Latest ArticlesThe interpretation of heterometallic bonding nature is a basic work of inorganic chemistry. By means of intermetallic substitution of germylene anions with iron halide complexes CpFe(CO)2I and β-diketiminato FeⅡ chloride, the ferrogermylene complexes 3a, 3b and 4a were synthesized and structurally characterized. The structural and IR characterizations show the presence of the Ge←Fe π backbonding in molecules 3a, 3b and 4a. The computational works on frontier molecular orbitals and their comparison of energy states confirmed that σ donation and π backbonding are both weak in these molecules, despite three complexes have longer Ge-Fe bonds, whose strength decreases slightly with the degressive electron density around Fe environment in a sequence from 3a, 3b to 4a.
Sulfide oxidation under aerobic conditions can produce active oxygen for the transformation of organic pollutants in aquatic environments. However, the catalytic performance of transition metal-supported carbon material on this process is poor understood. This study found that Co-loaded carbon nanotubes (CNTs) was able to realize the efficient aerobic transformation of antibiotic ciprofloxacin (CIP) by sulfide, with the pseudo-first order reaction rate constant improved from 0.013 h−1 without catalyst to 0.44–0.71 h−1 with 100 mg/L Co-loaded CNTs. Singlet oxygen (1O2) was the main active specie playing key roles in the process of CIP aerobic transformation with presence of Co-loaded CNTs. Mechanism studies indicated that the excellent electron transfer ability of Co-loaded CNTs might play an important role to promote the electron transfer and facilitate the formation of intermediate H2O2 and 1O2. Additionally, the Co-loaded CNTs/sulfide system effectively reduced the acute toxicity of organic pollutant, and Co-loaded CNTs showed remarkable cycling stability and negligible leaching. This study gives a better understanding for the Co-loaded CNTs mediated aerobic antibiotics transformation by sulfide, and provide a reference for the application of Co-loaded carbon materials on organics aerobic transformation by sulfide.
Available online Immunoglobulins G (IgGs) are Y-shaped globular proteins, however, their high flexibility and heterogeneity pose great challenges to their structure and conformation determinations. Geometric structure of IgG closely correlates to its biofunctions, such as the antibody escape of human immunodeficiency virus (HIV) could attribute to the distance mismatch between the ends of two Fab arms (antigen-binding sites) and envelope glycoprotein spikes on virion surface. Herein, we report the first use of mobility capillary electrophoresis (MCE) and native mass spectrometry (nMS) to resolve the internal geometric structure and conformation of an IgG (trastuzumab) in solution phase. After proteolysis, the ellipsoid dimensions of IgG and its subunits were measured by MCE-nMS experiments. IgG was then reconstructed, in which the sizes and relative positions of these three subunits in three-dimensional space were characterized. It was found that the two Fab arms have an angle of ~102.1° and a distance of ~11.0 nm between the two antigen-binding sites under native condition, and the Fc arm was tilted ~16.0° towards one of the Fab arms. Fc was not on the plane of Fab-Fab, but has an angle of no larger than 103.1°. Under acidic environment (pH 3.0), each subunit of the IgG would unfold into larger dimensions, and the angles between these subunits also change. With great potential for tumor imaging and therapy, the structure of F(ab′)2 fragments was also measured and validated by molecular dynamic simulation. It was found that the electrostatic force among these three subunits and steric hindrance stemming from Fc help maintaining the angle between two Fab arms.
Electrochemical oxidation is an effective method to degrade persistent organic pollutants. However, due to the limited catalytic activity of traditional thin film electrodes, the anodic oxidation process is slow and usually requires high energy consumption. Herein, Ti/SnO2-Sb electrode with regulated surface structure was reported to enhance the performance for electrochemical oxidation of persistent organic pollutants. The electrode deposited with SnO2-Sb nanoneedles (Ti/N-SnO2-Sb) showed higher oxidation activity. Its kinetic constant for perfluorooctanoic acid (PFOA) oxidation was 2.0 h−1 and the total organic carbon removal rate was 81.7% (4 h) at a relatively low current density of 6 mA/cm2. Compared with Ti/SnO2-Sb thin film and nanoparticles, Ti/N-SnO2-Sb significantly improved the electrochemical active area and •OH yield, and simultaneously reduced the electron transfer resistance, which enabled it to oxidize PFOA more rapidly even at a lower potential. This work provides a new strategy for promoting the electrochemical oxidation performance.
Therapeutic cancer vaccines have undergone a resurgence in the past decade. Because of the high level of immune cell accumulation and abundant capillary lymphatic system in the dermis, percutaneous vaccination is considered to be an ideal treatment route. For convenient administration, the recent development of microneedles (MNs) provides a safe, painless, and low-cost transdermal delivery strategy, which could bypass the first-pass metabolism of vaccines for enhanced stability and bioavailability. However, the therapeutic effect of MNs-based cancer vaccines is not optimal, which is limited by the complex set of host, tumor, and environmental factors, as well as the limited vaccine loading capacity. Therefore, further improvements are still required to push their clinical translation. In this critical review, we deliberate on how to improve the therapeutic effect of MNs-based vaccines for cancer immunotherapy, summarize the recent advances in MNs-based cancer vaccination, and provide an overview of various design strategies and mechanisms for active or passive targeting delivery, aiming to develop safer, more effective, and more stable MNs-based cancer vaccines. Finally, we briefly describe the potential of vaccine platforms in combination with other therapies, suggest the need to design vaccines according to specific circumstances, and discuss the biosafety of repeated administration for enhancing clinical efficacy.
