Energy Band Positions Research Articles

Z-Scheme ZnV2O4/g-C3N4 Heterojunction Catalyst Produced by the One-Pot Method for the Degradation of Tetracycline under Visible Light

A novel Z-scheme ZnV2O4/g-C3N4 composite catalyst was prepared using a one-pot calcination method, and the photodegradation performance of the ZnV2O4/g-C3N4 heterojunction was studied under simulated sunlight condition. Under visible-light treatment, the ZnV2O4/g-C3N4 catalyst showed excellent catalytic activity in the degradation of tetracycline (TC), and compared with pure g-C3N4 and ZnV2O4, its photocatalytic degradation efficiency was significantly improved. The performances of the ZnV2O4/g-C3N4 catalyst were compared under different ZnV2O4 loading rates, catalyst dosage, pollutant concentrations, and initial pH values of the solution. The experimental results showed that the 35 wt % ZnV2O4/g-C3N4 (35ZVO/CN) had the best photocatalytic activity. The appreciable improvement in performance was mainly due to the construction of the Z-scheme structure between ZnV2O4 and g-C3N4, which promoted the effective separation of charge carriers. In addition, a possible mechanism of the photodegradation process of 35ZVO/CN was discussed based on the energy band position analyses and active radical capture experiments. That superoxide radical was the main reaction specie confirmed the Z-scheme mechanism. By forming the Z-scheme heterojunction, the efficiency of charge separation and transfer was improved, and the catalyst had strong oxidation and reduction abilities. This research provided a new enlightenment for the construction and synthesis of a low-cost Z-scheme heterojunction photocatalyst and the treatment of antibiotics in water.

Nanomaterials as Photocatalysts—Synthesis and Their Potential Applications

Increasing demand for energy and environmental degradation are the most serious problems facing the man. An interesting issue that can contribute to solving these problems is the use of photocatalysis. According to literature, solar energy in the presence of a photocatalyst can effectively (i) be converted into electricity/fuel, (ii) break down chemical and microbial pollutants, and (iii) help water purification. Therefore, the search for new, efficient, and stable photocatalysts with high application potential is a point of great interest. The photocatalysts must be characterized by the ability to absorb radiation from a wide spectral range of light, the appropriate position of the semiconductor energy bands in relation to the redox reaction potentials, and the long diffusion path of charge carriers, besides the thermodynamic, electrochemical, and photoelectrochemical stabilities. Meeting these requirements by semiconductors is very difficult. Therefore, efforts are being made to increase the efficiency of photo processes by changing the electron structure, surface morphology, and crystal structure of semiconductors. This paper reviews the recent literature covering the synthesis and application of nanomaterials in photocatalysis.

Fabrication of Novel g-C3N4@Bi/Bi2O2CO3 Z-Scheme Heterojunction with Meliorated Light Absorption and Efficient Charge Separation for Superior Photocatalytic Performance

Herein, a novel g-C3N4@Bi/Bi2O2CO3 Z-scheme heterojunction was synthesized via simple methods. UV/Vis diffuse reflectance spectroscopy (DRS) revealed that the visible light absorption range of heterojunction composites was broadened from 400 nm to 500 nm compared to bare Bi2O2CO3. The XRD, XPS and TEM results demonstrated that metal Bi was introduced into g-C3N4@Bi/Bi2O2CO3 composites, and Bi may act as an electronic bridge in the heterojunction. Metal Bi elevated the separation efficiency of carriers, which was demonstrated by photocurrent and photoluminescence. The performance of samples was assessed via the degradation of Rhodamine B (RhB), and the results exhibited that g-C3N4@Bi/Bi2O2CO3 possessed notably boosted photocatalytic activity compared with g-C3N4, Bi2O2CO3 and other binary composites. The heterojunction photocatalysts possessed good photostability and recyclability in triplicate cycling tests. Radical trapping studies identified that h+ and •O2- were two primary active species during the degradation reaction. Based on the energy band position and trapping radical experiments, the possible reaction mechanism of the indirect Z-scheme heterojunction was also proposed. This work could provide an effective reference to design and establish a heterojunction for improving the photocatalytic activity of Bi2O2CO3.

