It is a challenge to fabricate atomically dispersed metal clusters in polymeric carbon nitride (PCN) for durable photocatalytic reactions owing to the thermodynamic stability limitation. Herein, atomically dispersed Ru clusters are implanted into the PCN skeleton matrix based on an ionic diffusion and coordination (IDC) strategy, the stability of which is improved owing to the robust Ru−N bonds in the formed RuN 4 and RuN 3 configurations. Additionally, RuN 4 and RuN 3 as charge transport bridges between two adjacent melon strands efficaciously conquer hydrogen bond restriction in the skeleton to facilitate the in-plane mobility and separation of charge carriers. Moreover, the synergistic effect of adjacent Ru atoms is triggered on the assembled RuN 3 −RuN 4 and RuN 3 −RuN 3 in the atomically dispersed Ru clusters to significantly decrease hydrogen adsorption energy. As a result, the optimal PCN-Ru photocatalyst achieves nearly 6 times higher than the photocatalytic hydrogen evolution (PHE) rate of the Pt/PCN benchmark and maintains the long-term stable running for 104 h of 26 cycles; its overall PHE performance is far superior to the most of single atoms supported on g-C 3 N 4 photocatalysts reported. The findings here gain new insight into the preparation strategy, structure configuration, and reaction mechanism for atomically dispersed metal clusters supported on PCN, which further stimulates the intensive investigations toward developing more efficient and stable PCN-like photocatalytic materials.
In this work, we design and successfully fabricate a novel Bi 2 O 3 quantum dots (QDs) decorated BiVO 4 nanofibers by a direct heat treatment of as-spun fibers. The Bi 2 O 3 quantum dots with a size of 5-15 nm are well dispersed on the surface of the BiVO 4 nanofibers with a diameter of 400-700 nm to form a Bi 2 O 3 QDs decorated BiVO 4 nanofibers photocatalyst. Based on the phase separation mechanism and the 10 properties of solvents, a possible formation process of the Bi 2 O 3 QDs decorated BiVO 4 nanofibers has been proposed. The BiVO 4 nanofibers with the decoration of Bi 2 O 3 QDs exhibit much better photocatalytic performance than pure BiVO 4 nanofibers. Photocurrent responses and electrochemical impedance spectra prove that decorating BiVO 4 nanofibers with tiny size Bi 2 O 3 QDs can effectively promote the separation of photoinduced carriers, which is benefit for photocatalytic properties. More 15 significantly, this work is avail to environmental purification and photoelectrochemical. 65 photocatalysts, including hydrothermal method, refluxing, pyrolysis of the organometallic precursors, ultrasonic method, and so on. 28-31 Nevertheless, electrospinning can solve the problem more perfectly because electrospinning is a facile preparation method to fabricate photocatalysts with stable 70 structure and large specific area for preventing quantum dots from aggregation. The quantum dots can well dispersed on/into the one-dimensional (1D) photocatalysts to form composite
Micro/nanostructure control of heterostructures is still a challenge for achieving high efficiency and selectivity of photocatalytic CO 2 conversion. In this work, a new three-dimensiona/two-dimensional (3D/2D) heterostructure is fabricated by encapsulating RuS 2 nanospheres in the interlayer of mesoporous polymeric carbon nitride (PCN) nanosheets based on an in situ growth and polymerization strategy. The unique microstructure of the obtained 3D/2D RuS 2 / PCN heterojunction can effectively improve the transfer and separation efficiency of photogenerated charge carriers, reduce the mass transfer resistance of CO 2 toward active sites, and provide a confined reaction space, thus propelling the photocatalytic CO 2 reduction to CO with high selectivity. The CO yield over the optimal 5%-RuS 2 / PCN sample reaches 4.2 and 2.8 times as high as that of single PCN and RuS 2 within 4 h, respectively. Furthermore, the plausible charge transfer mechanism and CO 2 reduction path are revealed by time-dependent in situ Fourier transform infrared (FT-IR) spectra combined with photophysical, electrochemical, and photoelectrochemical techniques and density functional theory (DFT) calculations. This work develops the microstructural engineering design strategy of PCN-based heterojunctions for selective photocatalytic CO 2 fuel conversion.
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