Defect Engineering in Bi-Based Photo/Electrocatalysts for Nitrogen Reduction to Ammonia.

Main group Bi-based materials have gained popularity as N2 reduction reaction (NRR) photo/electrocatalysts due to their ability to inhibit competitive H2 evolution reactions (HER) and the unique N2 adsorption activities. The introduction of defects in Bi-based catalysts represents a highly effective strategy for enhancing light absorption, promoting efficient separation of photogenerated carriers, optimizing the activity of free radicals, regulating electronic structure, and improving catalytic performance. In this review, we outline the various applications of state of the defect engineering in Bi-based catalysts and elucidate the impact of vacancies on NRR performance. In particular, the types of defects, methods of defects tailoring, advanced characterization techniques, as well as the Bi-based catalysts with abundant defects and their corresponding catalytic behavior in NRR were elucidated in detail. Finally, the main challenges and opportunities for future development of defective Bi-based NRR catalysts are discussed, which provides a comprehensive theoretical guidance for this field.

C-X-C motif chemokine ligand 12 improves the developmental potential of bovine oocytes by activating SH2 domain-containing tyrosine phosphatase 2 during maturation†.

In vitro maturation of mammalian oocytes is an important means in assisted reproductive technology. Most bovine immature oocytes complete nuclear maturation, but less than half develop to the blastocyst stage after fertilization. Thus, inefficient in vitro production is mainly caused by a suboptimal in vitro culture process, in which oocyte quality appears to be the limiting factor. In our study, a potential maternal regulator, C-X-C motif chemokine ligand 12, was identified by analyzing transcriptome data. C-X-C motif chemokine ligand 12 supplementation promoted the developmental potential of oocytes by improving protein synthesis and reorganizing cortical granules and mitochondria during in vitro maturation, which eventually increased blastocyst formation efficiency and cell number after parthenogenesis, fertilization, and cloning. All these promoting effects by C-X-C motif chemokine ligand 12 were achieved by activating SH2 domain-containing tyrosine phosphatase 2, thereby promoting the mitogen-activated protein kinase signaling pathway. These findings provide an in vitro maturation system that closely resembles the maternal environment to provide high-quality oocytes for in vitro production.

Multi-wavelength unidirectional forward scattering properties of the arrow-shaped gallium phosphide nanoantenna.

An arrow-shaped gallium phosphide nanoantenna exhibits both near-field electric field enhancement and far-field unidirectional scattering, and the interference conditions involve electric and magnetic quadrupoles as well as toroidal dipoles. By using long-wavelength approximation and exact multipole decomposition, the interference conditions required for far-field unidirectional transverse light scattering and backward near-zero scattering at multiple wavelengths are determined. The near-field properties are excellent, as exemplified by large Purcell factors of 4.5×109 for electric dipole source excitation, 464.68 for magnetic dipole source excitation, and 700 V/m for the field enhancement factor. The degree of enhancement of unidirectional scattering is affected by structural parameters such as the angle and thickness of the nanoantenna. The arrow-shaped nanoantenna is an efficient platform to enhance the electric field and achieve high directionality of light scattering. Moreover, the nanostructure enables flexible manipulation of light waves and materials, giving rise to superior near-field and far-field performances, which are of great importance pertaining to the practicability and application potential of optical antennas in applications such as spectroscopy, sensing, displays, and optoelectronic devices.

Design of optical anapole modes of all-dielectric nanoantennas for SERS applications.

To obtain large electric field enhancement while mitigating material losses, an all-dielectric nanoantenna composed of a heptamer and nanocubes is designed and analyzed. A numerical simulation by the finite element method reveals that the nanoantenna achieves the optical electric anapole modes, thereby significantly enhancing the coupling between different dielectrics to further improve the near-field enhancement and spontaneous radiation. Field enhancement factors |E/E 0|2 of 3,563 and 5,395 (AM1 and AM2) and a Purcell factor of 3,872 are observed in the wavelength range between 350 and 800 nm. This nanoantenna has promising potential in applications involving surface-enhanced Raman scattering and nonlinearities due to its low cost and excellent compatibility.