A facile chemical method for the development of photocatalytic coating products was proposed based on practical application perspective for the Hong Kong roadside nitrogen oxides (NOx) mitigation. TiO2-based photocatalytic coating PC-C film with crystallized size of around 5–6 nm was synthesized with the peptization of H2O2. The PC-C coating possesses a super-hydrophilicity surface and is proven to have a NOx degradation rate of 46.8% with an optimum pH level of 7. In addition, the PC-C coating presents a promising photocatalytic NOx degradation compared with other commercially available coating products and P25 when applied on two building materials of poly-methyl methacrylate (PMMA) and concrete surface. A weather resistance simulation and a 180-day on-site field trial were carried out the attenuation effects of photocatalytic coating applied in outdoor exposure. Based on epidemiological estimation and field investigation, hospital admissions for respiratory diseases (HARD) and mortality cases (MC) could be reduced with the application of PC-C coating along the street canyon. This work demonstrates the feasibility of air pollution control measures for the local roadside NOx using photocatalytic technology, offering promising health benefits with environmental remediation.
A meso-molecular muscle was prepared by capping the [c2]daisy chain based on a mono-functionalized copillar[5]arene with an imidazolium group in its axle. From its crystal structure, we observed that it was a cyclic dimer composed of two mirror image subcomponents, a pR- and a pS-copillar[5]arene. Their conformations were fixed by the doubly interlocked mechanical bond. By comparison of the 1H NMR and COSY spectra, we found that the length of this meso-molecular muscle could be controlled not only by the solvents, but also by the counter anions.
Biomass is the most bountiful renewable carbon resource on earth. Photocatalytic transformation is a promising method to utilize biomass to obtain high-value-added chemicals and it has more obvious advantages compared with thermochemical and biological processes due to the milder operational conditions, fewer reagents and equipment. Semiconductor material is one of the most common kinds of heterogeneous biomass photocatalysts, which has the advantages of high selectivity, stable catalytic performance, long activation time, and low cost. In this paper, the significant research progress on the photocatalytic transformation of biomass with semiconductor materials to produce high-value-added chemicals is reviewed, and the three most typical semiconductor photocatalysts (TiO2, CdS, and g-C3N4) are detailed. The photocatalytic mechanism and photocatalytic system optimization including structural modification, metal co-catalyst loading, and introduction of heterojunction are presented. Besides, the main problems, the development direction and trend of semiconductor materials in photocatalytic transformations of biomass in the future are prospected, which provide guidance and inspiration for the further development of semiconductor photocatalysts and make contributions to the progress in efficient utilization of biomass.
Artificial Z(S)-scheme photocatalytic water splitting systems have attracted extensive attention due to their advantages such as wide light absorption range, high charge separation efficiency and strong carrier redox ability. However, it is still challenging to design and prepare Z(S)-scheme photocatalysts with low-cost and highly stability for efficiently photocatalytic overall water splitting using solar energy. This review mainly introduces various strategies to improve the photocatalytic water splitting performance of Z(S)-scheme systems. These strategies mainly focus on enhancing or extending the range of light absorption, promoting charge separation, and enhancing surface redox reaction in Z(S)-scheme systems. Finally, the main challenges of Z(S)-scheme photocatalytic water splitting systems and their future development directions are pointed out. This review would be beneficial to understanding the challenges and opportunities faced by the research field of Z(S)-scheme photocatalytic systems, and has important guiding significance for the development and utilization of high-performance Z(S)-scheme photocatalytic reaction system in the future.
Molecular structure of organic semiconductor plays a critical role in determining the performance and functionality of organic electronic devices, by optimizing the electrical, optical and physicochemical properties. Substituted alkyl chains are fundamental units in tailering the solubility and assemblability, among which the asymmetric properties have been reported as key element for controlling the packing motifs and intrinsic charge transport. Here, we expanded the scope of molecular asymmetry dependent sensing features based on a new series of naphthalene diimides (NDI)-based derivatives substituted with a same branching alkyl chain but various linear-shaped alkyl chains (Cn-). A clear molecular stacking change, from head-to-head bilayer to head-to-tail monolayer packing model, is observed based on the features of anisotropic molecular interactions with the change in the chain length. Most importantly, a unique LUMO level shift of 0.17 eV is validated for NDI-PhC4, providing a record sensitivity up to 150% to 0.01 ppb ammonia, due to the desired molecular reactivity and device amplification properties. These results indicate that asymmetric side-chain engineering opens a route for breath healthcare.
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