Performance and mechanism of a novel S-scheme heterojunction sonocatalyst CuS/BaWO4 for degradation of bisphenol A by ultrasonic activation

A novel CuS/BaWO4 heterojunction catalyst was prepared and characterized. Taking bisphenol A as the target pollutant for catalytic degradation, the sonocatalytic activity of CuS/BaWO4 composite was evaluated, and the combination with persulfate improved the sonocatalytic degradation of bisphenol A. The results showed that CuS/BaWO4 composite had good sonocatalytic degradation activity for bisphenol A, and the degradation rate was 70.99% ± 1.46%. After combined with persulfate, the degradation rate was further increased to 95.34% ± 0.10%, and the reaction time was relatively shortened. The results of the trapping experiment and calculated energy band positions showed that the formation of S-scheme heterojunction and the formation of hydroxyl radicals and holes were the key to the catalytic degradation of bisphenol A by CuS/BaWO4 composite. In this study, a new CuS/BaWO4 heterojunction sonocatalyst was synthesized. The catalyst can efficiently remove bisphenol A from the water environment and can be used as a potential solution for endocrine disruptor pollution in the water environment.

Design and synthesis of black phosphorus quantum dot sensitized inverse opal TiO2 photonic crystal with outstanding photocatalytic activities

Quantum dot sensitized photocatalyst is designed and applied in purification of dye wastewater, using black phosphorus nanoparticles (BPQDs) as the quantum dot and inverse opal (IO) TiO2 photonic crystal as the main photocatalyst. Due to electron density change within the composite, electrons can transfer from BPQDs to IO TiO2 directionally. Bandgap energies and relative energy band positions of BPQDs and IO TiO2 further provide efficient electronic transmission channels at the heterojunction interface. Therefore, interfacial resistance for charge transfer is reduced, the production of active oxidative species is promoted, and the photo induced charge transfer proceeds through a typical type-II route. Finally, excellent photocatalytic properties of BPQDs-IO TiO2 are achieved with the highest apparent kinetic constant (kapp) of 0.046 min−1, which is more than 3 times for bare IO TiO2 (0.014 min−1) and nearly 2 times for commercial P25 TiO2 (0.027 min−1). Furthermore, long-term stability and non-toxicity make the quantum dot sensitized photocatalyst have great applications in purifying environmental water pollution.

Increasing the Photocatalytic Activity of BiVO4 by Naked Co(OH)2 Nanoparticle Cocatalysts

Bismuth vanadate (BiVO4 or BVO) is one of the most studied photocatalysts for water oxidation because of its excellent visible light absorption and appropriate band energy positions. However, BVO presents a low charge mobility and a high electron–hole recombination rate. To address these fundamental limitations, this study proposes the coating of previously synthesized phase-pure monoclinic scheelite BVO with different amounts of naked cobalt (further oxidized to cobalt hydroxide) nanoparticles (NPs) via a modified magnetron sputtering deposition. The resulting BVO/Co photocatalysts were investigated for methylene blue (MB) photodegradation, photocatalytic oxygen evolution, and photoelectrochemical (PEC) water oxidation. In the MB photodegradation tests, the BVO/Co sample prepared with a deposition time of 5 min (BVO/Co(5 min)) presented the highest photoactivity (k = 0.06 min−1) compared with the other sputtering investigated times (k = 0.01–0.02 min−1), as well as the pristine BVO sample (k = 0.04 min−1). A similar trend was evidenced for the PEC water oxidation, where a photocurrent density of 23 µA.cm−2 at 1.23 V (vs. RHE) was observed for the BVO/Co(5 min) sample, a value 4.6 times higher compared with pristine BVO. Finally, the BVO/Co(5 min) presented an O2 evolution more than two times higher than that of the pristine BVO. The increased photocatalytic performance was ascribed to increased visible-light absorption, lesser electron–hole recombination, and enhanced charge transfer at the liquid/solid interface. The deposition of Co(OH)2 NPs via magnetron sputtering can be considered an effective strategy to improve the photocatalytic performance of BVO for different target catalytic reactions, including oxygen evolution, water oxidation, and pollutant photodegradation.

High detectivity graphene/si heterostructure photodetector with a single hydrogenated graphene atomic interlayer for passivation and carrier tunneling

