Designing ultrathin Fe doped Ta2O5-x nanobelts for highly enhanced ammonia photosynthesis.

Solar-light photosynthesis of ammonia form N2 reduction in ultrapure water over the artificial photocatalysts is attractive but still challenging compared with Haber-Bosch process. In this work, ultrathin Fe-Ta2O5-x nanobelts were fabricated via the controllable solvothermal process for ammonia photosynthesis. The formed oxygen vacancies and Fe doping narrowed their bandgap energies and promoted the carriers' separation and transfer for Fe-Ta2O5-x nanobelts. In addition, Fe doping also resulted in the reduced working functions of the samples, indicating a weaker electron binding restriction and stronger separation and transfer of photo-induced carriers. The experimental results showed that Fe-Ta2O5-x nanobelts showed remarkably enhanced photocatalytic ammonia production performance under simulated sunlight irradiation, and the relevant ammonia production rate reached approximately 3030.86 µM g-1 h-1, which was 9.63 times of pristine Ta2O5-x and 491.0 times of commercial Ta2O5, and a relatively stable photocatalytic ammonia production performance under simulated sunlight irradiation for Fe-Ta2O5-x nanobelts. Meanwhile, it was also found that Fe doping has great influences on the photocatalytic performance under visible light and simulated sunlight irradiation, mainly because of their suitable bandgap energies and enhanced solar-light harvesting capacity. Current work indicates the great potentials of ultrathin tantalum-based functional materials for high-efficiency ammonia photosynthesis.

Designing step-scheme AgI decorated Ta2O5-x heterojunctions for boosted photodegradation of organic pollutants.

Step-scheme (S-scheme) AgI decorated Ta2O5-x heterojunctions have been designed and synthesized via a combination of solvothermal and chemical deposition methods for enhanced visible-light harvesting and high-performance photocatalysis. The AgI nanoparticles showed great influences on the visible-light absorption and charge separation between AgI and Ta2O5-x microspheres. The experimental results indicated that the as-prepare AgI/Ta2O5-x composites achieved enhanced photocatalytic performance towards tetracycline degradation under visible light, and the AgI/Ta2O5-x-11 sample displayed the highest photocatalytic performance and the maximum rate constant of approximately 0.09483 min-1, which was 7.22 times that of Ta2O5-x microspheres and 2.56 times that of AgI, respectively. The highly enhanced photocatalytic performance was mainly attributed to the construction of S-scheme heterostructure and formation of oxygen vacancies in Ta2O5-x microspheres. In addition, the trapping experimental and DMPO spin-trapping ESR spectra confirmed the ⸱O2- and ⸱OH species as the main radicals during tetracycline degradation. Current work indicates an S-scheme tantalum-based composites for high-performance environmental photocatalysis.

Rational design of S-scheme AgI/ZrTiO4-x heterojunctions for remarkably boosted norfloxacin degradation.

Emerging S-scheme heterojunction photocatalysts endowed with efficient charge separation and strong redox capacity have stimulated wide interests in dealing with environmental issues nowadays. In this work, we firstly fabricated the oxygen vacancy modified ZrTiO4-x nanocrystals, which was further combined with AgI to build the defective S-scheme AgI/ZrTiO4-x heterojunctions for visible-light photocatalytic norfloxacin degradation. The synthesized ZrTiO4-x nanocrystals and AgI/ZrTiO4-x heterojunctions displayed remarkably boosted norfloxacin degradation performance under visible-light irradiation. The reaction rate constant of the optimized AgI/ZrTiO4-x-5% heterojunction is as high as 0.01419 min-1, which is approximately 43.35 times that of AgI and 7.93 times that of ZrTiO4-x nanocrystals, and far superior to those of commercial TiO2 and commercial ZrO2. The high-performance photocatalytic norfloxacin degradation could be mainly attributed to the formation of S-scheme charge transfer pathways and oxygen vacancy defects. More significantly, AgI/ZrTiO4-x could also realize the effective photo-decomposition of other emerging pollutants. Finally, the visible-light photocatalytic performance and photocatalysis mechanism were investigated.

Construction of Au and C60 quantum dots modified materials of Institute Lavoisier-125(Ti) architectures for antibiotic degradation: Performance, toxicity assessment, and mechanistic insight.

High-performance and stabilized photocatalytic degradation of antibiotic contaminants still remains a challenge in environmental photocatalysis and has been studied worldwide. In this work, hybrid Au and C60 quantum dots decorated Materials of Institute Lavoisier-125(Ti) (MIL-125(Ti)) composites were successfully fabricated for visible-light photocatalytic tetracycline degradation with pristine MIL-125(Ti) as a comparison. The experimental results revealed that the introduction of C60 quantum dots and Au nanoparticles resulted in highly enhanced visible-light harvesting and charge separation for efficient tetracycline degradation. The optimal Au/C60-MIL-125(Ti)-1.0% sample exhibited the highest visible-light photocatalytic performance, and the corresponding rate constant was approximately 9.19 times of MIL-125(Ti), indicating the significant roles of Au and C60 quantum dots in boosting visible-light absorption and charge separation. Furthermore, the radical species, possible degradation pathways and toxicity assessment, and photocatalytic mechanism were also investigated. Current work indicates a synergistic strategy for enhancing visible-light harvesting and charge separation to fabricate high-performance composite photocatalysts.

Topotactic formation of poriferous (Al,C)-Ta2O5 mesocrystals for improved visible-light photocatalysis.

Poriferous monocrystal-like nanostructures are contributing to fabricate long-distance charge transfer pathways and rapid diffusions of the degraded products, and attracts wide attentions. In this work, layered and poriferous (Al,C)-Ta2O5 mesocrystals were fabricated by topotactic transformation strategy with Ta4AlC3 MAX as starting materials for visible-light photocatalytic antibiotic degradation. The prepared sample exhibited enhanced visible-light absorption and visible-light photocatalytic performance, far superior to those of commercial Ta2O5 and Ta4AlC3 MAX, which was mainly because of the elemental doping in the samples. The experimental results also indicated that continuous attacks of the photo-generated holes and ·O2- species efficiently induced efficient visible-light photodegradation of tetracycline. Current work also indicates a new and potential tantalum-based semiconductors for high-performance environmental photocatalysis.

Oxyfunctionalization of Alkanes Based on a Tricobalt(II)-Substituted Dawson-Type Rhenium Carbonyl Derivative as Catalyst.

POM-supported metal carbonyl derivatives (PMCDs) represent a family of tremendous potential catalysts owing to their peculiar physical and chemical properties. Yet low-valence transition metal-substituted Dawson-type PMCD catalysts are uncommon. Hence, we synthesized a tricobalt-substituted PMCDs by conventional aqueous solution method, [Na(H2O)5](NH4)7[P2W15O56Co3(H2O)3(OH)3Re(CO)3]·13H2O (1), and characterized by single crystal X-ray diffraction crystallography, IR, and thermogravimetric analyses (TGA), etc. The obtained compound 1 was employed as a catalyst for the oxidation of diphenylmethane (DPM) to benzophenone, giving 96.8% yield in the presence of tert-butyl hydroperoxide (TBHP) and pyridine. The control experiments indicate that Co metal ion plays an important role in the catalytic reactions. As a side note, the electrospray ionization mass spectrometry (ESI-MS) and UV spectroscopy showed that 1 can retain its integrity in solution, and magnetic measurements indicated that 1 exhibited a weaker ferromagnetic interaction at low temperature.