band center to the Fermi level results in higher electron transfer efficiency and lower decomposition energy of PMS to SO4•-. Moreover, the reactive sites of pazufloxacin for SO4•- attack were precisely identified based on DFT calculation on the Fukui index. The pazufloxacin pathways proceeded as decarboxylation, nitroheterocyclic ring opening reaction, defluorination, and hydroxylation. This work can provide a potential route in developing advanced catalysts based on manipulation of the interface and electronic structure for enhanced Fenton-like reaction such as PMS activation.

Interface Engineering of Co(OH)2 Nanosheets Growing on the KNbO3 Perovskite Based on Electronic Structure Modulation for Enhanced Peroxymonosulfate Activation.

ZnIn2S4-based photocatalysts for photocatalytic hydrogen evolution via water splitting

g-C3N4-Based 2D/2D Composite Heterojunction Photocatalyst

Ultrathin 2D/2D ZnIn2S4/g-C3N4 Nanosheet Heterojunction with Atomic-Level Intimate Interface for Photocatalytic Hydrogen Evolution under Visible Light

By an in situ modification of CdIn2S4 nano-octahedron on the surface of ZnIn2S4 nanosheets, ZnIn2S4/CdIn2S4 nano-composites with tight interface contact were obtained by a one-step solvothermal method. Because of the existence of ZnIn2S4/CdIn2S4 nano-heterostructure, the optimized sample (ZCIS-50) exhibited excellent photocatalytic H2 generation activity (12.67 mmol h−1 g−1) under visible light, which was approximately 15.1 times that of pure CdIn2S4 (0.84 mmol h−1 g−1) and 5.9 times that of ZnIn2S4 (2.13 mmol h−1 g−1). Based on experiments and simulation studies, the remarkable improvement of the photocatalytic performance of ZnIn2S4/CdIn2S4 can be ascribed to the presence of a large number of Cd–S–Zn atomic bridges between ZnIn2S4 nanosheets and CdIn2S4 nano-octahedrons, which not only promoted the interfacial charge transfer but also inhibited the recombination of light-induced carriers. In Na2S/Na2SO3 solution, the apparent quantum yield of the ZCIS-50 sample at 420 nm was 18.73% with good stability under long-term irradiation. This work emphasizes the key role of interface design and defect engineering of in situ nano heterostructures. It may provide a promising strategy for the progress of high-efficiency photocatalytic water-splitting catalysts.

The in situ construction of ZnIn2S4/CdIn2S4 2D/3D nano hetero-structure for an enhanced visible-light-driven hydrogen production

The atomically dispersed metal is expected as one of the most promising Fenton-like catalysts for the degradation of recalcitrant organic pollutants (ROPs) by the strong "electronic metal-support interactions" (EMSIs). Here, we develop an atomically dispersed metal-atom alloy made by guest Au atoms substitute host V atoms in the two-dimensional VO2 (B) nanobelt support (Au/VO2 ) to activate Fenton-like oxidation for elimination of ROPs. The 2D nanobelt structure enlarges the exposure of atomically Au thus increasing the number of active sites to absorb more S2 O8 2- ions. And the EMSIs regulate the charge density in Au atoms to present positive charge Au+ , lowering the energy barrier of S2 O8 2- decomposition to produce SO4 .- . The Au/VO2 catalyst possesses excellent durable and reliable characteristics and exhibits record-breaking efficiency with TOF as high as 21.42 min-1 , 16.19 min-1 , and 80.89 min-1 for rhodamine, phenol, and bisphenol A degradation, respectively.

Tailoring the electronic metal-support interactions in supported atomically dispersed gold catalysts for efficient Fenton-like reaction.

Luminol, as a classical luminophore, plays a crucial role in electrochemiluminescence (ECL). However, the traditional luminol-H2O2 ECL system suffers from the self-decomposition of H2O2 at ambient temperature, which hinders its further application in quantitative analysis. In this work, for the first time, we developed atomically gold-supported two-dimensional VO2 nanobelts (Au/VO2) as an advanced co-reaction promoter to speed up the reduction of dissolved oxygen to superoxide radicals (O2•-), which react with the luminol anion radical and greatly promote the ECL emission. The ECL resonance energy transfer (ECL-RET) between the hollow manganese dioxide nanospheres and luminol results in a conspicuously decreased ECL signal response, and in the presence of glutathione (GSH), effective redox reaction between manganese dioxide and GSH restores the ECL signal. As a consequence, the designed sensor based on ECL-RET-assisted Au/VO2 signal amplification showed outstanding performance for "signal-on" detection of GSH in the concentration range of 10-3 to 10-10 M, and the detection limit was as low as 0.03 nM. The ECL sensor displayed excellent specificity and was successfully utilized to target GSH in real human serum samples. Importantly, this work not only highlights a powerful avenue for constructing an ultrasensitive ECL sensor for GSH but also provides some inspiration for the further design of high-performance co-reaction accelerators using the ECL technique.

Signal Amplification Strategy Using Atomically Gold-Supported VO2 Nanobelts as a Co-reaction Accelerator for Ultrasensitive Electrochemiluminescent Sensor Construction Based on the Resonance Energy Transfer Platform.

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Ultrathin 2D/2D ZnIn2S4/g-C3N4 Nanosheet Heterojunction with Atomic-Level Intimate Interface for Photocatalytic Hydrogen Evolution under Visible Light

The in situ construction of ZnIn2S4/CdIn2S4 2D/3D nano hetero-structure for an enhanced visible-light-driven hydrogen production

Tailoring the electronic metal-support interactions in supported atomically dispersed gold catalysts for efficient Fenton-like reaction.

Signal Amplification Strategy Using Atomically Gold-Supported VO2 Nanobelts as a Co-reaction Accelerator for Ultrasensitive Electrochemiluminescent Sensor Construction Based on the Resonance Energy Transfer Platform.