Sigma-1 Receptor Agonist TS-157 Improves Motor Functional Recovery by Promoting Neurite Outgrowth and pERK in Rats with Focal Cerebral Ischemia

Sigma-1 (σ-1) receptor agonists are considered as potential treatment for stroke. TS-157 is an alkoxyisoxazole-based σ-1 receptor agonist previously discovered in our group. The present study describes TS-157 profile in a battery of tests for cerebral ischemia. Initial evaluation demonstrated the compound’s safety profile and blood–brain barrier permeability, as well as its ability to induce neurite outgrowth in vitro. The neurite outgrowth was shown to be mediated via σ-1 receptor agonism and involves upregulation of ERK phosphorylation (pERK). In particular, TS-157 also significantly accelerated the recovery of motor function in rats with transient middle cerebral artery occlusion (tMCAO). Overall, the results herein support the notion that σ-1 receptor agonists are potential therapeutics for stroke and further animal efficacy studies are warranted.     

Modulating Hydroxyl-Rich Interfaces on Nickel–Copper Double Hydroxide Nanotyres to Pre-activate Alkaline Ammonia Oxidation Reactivity

The surface hydroxyl groups of Ni_xCu_1−x(OH)₂ play a crucial role in governing their conversion efficiency into Ni_xCu_1−xO_x(OH)_2−x during the electro-chemical pre-activation process, thus affecting the integral ammonia oxidation reaction (AOR) reactivity. Herein, the rational design of hierarchical porous NiCu double hydroxide nanotyres (NiCu DHTs) was reported for the first time by considering hydroxyl-rich interfaces to promote pre-activation efficiency and intrinsic structural superiority (i.e., annulus, porosity) to accelerate AOR kinetics. A systematic investigation of the structure–function relationship was conducted by manipulating a series of NiCu DHs with tunable intercalations and morphologies. Remarkably, the NiCu DHTs exhibit superior AOR activity (onset potential of 1.31 V with 7.52 mA cm⁻² at 1.5 V) and high ammonia sensitivity (detection limit of 9 μm ), manifesting one of the best non-noble metal AOR electrocatalysts and electro-analytical electrodetectors. This work deepens the understanding of the crucial role of surface hydroxyl groups on determining the catalytic performance in alkaline medium.     

Synergistic Effect of Boron Nitride and Carbon Domains in Boron Carbide Nitride Nanotube Supported Single-Atom Catalysts for Efficient Nitrogen Fixation

Developing the low-cost and efficient single-atom catalysts (SACs) for nitrogen reduction reaction (NRR) is of great importance while remains as a great challenge. The catalytic activity, selectivity and durability are all fundamentally related to the elaborate coordination environment of SACs. Using first-principles calculations, we investigated the SACs with single transition metal (TM) atom supported on defective boron carbide nitride nanotubes (BCNTs) as NRR electrocatalysts. Our results suggest that boron-vacancy defects on BCNTs can strongly immobilize TM atoms with large enough binding energy and high thermal/structural stability. Importantly, the synergistic effect of boron nitride (BN) and carbon domains comes up with the modifications of the charge polarization of single-TM-atom active site and the electronic properties of material, which has been proven to be the essential key to promote N₂ adsorption, activation, and reduction. Specifically, six SACs (namely V, Mn, Fe, Mo, Ru, and W atoms embedded into defective BCNTs) can be used as promising candidates for NRR electrocatalysts as their NRR activity is higher than the state-of-the art Ru(0001) catalyst. In particular, single Mo atom supported on defective BCNTs with large tube diameter possesses the highest NRR activity while suppressing the competitive hydrogen evolution reaction, with a low limiting potential of −0.62 V via associative distal path. This work suggests new opportunities for driving NH₃ production by carbon-based single-atom electrocatalysts under ambient conditions.     

Asymmetric Catalytic Approach to Multilayer 3D Chirality

The first asymmetric catalytic approach to multilayer 3D chirality has been achieved by using Suzuki-Miyaura cross-couplings. New chiral catalysts were designed and screened under various catalytic systems that proved chiral amide-phosphines to be more efficient ligands than other candidates. The multilayer 3D framework was unambiguously determined by X-ray structural analysis showing a parallel pattern of three layers consisting of top, middle and bottom aromatic rings. The X-ray structure of a catalyst complex, dichloride complex of Pd-phosphine amide, was obtained revealing an interesting asymmetric environment nearby the Pd metal center. Three rings of multilayer 3D products can be readily changed by varying aromatic ring-anchored starting materials. The resulting multilayer products displayed strong luminescence under UV irradiation and strong aggregation-induced emission (AIE). In the future, this work would benefit not only the field of asymmetric synthesis but also materials science, in particular polarized organic electronics, optoelectronics and photovoltaics.     

