An ultra pH-responsive peptide nanocarrier for cancer gene therapy.

The tumor microenvironment is a very complex and dynamic ecosystem. Although a variety of pH-responsive peptides have been reported to deliver nucleic acid drugs for cancer treatment, these responses typically only target the acidic microenvironment of the tumor or the lysosome, and the carrier suffers from issues such as low transfection efficiency and poor lysosomal escape within the cell. To address this problem, we have developed an ultra pH-responsive peptide nanocarrier that can efficiently deliver siRNA, pDNA, and mRNA into cancer cells by performing progressive dynamic assembly in response to pH changes in the acidic tumor microenvironment (pH 6.

Distinct Selectivity Control in Solar-Driven Bio-Based α-Hydroxyl Acid Conversion: A Comparison of Pt Nanoparticles and Atomically Dispersed Pt on CdS.

Solar-driven photocatalytic lignocellulose conversion is a promising strategy for the sustainable production of high-value chemicals, but selectivity control remains a challenging goal in this field. Here, we report efficient and selective conversion of lignocellulose-derived α-hydroxyl acids to tartaric acid derivatives, α-keto acids, and H using Pt-modified CdS catalysts. Pt nanoparticles on CdS selectively produce tartaric acid derivatives via C-C coupling, while atomically dispersed Pt on CdS switches product selectivity to the oxidation reaction to produce α-keto acids.

Independent component analysis of Corynebacterium glutamicum transcriptomes reveals its transcriptional regulatory network.

Gene expression in bacteria is regulated by multiple transcription factors. Clarifying the regulation mechanism of gene expression is necessary to understand bacterial physiological activities. To further understand the structure of the transcriptional regulatory network of Corynebacterium glutamicum, we applied independent component analysis, an unsupervised machine learning algorithm, to the high-quality C.

Lewis Base-Catalyzed Intramolecular Vinylogous Aldol Reaction and Chemoselective Syntheses of 3-Hydroxy-2,3-Disubstituted Dihydrobenzofurans and Indolines.

A Lewis base-catalyzed intramolecular vinylogous aldol reaction of -(allyloxy)phenyl ketoesters or -(allylamino)phenyl ketoesters has been developed. This reaction provides ready access to 3-hydroxy-2,3-disubstituted dihydrobenzofurans and indolines in high yields with excellent chemoselectivity and diastereoselectivity. An acid-promoted dehydration of such products further extends the utility of the reaction to the synthesis of 2-alkenyl benzofurans and indoles.

Proton is Essential or Not: A Fresh Look on Pseudocapacitive Energy Storage of PANI Composites.

Protonation has been considered essential for the pseudocapacitive energy storage of polyaniline (PANI) for years, as proton doping in PANI chains not only activates electron transport pathways, but also promotes the proceeding of redox reactions. Rarely has the ability for PANI of storing energy without protonation been investigated, and it remains uncertain whether PANI has pseudocapacitive charge storage properties in an alkaline electrolyte. Here, this work first demonstrates the pseudocapacitive energy storage for PANI without protonation using a PANI/graphene composite as a model material in an alkaline electrolyte.

NADH Photosynthesis System with Affordable Electron Supply and Inhibited NADH Oxidation.

Photosynthesis offers a green approach for the recycling of nicotinamide cofactors primarily NADH in bio-redox reactions. Herein, we report an NADH photosynthesis system where the oxidation of biomass derivatives is designed as an electron supply module (ESM) to afford electrons and superoxide dismutase/catalase (SOD/CAT) cascade catalysis is designed as a reactive oxygen species (ROS) elimination module (REM) to inhibit NADH degradation. Glucose as the electron donor guarantees the reaction sustainability accompanied with oxidative products of gluconic acid and formic acid.

Tailoring Phase Distribution of Quasi-2D Perovskites via Taurine-Assistance Enables Efficient Blue Light-Emitting Diodes.

Quasi-2D (Q-2D) perovskites with typical varied n-phase structures deserve promising candidates in pursuing high-performance perovskite light-emitting diodes (PeLEDs). Whereas their weakness in precise n-phase distribution control disables the optical property of PeLEDs since the n = 1 phase is dominated by severe nonradiative recombination. Here, an effective phase distribution tailoring strategy is developed for pure blue PeLEDs by introducing taurine (TAU) into mixed halide Q-2D perovskites.

Selective Chiral Recognition between Amino Acids and Growing Gypsum Crystals.

In nature, selective chiral interactions between biomolecules and minerals provide insight into the mysterious origin of homochirality. Here, we show growing gypsum crystals in a nonequilibrium state can recognize chiral enantiomers of amino acids. The chiral selection for amino acids with different functional groups by growing minerals are distinct.

Retinal Microenvironment-Protected Rhein-GFFYE Nanofibers Attenuate Retinal Ischemia-Reperfusion Injury via Inhibiting Oxidative Stress and Regulating Microglial/Macrophage M1/M2 Polarization.

