3D-MoS 2 can adsorb organic molecules and provide multidimensional electron transport pathways, implying ap otential application for environment remediation. Here,w e study the degradation of aromatic organics in advanced oxidation processes (AOPs) by a3 D-MoS 2 sponge loaded with MoS 2 nanospheres and graphene oxide (GO). Exposed Mo 4+ active sites on 3D-MoS 2 can significantly improve the concentration and stability of Fe 2+ in AOPs and keep the Fe 3+ / Fe 2+ in as table dynamic cycle,t hus effectively promoting the activation of H 2 O 2 /peroxymonosulfate (PMS). The degradation rate of organic pollutants in the 3D-MoS 2 system is about 50 times higher than without cocatalyst. After a1 40 Lp ilotscale experiment, it still maintains high efficiency and stable AOPs activity.A fter 16 days of continuous reaction, the 3D-MoS 2 achieves ad egradation rate of 120 mg L À1 antibiotic wastewater up to 97.87 %. The operating cost of treating aton of wastewater is only US$ 0.33, suggesting huge industrial applications.
Photodriven nonoxidative coupling of CH4 (NOCM) is an attractive potential way to use abundant methane resources. Herein, an n‐type doped photocatalyst for NOCM is created by doping single‐atom Nb into hierarchical porous TiO2–SiO2 (TS) microarray, which exhibits a high conversion rate of 3.57 μmol g−1 h−1 with good recyclability. The Nb dopant replaces the 6‐coordinated titanium on the (1 0 1) plane and forms shallow electron‐trapped surface polarons along [0 1 0] direction and the comparison of different models proves that the electron localization caused by the n‐type doping is beneficial to both methane activation and ethane desorption. The positive effect of n‐type dopant on CH4 conversion is further verified on Mo‐, W‐ and Ta‐doped composites. In contrast, the doping of p‐type dopant (Ga, Cu, Fe) shows a less active influence.
Synergistic
nitrogen reduction and water oxidation process is significant
to the photocatalytic fixation of nitrogen. However, the coupling
mechanism remains ambiguous and lacks study. Herein, we report enhanced
photocatalytic nitrogen fixation on single-atom Fe-modified macro-/mesoporous
TiO2-SiO2 (Fe-T-S), with a high ammonia generation
rate of 32 μmol g–1 h–1 without
any sacrificial agent and cocatalysts. Experimental and theoretic
calculation studies confirmed the formation of a photoinduced hole-trapping
polaron on the Fe dopant, resulting in the high-valent Fe(IV) species.
The single-atom Fe(IV) site is responsible for water oxidation and
helps promote N2 hydrogenation on neighboring oxygen vacancy.
This study explicitly unravels the key to achieve the coupling between
photocatalytic N2 hydrogenation and water oxidation through
a doping strategy and provides significant guidance for the rational
design of photocatalysts for ammonia synthesis.
It is important to develop self‐producing reactive oxygen species (ROSs) systems and maintain the continuous and effective degradation of organic pollutants. Herein, for the first time, a system of ultrasound‐treated CoS2−x mixed with Fe2+ is constructed to sustainably release singlet oxygen (1O2) for the effective degradation of various organic pollutants, including dyes, phenols, and antibiotics. Ultrasonic treatment produces defects on the surface of CoS2 which promote the production of ROSs and the circulation of Fe3+/Fe2+. With the help of Co4+/Co3+ exposed on the surface of CoS2−x, the directional conversion of superoxide radical (.O2−) to 1O2 is realized. The CoS2−x/Fe2+ system can degrade organic pollutants efficiently for up to 30 days, which is significantly better than the currently recognized CuPx system (<3 days). Therefore, CoS2−x provides a new choice for the long‐term remediation of organic pollutants in controlling large area river pollution.
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