Constructing In2S3/CdS/N-rGO Hybrid Nanosheets via One-Pot Pyrolysis for Boosting and Stabilizing Visible Light-Driven Hydrogen Evolution.

The construction of hybrid junctions remains challenging for the rational design of visible light-driven photocatalysts. Herein, In2S3/CdS/N-rGO hybrid nanosheets were successfully prepared via a one-step pyrolysis method using deep eutectic solvents as precursors. Benefiting from the surfactant-free pyrolysis method, the obtained ultrathin hybrid nanosheets assemble into stable three-dimensional self-standing superstructures. The tremella-like structure of hybrid In2S3/N-rGO exhibits excellent photocatalytic hydrogen production performance. The hydrogen evolution rate is 10.9 mmol·g-1·h-1, which is greatly superior to CdS/N-rGO (3.7 mmol·g-1·h-1) and In2S3/N-rGO (2.6 mmol·g-1·h-1). This work provides more opportunities for the rational design and fabrication of hybrid ultrathin nanosheets for broad catalytic applications in sustainable energy and the environment.

Contribution of ultrasound in combination with chlorogenic acid against Salmonella enteritidis under biofilm and planktonic condition.

The antibacterial and antibiofilm mechanisms of ultrasound combined with chlorogenic acid treatment for Salmonella enteritidis under biofilm and planktonic condition were investigated. S. enteritidis under biofilm and planktonic cells were treated with ultrasound, chlorogenic acid, and their combination for 5, 10, 20, 30, and 60 min. Results showed that the combined treatments exhibited synergistic effects that inactivated the S. enteritidis biofilm and planktonic cells. The nucleic acids and ATP leakage and CLSM imagines showed that the combining chlorogenic acid and ultrasound treatment significantly increased the permeability of the S. enteritidis cell membrane. SEM indicated that the combining chlorogenic acid and ultrasound treatment quickly destroyed the integrity of the S. enteritidis cell membrane, and the activity of respiratory chain dehydrogenase sharply decreased. Additionally, the amounts of polysaccharides in the S. enteritidis biofilms significantly decreased after the combined treatments. Hence, the combining chlorogenic acid and ultrasound treatment have potential applications in food preservation.

Antibacterial and Antibiofilm Effect of Ultrasound and Mild Heat Against a Multidrug-Resistant Klebsiella pneumoniae Stain Isolated from Meat of Yellow-Feathered Chicken.

Klebsiella pneumoniae is an important foodborne pathogen with high biofilm-forming ability, which is continuously detected in food products in recent years. The antibacterial and antibiofilm activities and mechanism of ultrasonication in combination with heat treatment against K. pneumoniae were studied. K. pneumoniae planktonic and biofilm cells were treated with ultrasound (US), mild heat treatment (HT50, HT60, and HT70), and combinations of US and mild heat treatment (UH50, UH60, and UH70) for 5, 10, 20, 30, and 60 min. Results showed that the combination of US and mild heat treatment was more effective in inactivating K. pneumoniae planktonic and biofilm cells than the single treatment by counting viable bacteria. In addition, confocal laser scanning microscopy, scanning electron microscopy, and analysis of leakage of intracellular substances have revealed that the combination treatment effectively damaged the integrity of bacterial cell membrane and increased cell permeability, which led to the quick release of adenosine triphosphate (ATP) and macromolecular substances of nucleic acids and proteins. Moreover, the activities of respiratory chain dehydrogenase in planktonic and biofilm cells significantly decreased after UH treatment. The results indicated that ultrasonication and mild heat treatment had a synergistic effect on the inactivation of K. pneumoniae planktonic and biofilm cells by damaging the cell membrane and inhibiting intercellular cell respiration.

