Designing photocatalysts with high light utilization and efficient photogenerated carrier separation for pollutant degradation is one of the important topics for sustainable development. In this study, hierarchical core–shell material α-Fe2O3@ZnIn2S4 with a step-scheme (S-scheme) heterojunction is synthesized by in situ growth technique, and MXene Ti3C2 quantum dots (QDs) are introduced to construct a double-heterojunction tandem mechanism. The photodegradation efficiency of α-Fe2O3@ZnIn2S4/Ti3C2 QDs to bisphenol A is 96.1% and its reaction rate constant attained 0.02595 min−1, which is 12.3 times that of pure α-Fe2O3. Meanwhile, a series of characterizations analyze the reasons for the enhanced photocatalytic activity, and the charge transport path of the S-scheme heterojunction/Schottky junction tandem is investigated. The construction of the S-scheme heterojunction enables the photo-generated electrons of α-Fe2O3 and the holes of ZnIn2S4 to transfer and combine under the action of the reverse built-in electric field. Due to the metallic conductivity of Ti3C2 QDs, the photogenerated electrons of ZnIn2S4 are further transferred to Ti3C2 QDs to form a Schottky junction, which in turn forms a double-heterojunction tandem mechanism, showing a remarkable charge separation efficiency. This work provides a new opinion for the construction of tandem double heterojunctions to degrade harmful pollutants.
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The formation of chemical bonds between metal ions and their supports is an effective strategy to achieve good catalytic activity. However, both the synthesis of active metal species on a support and control of their coordination environment are still challenging. Here, we show the use of an organic compound to produce tubular carbon nitride (TCN) as a support for Pd nanoparticles (NPs), creating a composite material (NP-Pd-TCN). It was found that Pd ions preferentially bind with the electron-rich N atoms of TCN, leading to strong metal–support interactions that benefit charge transfer from g-C3N4 to Pd. X-ray absorption spectroscopy further revealed that the metal–support interactions resulted in the formation of Pd–N bonds, which are responsible for the improvement in the charge dynamics as evidenced by the results from various techniques including photoluminescence (PL) spectroscopy, photocurrent measurements, and electrochemical impedance spectroscopy (EIS). Owing to the good dynamical properties, NP-Pd-TCN was used for photocatalytic hydrogen evolution under visible-light irradiation (λ > 420 nm) and an excellent evolution rate of ~ 381 μmol·h −1 (0.02 g of the photocatalyst) was attained. This work aims to promote a strategy to synthesize efficient photocatalysts for hydrogen production by controllably introducing metal nanoparticles on a support and in the meantime forming chemical bonds to achieve intimate metal-support contact.
Fenton or photocatalytic degradations of organic contaminants are recognized as promising approaches to address the increasing environmental pollution issues. Herein, we develop the effective synergistic catalysis reaction of Fenton and photocatalysis based on a loofah sponge-like Fe2Ox/C nanocomposite, which exhibits excellent nitrobenzene photocatalytic degradation property. It is noted that Fe2O3 nanoparticles with surface Fe2+ species were encapsulated with an ultrathin carbon layer (denoted as Fe2Ox/C) via a supramolecular self-sacrificing template and following thermal treatment process. The experimental results indicated that the thin layer carbon coating not only inhibited the Fe iron leaching from the Fe2Ox but also prompted the separation and transferring of electrons–hole pairs. The introduction of Fe2Ox/C enables the Fenton reaction to induce a rapid Fe2+/Fe3+ cycle, and meanwhile, together with the photocatalytic reaction to produce continuous active substances for the subsequent degradation catalytic reaction without successive H2O2, resulting in the inexpensive and the effective photocatalytic procedure. As a result, 100% nitrobenzene (100 mg/L) was degraded and 97% of the organic carbon was mineralized in 90 min using the Fe2Ox/C (0.1 g/L) at a low H2O2 dosage (0.50 mM), under air mass (AM) 1.5 irradiation. Theoretical calculations confirmed that the Fe2Ox/C-600 with thin carbon layer promoted the dissociation of H2O2 and the ·OH desorption. The synergistic catalysis of this work may provide new ideas for low-cost and more efficient treatment of pollutants.