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Quadruple bonding between iron and boron in the BFe(CO)3- complex.
While main group elements have four valence orbitals accessible for bonding, quadruple bonding to main group elements is extremely rare. Here we report that main group element boron is able to form quadruple bonding interactions with iron in the BFe(CO)3- anion complex, which has been revealed by quantum chemical investigation and identified by mass-selected infrared photodissociation spectroscopy in the gas phase. The complex is characterized to have a B-Fe(CO)3- structure of C3v symmetry and features a B-Fe bond distance that is much shorter than that expected for a triple bond. Various chemical bonding analyses indicate that the complex involves unprecedented BâŁFe quadruple bonding interactions. Besides the common one electron-sharing Ï bond and two FeâB dative Ï bonds, there is an additional weak BâFe dative Ï bonding interaction. This finding of the new quadruple bonding indicates that there might exist a wide range of boron-metal complexes that contain such high multiplicity of chemical bonds
Efficient depolymerization of lignin through microwave-assisted Ru/C catalyst cooperated with metal chloride in methanol/formic acid media
Lignin, an abundant aromatic biopolymer, has the potential to produce various biofuels and chemicals through biorefinery activities and is expected to benefit the future circular economy. Microwave-assisted efficient degradation of lignin in methanol/formic acid over Ru/C catalyst cooperated with metal chloride was investigated, concerning the effect of type and dosage of metal chloride, dosage of Ru/C, reaction temperature, and reaction time on depolymerized product yield and distribution. Results showed that 91.1Â wt% yield of bio-oil including 13.4Â wt% monomers was obtained under the optimum condition. Yields of guaiacol-type compounds and 2,3-dihydrobenzofuran were promoted in the presence of ZnCl2. Formic acid played two roles: (1) acid-catalyzed cleavage of linkages; (2) acted as an in situ hydrogen donor for hydrodeoxygenation in the presence of Ru/C. A possible mechanism for lignin degradation was proposed. This work will provide a beneficial approach for efficient depolymerization of lignin and controllable product distribution
Managing Excess Lead Iodide with Functionalized OxoâGraphene Nanosheets for Stable Perovskite Solar Cells
Stability issues could prevent lead halide perovskite solar cells (PSCs) from commercialization despite it having a comparable power conversion efficiency (PCE) to silicon solar cells. Overcoming drawbacks affecting their long-term stability is gaining incremental importance. Excess lead iodide (PbI2) causes perovskite degradation, although it aids in crystal growth and defect passivation. Herein, we synthesized functionalized oxo-graphene nanosheets (Dec-oxoG NSs) to effectively manage the excess PbI2. Dec-oxoG NSs provide anchoring sites to bind the excess PbI2 and passivate perovskite grain boundaries, thereby reducing charge recombination loss and significantly boosting the extraction of free electrons. The inclusion of Dec-oxoG NSs leads to a PCE of 23.7â% in inverted (p-i-n) PSCs. The devices retain 93.8â% of their initial efficiency after 1,000â
hours of tracking at maximum power points under continuous one-sun illumination and exhibit high stability under thermal and ambient conditions
Self-adaptive logit balancing for deep neural network robustness: Defence and detection of adversarial attacks
With the widespread applications of Deep Neural Networks (DNNs), the safety of DNNs has become a significant issue. The vulnerability of the neural networks against adversarial examples deepens concerns about the safety of DNNs applications. This paper proposed a novel defence method to improve the adversarial robustness of DNN classifiers without using adversarial training. This method introduces two new loss functions. First, a zero-cross-entropy loss is used to punish overconfidence and find the appropriate confidence for different instances. Second, a logit balancing loss is proposed to protect DNNs from non-targeted attacks by regularising incorrect classesâ logits distribution. This method achieved competitive adversarial robustness compared to advanced adversarial training methods. Meanwhile, a novel robustness diagram is proposed to analyse, interpret and visualise the robustness of DNN classifiers against adversarial attacks. Furthermore, a Log-Softmax-pattern-based adversarial attack detection method is proposed. This detection method can distinguish clean inputs and multiple adversarial attacks via one multi-classification MLP. In particular, it is state-of-the-art in identifying white-box gradient-based attacks; it achieved at least 95.5% accuracy for classifying four white-box gradient-based attacks with maximum 0.1% false positive ratio
Synergistic Hydrolysis of Soy Proteins Using Immobilized Proteases: Assessing Peptide Profiles
Because of the health benefits and economic opportunities, extracting bioactive peptides from plant proteins, often food processing by-products, garners significant interest. However, the high enzyme costs and the emergence of bitter peptides have posed significant challenges in production. This study achieved the immobilization of Alcalase and Flavorzyme using cost-effective SiO2 microparticles. Mussel-inspired chemistry and biocompatible polymers were employed, with genipin replacing glutaraldehyde for safer crosslinking. This approach yielded an enzyme loading capacity of approximately 25 mg/g support, with specific activity levels reaching around 180 U/mg for immobilized Alcalase (IA) and 35 U/mg for immobilized Flavorzyme (IF). These immobilized proteases exhibited improved activity and stability across a broader pH and temperature range. During the hydrolysis of soy proteins, the use of immobilized proteases avoided the thermal inactivation step, resulting in fewer peptide aggregates. Moreover, this study applied peptidomics and bioinformatics to profile peptides in each hydrolysate and identify bioactive ones. Cascade hydrolysis with IA and IF reduced the presence of bitter peptides by approximately 20%. Additionally, 50% of the identified peptides were predicted to have bioactive properties after in silico digestion simulation. This work offers a cost-effective way of generating bioactive peptides from soy proteins with reducing potential bitterness
Risk factors associated with severe scrub typhus in Shandong, northern China
Objectives: The aim of this study was to identify risk factors associated with severe scrub typhus, in order to provide a reference for clinical decision-making.