Polymeric Carbon Nitride-Derived Photocatalysts for Water Splitting and Nitrogen Fixation.

Photocatalysis is a promising energy conversion and environmental restoration technology. The main focus of photocatalysis is the development and manufacture of highly efficient photocatalysts. Semiconductor-based photocatalysis technology based on harnessing solar energy is considered as an attractive approach to solve the problems of global energy shortage and environmental pollution. Since 2009 pioneering work has been carried out on polymeric carbon nitride (PCN) for visible photocatalytic water splitting, thus PCN-based photocatalysis has become a hot research topic, demanding significant research attention. This article reviews the physical and chemical properties, synthesis methods, and the methods to control the morphology, heteroatom doping, and construction of heterojunctions to improve the performance of PCN-based photocatalysts in water splitting and nitrogen fixation. Through different design strategies, the photo-generated electron-hole pair separation efficiency of PCN materials can be effectively improved, thereby improving their photocatalytic performance. Finally, the challenges of PCN-based photocatalysts in water splitting and nitrogen fixation applications are discussed herein. It is strongly believed that through different design strategies, efficient PCN-based photocatalysts can be constructed for both water splitting and nitrogen reduction. These excellent modification strategies can be used as a guiding theory for photocatalytic reactions of other promising catalysts and further promote the development of photocatalysis.

Transcriptional memory inherited from donor cells is a developmental defect of bovine cloned embryos.

Studies on the effects of transcriptional memory on clone reprogramming in mammals are limited. In the present study, we observed higher levels of active histone H3 lysine 4 trimethylation (H3K4me3 and 5-hydroxymethylcytosine) and repressive (5-methylcytosine) epigenetic modifications in bovine early cloned embryos than in in vitro fertilized embryos. We hypothesized that aberrant epigenetic modification may result in transcriptional disorders in bovine somatic cell nuclear transfer (SCNT) embryos. RNA sequencing results confirmed that both abnormal transcriptional silencing and transcriptional activation are involved in bovine SCNT reprogramming. The cloned embryos exhibited excessive transcription in RNA processing- and translation-related genes as well as transcriptional defects in reproduction-related genes whose transcriptional profiles were similar to those in donor cells. These results demonstrated the existence of active and silent memory genes inherited from donor cells in early bovine SCNT embryos. Further, H3K4me3-specific demethylase 5B (KDM5B) mRNA was injected into the reconstructed embryos to reduce the increased H3K4me3 modification. KDM5B overexpression not only reduced the transcriptional level of active memory genes, but also promoted the expression of silent memory genes; in particular, it rescued the expression of multiple development-related genes. These results showed that transcriptional memory acts as a reprogramming barrier and KDM5B improves SCNT reprogramming via bidirectional regulation effects on transcriptional memory genes in bovines.

Rumen bacteria and meat fatty acid composition of Sunit sheep reared under different feeding regimens in China.

BACKGROUND: Rumen bacteria play a critical role in feed degradation and productivity. This study evaluated the impact of feeding regimen on the rumen microbial populations and fatty acid composition of the meat of sheep. Twenty-four Sunit sheep were raised on a grass pasture from birth to 9 months of age, at which time they were randomly divided into two feeding groups: pasture feeding (PF) and barn feeding (BF). Sheep in the PF group were allowed to graze freely on wild grassland for 3 months. Sheep in the BF group were confined for 3 months to a dry barn, in which they roamed freely with corn straw and corn. RESULTS: Sheep in the PF group had greater rumen bacteria diversity. The relative abundances of the genera Butyrivibrio_2, Saccharofermentans and Succiniclasticum were increased, and that of the genus RC9_gut_group was decreased, in the PF compared to the BF sheep. The n-3 polyunsaturated fatty acid contents were greater in meat from PF sheep than from BF sheep. In addition, the α-linolenic acid (C18:3 n-3, ALA) and conjugated linoleic acid (CLA) contents were positively correlated with the abundance of Butyrivibrio_2. CONCLUSION: Grazing may improve the diversity of rumen bacteria and increase the proportion of ALA and CLA in sheep meat. © 2020 Society of Chemical Industry.

