查看更多>>摘要：Effective removal of pollutants that affect human health and ecosystem stability is a crucial challenge. Here, the structural confinement engineering strategy realizes the effective anchoring of atomically dispersed Co in the Bdoped-CN network (BCN) (BCN/CoN[2 +2]). The advanced oxidation process (AOP) involved BCN/CoN[2 + 2] has realized the rapid and complete degradation to tetracycline (TCL), the removal of approximately 80% and 100% of tetracycline was achieved in 5 min and 30 min, respectively. The AOP with BCN/CoN[2 + 2] can degrade TCL over a wide pH; in addition, BCN/CoN[2 + 2] has the ability to efficiently degrade common pollutants, and its catalytic activity did not decay even if it was used repeated five times. Electron paramagnetic resonance (EPR) spectroscopy shows that BCN/CoN[2 + 2] drives the complete conversion of peroxymonosulfate (PMS) to 1O2, and density functional theory calculations demonstrate that the base for the conversion of PMS to 1O2 is from the isolated state of the active site Co.
查看更多>>摘要：Nearly 100% exposure of pi-conjugated planes, whose structure inherently exhibits large electron delocalization and fast charge transfer, has been achieved in perylene diimide (PDI) supramolecular photocatalysts by a solvent-induced self-assembly method. The high exposure ratio of pi-conjugated planes is found to cause a larger surface potential and higher surface charge density by experimental data, and higher electron distribution by DFT calculations, relative to pi-stacked planes exposed on PDI nanorods or (020) planes exposed on PDI particles, resulting in a strong internal electric field. This gives pi-conjugated PDI ca. 8-17 times higher activity on phenols photodegradation than reported PDI, and 4-6 times higher activity than well-known photocatalysts like Bi2WO6 or g-C3N4. The successful control of PDI to preferentially expose pi-conjugated planes may not only boost the photocatalytic activity in this system, but also give some guidelines in the design and development of more efficient organic photocatalysts with wide spectrum response.
查看更多>>摘要：Photocatalysis has been facing challenging problems especially the inefficient photocarriers transfer at the interfaces. Here, based on Ksp difference, we prepare the sequential heterojunction of CoS/CdS/CuS via sequential cation exchange strategy, and propose the concept of "electron-welcome zone", where the point-to-point contact can be formed at the interface, thus providing continuous electron transport channels. HAADF-STEM EDS line test indicates the formation of designed structures, and the p/n junction is confirmed by band structure and Mott Schottky analysis. Theoretical calculation indicates that CoS reduces the Gibbs free energy of the reaction. TRPL spectra show that the existence of "electron welcome zone" greatly improves the lifetime of electrons. This sequential structure enable the optimal H-2 production rate to reach 123.2 mmol g(-1) h(-1) with AQE of 45.6%, which is among the highest values of CdS-based photocatalysts. This work opens new way to efficient photo generated carrier transfer channel for solar-energy conversion.
NSTL
Elsevier