The Versatile Electronic,Magnetic and Photo-Electro Catalytic Activity of a New 2D MA2Z4 Family**

The recent successful growth of MoSi₂N₄ and WSi₂N₄ monolayers led to the discovery of a new class of the two-dimensional (2D) MA₂Z₄ materials with no known 3D layered allotropes, which renders great possibilities to integrate diverse properties by proper design of sandwiched “MZ₂” building blocks and “A−Z” passivation layers. In this work, the dynamic stability, electronic properties, and surface reactivity of the new MA₂Z₄ family, in which M is Ti, Zr, Hf, V, Nb, Ta, Cr, Mo, W, A refers to Si or Ge, and Z is N, P or As, is theoretically probed. Among the proposed 54 possible combinations, about 42 compositions are dynamically stable, which vary from non-magnetic, anti-ferromagnetic, to ferromagnetic semiconductors, metals and half-metals. In particular, the VB (V, Nb, Ta) MA₂Z₄ possesses robust intrinsic ferromagnetism that is essential for spintronics applications. In regard to surface activity, most MA₂Z₄, particularly N- or P-terminated IVB and VB MA₂Z₄, have high catalytic potential for hydrogen evolution, and the ▵G_H of non-magnetic MA₂Z₄ is highly correlated to the highest occupied p electronic states of the surface Z atoms. The photocatalytic activity is also evaluated. MoSi₂N₄ and WSi₂N₄ within 4 % tensile strain are capable of photocatalytic overall water splitting. The findings indicate the new 2D MA₂Z₄ family has fascinating properties and possesses strong potential for applications but not limited to electronics, spintronics and catalysts, which will stimulate the interests of experimental synthesis.     

Cell-Penetrating Mitochondrion-Targeting Ligands for the Universal Delivery of Small Molecules,Proteins and Nanomaterials

Mitochondria are key organelles that perform vital cellular functions such as those related to cell survival and death. The targeted delivery of different types of cargos to mitochondria is a well-established strategy to study mitochondrial biology and diseases. Of the various existing mitochondrion-transporting vehicles, most suffer from poor cytosolic entry, low delivery efficiency, limited cargo types, and cumbersome preparation protocols, and none was known to be universally applicable for mitochondrial delivery of different types of cargos (small molecules, proteins, and nanomaterials). Herein, two new cell-penetrating, mitochondrion-targeting ligands (named Mito^Ligand) that are capable of effectively “tagging” small-molecule drugs, native proteins and nanomaterials are disclosed, as well as their corresponding chemoselective conjugation chemistry. Upon successful cellular delivery and rapid endosome escape, the released native cargos were found to be predominantly localized inside mitochondria. Finally, by successfully delivering doxorubicin, a well-known anticancer drug, to the mitochondria of HeLa cells, we showed that the released drug possessed potent cell cytotoxicity, disrupted the mitochondrial membrane potential and finally led to apoptosis. Our strategy thus paves the way for future mitochondrion-targeted therapy with a variety of biologically active agents.     

Facile preparation of MgAl2O4/CeO2/Mn3O4 heterojunction photocatalyst and enhanced photocatalytic activity

Novel Mn₃O₄-promoted double p?n junction MgAl₂O₄/CeO₂/Mn₃O₄ heterojunction photocatalyst was constructed by one-step synthesis method and two-step synthesis method. The X-ray powder diffraction, Fourier transform infrared spectrum, X-ray photoelectron spectroscopy, optical and photoluminescence demonstrated that the MgAl₂O₄/CeO₂/Mn₃O₄ heterojunction photocatalyst was synthesized by the two-step synthesis method comprehends a high crystallinity, charge carrier migration and separation efficiency, and relatively low optical absorption coefficient. The MgAl₂O₄/CeO₂/Mn₃O₄ heterojunction photocatalysts were efficiently used as simulated sunlight-driven n-n and p-n double junction photocatalyst for the simultaneous degradation of methylene blue (MB) dye. The continuous double p?n junction MgAl₂O₄/CeO₂/Mn₃O₄ heterojunctions strengthened the function of single n-n or p-n junction and guided the charge carrier migration and separation direction; thus, the oxidation and reduction reactions occur at the active site of spatial separation and prevent the recombination of electrons and holes. The results suggest that the continuous double p?n junction MgAl₂O₄/CeO₂/Mn₃O₄ heterojunctions are very promising candidate material for enhancing the photocatalytic activity in the photocatalytic degradation of MB dye.     

Photocatalytic Carboxylation of Phenyl Halides with CO2 by Metal-Organic Frameworks Materials

In this work,important commercial pharmaceutical intermediates,phenylpropionic acid compounds,are successfully obtained by catalyzing the reaction of carbon dioxide with phenyl halides using MOF-5,a typical metal-organic framework(MOF)material.The influence of temperature,pressure,catalyst type and light on the reaction is investigated,and a 90.3%selectivity towards fluorophenylpropionic acid is reached.Significantly,the catalysts are effective for varied benzyl compounds containing different substituent groups.The catalysts are stable and remain active after three cycles.     

Pyrazole-based trinuclear and mononuclear complexes: synthesis,characterization, DNA interactions and cytotoxicity studies

Transition Metal Chemistry - A new trinuclear Cu(II) complex [Cu3(μ3-OH)(μ-pz)3(Hpz)2(HCOO)(BTAO)Cl] (1) (Hpz = pyrazole, BTAO = 4,6-bis(dimethylamino)-1,3,5-triazin-2(1H)-one) and four...