In Situ Growth of Ag Nanodots Decorated Cu2 O Porous Nanobelts Networks on Copper Foam for Efficient HER Electrocatalysis.

Developing earth-abundant electrocatalysts for high-efficiency hydrogen evolution reaction (HER) has become one of the leading research frontiers in energy conversion. Here, the design and in situ growth of Ag nanodots decorated Cu2 O porous nanobelts networks on Cu foam (denoted as Ag@Cu2 O/CF) are carried out via a simple one-pot solution strategy at room temperature. Serving as self-supporting electrocatalysts, Ag@Cu2 O porous nanobelts provide plentiful active sites, and the 3D hybrid foams provide fast transportation for electrolyte and short diffusion path for newly formed H2 bubbles, which result in excellent electrocatalytic HER activity and long-term stability. Owing to the synergistic effect between Ag nanodots and Cu2 O porous nanobelts and CF, the hybrid electrocatalyst exhibits a low Tafel slope of 58 mV dec-1 , a small overpotential of 108 mV at 10 mA cm-2 , and high durability for more than 20 h at a potential of 200 mV for HER in 1.0 mol L-1 KOH solution.

Allopurinol treatment improves renal function in patients with type 2 diabetes and asymptomatic hyperuricemia: 3-year randomized parallel-controlled study.

OBJECTIVE: To investigate the effects of long-term effective control of serum uric acid on renal function in patients with type 2 diabetes and asymptomatic hyperuricemia. METHODS: Application of randomized open parallel-controlled methods, a total of 176 patients with type 2 diabetes and asymptomatic hyperuricemia were selected, and was randomly divided into two groups for allopurinol or conventional treatments, respectively. Changes in urinary albumin excretion rate (UAER), the levels of serum creatinine and glomerular filtration rate (GFR) and the incidence of new-onset diabetic nephropathy (DN) and hypertension in patients before and after 3 years of treatment were measured and compared between groups. RESULTS: There were no statistically significant difference in the baseline clinical characteristics of study participants between two treatment groups (P > 0·05 for all). After 3 years of treatment, compared to the conventional treatment, the allopurinol treatment was more effective in reducing serum uric acid, UAER, serum creatinine (P < 0·01 for all) and increasing GFR (P < 0·01). The intention-to-treat (ITT) analysis indicated that the incidence of new-onset DN and hypertension in the allopurinol group showed a declining trend compared to that in the conventional treatment group, despite a lack of significant difference (P > 0·05). CONCLUSION: Long-term effective control of serum uric acid can decrease UAER and serum creatinine, increase GFR and may exert kidney protection effects in patients with type 2 diabetes and asymptomatic hyperuricemia.

S-vacancy-assisted fast charge transport and oriented ReS2 growth in twin crystal ZnxCd1-xS: an atomic-level heterostructure for dual-functional photocatalytic conversion.

