Latest ArticlesParticle engineering has opened the floodgates to material science in both fundamental and application field. However, covalent interactions have not yet been adequately designed in the particle engineering for functional colloidal photonic crystals (CPCs). Herein, we achieved covalent coupling between carboxyl-rich poly(styrene-acrylic acid) (P(St-AA)) monodispersed colloidal particles and amine-rich carbon dots (CDs) based on an feasible and universal particle engineering strategy. The designed CDs-grafted P(St-AA) monodispersed colloidal particles initiate a hydrogen bond-driven assembly mode and ensure the construction of large-scale crack-free CPCs. Moreover, the CDs equipped with selective broad-band absorption capacity could improve the saturation of structural colors for high-visibility CPCs. Furthermore, an injectable photonic hydrogel (IPH) is developed to design CPC supraball hydrogel via integrating the CDs-grafted P(St-AA) CPC supraballs with supramolecular hydrogel. Combining superior flexibility, sufficient self-healing capacity of supramolecular hydrogel with visual optical information of our CPC supraballs, a cyclically reversible coding and decoding system was developed. Meanwhile, we firstly demonstrated the novel strategy of 3D supraballs-based passive cooling. The designed 3D CPC supraball hydrogel presents nearly full observation angle reflections behavior and excellent water evaporation capacity and achieves 3.6 ℃ temperature drops, showing the application advantages in 3D thermal management. This work not only provides a new insight for manipulating optical properties of CPCs, but also demonstrates an easy-to-perform platform, as well as indicates the direction for the promising application of CPCs.
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.
Geminal diboronates and diarylmethyl boronates are versatile building blocks in synthetic chemistry. We here reported a highly efficient approach for the synthesis of gem-bisborylalkanes and diarylmethyl boronates via cobalt-catalyzed deoxygenative borylation of diaryl ketones. This borylation protocol is compatible with a broad range of functionalized aryl groups, providing access to a wide array of boronic esters. The resulting boronic esters can be further transformed to various cross-coupling products and TPEs that represent important structural motifs in organic chemistry and materials science.
The pharmaceutical industry is now paying increased attention to continuous manufacturing. While the revolution to continuous and automated manufacturing is deepening in most of the top pharma companies in the world, the advancement of automated pharmaceutical continuous manufacturing in China is relatively slow due to some key challenges including the lack of knowledge on the related technologies and shortage of qualified personnels. In this review, emphasis is given to two of the crucial technologies in automated pharmaceutical continuous manufacturing, i.e., process analytical technology (PAT) and self-optimizing algorithm. Research work published in recent 5 years employing advanced PAT tools and self-optimization algorithms is introduced, which represents the great progress that has been made in automated pharmaceutical continuous manufacturing.
Plasmonic metal nanomaterials with intrinsic surface–enhanced Raman scattering (SERS) and photothermal properties, especially AuAg nanoalloys with both the outstanding merits of Au and Ag nanocrystals, show huge application prospects in bacterial theranostics. However, the direct exposure of AuAg nanoalloys in external conditions probably cause undesirable reactions and poisonous metal ion leakage during SERS detection and photothermal antibacterial therapy process, which severely hinder bacterial theranostics applications. Herein, we report an ultrastable graphene–isolated AuAg nanoalloy (GAA) with AuAg core confined in few–layer graphitic shell as a versatile platform for bacterial detection and therapy. The encapsulation of graphene ensures the good stability of AuAg core, that its superior SERS and photothermal properties are therefore further guaranteed. GAA is used for SERS detection of two vital bacterial biomarkers (including corrosive cyanide and pyocyanin), exhibiting good SERS quantitative and multiplexing ability. GAA is further used for photothermal antibacterial therapy application, and ultrahigh antibacterial efficacies for both Gram–negative Escherichia coli and Gram–positive Staphylococcus aureus are achieved under 808 nm laser irradiation. This work proposes a valuable method to develop robust bacterial theranostic platform.
The 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.
Polymerase chain reactions (PCR) are a very important tool for use in cloning, nucleic acid sequencing and diagnostic testing. The storage conditions of PCR reagents are limited to freezing and a lot of mixing steps are needed. In this paper, we report using metal ions to form coordination nanomaterials with the intrinsic components of the PCR reagents including dNTP, DNA primers and DNA polymerase as an integrated PCR reaction system. To complete PCR reactions, users need only to dissolve the coordination nanomaterials with a buffer and add template DNA. A few transition metal ions were screened and Cu2+ was found to be the most effective metal ion for this purpose. Then the encapsulation efficiency of PCR reagents was measured, which can reach close to 100% for the primers and DNA polymerase, but only 10% for dNTP because dNTP was excess. Further study also exhibited this integrated PCR reaction system can be used for DNA detection with a similar detection limit to the normal PCR, and showed good stability of encapsulated PCR nanomaterial after storage for a week.
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.
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.
Nitrogen oxide (NOx) is one of the most critical contaminants in the air, and the control of NOx emission from diesel vehicles is very important. Cu-based small-pore zeolites have already been applied for NOx abatement on diesel vehicles. Among the small-pore zeolites, Cu-SSZ-50 catalysts with good NH3-SCR catalytic activity were believed to have potential for application. In this study, a one-pot synthesis method for Cu-SSZ-50 catalysts was developed for the first time, using the co-templates of Cu-TEPA and 2,6-dimethyl-N-methylpyridinium hydroxide. In this synthesis method, Cu-SSZ-50 with various Cu contents can be obtained by adjusting the amount of Cu-TEPA without the need for a further after-treatment process. The addition of Cu-TEPA affected the framework atoms and Cu species, and a lower Si/Al ratio and more SCR active Cu species were obtained. The synthesized catalyst with a Cu/Al ratio of 0.40 exhibited over 90% NOx conversion between 200 ℃ and 450 ℃ for the selective catalytic reduction of NOx with NH3 (NH3-SCR). Meanwhile, over 80% NOx conversion could be obtained from 250 ℃ to 450 ℃ after hydrothermal aging at 750 ℃ for 16 h. In addition, both L-H and E-R mechanisms were proven to exist for the one-pot-synthesized Cu-SSZ-50 by in situ DRIFTS experiments. The simple synthesis procedure, excellent catalytic activity and hydrothermal stability brighten the prospects for the application of Cu-SSZ-50.
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