Methods: A caseâcontrol study was conducted of scrub typhus patients who presented at local hospitals between 2010 and 2013. In total, 46 patients with severe scrub typhus complications (cases) and 194 without severe complications (controls) were included.
Results: There were significant differences in the duration of illness before effective antibiotic therapy, lymphadenopathy, rash, blood platelet count, white blood cell (WBC) count, percentage neutrophils, and percentage lymphocytes between the case and control groups. Multivariate analysis demonstrated that the following four factors were significantly associated with the severe complications of scrub typhus: (1) duration of illness before effective antibiotic therapy (odds ratio (OR) 2.287, 95% confidence interval (CI) 1.096â4.770); (2) the presence of a rash (OR 3.694, 95% CI 1.300â10.495); (3) lymphadenopathy (OR 2.438, 95% CI 1.090â5.458); (4) blood platelet count <100Â ĂÂ 109/l (OR 2.226, 95% CI 1.002â4.946).
Conclusions: This study indicates that improved diagnosis and timely treatment are important factors for the prevention of severe scrub typhus. When scrub typhus patients present with a rash, lymphadenopathy, or blood platelet count <100Â ĂÂ 109/l, clinicians should be alert to the appearance of severe complications
Large Red-Shifted Fluorescent Emission via Intermolecular ÏâÏ Stacking in 4âEthynyl-1,8-naphthalimide-Based Supramolecular Assemblies
Two low molecular weight gelators
containing 4-ethynyl-1,8-naphthalimide
groups with large conjugated structure via different length of alkyl
chains were synthesized and fully characterized. The gelation properties,
structural character, and fluorescence of the gels were investigated
via methods of scanning electron microscopy, X-ray diffraction, and
spectral studies. The gelators have high fluorescence quantum yields
in both solution and solid state. Interestingly, the wavelength of
the fluorescent emission in the reversible solâgel transition
process of the gels has a large red-shift of 80 nm in DMF, which is
extremely sparse for 1,8-naphthalimide derivatives in the literature.
The intermolecular ÏâÏ stacking between naphthalimide
is suggested to be the main driving force for the gel formation and
fluorescent variation by means of temperature-dependent <sup>1</sup>H NMR study and theoretical calculation
Stabilisation of Inorganic Perovskite Solar Cells with A 2d Dion-Jacobson Passivating Layer
Wu L, Li G, Prashanthan K, et al. Stabilisation of Inorganic Perovskite Solar Cells with A 2d Dion-Jacobson Passivating Layer. Advanced Materials . 2023: e2304150.Inorganic metal halide perovskites such as CsPbI3 are promising for high-performance, reproducible and robust solar cells. However, inorganic perovskites are sensitive to humidity, which causes the transformation from the black phase to the yellow delta, non-perovskite phase. Such phase instability has been a significant challenge to long-term operational stability. Here, we report a surface dimensionality reduction strategy, using 2-(4-aminophenyl) ethylamine cation to construct a Dion-Jacobson 2D phase that covers the surface of the 3D inorganic perovskite structure. The Dion-Jacobson layer mainly grew at the grain boundaries of the perovskite, effectively passivating surface defects and providing favourable interfacial charge transfer. The resulting inorganic perovskite films exhibited excellent humidity resistance when submerged in an aqueous solution (Isopropanol: Water = 4: 1v/v) and exposed to a 50% humidity air atmosphere. The DJ 2D/3D inorganic perovskite solar cell (PSC) achieved a power conversion efficiency (PCE) of 19.5% with a Voc of 1.197eV. It retained 83% of initial PCE after 1260h of maximum power point tracking under 1.2 sun illumination. Our work demonstrates an effective way for stabilising efficient inorganic perovskite solar cells. This article is protected by copyright. All rights reserved. This article is protected by copyright. All rights reserved