The achievement of dual-functional photocatalytic technology requires a photocatalyst with accelerated charge flow and purposeful active-site arrangement. In this study, we developed an oriented embedding strategy to induce ReS2 growth at the S vacancy in twin-crystal Zn0.5Cd0.5S solid solution (Sv-ZCS), obtaining an atomic-level heterostructure (ReS2/Sv-ZCS). The electronic structure calculations demonstrate that the charge density of the Zn atom around the S vacancy is higher than for other Zn atoms and the introduced S vacancy establishes a high-speed channel for electron transport via formed Zn-S-Re bonds at the interface between ReS2 and Sv-ZCS. Photogenerated electrons and holes gathered on Re atoms and Sv-ZCS, respectively, which achieves spatial charge separation and separated arrangement for redox sites. As a result, the optimized ReS2/Sv-ZCS heterostructure possesses high efficiency of electron injection (2.6-fold) and charge separation (8.44-fold), as well as excellent conductivity capability (20.16-fold). The photocatalytic performance of the ReS2/Sv-ZCS composite exhibits highly improved dual-functional activity with simultaneous H2 evolution and selective oxidation of benzyl alcohol. The reaction rate of benzaldehyde and H2 evolution reaches 125 mmol gcat-1 h-1 and 159 mmol gcat-1 h-1, which is the highest efficiency achieved so far for simultaneous coproduction of H2 fuel and organic chemicals on ReS2-based composites. This work enriches the application of ReS2-modified composites in a dual-functional photoredox system and also gives insight into the role of defects in electronic structure modification and activity improvement.

Effects of different electrostatic field intensities assisted controlled freezing point storage on water holding capacity of fresh meat during the early postmortem period.

In this study, the effect of different intensity electrostatic fields on the water holding capacity (WHC) of fresh meat during the early postmortem period in controlled freezing point storage (CFPS) were investigated. Significantly lower cooking loss were found in low voltage electrostatic field (LVEF) and high voltage electrostatic field (HVEF) compared to the control group (CK) (p < 0.05). The myofibril fragmentation index and microstructure results suggested that the sample under HVEF treatment remained relatively intact. It has been revealed that the changes in actomyosin properties under electrostatic field treatment groups were due to the combination and dissociation of actomyosin binding into myofilament concentration, which consequently affects the muscle WHC. The study further demonstrated that the electrostatic field, especially HVEF, might increase the WHC of fresh meat by affecting the distribution of water molecules and physiochemical properties of actomyosin during the early postmortem period.

The rice E3 ubiquitin ligase-transcription factor module targets two trypsin inhibitors to enhance broad-spectrum disease resistance.

Broad-spectrum disease resistance (BSR) is crucial for controlling plant diseases and relies on immune signals that are subject to transcriptional and post-translational regulation. How plants integrate and coordinate these signals remains unclear. We show here that the rice really interesting new gene (RING)-type E3 ubiquitin ligase OsRING113 targets APIP5, a negative regulator of plant immunity and programmed cell death (PCD), for 26S proteasomal degradation. The osring113 mutants in Nipponbare exhibited decreased BSR, while the overexpressing OsRING113 plants showed enhanced BSR against Magnaporthe oryzae (M. oryzae) and Xanthomonas oryzae pv. oryzae (Xoo). Furthermore, APIP5 directly suppressed the transcription of the Bowman-Birk trypsin inhibitor genes OsBBTI5 and AvrPiz-t-interacting protein 4 (APIP4). Overexpression of these two genes, which are partially required for APIP5-mediated PCD and disease resistance, conferred BSR. OsBBTI5 and APIP4 associated with and stabilized the pathogenesis-related protein OsPR1aL, which promotes M. oryzae resistance. Our results identify an immune module with integrated and coordinated hierarchical regulations that confer BSR in plants.

Zein and tannic acid hybrid particles improving physical stability, controlled release properties, and antimicrobial activity of cinnamon essential oil loaded Pickering emulsions.

Pickering emulsion loading essential oil has demonstrated a promising strategy as delivery system in food preservation, but localization in stability and antimicrobial activity limits application. In this study, Pickering emulsions co-loaded with tannic acid and cinnamon essential oil (ZTC) have been developed based on zein and tannic acid complexes (ZT) mediated interfacial engineering. Fourier transform infrared, fluorescence spectroscopy, and molecular docking results indicated tannic acid altered the structural of zein. Interfacial tension results indicated that tannic acid accelerated the adsorbed speed of zein particles by decreased interfacial tension (11.99-9.96 mN/m). ZT5 formed a viscoelastic and dense layer in oil-water interface than that for other ZTs, which improved stability and control release performance of ZTC. Furthermore, the ZTC showed an effective antimicrobial activity against spoilage organisms Pseudomonad paralactis MN10 and Lactobacillus sakei VMR17. These findings provide new insight for developing co-loaded multiple antimicrobial agents within Pickering emulsion as a delivery system.

