Heterojunction and direct Z-scheme nanostructures are two typical representatives of an efficient photocatalyst, which is composed of two semiconductors. However, it is a great challenge to construct each of them on purpose. The photodeposition technique can be a potentially powerful tool to regulate the electron flow direction for constructing these nanostructures. In this report, CdS nanoparticles were deposited on the g-C3N4 nanosheets by photodeposition and chemical deposition methods for comparison. In the photodeposition case, PL and charge flow tracking demonstrate that a type II heterojunction is constructed because CdS is selectively deposited at the electron transfer site of g-C3N4, which leads to the photoexcited electron from g–C3N4 tending to transfer to CdS in the composites. In the latter, the CdS is randomly deposited onto the g-C3N4 nanosheets through chemical deposition. There is no preferred site for deposition or charge transfer in the composite. The results illustrate that the electron of CdS tends to recombine with the hole from g-C3N4. The direct Z-scheme is predominant for the CdS/g-C3N4 prepared by the chemical deposition route. Furthermore, the photocatalytic performance and stability also confirm the above results. On the of these, we can deduce that the photodeposition method can be used to regulating the electron transfer route. We expect this report to shed light on the rational design of heterojunction or direct Z-scheme type composites.
Photocatalytic ammonia synthesis is another important reaction to mimic natural nitrogen fixation, which has attracted more and more attention. In recent reports, sacrificial agents are often used to promote charge separation, and high-activity photocatalysts are discovered by using Nessler’s reagent method as a detection technique of ammonia production. However, there is an open question on the rationality and accuracy of the ammonia production amount in the presence of the sacrificial agent and Nessler’s reagent detection method. In this report, P25 TiO2 is employed as a model photocatalyst and alcohol as sacrificial agent, and both Nessler’s reagent and cation exchange chromatography are employed as ammonia detection methods. The different ammonia production amount was found by the different detection method. HPLC and 1H NMR results indicate that carbonyl compounds (formaldehyde, acetaldehyde, and acetone) are produced in the reaction. When the carbonyl compound was added to the ammonia standard solution, the interference effect on the detection of ammonia was found in the Nessler’s reagent method. No interference effect was found in the cation exchange chromatography. Thus, the Nessler’s reagent is not suitable for ammonia detection in the presence of alcohol as the sacrificial agent.
A photocatalyst system is generally comprises a catalyst and cocatalyst to achieve light absorption, electron‐hole separation, and surface reaction. It is a challenge to develop a single photocatalyst having all functions so as to lower the efficiency loss. Herein, the active GaN4 site is integrated into a polymeric carbon nitride (CN) photocatalyst (GCN), which displays an excellent H2 production rate of 9904 μmol h−1 g−1. It is 162 and 3.3 times higher than that of CN with the absence (61 μmol h−1 g−1) and presence (2981 μmol h−1 g−1), respectively, of 1.0 wt % Pt. Under light irradiation the electron is injected and stored at the GaN4 site, where the LUMO locates. The HOMO distributes on the aromatic ring resulting in spatial charge separation. Transient photovoltage discloses the electron‐storage capability of GCN. The negative GaN4 promotes proton adsorption in the excited state. The positive adsorption energy drives H2 desorption from GaN4 after passing the electron to the proton. This work opens up opportunities for exploring a novel catalyst for H2 production.
Carbon dots (CDs) as the advancing fluorescent carbon nanomaterial have superior potential and prospective. However, the ambiguous photoluminescence (PL) mechanism and intricate structure-function relationship become the greatest hindrances in the development and applications of CDs. Herein, red emissive CDs were synthesized in high yield from o-phenylenediamine (oPD) and catechol (CAT). The PL mechanism of the CDs is considered as the molecular state fluorophores because 5,14-dihydroquinoxalino[2,3-b] phenazine (DHQP) is separated and exhibits the same PL properties and behavior as the CDs. These include the peak position and shape of the PL emission and PL excitation and the emission dependence on pH and solvent polarity. Both of them display close PL lifetime decays. Based on these, we deduce that DHQP is the fluorophore of the red emissive CDs and the PL mechanism of CDs is similar to DHQP. During the PL emission of CDs, the electron of the molecule state can transfer to CDs. The formation process of DHQP is further confirmed by the reaction intermediates (phthalazine, dimers) and oPD. These findings provide insights into the PL mechanism of this type of CDs and may guide the further development of tunable CDs for tailored properties.
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