Hydrogenated graphene is easy to prepare and chemically stable. Besides, hydrogenation of graphene can open the band gap, which is vital for electronic and optoelectronic applications. Graphene/Si photodetector (PD) has been widely studied in imaging, telecommunications, and other fields. The direct contact between graphene and Si can form a Schottky junction. However, it suffers from poor interface state, where the carrier recombination at the interface causes serious leakage current, which in turn leads to a decrease in the detectivity. Hence, in this study, hydrogenated graphene is used as an interfacial layer, which passivates the interface of graphene/Si (Gr/Si) heterostructure. Besides, the single atomic layer thickness of hydrogenated graphene is also crucial for the tunneling transport of charge carriers and its suitable energy band position reduces the recombination of carrier. The fabricated graphene/hydrogenated-graphene/Si (Gr/H–Gr/Si) heterostructure PD showed an extremely low dark current about 10−7 A. As a result, it had low noise current and exhibited a high specific detectivity of ∼2.3 × 1011 Jones at 0 V bias with 532 nm laser illumination. Moreover, the responsivity of the fabricated PD was found to be 0.245 A W−1 at 532 nm illumination with 10 μW power. These promising results show a great potential of hydrogenated graphene to be used as an interface passivation and carrier tunneling layer for the fabrication of high-performance Gr/Si heterostructure PDs.

Integrated p-n Junctions for Efficient Solar Water Splitting upon TiO2/CdS/BiSbS3 Ternary Hybrids for Improved Hydrogen Evolution and Mechanistic Insights

The development of efficient and novel p-n heterojunctions for photoelectrochemical (PEC) water splitting is still a challenging problem. We have demonstrated the complementary nature of (p-type) BiSbS3 as a sensitizer when coupled with (n-type) TiO2/CdS to improve the photocatalytic activity and solar to hydrogen conversion efficiency. The as-prepared p-n heterojunction TiO2/CdS/BiSbS3 exhibits good visible light harvesting capacity and high charge separation over the binary heterojunction, which are confirmed by photoluminescence (PL) and electrical impedance spectroscopy (EIS). The ternary heterojunction produces higher H2 than the binary systems TiO2/CdS and TiO2/BiSbS3. This ternary heterojunction system displayed the highest photocurrent density of 5 mA·cm−2 at 1.23 V vs. reversible hydrogen electrode (RHE) in neutral conditions, and STH of 3.8% at 0.52 V vs. RHE is observed. The improved photocatalytic response was due to the favorable energy band positions of CdS and BiSbS3. This study highlights the p-n junction made up of TiO2/CdS/BiSbS3, which promises efficient charge formation, separation, and suppression of charge recombination for improved PEC water splitting efficiency. Further, no appreciable loss of activity was observed for the photoanode over 2500 s. Band alignment and interfaces mechanisms have been studied as well.

Controllable synthesis of Bi2SiO5/Bi4Si3O12 heterostructure and it's specific adsorption and photocatalytic performance

Nanosheets of Bi2SiO5/Bi4Si3O12 composite material was prepared by a one-step hydrothermal method with HNO3 solution as the solvent. In the same hydrothermal condition, the nanosheets of Bi2SiO5 and hollow spherical of Bi4Si3O12 were prepared by substituting HNO3 solution with ethylene glycol and benzyl alcohol as solvent, respectively. The obtained materials were characterized by the XRD, XPS, SEM, TEM, BET, UV–vis spectroscopy and PL. The Bi2SiO5, Bi2SiO5/Bi4Si3O12 and Bi4Si3O12 photocatalysts were applied to remove 17α-ethynylestradiol (EE2), and the EE2 removal rates were 47.6%, 99.4% and 25.4% after 12 min of UV-light irradiation, respectively. Photocatalytic activity of Bi2SiO5/Bi4Si3O12was better than that of Bi2SiO5 and Bi4Si3O12, because that heterojunction of Bi2SiO5/Bi4Si3O12 had the matching band structure between Bi2SiO5 and Bi4Si3O12, the carrier separation efficiency and transport efficiency were improved. The Bi2SiO5/Bi4Si3O12 shows the highest reaction rate, which is 9.69, 26.41, 27.29 and 124.96 times higher than that of Bi2SiO5, Bi4Si3O12, P25 and EE2 photolysis, respectively. The effects of pH value and photocatalyst dosage were optimized for removing EE2 in water. The possible photocatalytic mechanism was proposed based on the trapping photocatalytic experiments and the energy band positions. Surprisingly, the Bi2SiO5/Bi4Si3O12 photocatalyst had specific adsorption performance on EE2 comparing to BPA due to the EE2 has stronger hydrophobicity than BPA, while it can photodegrade both EE2 and bisphenol A (BPA). Results in this work provide new insights for controlled synthesized the Bi2SiO5, Bi2SiO5/Bi4Si3O12 and Bi4Si3O12 only by changing the solvent in hydrothermal process. The Bi2SiO5/Bi4Si3O12 possess a synergistic effect of adsorption and photocatalysis for hydrophobic organic molecules, which indicates that it can be used as an efficient material for removing hydrophobic molecules. Meanwhile, Bi2SiO5/Bi4Si3O12 composite was considered a promising photocatalyst for removing all kinds of Endocrine Disrupting Chemicals (EDCs) organic pollutants.