Modulating Lewis acidic active sites of Fe doped Bi2MoO6 nanosheets for enhanced electrochemical nitrogen fixation.

Electrocatalytic nitrogen reduction reaction (NRR) for artificial ammonia synthesis under mild conditions has been considered as a promising alternative to the conventional Haber-Bosch method. The highly desired efficient NRR still faced with the mulriple challenges of adsorption and activation of N2 and limited Faraday efficiency. Here, Fe-doped Bi2MoO6 nanosheets fabricated by one step synthesis exhibits high NH3 yield rate of 71.01 µg·h-1·mg-1 and Faraday Efficiency of 80.12%. The decreased electron density of Bi in collaboration with Lewis acid active sites on Fe-doped Bi2MoO6, jointly enhance the adsorption and activation of Lewis basic N2. Benefited from surface texture optimization and the superior ability of N2 adsorption and activation, the increasing density of effective active sites greatly improve the NRR behavior. This work provides new opportunities for developing efficient and highly selective catalysts for NH3 synthesis via NRR.

Characterisation, slow-release, and antibacterial properties of carboxymethyl chitosan/inulin hydrogel film loaded with novel antilisterial durancin GL.

This paper reports the development of a hydrogel film with antibacterial activity and controlled release characteristics. Carboxymethyl chitosan (CMCS) is grafted onto durancin GL and inulin via a mediated reaction between N-hydroxysuccinimide and 1-(3-dimethylaminopropyl)-3-ethylcarbodiimide hydrochloride. Rheology tests, Fourier transform infrared (FTIR) spectroscopy, X-ray photoelectron spectroscopy, and lap shear tests confirmed the formation of a stable chemical cross-linking and excellent adhesion hydrogel with 4 % CMCS and 8 % inulin. The CMCS/inulin hydrogel film loaded with durancin GL appears transparent and uniform. FTIR spectroscopy results reveal the interaction mode among CMCS, inulin, durancin GL, and the hydrogel film structure. Cross-linking improved thermal stability and water-vapour barrier performance. The hydrophobicity of CMCS/inulin @Durancin GL increased under a durancin GL concentration of 0.036 g/30 mL, and the release of active substances is prolonged. In-vitro antibacterial capacity and salmon preservation experiments show that the addition of durancin GL enhanced the antibacterial activity of the hydrogel film. Therefore, CMCS/inulin@Durancin GL hydrogel films can be used as fresh-keeping packaging materials in practical applications.

Construction of S-Scheme heterojunction Ni11(HPO3)8(OH)6/CdS photocatalysts with open framework surface for enhanced H2 evolution activity.

The emerging S-scheme heterojunction shows a particular superiority in enhancing the efficiency of charge separation in photocatalyst. Herein, a Ni11(HPO3)8(OH)6/CdS heterojunctions (NiPO/CdS) are constructed for the first time by loading open framework structure NiPO on the surface of CdS nanoparticles (CdS NPs). The built-in electric field generated at the interface promotes the directional migration of photogenerated electrons from NiPO to CdS. This S-scheme pathway achieves a strong redox capacity and efficient carrier separation. More importantly, the unique triangular and hexagonal channels of NiPO facilitate the exposure of CdS active sites for proton adsorption, H2 production and escape. The hydrogen evolution rate of NiPO/CdS is 39 mmol g-1 h-1 under visible light irradiation, which is 6.5 times higher than that of pure CdS. The NiPO/CdS heterojunction also exhibits remarkable long-term stability. This study provides a new strategy for the ingenious design of S-scheme photocatalysts with excellent photocatalytic performance.