2D-g-C3N4 nanosheet was prepared and employed for the adsorption of elemental mercury (Hg0). The g-C3N4 was analyzed through X-ray diffraction (XRD), scanning electron microscope (SEM) and Fourier transform infrared spectroscopy (FT-IR) methods, and the results showed that the prepared sample was well-defined 2D-nanosheet. The 2D-g-C3N4 sorbent exhibited a high Hg0 removal efficiency (> 90%) at the condition of temperature 120 °C. To investigate the mechanism of Hg0 adsorption on the 2D-g-C3N4 surface, corresponding theoretical exploration based on the first principle prediction and X-ray photoelectron spectroscopy (XPS) test was implemented. The DFT calculation results showed that Hg0 was strongly bound to the B1 site of the g-C3N4 surface with an adsorption energy change of -162.2 kJ mol−1, the equilibrium distance of Hg-C was 3.473 Å, and electron transfer between Hg and C atoms was 0.02. The results of XPS showed the main species of mercury was HgO on the surface of 2D-g-C3N4 sample and the interaction between C3N4 surface and Hg0 was physisorption. This study provides a demonstration of proof-of-concept demonstration that g-C3N4 is a promising sorbent capable of capturing Hg0, and presents in-depth understanding of Hg0 adsorption mechanism on 2D-g-C3N4 sorbent.@en

To guarantee drinking water security, removal of bromate (BrO3 −) has garnered plenty of attention in water treatment. In current study, we have developed a novel conjugated donor-acceptor (D-A) photocatalyst (4,4′'-bis(diphenylamino)-[1,1′:4′,1′'-terphenyl]-2′,5′-dicarbaldehyde, BDTD) with supramolecule architecture assembling via intermolecular C–H···O hydrogen bonds and C–H···π interactions. Both diffuse reflectance spectrum (DRS) and density functional theoretical (DFT) calculations gave the bandgap of Eg = 2.21 eV, clearly indicating the visible-light response of BDTD supramolecule. The calculations showed that BDTD supramolecule could induce nearly 100% removal of BrO3 − stably at pH-neutral condition driven by visible light, accounting for a first-order kinetic constant being one order of magnitude higher than most of the photocatalysts previous reported. As demonstrated by our electron scavenger experiment and DFT calculations, the BDTD supramolecule should undergo the photocatalytic reduction of BrO3 − through direct reduced by the lowest unoccupied molecular orbital of conduction band (potential of −1.705 V versus standard hydrogen electrode) electron. The BDTD supramolecule may serve as an attractive photocatalyst by virtue of response to visible light, efficient charge transfer and separation as well as high photocatalytic activity, which will make the removal of BrO3 − in water much easier, more economical and more sustainable.@en

This work focuses on the photocatalytic removal of recalcitrant organic pollutants in water treatment. Based on facile precipitation reaction, we fabricated a photocatalyst (PbCrO4) in single crystals that present evident response to visible light and employed the catalyst in the photocatalytic decomposition of microcystin-LR (MC-LR). In the degradation test using the nanorods with prepared PbCrO4 photocatalyst, a 100% removal efficiency (27 min reaction) and a kinetics constant of 0.1356 min−1 were achieved. Such a high performance of PbCrO4 in photocatalytic conversion of MC-LR was ascribed to its high carrier separation efficiency, positive valence band (VB) position, and good delocalization of VB and conduction band (CB). The test of electron spin-resonance resonance (ESR) demonstrated that excessive free [rad]OH radicals were produced during the PbCrO4 photocatalysis of MC-LR. The density functional theory (DFT) and LC/MS/MS technology were employed to ascertain the intermediates during the MC-LR photocatalytic degradation. The major intermediates were resulted from the attack of hydroxyl radicals to the ADDA side chains of MC-LR structure. This study provides a proof-of-concept strategy to develop effective photocatalysts to efficiently produce [rad]OH radicals for the visible-light induced photocatalytic degradation of MC-LR in water.@en

This work focuses on the photocatalytic removal of recalcitrant organic pollutants in water treatment. Based on facile precipitation reaction, we fabricated a photocatalyst (PbCrO4) in single crystals that present evident response to visible light and employed the catalyst in the photocatalytic decomposition of microcystin-LR (MC-LR). In the degradation test using the nanorods with prepared PbCrO4 photocatalyst, a 100% removal efficiency (27 min reaction) and a kinetics constant of 0.1356 min−1 were achieved. Such a high performance of PbCrO4 in photocatalytic conversion of MC-LR was ascribed to its high carrier separation efficiency, positive valence band (VB) position, and good delocalization of VB and conduction band (CB). The test of electron spin-resonance resonance (ESR) demonstrated that excessive free [rad]OH radicals were produced during the PbCrO4 photocatalysis of MC-LR. The density functional theory (DFT) and LC/MS/MS technology were employed to ascertain the intermediates during the MC-LR photocatalytic degradation. The major intermediates were resulted from the attack of hydroxyl radicals to the ADDA side chains of MC-LR structure. This study provides a proof-of-concept strategy to develop effective photocatalysts to efficiently produce [rad]OH radicals for the visible-light induced photocatalytic degradation of MC-LR in water.@en