CdS-based ternary composite material for high-efficiency photocatalytic CO2 reduction via a cascade electron transfer

CdS conductor has a suitable band gap (~2.4 eV), and the energy band position is conducive to photocatalytic CO2 reduction. However, its photocatalytic efficiency is highly confined by its unfavored carrier transfer. In this study, a moderately in-situ growth method is harnessed to insert commercial TiO2 particles (P25) into the CdS grains in the first place, and the resulted CdS-P25 composite is further integrated with to a mixed-ligand-based metal organic framework (MOF), CuTCPP⊂UiO-66 (CTU), which is structure-analogous to regular UiO-66 MOF but with visible light response thanks to the involvement of copper(II) tetra(4-carboxyphenyl) porphyrin (CuTCPP) ligand. The eventually attained ternary composite (CTU/CdS-P25) by solvothermal approach presents a broadened light absorption and an impressive delivery for photo-induced carriers. The light-driven catalytic assessment of CTU/CdS-P25 for CO2 reduction furnishes the CO production rate as great as 2.38 μmol·h−1, as much as 3.9 and 8.8 times that of UiO/CdS-P25 and CdS-P25, respectively. According to the value determination of band edge for each component of the ternary composite, we proposed that the established heterojunction facilitates a cascade electron transfer mode within the structure, which highly suppresses the adverse recombination of carriers and thereafter significantly enhances the photocatalytic behavior. Our work provides an effective perspective for the melioration of CdS semiconductor.

Laser-Reduced BiVO4 for Enhanced Photoelectrochemical Water Splitting.

The present study proposes a laser irradiation method to superficially reduce BiVO4 photoelectrodes and boost their water oxidation reaction performance. The origin of this enhanced performance toward oxygen evolution reaction (OER) was studied using a combination of a suite of structural, chemical, and mechanistic advanced characterization techniques including X-ray photoelectron (XPS), X-ray absorption spectroscopy (XAS), electrochemical impedance spectroscopy (EIS), and transient absorption spectroscopy (TAS), among others. We found that the reduction of the material is localized at the surface of the sample and that this effect creates effective n-type doping and a shift to more favorable energy band positions toward water oxidation. This thermodynamic effect, together with the change in sample morphology to larger and denser domains, results in an extended lifetime of the photogenerated carriers and improved charge extraction. In addition, the stability of the reduced sample in water was also confirmed. All of these effects result in a two-fold increase in the photocurrent density of the laser-treated samples.

Optimal monolayer WO3 nanosheets/TiO2 heterostructure and its photocatalytic performance under solar light

Highly efficient photocatalysts were formed via high-temperature calcination of monolayer WO3 prepared by a space-constrained method combined with commercial TiO2, and the optimal ratio of these components was explored. These synthetic catalysts were also characterized. During photocatalysis, the decomposition rate of MB achieved by the 1 mol% ML-WO3/TiO2 composite reached 98.05% within 10 min under solar light. Moreover, the photocatalytic efficiency of the composite catalyst did not decrease substantially after 5 cycles of operation. In addition, energy band position and active gene capture experiments revealed that the prepared photocatalysts conform to the transfer theory of Z-scheme heterojunctions.

Photocatalytic degradation of MB by novel and environmental ZnO/Bi2WO6-CC hierarchical heterostructures

ZnO-CC and ZnO/Bi2WO6-CC with different Bi2WO6 loadings layered heterostructures photocatalysts were synthesized on flexible carbon clothes (CC) substrate by the thermal decomposition-hydrothermal method. By characterizing the degradation of methylene blue (MB) under ultraviolet light irradiation, Z3B-CC (3 wt% Bi2WO6) showed the best photocatalytic effect, and the photodegradation rate of MB was as high as 96.9% in about 100 min. This new ZnO/Bi2WO6-CC layered heterostructure exhibits prominent photocatalytic performance, which is mainly ascribed to the type II band structure formed by ZnO and Bi2WO6. The appropriate energy band position further facilities the effective transfer of carriers and realizes the photocatalytic process of the heterostructure. This study is prospective to provide new ideas for the synthesis of other high-efficiency heterostructure photocatalytic designs, and it also has reference value for the synthesis of flexible photocatalytic materials with excellent performance.