Retinal ischemia is involved in the occurrence and development of various eye diseases, including glaucoma, diabetic retinopathy, and central retinal artery occlusion. To the best of our knowledge, few studies have reported self-assembling peptide natural products for the suppression of ocular inflammation and oxidative stress. Herein, a self-assembling peptide GFFYE is designed and synthesized, which can transform the non-hydrophilicity of rhein into an amphiphilic sustained-release therapeutic agent, and rhein-based therapeutic nanofibers (abbreviated as Rh-GFFYE) are constructed for the treatment of retinal ischemia-reperfusion (RIR) injury.

Conjugated Polymers from Direct Arylation Polycondensation of 3,4-Difluorothiophene-Substituted Aryls: Synthesis and Properties.

3,4-Difluorothiophene-substituted aryls, i.e., 1,4-bis(3,4-difluorothiophen-2-yl)-benzene (Ph-2FTh), 1,4-bis(3,4-difluorothiophen-2-yl)-2,5-difluorobenzene (2FPh-2FTh), and 4,7-bis(3,4-difluorothiophen-2-yl)-2,1,3-benzothiadiazole (BTz-2FTh), are synthesized as C─H monomers for the synthesis of conjugated polymers (CPs) via direct arylation polycondensation (DArP) with diketopyrrolopyrrole (DPP) and isoindigo (IID) derivatives as C─Br monomers.

Dibenzothiophene Sulfone-Based Ambipolar-Transporting Blue-Emissive Organic Semiconductors Towards Simple-Structured Organic Light-Emitting Transistors.

The development of blue-emissive ambipolar organic semiconductor is an arduous target due to the large energy gap, but is an indispensable part for electroluminescent device, especially for the transformative display technology of simple-structured organic light-emitting transistor (SS-OLET). Herein, we designed and synthesized two new dibenzothiophene sulfone-based high mobility blue-emissive organic semiconductors (DNaDBSOs), which demonstrate superior optical property with solid-state photoluminescent quantum yield of 46-67 % and typical ambipolar-transporting properties in SS-OLETs with symmetric gold electrodes. Comprehensive experimental and theoretical characterizations reveal the natural of ambipolar property for such blue-emissive DNaDBSOs-based materials is ascribed to a synergistic effect on lowering LUMO level and reduced electron injection barrier induced by the interfacial dipoles effect on gold electrodes due to the incorporation of appropriate DBSO unit.

Accessing complex reconstructed material structures with hybrid global optimization accelerated on-the-fly machine learning.

The complex reconstructed structure of materials can be revealed by global optimization. This paper describes a hybrid evolutionary algorithm (HEA) that combines differential evolution and genetic algorithms with a multi-tribe framework. An on-the-fly machine learning calculator is adopted to expedite the identification of low-lying structures.

Multicomponent structural color membrane based on soft lithography array for high-sensitive Raman detection.

Inspired by ordered photonic crystals and structural color materials in nature, we successfully prepared hydroxypropyl cellulose (HPC) photonic films with ordered surface arrays by double-imprint soft lithography. Then we introduced another important material of the cellulose family, cellulose nanocrystals (CNC), which has liquid crystal nature and birefringent properties of the particles, into the system to realize the single-point shrinkage of the film array and the control of structural color. Through multi-component doping and concentration control, we further optimized the multi-scale structure of the materials, and obtained HPC/CNCs composite photonic films with excellent properties in color, stability and flexibility, whose elastic modulus and tensile properties are significantly higher than those of single-component.

Reversed Electron Transfer in Dual Single Atom Catalyst for Boosted Photoreduction of CO.

Photogenerated charge localization on material surfaces significantly affects photocatalytic performance, especially for multi-electron CO reduction. Dual single atom (DSA) catalysts with flexibly designed reactive sites have received significant research attention for CO photoreduction. However, the charge transfer mechanism in DSA catalysts remains poorly understood.

The strong metal-support interactions induced electrocatalytic three-electron oxygen reduction to hydroxyl radicals for water treatment.

As a promising environmental remediation technology, the electro-Fenton (EF) process is mainly limited by the two rate-limiting steps, which are HO generation and activation. The electrocatalytic three-electron oxygen reduction reaction (3e ORR) can directly activate oxygen to hydroxyl radicals (•OH), which is expected to break through the rate-limiting steps of the EF process. However, limited success has been achieved in the design of 3e ORR electrocatalysts.

Enzyme-Driven, Switchable Catalysis Based on Dynamic Self-Assembly of Peptides.

