Structure-phase transformation of bismuth oxide to BiOCl/Bi24O31Cl10 shoulder-by-shoulder heterojunctions for efficient photocatalytic removal of antibiotic.

Developing heterojunction photocatalyst with well-matched interfaces and multiple charge transfer paths is vital to boost carrier separation efficiency for photocatalytic antibiotics removal, but still remains a great challenge. In present work, a new strategy of chloride anion intercalation in Bi2O3 via one-pot hydrothermal process is proposed. The as-prepared Ta-BiOCl/Bi24O31Cl10 (TBB) heterojunctions are featured with Ta-Bi24O31Cl10 and Ta-BiOCl lined shoulder-by-shouleder via semi-coherent interfaces. In this TBB heterojunctions, the well-matched semi-coherent interfaces and shoulder-by-shoulder structures provide fast electron transfer and multiple transfer paths, respectively, leading to enhanced visible light response and improved photogenerated charge separation. Meanwhile, a type-II heterojunction for photocharge separation has been obtained, in which photogenerated electrons are drove from the CB (conduction band) of Ta-Bi24O31Cl10 to the both of bilateral empty CB of Ta-BiOCl and gathered on the CB of Ta-BiOCl, while the photogenerated holes are left on the VB (valence band) of Ta-Bi24O31Cl10, effectively hindering the recombination of photogenerated electron-hole pairs. Furthermore, the separated electrons can effectively activate dissolved oxygen for the generation of reactive oxygen species (·O2-). Such TBB heterojunctions exhibit remarkably superior photocatalytic degradation activity for tetracycline hydrochloride (TCH) solution to Bi2O3, Ta-BiOCl and Ta-Bi24O31Cl10. This work not only proposes a Ta-BiOCl/Bi24O31Cl10 shoulder-by-shoulder micro-ribbon architectures with semi-coherent interfaces and successive type-II heterojunction for highly efficient photocatalytic activity, but offers a new insight into the design of highly efficient heterojunction through phase-structure synergistic transformation strategy.

Healthier Dietary Patterns Are Associated with Better Sleep Quality among Shanghai Suburban Adults: A Cross-Sectional Study.

BACKGROUND: More is to be explored between dietary patterns and sleep quality in the Chinese adult population. METHODS: A cross-sectional study including 7987 Shanghai suburban adults aged 20-74 years was conducted. Dietary information was obtained using a validated food frequency questionnaire. Adherence to a priori dietary patterns, such as the Chinese Healthy Eating Index (CHEI), Dietary Approaches to Stop Hypertension (DASH) diet and Mediterranean diet (MD), was assessed. Sleep quality was assessed from self-reported responses to the Pittsburgh Sleep Quality Index (PSQI) questionnaire. Logistic regression models adjusting for confounders were employed to examine the associations. RESULTS: The overall prevalence of poor sleep (PSQI score ≥ 5) was 28.46%. Factor analysis demonstrated four a posteriori dietary patterns. Participants with a higher CHEI (ORQ4 vs. Q1: 0.81, 95% CI: 0.70-0.95), DASH (ORQ4 vs. Q1: 0.70, 95% CI: 0.60-0.82) or MD (ORQ4 vs. Q1: 0.75, 95% CI: 0.64-0.87) had a lower poor sleep prevalence, while participants with a higher "Beverages" score had a higher poor sleep prevalence (ORQ4 vs. Q1: 1.18, 95% CI: 1.02-1.27). CONCLUSIONS: In Shanghai suburban adults, healthier dietary patterns and lower consumption of beverages were associated with better sleep quality.

Cage-modified hypocrellin against multidrug-resistant Candida spp. with unprecedented activity in light-triggered combinational photodynamic therapy.