A newly-constructed double p-n heterojunction based on g-C3N4@NiO/Ni@MIL-101 ternary composite with enhanced photocatalytic performance for wastewater purification

In this study, a double p-n heterojunction based on g-C3N4@NiO/Ni@MIL-101 ternary composite was successfully prepared by a feasible method. Results suggested that the rational growth of NiO and MIL-101 on the surface of g-C3N4 can improve the absorption capacity for visible light. Importantly, the formation of double p-n heterojunction can effectively inhibit the recombination of photogenerated electrons and holes. Due to the significant Fermi level differences among NiO, MIL-101 and g-C3N4, the internal electric fields were established on the interface after constructing the composite, consequently reducing the electrical resistance and accelerating the transfer of photoinduced charge carriers. As expected, the g-C3N4@NiO/Ni@MIL-101 ternary composite with good stability had excellent photocatalytic performance in the degradation of emerging pollutants, and the removal efficiency of ibuprofen was as high as 95.6%. The •O2−, •OH and 1O2 were the major active species in the reaction system. Furthermore, developed photocatalytic oxidation system can also achieve the rapid inactivation of bacteria. Based on the synergistic effects of energy band position and double internal electric fields, the separation and transfer of photogenerated charge carriers followed a traditional type-II route. In short, current work not only constructed a promising photocatalyst, but also shared an effective strategy for boosting the photocatalytic activity.

Investigation of the nature of polypropylene absorption bands before and after electron irradiation

The results of studies of reflection spectra in the UV, visible and near IR spectral regions for polypropylene films before and after electron irradiation (E = 30 keV, F = 1...3·1016 cm−2) are presented. The spectra were recorded in high vacuum at the irradiation site (in situ). Before irradiation, bands at 1200, 1400 and 1700 nm, caused by overtones of vibrational frequencies of CH, CH2 and CH3 molecular groups, and sorbed OH groups, were recorded. After irradiation and decomposition of the spectra into components, the absorption bands of the following radicals were detected: C3H5 –, – C3H6 –, – C4H6 –, – C4H7 –, – C4H8–, – C4H12 –, – C5H7 –, and – C5H10 –. A linear dependence of the energy position of absorption bands on the mass of the radicals that determine these bands was confirmed. The contribution of each band to the integral absorption band of a complex shape and its dependence on the electron fluence were determined. The mechanism behind the formation of radiation defects during irradiation of polypropylene is proposed.

Photocatalytic dye degradation using nickel ferrite spinel and its nanocomposite.

Coloured wastewater is a major issue of today for human health and ecology. Among all available processes such as physical, chemical, biological and electrochemical methods, photocatalysis can be a promising solution because of its ability to degrade colour-causing compounds completely by converting them into simpler molecules (H2O, CO2) depending on dye structure. In this work, NiFe2O4was synthesized by the co-precipitation method. Furthermore, the composites of NiFe2O4 with TiO2 were synthesized by varying amounts of TiO2. The spinel and composites were characterized by XRD, ZETA analysis and UV-DRS. Their photocatalytic activities were investigated using the photocatalyticdegradation ofreactive turquoise blue 21 (RB 21)dye as model pollutants under sunlight.The increased absorption of the visible light and the enhanced separation of the electron-hole pairs due to the relative energy band positions in NiFe2O4 and TiO2 are considered as the main advantages.Our results showed that NiFe2O4-based nanocomposites could be used as an effective and magnetic retrievable photocatalyst.

Boosting the Photocatalytic Activity and Resistance of Photostability of ZnS Nanoparticles.

Defects play a vital role in improving photocatalytic performance. However, the specific influence mechanism of sulfur defects (DSS) on sulfide photocatalytic performance and stability is still unclear. In this work, an ingenious solvent-free self-overflow strategy is designed to introduce DSS into ZnS nanoparticles and explore the specific promotion mechanism of photocatalytic performance and photostability. The results indicate that the introduced DSS in ZnS nanoparticles can simultaneously boost the photocatalytic hydrogen production (PHE) performance and photostability of ZnS: the PHE rate of the defective ZnS can increase up to 21350.23 μmol·h-1·g-1, which is roughly 4.7 times higher than that of pristine ZnS. Both experiments and theoretical calculationsshow that the enhanced photocatalytic performance could be attributed to the change of energy band position after introducing DSS. Specifically, the introduction of DSS can raise the conduction band (CB) position of ZnS to enhance the reducing ability of photogenerated electrons. Besides, the valence band (VB) position can also be raised to boost the light absorption ability of ZnS and restrain the photocorrosion by weakening the oxidation capacity of the photogenerated holes. The ingenious strategy and interesting mechanism in this job provide a simple artful tactic to fabricate other defective sulfide photocatalysts and open up a particular path to promote the photostability of the photocatalysts.