Covalent regulatory systems of enzymes are widely used to modulate biological enzyme activities. Inspired by the regulation of reactive-site phosphorylation in organisms, we developed peptide-based catecholase mimetics with switchable catalytic activity and high selectivity through the co-assembly of nanofibers comprising peptides and copper ions (Cu ). Through careful design and modification of the peptide backbone structure based on the change in the free energy of the system, we identified the peptide with the most effective reversible catalytic activity.

Cerium Methacrylate Assisted Preparation of Highly Thermally Conductive and Anticorrosive Multifunctional Coatings for Heat Conduction Metals Protection.

Preparing polymeric coatings with well corrosion resistance and high thermal conductivity (TC) to prolong operational life and ensure service reliability of heat conductive metallic materials has long been a substantive and urgent need while a difficult task. Here we report a multifunctional epoxy composite coating (F-CB/CEP) by synthesizing cerium methacrylate and ingeniously using it as a novel curing agent with corrosion inhibit for epoxy resin and modifier for boron nitride through "cation-π" interaction. The prepared F-CB/CEP coating presents a high TC of 4.

Highly selective NH synthesis from N on electron-rich Bi in a pressurized electrolyzer.

Electrochemical conversion of N into ammonia presents a sustainable pathway to produce hydrogen storage carrier but yet requires further advancement in electrocatalyst design and electrolyzer integration. This technology suffers from low selectivity and yield owing to the extremely strong N≡N bond and the exceptionally low solubility of N in aqueous systems. A high NH synthesis performance is restricted by the high activation energy of N≡N bond and the supply insufficiency of N to active sites.

p-Type Conjugated Polymers Containing Electron-Deficient Pentacyclic Azepinedione.

Bisthienoazepinedione (BTA) has been reported for constructing high-performing p-type conjugated polymers in organic electronics, but the ring extended version of BTA is not well explored. In this work, we report a new synthesis of a key building block to the ring expanded electron-deficient pentacyclic azepinedione (BTTA). Three copolymers of BTAA with benzodithiophene substituted by different side chains are prepared.

Preparation and Characterization of Body-Temperature-Responsive Thermoset Shape Memory Polyurethane for Medical Applications.

Shape memory polymers (SMPs) are currently one of the most attractive smart materials expected to replace traditional shape memory alloys and ceramics (SMAs and SMCs, respectively) in some fields because of their unique properties of high deformability, low density, easy processing, and low cost. As one of the most popular SMPs, shape memory polyurethane (SMPU) has received extensive attention in the fields of biomedicine and smart textiles due to its biocompatibility and adjustable thermal transition temperature. However, its laborious synthesis, limitation to thermal response, poor conductivity, and low modulus limit its wider application.

Conformationally confined three-armed supramolecular folding for boosting near-infrared biological imaging.

Herein, a triphenylamine derivative (TP-3PY) possessing 4-(4-bromophenyl)pyridine (PY) as an electron-accepting group and tris[-(4-pyridylvinyl)phenyl]amine (TPA) with large two-photon absorption cross-sections as an electron-donating group was obtained, and showed intense absorption in the visible light region ( = 509 nm) and weak near-infrared (NIR) fluorescence emission at 750 nm. After complexation with cucurbit[8]uril (CB[8]), TP-3PY showed bright NIR fluorescence emission at 727 nm and phosphorescence emission at 800 nm. When the supramolecular assembly (TP-3PY⊂CB[8]) further interacted with dodecyl-modified sulfonatocalix[4]arene (SC4AD), the fluorescence and phosphorescence emissions were further enhanced at 710 and 734 nm, respectively.

Crystal Facet Structure Dependence and Promising Pd-Pt Catalytic Materials for Perhydroacenaphthene Dehydrogenation.

Designing an effective Pd-Pt catalytic material with excellent catalytic performance for perhydroacenaphthene (PHAN) dehydrogenation is a great challenge. In this work, in order to explore the crystal facet structure over the bimetallic Pd-Pt catalyst on the dehydrogenation performance of PHAN, the surface compositions of two kinds of Pd (Pt) atoms with different coverage on Pd modulated Pt (PdPt) and Pt modulated Pd (PtPd) catalysts were designed and studied by means of density functional theory (DFT). Through the investigation of the reaction path of PHAN dehydrogenation on PdPt(111) and PtPd(111) surfaces, it was found that PdPt(111) was advantageous to PHAN dehydrogenation ( = 2.

Theoretical investigation on the functional group modulation of UV-Vis absorption profiles of triphenylamine derivatives.

Understanding the functional group modulation of electronic structure and excitation is pivotal to the design of organic small molecules (OSMs) for photoelectric applications. In this study, we employed density functional theory (DFT) and time-dependent DFT (TDDFT) calculations to explore the unique absorption character of four triphenylamine photosensitizers. The various conformations were investigated given the multiple single bonds in the compounds, and the resemblance in the electronic structure of different conformations is affirmed because the coplanarity and consequent long-range conjugation is maintained regardless of the orientation of the flexible blocks.