Infections caused by multidrug-resistant fungi pose a devastating threat to human health worldwide, making new antifungal strategies urgently desired. Antimicrobial photodynamic therapy (aPDT) has gained increasing attention due to its potential in fighting against fungal infection. However, the preparation of highly efficient and water-soluble photosensitizers (PSs) for this purpose remains a challenge. Herein, we present a new strategy to prepare powerful PSs for efficient aPDT by introducing a porous cage compound, which could facilitate the transportation of O2 and reactive oxygen species (ROS). Specifically, the natural PS hypocrellin A (HA) was attached to a novel organic cage compound (covalent organic polyhedra 1 tied, COP1T) with polyethylene glycol (PEG) chains to improve its water solubility. It was found that the resulting COP1T-HA exhibited in vitro antifungal efficiency several folds higher compared to the free HA in fighting against four types of multidrug-resistant fungal planktonic cells and biofilms, including the "super fungus" Candida auris. Interestingly, the red-shift of COP1T-HA adsorption led to the realization of phototheranostic aPDT for cage-modified HA or derivatives. Additionally, COP1T-HA exhibited good biocompatibility, excellent disinfection capacity and wound healing efficiency without obvious toxic effects in vivo of rat model. With further development and optimization, COP1T-HA has great potential to become a new class of antifungal agent to fight against drug-resistant pathogens.

Chemocatalytic Conversion of Cellulosic Biomass to Methyl Glycolate, Ethylene Glycol, and Ethanol.

Production of chemicals and fuels from renewable cellulosic biomass is important for the creation of a sustainable society, and it critically relies on the development of new and efficient transformation routes starting from cellulose. Here, a chemocatalytic conversion route from cellulosic biomass to methyl glycolate (MG), ethylene glycol (EG), and ethanol (EtOH) is reported. By using a tungsten-based catalyst, cellulose is converted into MG with a yield as high as 57.7 C % in a one-pot reaction in methanol at 240 °C and 1 MPa O2 , and the obtained MG can be easily separated by distillation. Afterwards, it can be nearly quantitatively converted to EG at 200 °C and to EtOH at 280 °C with a selectivity of 50 % through hydrogenation over a Cu/SiO2 catalyst. By this approach, the fine chemical MG, the bulk chemical EG, and the fuel additive EtOH can all be efficiently produced from renewable cellulosic materials, thus providing a new pathway towards mitigating the dependence on fossil resources.

Selective Hydrogenolysis of Glycerol to 1,3-Propanediol: Manipulating the Frustrated Lewis Pairs by Introducing Gold to Pt/WOx.

A highly dispersed Au and Pt catalyst supported on WOx was developed for high performance in the selective hydrogenolysis of glycerol to 1,3-propanediol (1,3-PD) under very mild reaction conditions (81.4 % glycerol conversion, 51.6 % 1,3-PD selectivity at 413 K, 1 MPa H2 ). The highly dispersed Au decreased the original surface Lewis-acid sites on Pt/WOx but greatly increased its in situ generated Brønsted-acid sites with the assistance of H2 through the formation of frustrated Lewis pairs. These in situ formed and spatially separated pairs of H+ and H- function as the active sites in glycerol conversion to 1,3-PD.

Hydrogenolysis of Glycerol to 1,3-propanediol under Low Hydrogen Pressure over WOx -Supported Single/Pseudo-Single Atom Pt Catalyst.

Single/pseudo-single atom Pt catalyst was prepared on mesoporous WOx . The large surface area and abundant oxygen vacancies of WOx improve the Pt dispersion and stabilize the Pt isolation. This newly prepared catalyst exhibited outstanding hydrogenolysis activity under 1 MPa H2 pressure with a very high space-time yield towards 1,3-propanediol (3.78 g gPt (-1) h(-1) ) in Pt-W catalysts. The highly isolated Pt structure is thought to contribute to the excellent H2 dissociation capacity over Pt/WOx . The high selectivity towards 1,3-propanediol is attributed to the heterolytic dissociation of H2 at the interface of Pt and WOx (providing specific Brønsted acid sites and the concerted dehydration-hydrogenation reaction) and the bond formation between glycerol and WOx , which favors/stabilizes the formation of a secondary carbocation intermediate as well as triggers the redox cycle of the W species (W(6+) ⇄W(5+) ).