Constructing Co3O4/La2Ti2O7 p-n Heterojunction for the Enhancement of Photocatalytic Hydrogen Evolution.

Layered perovskite-type semiconductor La2Ti2O7 has attracted lots of attention in photocatalytic hydrogen evolution, due to the suitable energy band position for water splitting, high specific surface area, and excellent physicochemical stability. However, the narrow light absorption range and the low separation efficiency of photogenerated carriers limit its photocatalytic activity. Herein, plate-like La2Ti2O7 with uniform crystal morphology was synthesized in molten NaCl salt. A p-n heterojunction was then constructed through the in situ hydrothermal growth of p-type Co3O4 nanoparticles on the surface of n-type plate-like La2Ti2O7. The effects of Co3O4 loading on photocatalytic hydrogen evolution performance were investigated in detail. The results demonstrate that composite Co3O4/La2Ti2O7 possesses much better photocatalytic activity than the pure component. The composite photocatalyst with 1 wt% Co3O4 exhibits the highest hydrogen evolution rate of 79.73 μmol·g−1·h−1 and a good cycling stability. The photoelectrochemistry characterizations illustrate that the improvement of photocatalytic activity is mainly attributed to both the enhanced light absorption from the Co3O4 ornament and the rapid separation of photogenerated electron-hole pairs driven by the built-in electric field close to the p-n heterojunction. The results may provide further insights into the design of high-efficiency La2Ti2O7-based heterojunctions for photocatalytic hydrogen evolution.

Fluorine-doped CuBi2O4 nanorod arrays for enhanced photoelectrochemical oxygen reduction reaction toward H2O2 production

CuBi2O4 (CBO) semiconductor composed of low cost and environmentally friendly Cu, Bi, and O elements possesses relatively narrow band gap, appropriate energy band position, and very positive photocurrent onset potential, which make it promising for photoelectrochemical (PEC) O2 reduction reaction (ORR). However, low separation and transfer efficiency of photogenerated carriers and poor product selectivity limit its further application in PEC ORR toward H2O2 production. In this work, we report F− ions doped CuBi2O4 (F-CBO) nanorod arrays with enhanced PEC ORR performance for H2O2 generation. PEC ORR activity of CBO nanorod arrays was obviously enhanced through decreasing the sizes of nanorods. Furthermore, the doping of F− ions into CBO lattice promoted the separation and transfer of photogenerated carriers and significantly improved the selectivity of ORR toward H2O2 path. As a result, 0.85 mmol/L of H2O2 could be achieved on the F-CBO photocathode within 45 min under simulated AM1.5G sunlight illumination (100 mW cm−2), which is 2.8 times higher than that obtained on the pristine counterpart. The roles of fluorine doping were revealed based on experimental results and density functional theory (DFT) calculations. The combination of morphology and surface doping engineering provides a new strategy for designing highly efficient photocathod for PEC ORR to H2O2 production.

Efficient splitting of alcohols into hydrogen and C–C coupled products over ultrathin Ni-doped ZnIn2S4 nanosheet photocatalyst

Integrating selective organic synthesis with hydrogen (H2) evolution in one photocatalytic redox reaction system sheds light on the underlying approach for concurrent employment of photogenerated electrons and holes towards efficient production of solar fuels and chemicals. In this work, a facile one-pot oil bath method has been proposed to fabricate a noble metal-free ultrathin Ni-doped ZnIn2S4 (ZIS/Ni) composite nanosheet for effective solar-driven selective dehydrocoupling of benzyl alcohol into value-added C–C coupled hydrobenzoin and H2 fuel, which exhibits higher performance than pure ZIS nanosheet. The remarkably improved photoredox activity of ZIS/Ni is mainly attributed to the optimized electron structure featuring narrower band gap and suitable energy band position, which facilitates the ability of light harvesting and photoexcited charge carrier separation and transfer. Furthermore, it has been demonstrated that it is feasible to employ ZIS/Ni for various aromatic alcohols dehydrocoupling to the corresponding C–C coupled products. It is expected that this work can stimulate further interest on the establishment of innovative photocatalytic redox platform coupling clean solar fuels synthesis and selective organic conversion in a sustainable manner.